Hydrogen Carriers: Production, Transmission, Decomposition, and Storage

Dionissios D. Papadias, Jui-Kun Peng, and Rajesh K. Ahluwalia

Argonne National Laboratory

9700 South Cass Avenue, Lemont, IL 60439

Abstract

Recognizing the potential role of liquid hydrogen carriers in overcoming the inherent limitations

in transporting and storing gaseous and liquid hydrogen, a complete production and use scenario

is postulated and analyzed for perspective one-way and two-way carriers. The carriers, methanol,

ammonia and toluene/MCH (methyl cyclohexane), are produced at commercially viable scales in

a central location, transmitted by rail or pipelines for 2000 miles, and decomposed near city gates

to generate fuel-cell quality hydrogen for distribution to refueling stations. In terms of the levelized

cost of H2 distributed to the stations, methanol is less expensive to produce ($1.22/kg-H2) than

MCH ($1.35/kg-H2) or ammonia ($2.20/kg-H2). Levelized train transmission cost is smaller for

methanol ($0.63/kg-H2) than ammonia ($1.29/kg-H2) or toluene/MCH system ($2.07/kg-H2).

Levelized decomposition cost is smaller for ammonia ($0.30-1.06/kg-H2) than MCH ($0.54-

1.22/kg-H2) or methanol ($0.43-1.12/kg-H2). Over the complete range of demand investigated, 10-

350 tpd-H2, the levelized cost of H2 distributed to stations is aligned as methanol << ammonia ~

MCH. With pipelines at much larger scale, 6000 tpd-H2, the levelized cost decreases by ~1 $/kg-

H2 for ammonia and MCH and much less for methanol. Methanol is a particularly attractive low-

risk carrier in the transition phase with lower than 50-tpd H2 demand.

Keywords: Bulk storage of hydrogen; hydrogen transport by trains and pipelines; liquid hydrogen

carriers: methanol ammonia and toluene

1
1.0 INTRODUCTION

A matured hydrogen economy as envisioned in the H2@Scale initiative involves hydrogen

utilization in transportation, utility and industrial sectors [1–4]. These applications require ability

to transmit hydrogen over long distances, including transoceanic, and agnostic methods to store

hydrogen in bulk quantities for short to extended periods of time. The current technologies based

on gaseous and liquid forms of hydrogen fail to meet these requirements [1-6].

Gaseous hydrogen can be transported over short distances in tube trailers using Type 1

tubes or Type 2, 3 or 4 carbon-fiber wound pressure vessels at 250-500 bar [5–9]. The capacity of

these tube trailers is limited to 280-1,000 kg H2 because of Department of Transportation’s height,

width and weight regulations [10]. Also, deployment of tube trailers for market penetration beyond

10% may not be feasible due to traffic congestion on road and at refueling stations [7]. Hydrogen

can be transported over longer distances and larger quantities (up to 4,300 kg) in vacuum-insulated

liquid tankers [6,11,12]. However, cost of liquefaction, power consumption (10 kWh/kg-H2), and

boil-off losses during delivery are major challenges [13,14]. Current regulations do not allow

transporting liquid hydrogen (LH2) by trains. A project is underway to demonstrate the feasibility

and determine the economics of transporting H2 from Australia to Japan in a 160,000-m3 (10,240

tonnes) LH2 tanker [15]. Hydrogen pipelines can also come into play if demand exists to transmit

large quantities of H2 over land, >6,000 tonnes per day (tpd).

The preferred method of bulk hydrogen storage depends on the relevant time and length

scales. At a small scale, up to 1,000 kg, hydrogen is generally stored as compressed gas at 350-

950 bar in carbon-fiber overwrapped pressure vessels. At a medium scale, <20 tonnes, gaseous

hydrogen can be stored in underground Type-1 pipe facilities at pressures below 100 bar [16].

Depending on the intended application, up to 250 tonnes of LH2 may be stored in an above-ground

2
spherical, insulated, cryogenic tank [16–18]. At very large scale, 100-3,000 tonnes, geologic

storage in underground salt caverns and lined rock caverns is likely the method of choice [19–22].

However, suitable sites for locating these types of caverns are limited by geology and are generally

not available where needed [21].

Hydrogen carriers, such as solid metal hydrides and liquid organic hydrocarbons (LOHC),

can address many of the inherent limitations in transporting and storing gaseous and liquid

hydrogen [23–26]. Whereas they have been investigated for onboard storage of hydrogen, the

interest in their use to facilitate off-board storage and transportation is relatively recent [26–32].

The scope of this work is limited to one inorganic and two organic liquid hydrogen carriers for

off-board applications: ammonia, methanol, and toluene/methyl cyclohexane (MCH). Formic acid,

perhydro-dibenzyltoluene, perhydro-N-ethylcarbazole are some of the other carriers that have been

proposed or analyzed.

Methanol is an important industrial feedstock for producing a wide range of chemicals

ranging from solvents, adhesives, plastics and fuel applications [33–35]. Nearly 30% of methanol

demand is as feedstock for formaldehyde, which is used in the adhesives for wood panels and

wood products. Nearly 21% of the methanol demand lies in the alternative fuels sector, i.e.,

gasoline blending, dimethyl ether (DME) and biodiesel. The third largest application is in methanol

to olefin (MTO) production (19%), followed by methyl tert-butyl ether (MTBE) and acetic acid

used to produce polyester fiber intermediates. Methanol is produced worldwide at an annual

production rate of ~118 million metric tons (MMT) in 2018, which is projected to increase to 140

MMT by the end of 2021 [36]. Most methanol plants in U.S. are located in the Gulf Coast region

due to a highly developed natural gas (NG) infrastructure which allows increased gas production

from the Permian Basin in western Texas. The total methanol production capacity in the U.S. is

3
estimated to reach 25,600 metric tons per day (tpd), ~ 45% higher than the level in 2018. Modern

methanol plants up to 5,000-tpd capacity have been built; even larger plants of 10,000-tpd are

considered feasible [37].

Ammonia is an important industrial commodity for supplying nutrients to the agricultural

industry. Over 90% of ammonia produced is used for fertilizers as diluted ammonia, urea and

ammonium salts [38]. In 2018, approximately 140,000 million tonnes of ammonia was produced

worldwide; the global ammonia capacity was expected to increase by 6% during the next three

years [39]. Because ammonia is synthesized from natural gas, ammonia production plants in U.S.

are largely concentrated on the Gulf coast region where NG is cheap and plentiful. Large pipelines

stretching from Louisiana to Nebraska and from Texas to Minnesota carry anhydrous ammonia

from its site of production to agricultural areas where it is used as fertilizer. These pipelines are

capable of annually transporting 3 million metric tons of ammonia and have a storage capacity of

1.5 million metric tons [40]. Ammonia can also be shipped in large refrigerated, low pressure

tanks. Barges on Mississippi river are often used for transporting refrigerated shipments. Haber-

Bosch process is the method of choice for synthesizing ammonia on an iron catalyst at 100-250

bar and 350-550°C. The largest ammonia plants have 2,200 – 2,700 tpd capacity [41].

Toluene is primarily produced by catalytic conversion of petroleum products,

aromatization of aliphatic hydrocarbons as well as being a byproduct from coke oven gases [42].

Its main industrial use is as a precursor to several chemicals (e.g., benzene, phenol, toluene

diisocyanate) accounting for approximately 50% of end use. Toluene is also a common solvent for

paints and coatings (10%) and also used as octane booster in gasoline (3%) [43]. As compared to

aromatics consumption, toluene is produced worldwide in smaller quantities. In 2012, worldwide

4
toluene production was estimated to be approximately 13 million tonnes with modest growth

projections [43]. Nearly 50% of toluene is consumed in China and U.S [44].

The objective of this work is to evaluate the efficiency and cost of hydrogen carriers,

considering the complete scenario involving carrier production, transmission, decomposition, and

storage. The scope is restricted to methanol, ammonia and toluene/MCH, as they are representative

of different classes of carriers, and to a particular scenario that allows a meaningful comparison

between transmission choices, daily throughput and H2 capacities.

2.0 CARRIER FORMATION, HYDROGEN RELEASE, AND TRANSMISSION

We selected three pathways to cover different classes of liquid hydrogen carriers:

methanol, ammonia, and methylcyclohexane (MCH)/toluene. Liquid methanol represents a class

of carriers that, depending on the synthesis method, may not require an explicit hydrogen

production step. Liquid methanol and ammonia are one-way carriers, while MCH/toluene is a two-

way carrier. Liquid ammonia and MCH are easier to produce using renewable hydrogen than

methanol that would also require a source for CO2.

As listed in Table 1, methanol and MCH/toluene are liquids over a broad range of

temperatures of interest, but the normal boiling point of ammonia is only -33.4oC so that high

pressures and/or low temperatures are required to maintain it in liquid form. Transporting ammonia

in refrigerated containers incurs additional cost. The H2 capacities by weight and volume are

similar for ammonia and methanol but only one-third for MCH. Thus, MCH can be more expensive

to transport than methanol, especially since it requires MCH to be moved from the hydrogenation

to dehydrogenation sites and toluene to be moved back from the dehydrogenation to hydrogenation

sites.

5
2.1 Baseline Gaseous H2 (GH2) Pathway

Figure 1 shows the reference GH2 pathway in which gaseous H2 is produced by steam-

reforming (SMR) of natural gas (NG) and purified by pressure swing adsorption (PSA). The SMR

plant is located 150 km from the city gate, and it consumes 0.165 TJ natural gas, 0.569 kWh

electricity and 12.7-liter water for each kg of H2 produced [45]. The plant supplies H2 to a mid-

size city like Sacramento, CA, with limited market in an early transition stage. The assumed

average daily use of H2 for the city in this scenario is 50 tons/day (tpd). We also assume that a

geologic facility is available to store 500 tons of H2 for annual plant outages lasting 10 days. This

assumption will need to be relaxed if a suitable geologic site is not available since storing 500 tons

of H2 by other methods, such as underground pipes, is not economically viable. Following

hydrogen delivery scenario model (HDSAM)[46], fuel cell quality H2 from PSA is compressed to

500 bar at the GH2 terminal and loaded in tube trailers for distribution to refueling stations in the

city. The GH2 terminal has multiple bays, each with two compressor trains, and tubes for holding

an amount of H2 equivalent to 1-day SMR plant capacity. HDSAM indicates that 100 trucks with

1042-kg payload are required, making on average two trips/day to distribute H2 to 125 refueling

stations that dispense 400 kg-H2/day.

2.2 Hydrogen Carrier Pathway

The capacity of a dedicated LHC production facility equivalent to the 50-tpd baseline GH2

pathway is 350 tpd for methanol and 370 tpd for ammonia, which are far too small to take

advantage of economies of scale. As shown in Fig. 2, most modern plants being constructed today

for methanol and ammonia (or urea) are 10-20 times larger. Since 2012, a large number of new

methanol (3,000-5,000 tpd) and ammonia (up to 2,500 tpd) plants have been in the planning stage

or commissioned to be built in the U.S. as a consequence of the low domestic NG prices. Most of

6
these plants are located on the Gulf Coast, taking advantage of low NG price outlook and plethora

of critical energy infrastructure [47].

To take advantage of economies of scale as well as favorable location specific feedstock

prices, we have formulated a large-plant pathway as shown in Fig. 2 for methanol. As in the

baseline GH2 pathway, the annual average daily use of H2 for the city is 50 tpd. We consider that

the necessary amount of LHC is syphoned from a large central production plant located on the

Gulf Coast in Texas. Transmission of LHC occurs by a unit-train from Texas to a storage terminal

near the city gate (3250 km), and by trucks from the storage facility to the city gate for

dehydrogenation (150 km). LHC is stored at the central production plant, railway terminal and city

gate. The large-plant pathway for ammonia as LHC is similar but the pathway for MCH includes

a transmission leg for return of toluene to the central production plant and also includes storage

facilities for toluene.

2.3 Methanol Production

As shown in Fig. 3a, commercial methanol production plants consist of three sections that

convert NG feedstock to syngas (H2/CO), react syngas to form methanol, and purify methanol [48–

51]. Syngas production, including air and CO2 separation, accounts for ~60% of the capital cost

and almost all the process energy consumption. Methanol plants are, therefore, distinguished

primarily by the method of producing syngas [35,37]. At scales below ~1,700 tpd, syngas is

produced by one-step tubular SMR co-fed with CO2. At larger scales up to 5,000 tpd, syngas is

produced by two-step reforming in tubular SMR followed by secondary oxygen-blown

autothermal reforming (ATR). At even larger scales up to 10,000 tpd, it is feasible to produce

syngas in a single train oxygen-blown ATR at low steam-to-carbon ratio (S/C).

7
 The one-step SMR process requires a supplemental CO2 source to the extent of CO2/C =

0.3, which can be CO2 contained in certain CO2-rich NG feedstock, cheaply available CO2 from

neighboring industry (rare occurrence), or CO2 recovered from the combustion products as shown

in Fig. 2.

SMR is an endothermic process and requires burning some NG to supply the heat of

reaction. Purge gas from the methanol synthesis section can also supply a portion of the heat of

reaction.
0
CH4 + H2O = CO + 3H2 ΔH298 = 206 kJ/mol
0
CO + H2O = CO2 + H2 ΔH298 = -41 kJ/mol
0
CH4 + 2O2 = CO2 + 2H2O ΔH298 = -802 kJ/mol

Methanol synthesis is exothermic, occurs over Cu/ZnO/Al2O3 catalyst with high selectivity

(>99.9%) at low temperatures and high pressures (50 bar), and can be described by the following

reactions [52].
0
CO2 + 3H2 = CH3OH + H2O ΔH298 = -40.9 kJ/mol
0
CO + 2H2 = CH3OH ΔH298 = -90.7 kJ/mol

Methanol synthesis is typically described in terms of its module (M) that refers to the syngas

stoichiometric molar ratio, M = (H2-CO2)/(CO+CO2). The syngas reaction is balanced if M equals

2. Favorable process economics dictates achieving high methanol conversion per pass by

efficiently removing heat of reaction at high temperature while allowing the reactions to equilibrate

at low temperature. Different reactor designs have been used for this purpose: quench reactors,

adiabatic reactors in series, and boiling water reactors (BWR).

A simple model was formulated to determine the component sizes and system performance

in terms of process variables for CO2 recycle (CO2/C), steam requirements for SMR and ATR

8
(S/C), oxygen requirement for ATR (O2/C), and syngas stoichiometry for methanol synthesis (M).

As summarized in Table 2, the model shows that the natural gas requirement is largest for the one-

step SMR and smallest for the one-step ATR. Also, sufficient by-product steam is generated in the

larger two-step SMR+ATR and one-step ATR plants that they can be net exporters of electricity.

The smaller one-step SMR plant, however, needs to import electricity.

Figure 3b presents the breakdown of capital costs estimated using the modeled component

sizes for representative 1,000 tpd one-step SMR, 2,200 tpd SMR+ATR and 5,000 tpd one-step

ATR plants [53]. Including CO2 recovery and air separation units (ASU), reformers account for

54%, 48%, and 50% of the total capital costs of one-step SMR, two-step SMR+ATR plants.

Methanol synthesis section represents 23-27% of the total capital costs. The electric plant accounts

for 11-13% of the total capital costs of plants larger than 2,000-tpd capacity. It is not economical

to incorporate steam turbines is plants smaller than 1,700-tpd capacity.

Figure 3c summarizes the estimated installed capital cost, presented as circle symbols,

validated with the literature data shown as square symbols [54]. The estimated cost is lowest for

one-step ATR plants for capacities larger than 3,000 tpd, two-step SMR+ATR plants for capacities

between 1,800 and 3,000 tpd, and one-step SMR for capacities below 1,500 tpd. There is more

than a factor of two difference between the largest (10,000 tpd) and smallest (350 tpd) plant

capacities in Fig. 3c.

2.4 Ammonia Production

Figure 4a is a simplified schematic of the Linde process in which ammonia is synthesized

by reacting H2 and N2 over an iron catalyst [55].

0
N2 + 3H2 = 2NH3 ΔH298 = -46 kJ/mol

9
The Linde Ammonia Concept (LAC) combines two established methods of producing ultra-pure

H2 from an SMR with PSA purification and ultra-pure N2 from cryogenic ASU. We estimated the

performance of LAC using the NETL process model for Haldor Topsoe S-300 Ammonia Synthesis

Loop [56]. The synthesis gas enters the reactor loop at 140 bar and 343°C. A radial bed reactor

converts ~30% of the feed to ammonia per pass due to equilibrium constraints. Equilibrium

constraints limit per-pass ammonia conversion to ~30% in the radial bed reactor. The process is

exothermic and generates superheated steam at 12 MPa and medium pressure steam at 4.14 MPa

in the synthesis loop. The ammonia is condensed and separated in a refrigeration system. A steam

turbine produces 0.98 kWhe/kg-NH3 electricity that is more than sufficient to meet the electrical

demand of all plant components, 0.9 kWhe/kg-NH3. A purge gas controls the build-up of inerts,

primarily argon from ASU and trace methane and other impurities from PSA raffinate.

The H2 production section of LAC includes low-temperature WGS. Our model indicates

that PSA can recover 80% H2 from the WGS reformate stream and the total NG consumption is

156 MJ/kg-H2 for S/C of 2.8 in SMR [57]. The total energy consumption in LAC is 30.6 MJ/kg-

NH3.

Figure 4b presents the installed cost of the LAC plant as estimated by scaling the cost data

a 2,500-tpd ammonia plant in NETL study [56], SMR data in DOE’s H2A production analysis

toolkit [58], and cost models for a low-temperature WGS reactor and PSA [57]. The estimated

capital cost is $385k/tpd for 2,500 tpd capacity increasing to $6555k/tpd for 500 tpd capacity. The

pie chart in Fig. 4c presents the cost breakdown for 1 2,500-tpd plant. The ammonia synthesis loop

accounts for the largest share of the total cost at 37%, followed by the reformer at 26%, electric

plant at 13% and ASU and BOP at 9%. Ammonia storage at -33°C and ambient pressure for 30

days of annual plant shut-down for maintenance accounts for only 6% of the total cost.

10
 The inset in Fig. 4b presents the configurations of more commonly built ammonia plants

by companies such as KBR and Haldor Topsoe. In this configuration, syngas is produced by

primary SMR followed by secondary air-blown ATR, and it is purified by a CO2 removal unit and

liquid nitrogen wash. This two-step reforming process is less capital intensive than the single-step

SMR in LAC. However, this cost advantage is almost entirely offset by the more expensive syngas

conditioning (CO2 removal and N2 wash) than PSA in LAC [54]. This type of plants offers an

economic advantage for subsequent urea production where already separated CO2 can be used as

a feedstock.

2.5 Toluene Hydrogenation

Figure 5a is a schematic of the toluene hydrogenation plant which consists of four main

sections for storage, hydrogenation, cooling, and recycle compression [59,60]. Toluene is pumped

from the storage tank and evaporated partially in a gas-liquid recuperator and completely in a heat

exchanger inside the hydrogenation reactor. Gaseous toluene mixes with hydrogen feed and enters

the reactor at 200°C. The inset in Fig. 5a presents toluene thermodynamic conversion as a function

of pressure and hydrogen-to-toluene ratio (H2/C7H8) at 250°C; it indicates that high conversion

can be achieved at modest pressures and excess hydrogen. On the basis of these results, we selected

10 bar, 240°C, and H2/ C7H8 of 4 as reactor operating conditions. Allowing for 0.5 bar pressure

drop through the reactor and heat exchanger, MCH is condensed at 9.5 bar and 40°C and pumped

to the MCH storage tank. Hydrogen and uncondensed MCH is compressed to 10 bar and mixed

with the primary hydrogen stream. The hydrogenation process is exothermic and requires an

external cooling loop with a heat-exchange fluid between 180 and 200°C.

Figure 5b shows that the estimated capital cost of the toluene hydrogenation process

decreases rapidly as the plant capacity increases to ~2,000 tpd MCH, but moderately thereafter.

11
The reactor was modeled as a shell and tube heat exchanger packed with catalyst; several parallel

reactor trains are required for throughput higher than 2000 tpd [61]. The maximum plant capacity

was restricted to 6,180 tpd for which size the H2 demand is 350 tpd - the largest available capacity

of a single train SMR. The pie chart in Fig. 5c provides a breakdown the capital cost at 6,180-tpd

plant capacity. A majority of the capital cost (51%) is attributed to the initial toluene inventory

equivalent to 10 days of storage capacity. Hydrogenation section (reactor, heat exchangers and

compressor) is the next expensive item at 31% whereas storage accounts for a small fraction of the

total capital cost.

2.6 Methanol Steam Reforming

Figure 6a depicts the methanol decomposition process consisting of separate sections for

steam reforming, water gas shift (WGS), steam raising and hydrogen purification [62]. We assume

that methanol is steam reformed over a conventional Cu/ZnO/Al2O3 [63] catalyst at 3 bar, 290oC,

and H2O/C of 2.
0
CH3OH + H2O = CO2 + 3H2 ΔH298 = 49.7 kJ/mol
0
CO + H2O = CO2 + 3H2 ΔH298 = -41.2 kJ/mol
0
CH3OH = CO + 2H2 ΔH298 = 90.7 kJ/mol

The overall reaction is endothermic and the heat of reaction is supplied by burning NG. The dry

composition of the reformate gas leaving the tubular reformer is 74.6% H2, 1.4% CO, and 24%

CO2. The water-gas shift section improves the H2 yield to 82% by conducting the exothermic WGS

reaction at 190oC over a copper-based catalyst. The enriched H2 stream exiting WGS rector is used

to preheat feed methanol, condensed to remove water, and compressed to 20 bar before it enters

the PSA beds. We estimate that PSA can recover 80 % H2 in the WGS exit stream [57]. The

remaining H2 in the PSA tail-gas is mixed with the NG combusted in the reformer burner. Figure

12
6a identifies the placement of various heat exchanges for raising process steam using the available

waste heat. Our performance model indicates that the methanol decomposition plant yields 0.15

kg-H2/kg-CH3OH while consuming 13.3 MJ-NG/kg-H2, 0.325 kWh electricity/kg-H2, and 1.12

kg-H2O/kg-H2.

Figure 6b presents the estimated capital cost of the methanol decomposition process as

function of plant capacity (tpd-H2). The capital cost is seen to decrease from $662k/tpd-H2 at 50-

tpd-H2 capacity to $396k/tpd-H2 at 350-tpd-H2 capacity. The pie chart in Fig. 6c provides a

breakdown of the capital cost at 350-tpd H2 capacity. The reforming section (tubular reactor and

heat exchangers), PSA, compressor, and miscellaneous (including steam raising) respectively

represent 53%, 25%, 13% and 8% of the total capital cost.

2.7 Ammonia Decomposition

Figure 7a depicts the ammonia decomposition process consisting of separate sections for

ammonia cracking, burner, storage, and hydrogen purification [64,65]. Ammonia cracking is

highly endothermic (30.6 kJ/mol-H2) and requires a Ni catalyst capable of operating at high

pressure (20 bar) and elevated temperature (800oC) [66]. This process does not have a wide

industrial application and likely requires development of a robust catalyst that is stable under the

harsh operating conditions [67]. The gas exiting the cracker contains near-stoichiometric amounts

of N2 and H2 with trace level of NH3 impurity (<0.5 mol%). The cracker operating pressure was

selected to eliminate any need for gas compression between ammonia cracker and hydrogen

purification sections.

Our performance model indicates that the ammonia decomposition plant yields 0.132 kg-

H2/kg-NH3 and consumes 10.6 MJ-NG/kg-H2, 0.07 kWh/kg-H2. We estimate that the PSA at 75%

recovery can supply fuel-cell quality hydrogen from the cracker outlet stream [57]. The PSA tail-

13
gas containing residual H2 is combined with NG and combusted in the burner to supply the heat

of decomposition required in ammonia cracker.

Figure 7b presents the estimated capital cost of the ammonia decomposition process as

function of plant capacity (tpd-H2). The capital cost is seen to decrease from $405k/tpd-H2 at 50-

tpd-H2 capacity to $275k/tpd-H2 at 350-tpd-H2 capacity. The pie chart in Fig. 7c provides a

breakdown of the capital cost at 350-tpd H2 capacity. The cracker (fired tubular reactor and heat

exchangers), PSA, and miscellaneous (including burner) sections respectively represent 59%,

31%, and 9% of the total capital cost.

2.8 MCH Dehydrogenation

Figure 8a depicts the dehydrogenation process comprising storage, dehydrogenation,

compression and hydrogen separation sections [59,60]. MCH is pumped from the storage tank,

vaporized completely and preheated to 255°C before entering the reactor. As shown in the inset,

high thermodynamic conversion (as calculated by Gibbs free energy minimization) is favored at

low pressures and high temperatures. Over 99.5% conversion is feasible at 350°C and 2 bar.

Higher temperatures are to be avoided due to risk of potential toluene decomposition. Depending

on the dehydrogenation catalyst used, hydrogen is recycled in Fig. 8a to maintain a H2/MCH molar

ratio of 0-0.2. Literature studies indicate that internal recirculation of hydrogen may prevent

catalyst deactivation, promote catalyst activity [68–70], and suppress by-product formation [71].

Experiments by Okada et al. [69] showed minor deactivation of a Pt-catalyst after 6,000 h of

operation, and that decreasing the H2 molar feed ratio from 20 to 5% did not affect catalyst

stability. Our calculations indicate that co-feeding up to 20% hydrogen does not significantly alter

the thermodynamic conversion at 350°C and 2 bar. The exit stream from the reactor containing

hydrogen and toluene is fed to a condenser where toluene is condensed at 40°C and 1.5 bar. 80%

14
of toluene is condensed at these conditions and is pumped to the toluene storage tanks. Hydrogen

and uncondensed toluene are compressed to 20 bar in a four-stage intercooled compression system.

Additional toluene condenses at higher pressures, bringing the total condensed fraction to 97.6%.

For fuel cell quality hydrogen, the stream is fed to a PSA unit to separate toluene and traces of

MCH from the hydrogen. Considering that aromatics have a high adsorption potential on activated

carbon, a PSA hydrogen recovery of 90% was assumed. The PSA beds are regenerated by lowering

the pressure to 1.3 bar. Because toluene is an expensive commodity ($0.6/kg), a further

condensation of toluene was included. Toluene and unrecovered hydrogen from the PSA tail-gas

is fed to a chiller at -20°C which increases the total amount of toluene being condensed in the

overall process to 99.62%. Unrecovered hydrogen and uncondensed toluene are mixed with natural

gas and fed to a burner to provide the necessary heat for the endothermic dehydrogenation reaction.

Figure 8b presents the capital cost of the dehydrogenation process as function of plant

capacity (tpd-H2). Capital cost decreases rapidly as plant capacity is increased but more modestly

at capacities exceeding ~250 tpd-H2. The dehydrogenation reactor is modeled as a reformer-like

tubular furnace that can be scaled to 350-tpd H2 using a single train. The compressor station,

however, needs more parallel trains for capacities exceeding 150-tpd H2. The pie chart in Fig. 8c

provides a breakdown of the capital cost at 350-tpd H2 capacity. Dehydrogenation section (reactor

and heat exchangers) dominates the capital cost at 44% with separation (PSA and chiller) and

compression section also account for a significant portion of the capital cost (29% and 20%,

respectively).

2.9 Transmission

Figures 1 and 2 distinguish the transmission and distribution steps as defined in this study.

The transmission step includes transport liquid hydrogen carrier from a) central production facility

15
to a storage terminal via rail, b) storage terminal to decomposition plant by trucks, and c)

decomposition plant to GH2 terminal at city gate by trucks. The distribution step refers to transport

of gaseous hydrogen from the GH2 terminal to local refueling stations. We consider two modes of

transmission, by rails and pipelines. Federal Railway Administration (FRA) regulations currently

only permit shipping of liquid carriers by rail, but not gaseous or liquid hydrogen. We assume that

pipelines, when used, extend to the decomposition plant for liquid carriers and GH2 terminal for

gaseous hydrogen.

We used actual cost data for transmission of ammonia, methanol and toluene/MCH by rail.

U.S. rail carriers shipping over 4,000 carloads annually are mandated to supply a sample of the

waybill for carloads and commodities shipped. We used the 2018 waybill data [72] and correlated

the transmission cost in terms of $/ton-mile as a function of shipping distance.

For pipeline transmission, we used HDSAM cost correlations for pipes, associated labor to

construct the pipeline, right of way (ROW), operation and maintenance, and compressors/pumps

[46]. In this study, the total length of the pipeline from Texas to northern California is 2,000 miles,

the maximum pipe diameter is restricted to 142 cm, the maximum pressure operating pressure is

80 bar, and the maximum pressure drop between pipe segments is 20 bar. To avoid erosion of the

inner wall of the pipe, the maximum velocity is restricted to 20 m/s for GH2 and 4 m/s for the

liquid carriers [73]. Given those restrictions, up to 14 compressor stations were needed over the

entire length of the pipeline for GH2 and 18 pumping stations were needed for the liquid carriers.

3.0 Economic Model

Total cost of ownership was evaluated using the U.S. Department of Energy (DOE)

standard economic tool (H2A) and assumptions [58]. As listed in Table 3, the following set of key

economic parameters was selected for our analyses: a) 2018 reference year, b) 10% after-tax

16
internal rate of return, c) 1.9% inflation rate, d) 30-year economic analysis period, e) modified

accelerated cost recovery system (MARCS) for depreciation period and schedule: 15 years with

an effective total tax rate of 38.9%, f) $0.0574/kWh electricity cost in Texas and 0.125/kWh in

California, and g) $2.51/TJ natural gas cost: in Texas and $6.45/TJ in California.

4.0 RESULTS AND DISCUSSION

Table 2 summarizes the various modeling tools, financial assumptions and performance

parameters used to analyze the production, transmission, decomposition and storage steps for the

carrier pathways shown in Fig. 1.

4.1 Baseline GH2 Pathway

Figure 9 presents the breakdown of the cost of hydrogen distributed to the refueling stations

in the baseline GH2 pathway with assumptions given in Table 1. The estimated cost of delivered

H2 in the baseline pathway is $4.95/kg-H2, split as 46% for hydrogen production by SMR accounts,

25% for GH2 terminal and storage, 22% for truck distribution of H2 from city gate to dispensing

stations, and 6% for truck transmission of H2 from production site to city gate. It is worth

emphasizing that the GH2 scenario includes 10-d (500 t-H2) of geologic storage which is not

available at all sites and it contributes $0.30/kg-H2 to the overall cost. Also, $4.95/kg-H2 does not

include the costs incurred at the dispensing station such as buffer storage, H2 compression above

900 bar, and refrigeration for cooling H2 to -40oC for 700-bar refueling. A recent study estimated

the dispensed cost as 13-16 $/kg-H2 at very low production volumes that are typically encountered

in a demonstration phase.

Nearly 54% of the $4.95/kg-H2 is due to the capital layout for SMR plant, trucks used for

H2 transmission and distribution, and GH2 terminal and storage facilities. The remaining 46% is

17
distributed as follows: 22% for fuel expenses, i.e., natural gas in SMR and truck diesel; 7% for

electrical and water utilities; and 17% for operations and maintenance.

The GH2 pathways consumes 1.42 kWh/kWh-H2 fuel energy and 1.71 kWh/kWh-H2 total

fuel energy assuming 33% electrical power generation efficiency. Thus, the overall efficiency is

58.5%.

4.2 Hydrogen Carrier Production Cost

Figure 10a presents the levelized cost of hydrogen production normalized on the basis of

H2 distributed to the refueling station. The normalization process reflects any carrier losses during

the decomposition step as well as any carrier and H2 losses during H2 purification by PSA; it also

accounts for an additional mole of H2 produced by steam reforming of methanol.

At $1.22/kg-H2, the levelized production cost is smallest for methanol carrier since it is

produced from natural gas in a very large one-step ATR plant (10,000 tpd) without requiring an

explicit step for pure H2 production by SMR.

At $2.20/kg-H2, the levelized production cost is highest for ammonia carrier since

ammonia plants are more capital intensive than methanol plants: the levelized capital cost is

$1.28/kg-H2 for ammonia plants compared to $0.56/kg-H2 for methanol plants. As discussed

earlier, ammonia plants require producing pure H2 and this step accounts for 44% of the levelized

production cost of ammonia.

At $1.35/kg-H2, the levelized production cost of MCH is competitive with methanol. Since

MCH is produced by a simple exothermic process for hydrogenating toluene, it has a low capital

cost, $0.30/kg-H2. However, it also requires producing pure H2 by SMR, that adds $0.32/kg-H2 to

the capital cost. SMR, bringing the total close to the capital cost for methanol production. The

SMR process accounts for nearly 2/3rd of the levelized cost of MCH production.

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 The levelized cost of distributed H2 production, $2.30/kg-H2, is included in Fig. 10a to

emphasize the benefit of natural gas price differential between gulf state and California and the

economy of scale. As a comparison, the levelized cost of centralized H2 production by SMR in a

gulf location is $0.96/kg-H2 in the ammonia plant and $0.89/kg-H2 in the MCH plant. Nearly 2/3rd

of the difference between the levelized costs of H2 production by SMR in California and in a Gulf

state is due to the cheaper natural gas price (2.51 $/TJ vs. 6.45 $/TJ); the remaining 1/3rd is due to

economy of scale (50 tpd-H2 vs. 350 tpd-H2). The net benefit is, however, smaller because of the

cost associated with the production of the carrier. The net result is that, compared to the baseline

GH2 scenario, the levelized production cost is smaller by $1.08/kg-H2 for methanol, $0.95/kg-H2

for MCH, and only $0.10/kg-H2 for ammonia.

4.3 Hydrogen Carrier Decomposition Cost

Figure 10b shows that, at 50 tpd-H2 scale, the levelized decomposition costs are comparable

for the three carriers, 0.61-0.78 $/kg-H2. As discussed earlier, the methanol decomposition method

is well established but requires steam reforming and water gas shift process step that make it capital

intensive, ammonia decomposes at high temperature (800oC) over a Ni catalyst that may require

further development and field testing, and MCH dehydrogenates on a recently-developed Pt/Al2O3

catalyst under mild conditions. The estimated levelized capital costs for decomposition using these

processes are aligned as follows: $0.53/kg-H2 for methanol, $0.43/kg-H2 for ammonia, and

$0.32/kg-H2 for MCH. Conversely, the levelized fuel and utilities costs for decomposition are

highest for MCH, $0.53/kg-H2, as it has a high heat of formation, 68.3 kJ/mol-H2, smallest for

ammonia, $0.07/kg-H2, and $0.10/kg-H2 for methanol, somewhat higher than for ammonia in spite

of lower H because of the steam raising step.

19
 The levelized decomposition costs in Fig. 10b scale more favorably for ammonia and methanol

than MCH. Absent published industrial data, a bottom-up costing method was used to project the

effect of throughput on the levelized cost of MCH dehydrogenation. A scaling factor of 0.6 was

applied in projecting the effect of throughput on the levelized cost of steam methanol reformer,

ammonia cracker and PSA in methanol and ammonia decomposition plants.

Further study is required to evaluate the possible benefit of methanol reforming at pressures

higher than 3 bar to reduce the capital and operating costs of a reformate compressor upstream of

the PSA unit. This cost saving needs to be evaluated against the offsetting cost of operating at

higher steam to carbon ratio to maintain the same methanol conversion. A similar trade-off study

is also recommended to evaluate the possible benefit of dehydrogenating MCH at combinations of

pressures and temperatures higher than 2 bar and 350oC.

4.4 Transmission Costs

4.41 Pipeline Transmission: Figure 11a presents the levelized transmission costs of gaseous H2

and liquid carriers as a function of pipeline length for 6,000 tpd-H2 equivalent capacity (left) and

as a function of capacity for 2000-mile pipeline (right). The results are for API 5L Grade X52

pipes, 60-80 bar operating pressure, 20-bar pressure drop between pumping/compressor stations,

and maximum flow velocity of 20 m/s for H2 and 4 m/s for liquids. At 6,000 tpd-H2 equivalent

capacity, Fig. 11a (left) shows that the optimum pipe OD for lowest levelized transmission cost is

46 cm for liquid methanol and ammonia pipelines, 76 cm for liquid MCH and toluene pipelines,

and 91 cm for gaseous H2 pipeline. Figure 11a (right) indicates that, for fixed pipeline length,

larger pipes are preferred at higher throughputs. As a reference, the initial capital outlay for a 6000

tpd-H2 pipeline is $3.6M/mile for H2 and about $1.6M/mile for methanol and ammonia.

20
 Co-locating supply (MCH) and return (toluene) pipelines for a two-way carrier provides

some cost relief in right-of-way and permitting activities. Figure 11a shows that the transmission

cost is a) lowest for methanol and ammonia, b) similar for H2 and MCH/toluene, c) decreases at

higher capacities, and d) unlikely to be economic for throughputs much below 5,000 tpd-H2. The

maximum capacity of the pipelines is limited to 20,000 - 25,000 tpd-H2; multiple pipelines may

be needed if the demand exceeds the maximum capacity.

For a perspective on the various contributors to the levelized transmission costs, Table 4

provides the data for 2000-mile pipelines with 6,000 tpd-H2 equivalent capacity, divided in three

categories: a) installed capex factors for pipe, labor, right of way, and compressor/pumping

stations, b) miscellaneous capex factors for engineering and design, project contingency, and

permitting and contractor, c) operating and maintenance for electricity (pumping and compression)

and maintenance.

4.42 Train Transmission: Figure 11b (left) presents the 2016 Railroad waybill data on

transmission costs ($/ton-mile) of methanol, ammonia and toluene as a function of distance. A

waybill is a receipt created by the railroad companies of every carload of freight that travels on

rails; it describes the commodities on each car, origin, destination, freight revenue, type of train

car, other modes of transportation (e.g., truck, ship) the freight travels on, freight weight, etc. The

freight revenue in $/ton-mile generally decreases with distance and number of freight cars per

train. The limiting rail transmission cost is related to the fuel consumption, about 380 ton-mile/gal,

fuel cost, perceived hazard in transporting material, and is slightly smaller for methanol ($0.04/ton-

mile) than for toluene ($0.044/ton-mile) and much smaller than for ammonia ($0.088/ton-mile).

Figure 11b (right) summarizes a representative set of results for the total levelized cost of

transmitting H2 carriers on a scenario consisting of unit trains at a capacity equivalent to 50-tpd

21
H2, storage at receiving rail terminal, and trucking from the receiving terminal to the city gate.

Consistent with the results in Fig. 11b (left), the levelized transmission cost is smallest for

methanol, $0.63/kg-H2, nearly double for ammonia, and more than triple for MCH.

4.5 Levelized Cost of Hydrogen Distributed to Stations

4.51 Baseline 50 tpd-H2 Distributed to Stations: Figure 12a presents the levelized cost of H2

broken down in terms of the costs for H2 production, LHC production, LHC transmission by the

train scenario, LHC decomposition and GH2 terminal & storage, and H2 distribution. To be

competitive with the baseline GH2 scenario, the combined cost of H2 & LHC production, LHC

decomposition, and LHC transmission needs to be less than $2.60/kg-H2. The LHC related costs

as analyzed are $2.63/kg-H2 for methanol, $3.42/kg-H2 for ammonia, and $3.45/kg-H2 for MCH.

Thus, only the methanol option is cost competitive with the $0.30/kg-H2 cost saving in the

combined production and decomposition cost offset by the 0.33 $/kg-H2 higher transmission cost.

As a carrier, ammonia is more expensive than methanol; it has $0.81/kg-H2 higher combined

production and decomposition cost and $0.69/kg-H2 higher transmission cost. The MCH scenario

is slightly more expensive than ammonia with $0.71/kg-H2 lower production and decomposition

cost offset by $0.87/kg-H2 higher transmission cost.

The levelized H2 cost can also be presented in terms of the initial capital investment,

operating and maintenance (O&M), fuel, and utilities; the data below were obtained by combining

the category costs in H2 production, LHC production, LHC transmission by the train scenario,

LHC decomposition and GH2 terminal & storage, and H2 distribution. The category costs are

aligned as follows. Capital: ammonia > methanol ~ MCH > GH2; O&M: MCH > ammonia >

methanol > GH2; fuel: GH2 > MCH > methanol > ammonia; and utilities: GH2 ~ MCH > ammonia

~ utilities.

22
▪ Methanol: $2.89/kg-H2 capital; $1.24/kg-H2 O&M; $0.71/kg-H2 fuel; $0.14/kg-H2 utilities

▪ Ammonia: $3.56/kg-H2 capital; $2.08/kg-H2 O&M; $0.66/kg-H2 fuel; $0.17/kg-H2 utilities

▪ MCH: $2.88/kg-H2 capital; $2.60/kg-H2 O&M; $0.86/kg-H2 fuel; $0.31/kg-H2 utilities

▪ GH2: $2.66/kg-H2 capital; $0.85/kg-H2 O&M; $1.10/kg-H2 fuel; $0.34/kg-H2 utilities

4.52 Effect of Demand: Figure 12b presents the levelized cost of H2 distributed to stations at 10

to 350 tpd-H2 and at 6,000 tpd-H2 using the train and pipeline scenarios, respectively. It is assumed

that, independent of demand, all carriers are produced centrally from natural gas as feedstock at

commercially viable scale, and, for simplicity in presentation, all levelized costs include fixed

$1.10/kg-H2 distribution cost. The results indicate that, in the market introductory phase with

demand below 50-tpd H2, methanol is an attractive H2 carrier as it offers $0.33/kg-H2 lower

levelized cost than the baseline GH2 option. It also carries lower investment risk because

construction of a new SMR plant at city gate is avoided and methanol may be siphoned from an

existing methanol production facility. In all cases, comparison between GH2 and liquid carriers is

sensitive to the prevailing natural gas price differential between the carrier production site and the

city gate, $3.93/TJ in this study.

In the other limit, the methanol option is also cost competitive with centralized SMR if

sufficient demand, 6,000 tpd-H2 equivalent capacity, exists to make pipelines viable. In this limit,

the levelized cost of H2 distributed to stations at 350 tpd-H2 demand per city gate is similar, albeit

slightly smaller, for methanol and H2 pathways, and is similar for ammonia and MCH pathways.

Compared to the train transmission scenario, the pipelines offer a cost saving of $0.27/kg-H2 for

methanol and ~$1/kg-H2 for ammonia and MCH. However, methanol is a lower cost option than

ammonia or MCH for both train and pipeline scenarios. Also, building gaseous pipeline is not cost

effective in that the baseline GH2 scenario has lower levelized H2 cost.

23
4.6 Energy Efficiency

Figure 13 compares the total (fuel plus electrical) energy consumed in the methanol,

ammonia and MCH options with the baseline GH2 pathway. The MCH option consumes the

maximum energy and has the lowest efficiency (42.2%), followed by ammonia with 44.4%

efficiency and methanol with 46.7% efficiency. The endothermic dehydrogenation step including

PSA at city gate is the largest contributor to the increase in energy consumption over the baseline

GH2 scenario (58.5% efficiency). Figure 13 includes the energy consumed in producing make-up

toluene as part of fuel energy.

4.7 CO2 Emissions

The primary source of CO2 emission in the scenario analyzed in this work is natural gas

used to produce H2, produce/hydrogenate carrier, and decompose/dehydrogenate carrier. We

estimate that a total of 14.6 (lowest for ammonia) to 15.5 (highest for methanol) kg-CO2/ kg-H2 is

emitted due to NG usage. Smaller amounts of CO2 are also emitted because of the electricity and

diesel consumed in these process steps and during the transmission/distribution step.

5.0 SUMMARY AND CONCLUSIONS

We have investigated a complete scenario involving H2 production, H2 carrier production,

H2 and carrier transmission, carrier decomposition, and H2 distribution. The study has included

three systems representing different classes of carriers: one-way vs. two-way, need for pure

hydrogen production, and ease of production by renewable sources. The following are the major

conclusions from this study.

• Since methanol is commercially produced at large scale and can be transmitted by rail, the

option of deploying it as a hydrogen carrier may offer lower risk in the transition phase with

<50-tpd H2 demand.

24
• Ranking of the three carriers by levelized production costs: methanol (1.22 $/kg-H2) < MCH

(1.35 $/kg-H2) << ammonia (2.20 $/kg-H2).

• H2 capacity of the carrier is an important factor in determining the transmission cost by trains.

Toluene has nearly the same train transmission cost as methanol on $/ton-mile basis but is >3

times costlier on $/kg-H2 basis.

• Toxicity and handling are also important factors in determining train transmission costs.

Ammonia has nearly the same H2 capacity as methanol but is >2 times costlier to move by train.

• Ranking of the three carriers by levelized decomposition cost: ammonia (0.61 $/kg-H2) < MCH

(0.75 $/kg-H2) ≤ ammonia (0.78 $/kg-H2).

• Ranking of the three carriers by levelized cost of H2 distributed to refueling stations at 350 tpd-

H2 demand: methanol (4.63 $/kg-H2) < MCH (6.17 $/kg-H2) < ammonia (6.44 $/kg-H2).

• At very high demands, 6,000 tpd-H2, compared to transmission by rail, 2,000-mile carrier

pipelines can reduce the levelized cost of H2 distributed to stations by $0.28-1.09/kg-H2. The

saving is larger for ammonia and MCH than for methanol. With pipelines, the levelized cost is

slightly lower for methanol than for gaseous H2.

• Hydrogen carriers are stored at each step in the scenario. Being a two-way carrier, MCH and

toluene require separate storage tanks at the production, rail terminal, and decomposition sites.

In the rail transmission option, the total estimated costs for carrier storage and terminal are

$0.10/kg-H2 for methanol, $0.198/kg-H2 for ammonia, and $0.248/kg-H2 for MCH.

• Further study is needed to evaluate the role of carriers as medium for bulk hydrogen storage.

Potential applications of hydrogen carriers of particular interest include renewable energy

storage (wind and solar) and steel industry. Further work is recommended to redefine TCO to

25
 incorporate costs associated with environmental impacts or benefits available from carbon

credits.

6.0 ACKNOWLEDGEMENTS

This work was supported by the U.S. Department of Energy’s Office of Energy Efficiency and

Renewable Energy. Mr. Jesse Adams of the Office of Hydrogen and Fuel Cell Technologies was

the Technology Development Manager for this study. Argonne National Laboratory, a

U.S. Department of Energy Office of Science laboratory, is operated by UChicago Argonne, LLC,

under Contract No. DE-AC02-06CH11357.

7.0 ATTRIBUTIONS
1
Courtesy by olafpictures from Pixabay. https://pixabay.com/photos/bulgaria-vratsa-abandoned-

industry-1351947/
2
Image HDSAM Manual. https://hdsam.es.anl.gov/
3
Photo courtesy from Lincoln Composites. https://www.energy.gov/eere/fuelcells/hydrogen-

tube-trailers
4
Image by gwav from Pixabay. https://pixabay.com/photos/cincinnati-train-yard-railway-

1384325/
5
https://commons.wikimedia.org/wiki/File:Sorting_tank_cars_on_the_Englewood_Hump_(5401

636867).jpg
6
https://pixabay.com/photos/marshalling-yard-germany-trains-3535659/
7
Image by pasja1000 from Pixabay. https://pixabay.com/photos/factory-the-industry-the-tank-

2915737/
8
https://pixabay.com/photos/tanks-petrochemistry-silos-406908/
9
https://pixabay.com/photos/petrochemical-plant-refinery-960296/

26
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35
 H2 Production 1 GH2 Terminal2
NG
Feed-stock H2
Utilities
Electricity,
Water SMR

Distribution 3

Baseline GH2

Figure 1 Baseline GH2 Scenario

36
 Annual average cost of NG ($/MBtua) in U.S. 2018
Source: U.S. Energy Information Admin. (EIA.gov)
a1 MBtu=1.055 TJ

7.47
2.62
5.73

5.0

6.80 2.43
8.04

2.65
3,000-5,000 tpd 3.11

Methanol Production1 Storage & Transportation

Infrastructure4
NG
MeOH
Water

Electricity

Liquid Methanol Carrier

Large Plant
Transmission5 Storage Terminal 6

GH2 Terminal2 H2 Purification PSA MeOH Decomposition10 Local Storage8 Transmission7

MeOH
H2
H2
+ NG
CO, CO2,
MeOH

Utilities

Figure 2 Hydrogen carrier pathway

37
 To Steam
HP Steam Turbine
ATR
Purge Gas
Oxygen Methanol Storage
Synthesis
H2
NG Sulphur Syngas Cooling &
Removal Compression
Waste Heat
ATR Boiler Condensate

To Steam
Two-Step HP Steam Turbine
(SMR+ATR)
Oxygen Purge Gas Methanol Storage
Synthesis

NG Sulphur Syngas Cooling &

SMR Compression
Removal
Waste Heat
ATR Boiler Condensate
To SMR
Furnace

One-Step CO2 Recovery Steam

(SMR) (Optional)

CO2 Purge Gas Methanol Storage

Synthesis

Sulphur Syngas Cooling &

SMR
Removal Compression
Waste Heat
To SMR Boiler Condensate
Furnace

(a) Industrial production of methanol at different scales (b) Breakdown of capital costs
Capital Cost, $M/tpd

Plant Capacity, tpd

(c) Projected capital costs
Figure 3 Projected capital costs for industrial production of methanol at different scales by one-
step SMR, two-step ATR and SMR, and one-step ATR

38
 Linde Ammonia Concept Steam To Steam
Turbine
(LAC)
Steam Ammonia Storage
Synthesis

NG PSA H2
Sulphur Syngas
SMR WGS
Removal Compression
Waste Heat
Boiler

O2
Fuel to SMR Furnace

Air
N2
ASU

0.70
Conventional Ammonia Process To Steam
Turbine
HP Steam
0.65 Air
$MM/Ton

Air N2
ASU Ammonia Storage
Cost,$M/tpd

Synthesis
0.60
Sulphur Syngas Cooling &
SMR WGS
Removal Compression
Waste Heat
To SMR ATR Boiler Condensate
N2 Wash
0.55
CapitalCost,

Furnace
CO2 Removal Off-gas
Total Capital

0.50

0.45

0.40

0.35
0 500 1000 1500 2000 2500 3000
Ammonia Plant
Plant Capacity,
Capacity, tpd MT/day
Breakdown of Capital Costs (2,500 tpd)

Figure 4 Industrial production of ammonia: schematic layouts of Linde concept (top) and
conventional process (inset middle), projected capital cost at different scales (middle), and
breakdown of capital costs

39
 Compression

Recycle H2/MCH
Storage 2
Makeup
Toluene

Storage 1
MCH Tank
Toluene Tank
Heat
Rejection C7H14(l)
From Dehydrogenation

C7H14 /H2
H2
Plant

240 °C
5

C7H8(l)
4

220 °C

C7H8(g)
H2/TOL = 3
180 °C

Heat
H2 Rejection
200 °C
(High Grade) T = 250 C
H2

Cooling Hydrogenation
System Boundary
H2 (a) Schematic of toluene hydrogenation plant

(b) Capital cost of MCH plant (c) Breakdown of capital cost, 6,764-tpd MCH plant
Figure 5 Toluene hydrogenation plant: schematic, capital cost, and breakdown of capital costs for
a plant requiring 350 tpd-H2 to produce 6,764 tpd-MCH

40
 Reformer Exhaust

H2
To
Superheater

PSA
PSA
tailgas

NG Compressor

From
Boiler

LT-WGS

Burner Water
Air
To
boiler

MeOH+H2O
(a) Schematic of methanol decomposition plant

(b) Capital cost of methanol decomposition plant (c) Breakdown of capital cost, 50-tpd H2
Figure 6 Methanol decomposition plant: schematic, capital cost, and breakdown of capital costs

41
 (a) Schematic of ammonia decomposition plant with PSA for H2 purification

(b) Capital cost of ammonia decomposition plant (c) Breakdown of capital cost, 50-tpd H2
Figure 7 Ammonia decomposition plant: schematic, capital cost, and breakdown of capital costs

42
 H2 Purification & Condensation H2
PSA 20 atm ISO/SAE Standard
Compression
Tailgas (1.3 atm) H2 Co-Feed
4 stages/Intercooled (H2 /MCH=0-0.2)

20.8.atm

Chiller
40 °C

H2/MCH/TOL

C7H8(l)
1.5 atm
To Storage
To Burner
Area 400
Storage 1
Area 300 Storage 2

MCH Tank Toluene Tank

40 °C
MCH (~100%)
TOL (~100%)

70 °C
1
Area 102
0.9

C7H14 (g)

MCH Equilibrium Conversion

C7H14(l)

250 °C
0.8
0.7
0.6
Area 101
350 °C 0.5
0.4
350 °C, 0% H₂
High grade
2 atm

0.3
waste heat 350 °C, 20% H₂
0.2
300 °C, 0% H₂
0.1
NG
Area 200

300 °C, 20% H₂

0.12 mol/s H2 0
255 °C
256 kWth 1 2 3 4 5 6 7 8 9 10
Pressure, bar
PSA Tailgas Dehydrogenation
System Boundary

(a) Schematic of MCH dehydrogenation plant

Storage
3%

Separation
31% Dehydrogenation
46%
Compression
20%

(b) Capital cost (c) Breakdown of 0.72 M$/tpd-H2 capital cost

Figure 8 MCH dehydrogenation plant: schematic, capital cost, and breakdown of capital costs for
a plant producing 50 tpd-H2

43
Figure 9 Cost and performance of the baseline gaseous H2 pathway producing 50 tpd-H2 by steam
reforming of methane at city gate

44
 a) Levelized costs of carrier production at industrial scale

b) Levelized cost of carrier decomposition as function of demand

Figure 10 Levelized costs of centralized production of carrier and carrier decomposition

45
 1.8 1.4
6,000 tpd-H2 (71 cm O.D.) 3,200 km Pipeline
1.6 1.2

Transmission Cost, $/kg-H2

Transmission Cost, $/kg-H2

MCH+Toluene
1.4
(76 cm O.D.) 1.0 (91)
1.2 (132) (157)
Hydrogen 0.8 Hydrogen
1.0 (97)
(102 cm O.D.)
0.8 (117)
0.6 (137)
(41) (152)
0.6
0.4 (56) MCH+Toluene
0.4 (71)
Methanol/Ammonia (81) (91)
0.2 0.2 Methanol/Ammonia
(46 cm O.D.)
0.0 0.0
0 1000 2000 3000 4000 5000 6000 0 5,000 10,000 15,000 20,000 25,000 30,000
Pipeline Length, km Hydrogen Equivalent Capacity, tpd

a) Carrier transmission by pipelines

b) Carrier transmission by trains

Figure 11 Levelized costs of carrier transmission by pipelines and trains

46
 a) Levelized costs of H2 distributed to stations at 50 tpd-H2

b) Levelized costs of H2 distributed to stations at different demand

Figure 12 Summary of levelized cost of hydrogen distributed to stations using hydrogen carriers

47
Figure 13 Energy efficiency of H2 carriers

48
Table 1 Hydrogen carriers: physical properties, production routes, and decomposition methods

MP BP H2 Capacity Production Decomposition

Carrier P, T,
o
C o
C wt% g/L P, bar T, oC bar o
C H, kJ/mol-H2
Ammonia -78 -33.4 17.6 121 150 375 20 800 30.6
Haber-Bosch Process High-Temperature Cracking
Fe Based Catalyst Ni Catalyst
Methanol -98 64.7 18.75 149 51 250 3 290 16.6
Cu/ZnO/Al2O3
Catalyst Steam Reforming
MCH1 -126 101 6.1 47 10 240 2 350 68.3
Non-PGM Catalyst Pt/Al2O3 Catalyst
1
Toluene MP and BP: MP=-95 °C, BP=111 °C

49
 Table 2 Performance of methanol production processes
Two-Step One-Step
One-Step SMR
SMR+ATR ATR
Capacity (tpd) < 1,700 2,000 - 4,000 5,000 - 10,000
Process Variables
CO2/C 0.3
S/C 3.5 1.8 0.6
O2/C 0.48 0.60
M 2.05 2.05 1.84
Component Sizes (Number)
Air Separation Units (ASU) 1 1-2
Methanol Synthesis Reactors 1 BWR or 1 Quench 1-2 BWRs 2-4 BWRs
System Performance
NG Consumption (MJ/kg-methanol) 33.44
Electricity Demand (kWh/kg-methanol) 0.14 0.33 0.4
Electricity Produced (kWh/kg-methanol) 0 0.48 0.5

50
 Table 3 Financial, cost and performance assumptions
Financial Assumptions City annual average daily use = 50 tpd-H2
Operating capacity factor = 90%
Internal rate of return (IRR) = 10%
Depreciation (MACRS) = 15 yrs
Tax rate, 35%; Inflation = 1.9%
Analysis period = 30 yrs; Construction period = 3 yrs
NG Electricity Water
Feedstock and Utilities, California 6.44 $/TJ 5.74 ₵/kWh 0.14 ₵/L
Feedstock and Utilities, Texas 2.51 $/TJ 12.5 ₵/kWh 0.14 ₵/L
SMR Consumption, /kg-H2 0.165 TJ 0.569 kWh 12.7 L
GH2 Terminal HDSAM v 3.1, Compressed Gas H2 Terminal
H2 Storage 10-days geologic storage of H2 for plant outages
H2 Distribution 400 kg/day H2 dispensing rate at refueling station
Tube Trailers Payload Volume
1042 kg 36 m3

51
Table 4. Capital cost of 2000-mile pipelines of comparable 12,000 tpd-H2 equivalent capacities

3,200 km pipeline Gaseous H2 Methanol/Ammonia MCH

Diameter (cm) 142 61 117
Thickness (cm) 3.0 1.3 2.2
Hydrogen equivalent flow (tpd) 12,000 11,740 14,469
Recompression station interval (km) 124 9 18
Production cost of pipes ($/km) 1,247,839 238,960 802,993
Pipe broker and logistics ($/km) 124,784 23,896 80,299
Packing for shipping from mill ($/km) 29,269 5,605 18,835
Total mill cost ($/km) 1,401,891 268,460 902,127
Surface coating ($/km) 200,961 86,127 165,076
Repacking at coating plant ($/km) 14,635 2,802 9,417
Rail shipment to coating plant ($/km) 27,101 5,190 17,440
Rail shipment to staging area ($/km) 21,681 4,152 13,952
Truck shipment to site area ($/km) 21,681 4,152 13,952
Misc. pipe cost ($/km) 286,059 102,422 219,836
Right of way ($/km) 139,752 139,752 139,752
Labor welding ($/km) 656,760 64,992 333,522
Weld inspection + hydrotesting ($/km) 209,858 214,165 218,112
Staging and pipe support ($/km) 61,732 61,732 61,732
Total labor ($/km) 1,068,101 480,640 753,117
Recompression station ($/km) 187,801 67,566 123,703
Eng. & Design ($/km) 187,801 85,152 187,508
Project Contingency ($/km) 274,806 127,729 281,262
Permitting & Contractor ($/km) 412,209 127,729 281,262
Total misc. costs ($/km) 1,062,617 408,175 873,735
Total costs ($/km) 3,818,668 1,259,698 2,748,816

52