Renewable and Sustainable Energy Reviews 82 (2018) 1969–1978

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Renewable and Sustainable Energy Reviews

journal homepage: www.elsevier.com/locate/rser

Potential flue gas desulfurization gypsum utilization in agriculture: A MARK

comprehensive review
⁎
Jinman Wanga,b, , Peiling Yangc
a
College of Land Science and Technology of China University of Geosciences, 29 Xueyuanlu, Haidian District, 100083 Beijing, People's Republic of China
b
Key Laboratory of Land Consolidation and Rehabilitation, Ministry of Land and Resources, 100035 Beijing, People's Republic of China
c
College of Hydraulic and Civil Engineering, China Agricultural University, 17 Qinghua Donglu, Haidian District, 100083 Beijing, People's Republic of China

A R T I C L E I N F O A BS T RAC T

Keywords: Over the past few decades, there has been wide interest in developing strategies for the utilization of flue gas
Flue gas desulfurization gypsum desulfurization gypsum (FGDG), a by-product of scrubbing sulfur from combustion gases in coal-fired power
Agriculture generation plants. FGDG has applications in agriculture due to its function in the remediation of soil quality and
Soil reclamation crop growth. It is often economical to use FGDG as a soil amendment; however, compared to other industries,
Soil erosion
the utilization of FGDG in agriculture is very limited. A comprehensive review of numerous studies in the last
Plant growth
few decades was conducted in this paper, which systematically covered the importance, scope, function, effect
and risk regarding the utilization of FGDG in agriculture. As a remediation material, FGDG has many benefits in
agriculture applications, such as improving soil physicochemical properties, controlling soil and nutrient loss,
supplementing trace elements for soil and increasing crop yield. However, FGDG also contains a number of
toxic trace elements. Therefore, proper attention should be paid to some important areas related to FGDG
utilization, such as long-term studies of the impact of FGDG on soil health, heavy metal uptake, crop growth and
quality, and continuous monitoring of the health of soil and water. The problems of salt accumulation and heavy
metal toxicity due to excess application should also be addressed when FGDG is used in agriculture. Moreover,
some measures and standards for the practical application of FGDG need to be proposed to promote the
utilization of FGD gypsum in agriculture.

1. Introduction amount of FGDG in the world is increasing, the comprehensive

The application of industrial wastes to agricultural land has been a
topic of considerable interest in recent years. Flue gas desulfurization
gypsum (FGDG) is a by-product of sulfur (S) removal from fuel
combustion gases in the flue gas desulfurization (FGD) system in
coal-fired power generation plants [1]. The removal is generally
achieved through a wet scrubbing process that injects a lime or
limestone reagent into the flue gas path to capture SO2 as CaSO3,
which is then converted to CaSO4 through forced air oxidation [2]. In
recent years, an increasing number of coal-fired power generation
plants have used the SO2 scrubbing process to satisfy environmental
standards that aimed to limit the atmospheric acidity caused by SO2
emission. The composition of FGDG shows that, it is a good source of
Ca and S, which can be beneficial for crop growth and production,
especially for soils with very low Ca levels [3].
In China, approximately 70 MT (million tons) of FGDG are
produced each year (Table 1) [4], and in the USA, the amount is
approximately 20 MT [2]. Although the comprehensive utilization
utilization rate is still relatively low due to the continuous increase of
its production. The disposal of such a huge quantity of FGDG is a big
problem in an area around the plant. Therefore, new and innovative
strategies are needed to reduce the negative impacts of FGDG on the
environment. FGDG is mostly utilized as a soil amendment in
agriculture by supplying Ca and S for plant nutrition [3,5], improving
physicochemical properties [6], increasing water infiltration and move-
ment through the profile, reclaiming saline and sodic soils [7],
mitigating subsoil acidity and Al toxicity [8,9], reducing soil erosion
and nutrient loss [10], etc. Sakai et al. [11] developed an evaluation
model for assessing the complete economic and environmental impact
of the application of FGDG on agriculture and found that it caused a
reduction in SO2 emissions and increases in GDP and agricultural
production following soil reclamation.
There are strong indications that FGDG production will continue to
increase in the coming years due to the air quality regulations for
environmental protection, making it an attractive fertilizer (Ca and Ca
and S) and conditioner for various types of degraded soils. Many

⁎
Corresponding author at: College of Land Science and Technology of China University of Geosciences, 29 Xueyuanlu, Haidian District, 100083 Beijing, People's Republic of China.
E-mail address: wangjinman2002@163.com (J. Wang).

http://dx.doi.org/10.1016/j.rser.2017.07.029
Received 26 October 2016; Received in revised form 8 April 2017; Accepted 9 July 2017
Available online 14 July 2017
1364-0321/ © 2017 Elsevier Ltd. All rights reserved.
J. Wang, P. Yang Renewable and Sustainable Energy Reviews 82 (2018) 1969–1978

Table 1
Generation and utiliazation of FGD gypsum in China and USA.
Source:Watts and Dick [2], Pan [4].

Country Year FGD gypsum production (MT) Utilization (%) Country Year FGD gypsum production (MT) Utilization (%)

China 2005 5.0 10.0 USA 2004 10.9 75.2

2006 9.5 20.0 2005 10.9 77.1
2007 17.0 33.0 2006 11.0 79.1
2008 35.0 45.1 2007 11.1 75.6
2009 43.0 55.8 2008 16.1 60.2
2010 52.3 68.8 2009 16.3 49.7
2011 67.7 70.9 2010 20.0 48.5
2012 69.0 71.7 2011 22.7 47.1
2013 72.1 72.3 2012 23.5 47.0

studies on the effect and potentiality of FGDG as an amendment in
agricultural applications have been conducted by various agencies and
research institutes at dispersed locations all over the world. In this
study, the utilization of FGDG as a beneficial product of agriculture is
reviewed with the objective of helping to increase the application of
FGDG and reduce the environmental and economic impacts of
disposal. The present review covers the positive and negative aspects
of FGDG utilization in agriculture. This review also discusses the
accumulation of toxic trace elements, especially heavy metals in the
plants and their response to the application of FGDG into the soil. The
control and reduction of negative effects of FGDG is important for its
sustainable utilization in agriculture.
2. Physicochemical properties of FGDG
FGDG has a similar moisture content and is a major component,
CaSO4·2H2O, of natural gypsum and has better technical character-
istics than natural gypsum [12]. The final FGDG is often > 95% pure,
and the crystals are mainly of a rhomboid shape. A microprobe analysis
showed that the concentration of CaO and SO3, which were the main
components of the FGDG from Florina in North West Greece, ranged
from 31.9% to 32.5% and from 45.90% to 46.40%, respectively [13].
FGDG and natural gypsum have similar chemical composition also in
terms of minor constituents, among which Mg and Si oxide, both in the
range of 3–4%, were the most important [14]. Moreover, it generally
has finer, more uniform particles than natural gypsum sources [2,5,15].
After crushing, the particle size of natural gypsum is approximately
140 µm, whereas it is mainly in the range of 30–50 µm for FGDG
[16,17]. The chemical compositions of FGDG and natural gypsum are
showed in Table 2.
The chemical composition of FGDG varies depending on the design
of the power plant, operating conditions, and materials used. The
physicochemical properties of FGDG are more closely associated with
the quality of the coal than the major combustion and scrubbing
Table 2
Chemical composition of FGD gypsum, natural gypsum and fly ash, mass %.
Source: Telesca et al. [14].
Chemical composition FGD gypsum Natural gypsum
technologies used to remove S [18]. Moreover, stabilized FGDG
generally has higher pH, calcium carbonate equivalent values, and
concentrations of mineral elements that are essential to plants com-
pared to non-stabilized FGDG [19]. The major exception is lower S in
stabilized FGDG compared to non-stabilized FGDG, which is expected
since most stabilizing materials added to FGDG contain relatively low S
[20]. An extensive physicochemical properties investigation of 59 dry
FGDG samples collected from 13 locations representing four major
FGD scrubbing technologies showed that FGDG was dominated by Ca,
S, Al, Fe, and Si and that there was strong preferential partitioning into
the acid-insoluble residue for Al, Ba, Be, Cr, Fe, Li, K, Pb, Si, and S, Ca,
and Mg, which occurred primarily in water- or acid-soluble forms
associated with sorbents or scrubber reaction products [18,21]. Chen
et al. [22] found that applying non-stabilized FGD-CaSO3 was also safe
for growing plants as the FGD-CaSO3 rapidly oxidized to SO42- on the
field surface during the first week and that much of the SO42- and Ca
moved downward into the 0–50 cm soil layer during a field experi-
mental period of two months.
Compared to other solid waste from the coal-fired power plant, fly
ash, the source of FGDG, had higher levels of Ca as well as S. Fly ash
contained lower Ca concentrations but higher concentrations of K, Mg,
Fe, and most trace elements compared to those in FGDG (Table 3).
FGDG may contain higher levels of metals than some mined solid
wastes, but the concentrations are lower than the background levels
stipulated for soils in Table 4 [26,27].
In summary, FGDG has the physicochemical properties that make
them suitable for beneficial use in agriculture.
3. Effects of FGDG on developing degraded soil properties
FGDG can reclaim both saline-sodic soil and acid soil [28]; more-
over, some degraded soils, e.g., mined soils and eroded soils, can also
be reclaimed using FGDG. Soil physicochemical properties that are
affected by FGDG application have been reported by some researchers
when utilizing it as a soil amendment [7,29,30]. The physicochemical
properties of soil due to FGDG addition vary according to the original
properties of soil and the FGDG, but certain generalization can be
made in most cases [2]. The mechanisms and effects of various
Fly ash
degraded soils reclaimed by FGDG are showed in Fig. 1.

SO3 36.90 36.20 0.77

CaO 31.90 30.10 4.34 3.1. Developing sodic soils
MgO 3.80 3.66 2.06
SiO2 3.30 3.00 48.48 Sodic soils are characterized by the occurrence of excess Na+ to
Al2O3 1.00 0.85 24.44 levels that can adversely affect the soil structure and disturb the
Fe2O3 0.30 0.25 8.43
TiO2 0.05 0.04 1.08
availability of some nutrients to plants [54]. Sodic soil reclamation
P2O5 0.01 0.01 0.77 involves an increase in Ca2+ on the cation exchange sites at the expense
Mn3O4 – – 0.05 of Na+ [55,56]. FGDG is a good Ca2+ source, which was effective in
Na2O – – 1.22 crusting-prevention and sodic soil reclamation [41]. The application of
K2O – – 1.86
FGDG significantly increased the concentrations of Ca2+ and SO42- in
l.o.i 22.40 24.60 6.50
Total 99.66 98.71 100.00 the leachate compared to the levels seen in the unamended soil and the
leaching of Mg2+ and K+ were also greater from FGDG amended

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J. Wang, P. Yang Renewable and Sustainable Energy Reviews 82 (2018) 1969–1978

Table 3 and sodium adsorption rate (SAR). The application of FGDG signifi-
Comparison of physicochemical properties in FGD gypsum, Natural gypsum and fly ash. cantly increased the stability of macro-aggregates ( > 0.25 mm), IR,
hydraulic conductivity and water-holding capacity of the saline-sodic
Physicochemical FGD Fly ashb Natural Coald
properties gypsuma gypsumc soils [31,35], and slightly improve bulk density and porosity
[29,35,61]. The FGDG treatment for soil carbon sequestration held a
pH (1:5) 7.5 8.8 6.5 — promise when it was applied to slightly soidic soils [62]. The improve-
EC (ms cm−1) 2.6 7.6 7.5 —
ment of soil physical properties facilitated the leaching of Na+ and
Organic carbon (%) 0.16 1.2 1.29 —
Total nitrogen (%) 0.01 0.02 0.13 1.2 salts, which led to significant decreases in soil salinity and sodicity
Total phosphorus (%) < 0.01 0.06– < 0.01 — [31,36,40]. A soil column leaching experiment conducted by Wang
0.12 et al. [6] and Amezketa et al. [41] presented the fast reductions of EC
Total potassium (%) 0.44–0.65 < 0.01 0.05 0.02– and SAR in their leachates after the application of FGDG. The research
0.43
from Xiao et al. [63] showed that after the application of FGDG in a
Major elements (g kg−1)
Ca 163–272 < 0.01 247 5.0–26.7 saline-sodic soil, the Na+ content, EC, SAR, and pH were reduced near
S 104–167 — 207 3.8–53.2 the surface layers, but the trend was reversed in deeper soil layers.
Si 0.56–0.64 — 1.2 5.8–60.9 With the increase of the applied FGDG, there was no significant
Mg 6.5–22.8 < 0.01 1.3 1.0–2.5
difference in the reclamation effect. Therefore, when the small amount
Fe 1.7–14.9 3.0–6.1 0.9 3.2–43.2
Al 5.5–12.3 < 0.01 1.5 4.3–30.4 of FGDG was added, a better leached effect of Na+ was achieved [63].
Trace elements (mg kg−1) However, Buckley and Wolkowski [29] found that FGDG application
Mn 90–403 500–750 31 6–181 had a negative effect on aggregate stability at sites tested in Wisconsin,
Mo 0.5–14.7 — 0.80 < 1–73 but the mechanism of FGDG decreasing aggregate stability was not
Zn 2.5–14.3 9.7–23.7 6.1 < 1–
clear. Some research showed that the application of FGDG resulted in
5600
Cu < 0.1–7.6 32–54 < 0.8 1.8–185 the decrease of soil EC [6,31,41]; however, some research showed that
Cr 65–91 144–488 4.8 < 1–610 applying FGDG increased soil EC [34,37]. With the application of
Cd < 0.01 5.0–10.0 0.30 < 1–6.5 FGDG, the salt content in the soil will increase [7,64]. Therefore,
Pb 3–218 26.5– 1.2 4–218
salinity should be controlled by leaching when sodic soils are reclaimed
121.3
Ni 1.5–17.3 33.3– 2.3 0.4–104
with FGDG [65]. The increase of soil EC may be from poor drainage
69.8 conditions or lack of leaching after applying FGDG [64]. Under field
As < 2.6 1.0–4.0 < 2.6 0.5–106 conditions, the salts should be immediately removed by constructing
Se 2.1 0.6–2.6 < 1.2 < 0.1– good drainage conditions [7,66]. Moreover, some materials used to
11.4
capture SO2 contain sufficient Na such that end-products could
Hg 0.25 — 0.02 0.01–1.6
B 98–175 17–38 168 — enhance Na dispersion of clay particles and reduce soil water infiltra-
tion. Caution is needed when using high-Na FGDG on sodic soil
a
Baligar et al. [19], DeSutter et al. [23],b Singh et al. [24], Mupambwa et al. [25]. c
reclamation [67].
DeSutter et al. [23], d Baligar et al. [19]. Some scholars also combined FGDG with other materials to reclaim
saline and sodic soils. For instance, Nan et al. [32,68] carried out a 3-
Table 4 year field experiment in a saline-sodic soil in coastal area of north
Concentration of heavy metals regulated by national standard of China (mg kg−1).
Jiangsu Province of China and found that application of FGDG with
Heavy metals Pb Cd Cr As Se Ni Cu Hg humic acid decreased soil pH, SAR, and ESP, and increased the EC and
saturated hydraulic conductivity; moreover, the effect of combing
GB8173–1987a 250 5 250 75 15 200 250 5 FGDG and humic acid was better than that of single FGDG.
Soil backgroundb ≤ 35 ≤ 0.2 ≤ 0.2 ≤ 15 — ≤ 40 ≤ 35 ≤ 0.15

a
Control Standards for Pollutants in Fly Ash for Agriculture Use, GB8173-87.
b
Environmental Quality Standard for Soils, GB15618-1995.
compared to the unamended soil [57]. It indicated that a high loading
of Ca2+ due to addition of FGDG appeared to displace and leach other
cations, such as K+ and or Mg2+, from the soil [57]. The ion solution
composition of sodic soils also plays an important role in the reclama-
tion process. After the FGDG and leaching, the soil soluble salts were
transformed from sodic salts containing Na2CO3 and NaHCO3 to
neutral salts containing NaCl and Na2SO4 [6,58]. Kukier et al. [59]
reported that application of FGDG resulted in a change in the
distribution of exchangeable cations. There was an increase in ex-
changeable Ca in the zone of incorporation and in the subsoil according
to a field experiment. The downward movement of Ca was dependent
on soil texture and on the rate of the FGDG applied. In two soils with
higher clay content, Ca moved downward much more slowly [59]. Chun
et al. [60] conducted a field experiment in the semiarid region of
Kangping in northeast China and found that the application of 23.1 Mg
ha−1 FGDG significantly increased electrical conductivity (EC), ex-
changeable and soluble Ca2+, SO42- and decreased CO32-, exchangeable
Na+, and soluble Na+.
The FGDG addition altered several soil physicochemical properties
such as its bulk density, water-holding capacity, hydraulic conductivity,
infiltration rate (IR), pH, EC, exchangeable sodium percentage (ESP),
3.2. Developing acid soils
Acid soils exist due to their formation from parent materials or
from the application of ammonium-based fertilizers [69]. The reclama-
tion of acid soils is commonly accomplished using liming materials.
The oxide anions from the dissolution of the liming material react with
H+ to form carbonic acid or water, hence neutralizing active soil acidity
[70]. Moreover, the cations from liming materials help replace
exchangeable Al3+ from the soil exchange sites, which react with OH-
to form an insoluble compound, thus reducing the effects of acidity and
toxicity of the Al for plants [71–73]. Due to the unspent sorbent
component during desulfurization, FGDG is usually highly sodic and
has significant neutralization potential. FGDG as a soil amendment is
as effective as gypsum for inhibiting soil crusting, improving water
infiltration, and promoting the movement of Ca2+ into acid subsoils
[42]. The unstable FGDG (CaSO3·0.5H2O) is fairly insoluble and can
decompose to release SO2 under highly acidic soil conditions; however,
it can also oxidize to form gypsum. Therefore, the autumn surface
applications of unstable FGDG in no-till systems should permit ample
time for oxidation/dissolution reactions to occur without introducing
biocidal effects related to oxygen scavenging, and soil and annual crops
can thus benefit from additions of soluble Ca and SO4 if FGDG is
applied in advance of spring planting [74].
The four mechanisms by which soil acidity can be reclaimed using
FGDG are summarized as (i) the self-liming effect; (ii) precipitation of

1971
J. Wang, P. Yang
Fig. 1. Mechanisms and effects of degraded soils reclaimed by FGDG [33,46,47,51].
solid phases; (iii) co-sorption of SO42- and Al3+; and (iv) ion pair
formation [75]. The liming capacity of FGDG makes them suitable for
increasing pH in acid soils [45]. High application rates of FGDG
effectively alleviated the subsoil acidity syndrome with a decrease in
exchangeable Al and/or increase in exchangeable Ca [59]. By applying
FGDG, the acidity of the red and crimson soil caused by weathering and
leaching and chronic acid rain in southern China was neutralized or
balanced. Field water capacity and bulk density were observed as
increasing and decreasing, respectively. Due to the addition of the
FGDG, the enhancement of the soil pH value and the reduction of Al
toxicity in acidic soil were also observed [44].
The correct application amount of FGDG didn’t exhibit negative
impact on acid soil microbial activities. Soil enzyme activities can be
used as indicators of soil quality, especially as related to the biological
functioning of the soil that pertains to nutrient cycling. FGDG can be
applied to soil at rates ranging up to 1.12 Mg ha−1 without affecting the
potential cycling of nutrients associated with soil enzymes [43]. No
significant differences in the activities of urease, β-glucosidase, alkaline
phosphatase, or arylsulfatase were observed compared to an untreated
control for an acid Platea soil with a pH of 4.0 [42]. Chen et al. [48]
found that after 17 years of reclamation using FGDG at a 280 Mg ha−1
application rate in a field study, β-glucosidase activity had increased at
0–5 cm and 5–10 cm depths compared to an adjacent untreated area.
Furthermore, β-glucosidase activity more than doubled in the treat-
ments with FGDG compared to the conventional soil treatment at 0–
5 cm depth.
3.3. Developing mined soils
Abandoned mined land is a worldwide concern due to their
potential negative environmental impacts, including erosion and the
development of acid mine drainage. The use of FGDG as a substitute
for agricultural limestone represents a potential beneficial use alter-
native to landfill disposal of these materials. Chen et al. [76] investi-
gated the use of FGDG for the reclamation of abandoned coal mined
land in a field study in Ohio of USA and found that use of FGDG for
remediating acidic surface coal mined sites could provide effective,
long-term reclamation. Soil pH at 0–20 cm depth increased from 3.1 to
approximately neutral and was sustained at this level for 15 years in the
treatments included FGDG at a rate of 280 Mg ha−1 FGDG [48].
Stehouwer et al. [49] reported that FGDG was effective in increasing
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Renewable and Sustainable Energy Reviews 82 (2018) 1969–1978
the pH of mine soils in a greenhouse column study and that leachate
pH, EC, dissolved organic C, Ca, Mg, and S tended to increase with the
increase of FGDG application rate. The application of FGDG increased
the soil pH from 4.5 to approximately 7.5 [50].
Bacterial populations and diversity and microbial biomass in the
reclaimed coal mine plots significantly increased compared to the
adjacent untreated area and were generally similar among different
reclamation treatments [77]. Mycorrhizal symbiosis may be partly
responsible for the increased productive capacity of the reclaimed sites.
Wilson et al. [78] found that the reclaimed sites using FGDG had 2.4
times the number of mycorrhizal spores, 5.1 times the root colonization,
and 2.2–28 times the inoculum potential of the abandoned sludge. In
reclaimed sites, 82–100% of all plants became mycorrhizal compared to
30–67% of plants in abandoned sites [78]. FGDG addition increased
microbial biomass, which indicates improved soil health and could
contribute to increased crop yield [38]. However, microbial properties
did not show linear trends with FGDG concentrations, which requires
further studies on threshold values and potential negative effects on soil
health in case of excessive application of FGDG. Soil microbial properties
presented a strong change over time, the future research should also
focus on the longer term dynamics of microbial biomass, activity, and
community composition in response to the FGDG addition.
3.4. Controlling soil and nutrient loss
The Ca in FGDG reduces the dispersion of soil particles by
promoting the flocculation and aggregation of clay particles. The highly
erodible Na-affected soils can be remediated with the addition of
FGDG. Runoff and soil loss decreased and infiltration increased as the
FGDG application rate increased [10,52], which also led to the
significant increase in aggregate stability and the decrease in surface
crusting [26,53]. There was a 71% increase in total infiltration, a 36%
decrease in total runoff, and a 77% decrease in soil loss at the
13.44 Mg ha−1 rate relative to the 0 treatment in the soil with a SAR
of 48 [53]. In addition, the decrease in soil loss and the reduction in
erodibility were evidenced by the increase in sediment sizes greater
than the 125–53 µm range and the accompanying decrease in the
percentage of sediment in the 5–2 µm and sizes less than 2-μm [53].
Therefore, the use of FGDG can improve the success rate of erosion
control structures installed in dispersive soils and aid in the develop-
ment of approaches to remediate streambank erosion problems [19].
J. Wang, P. Yang
Phosphorus (P), nitrogen (N), and carbon (C) are implicated in
eutrophication of surface waters [79]. After the addition of FGDG, the
reduction in finer size fractions means that runoff from soils will
transport lower concentrations of chemical contaminants in a sorbed
state. Some research results have shown that the use of FGDG as a soil
amendment has the potential to reduce P, N, and C losses in runoff
through increased infiltration and/or the formation of less soluble
pools [10,53,80]. Converting soil P to less soluble forms with the
application of FGDG may reduce the release of soil P to runoff [81–83].
FGDG application to pastures and crops showed promise as an
economical soil amendment to reduce dissolved P loss in runoff [84];
on grassed soils, the high application rate of FGDG reduced P in runoff
by 35% [85]. Treatment of high P soils with FGDG decreases water-
extractable P by conversion to soil inorganic P fractions that are stable
with time, does not decrease plant production [86]. Chen et al. [87]
reported that FGDG reduced the P loss through soil incubation tests
and that a greater decrease in water-extractable P occurred with a
greater dosage of FGDG. Compared to conventional coarse gypsum,
nano FGDG further reduced water-extractable P by providing a much
greater specific surface area, higher solubility, better contact with the
fertilizer and soil particles, and superior dispersibility. Although FGDG
readily lowers P solubility in soils, their impact on P losses in the runoff
can be undermined by erosional processes [88,89]. A 3-years field plot
experiment showed that FGDG lowered dissolved P in runoff by up to
47% below the untreated control in the first year; however, the effects
did not persist into the remaining years of the study. Total P losses
were not significantly affected by FGDG, which was likely because of
elevated particulate P losses. Water-extractable P was reduced by up to
40% in treated soils compared to untreated soils across the 3 years.
Alva et al. [90] investigated the effect of FGDG on the transport of
nitrate (NO3-) and ammonium (NH4+) in a Candler fine sand in a
leaching column experiment and found the application of FGDG at
4.5 Mg ha−1 decreased the leaching of NO3- from NH4NO3 by 22%
compared to that without the application of FGDG, and total-N
recovery with or without FGDG accounted for 62–67% and 69–78%
of total N applied as Ca(NO3)2 and NH4NO3, respectively.
4. Effects of FGDG on improving plant growth
4.1. Promoting plant growth
Since FGDG is a good source of Ca and S and contains many useful
trace elements, it may be beneficial as an amendment to improve plant
growth and increase crop yield for agricultural soils. Some studies are
available related to the use of FGDG as a soil amendment for the
benefit of a large number of field crops. FGDG application can improve
the yield and quality of high Ca-requiring plants, such as peanuts,
tomatoes, maize, wheat and citrus trees [19,91]. Effects of FGDG on
plant growth and nutrient uptake are shown in Table 5. The application
rate of 4.48 Mg ha−1 FGDG significantly increased the citrus fruit yield
and fruit quality in sandy soils that contain low levels of extractable Ca
[92]. The shoot concentration of Ca in alfalfa, white clover and tall
fescue generally increased as the level of FGDG increased in the soil
[93]. Ca increased in topsoil and subsoil at the high rate of 20 Mg ha−1
in FGDG in soils typically found in eastern Ohio and western
Pennsylvania [91]. The plant tissue content of Ca in fescue and alfalfa
was increased by FGDG amendment [50,94]. FGDG increased alfalfa
dry matter yield by as much as 14%, and in the subsoil, the soluble Al
decreased and the Ca content and Ca: Al ratio increased [95].
S fertilization is required for many crops, and FGDG can be an
effective source of S [19,96,97]. FGDG improved alfalfa and soybean
yields when applied to agricultural soils [98]. The application of FGDG
(33 kg S ha−1) promoted maize growth and the uptake of N in a silt
loam soil of Ohio [5]. Canola yields were more variable and depended
significantly on the S rate but not the S source; therefore, FGDG
appears to be a viable S fertilizer source for dryland canola, and the
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Renewable and Sustainable Energy Reviews 82 (2018) 1969–1978
recommended S application rate was about 22 kg ha−1 [99]. The plant
tissue content of S in fescue and alfalfa was increased through FGDG
amendment [50,94].
Other trace nutrients were also supplied by FGDG. FGDG has been
used as a source of B for maize [40,100], alfalfa [45,101], white clover
[101], and fescue [101]. Se, Mn, and Mg are the trace elements
required by many plants and can be supplied by FGDG. Mg deficiency
symptoms were induced in the leaves of plants grown with low Mg and
the Mg to Ca ratio. Mg increased and Ca decreased in maize shoots in
an acid soil amended with FGDG [102]. Shoot concentrations of Mg
and Mn in alfalfa, white clover and tall fescue increased as the levels of
soil in applied FGDG increased [93]. Feldhake and Ritchey [103] found
that the application of high FGDG to pastures in Appalachia has the
potential to improve root growth and functioning in acid subsoil
horizons and that the Mn content of leaf tissue increased significantly.
He and Shi [104] found that application of FGDG was effective in
increasing soil available P, K, Mg and Si in acidic soil and that the
application rate of 1.125 Mg ha−1 offered the best efficiency, which
increased rice grain yield by 21.6%. The elemental concentration of the
maize tissues indicated a characteristic elevation of B and Se after 56
days of FGDG application [105]. Applying FGDG as soil ameliorant
increased the total yield as well as the safety and quality of sweet
potatoes due to the enhancement of the soil mineral composition
contained in FGDG [106].
However, some research also showed that the application of FGDG
had no significant effects on crop yield. DeSutter et al. [23] found that
wheat grain yields were not affected by FGDG treatments. Applications
of 2.2, 4.4, or 8.8 Mg ha−1 CaSO3 to the pH 6.2 soil produced no effect
on wheat growth or the uptake of N, P, Ca2+ and Mg2+ [42]. Although B
is essential to plants, the differences between sufficiency and toxicity
are narrow. B toxicity can be a problem for plants grown in soils
amended with FGDG containing high B. After the FGD-stabilized
materials were leached, B toxicity is commonly alleviated [100].
4.2. Improving plant physiology
Stabilized FGDG normally contain many soluble salts. Soil saliniza-
tion in arid zones is a major factor that resulted in the reduction in the
yield and quality of many important crops. Plants vary in sensitivity to
soluble salts and, if inappropriate levels are present, seed germination,
plant establishment, and growth may be reduced. High doses of FGDG
has been reported to adversely affect the biochemical composition as
well as the yield of many crops. Shahandeh and Sumner [107] reported
that after the application of FGDG in a greenhouse experiment, the
growth of weeping lovegrass and lespedeza was poor due to the
presence of high levels of soluble salts. Wang et al. [7] reported that
the improvement effects had no positive correlation with FGDG rate in
a pot experiment, and the effect of a high leaching level was better than
that of a low leaching level. Initially, the increase of FGDG application
rate resulted in soil improvement, but beyond a certain application rate
threshold, the improvement effects began to decrease. Salinity should
be controlled by leaching when sodic soils are reclaimed with FGDG
because sunflower growth is very sensitive to salinity during its
seedling stage [7].
Mao et al. [108] analyzed the potential mechanism of FGDG-
mediated amendment of sodic soils in an oil sunflower model by
accessing the Ca2+ distribution and Ca2+-ATPase activity in leaf cells,
and found that the Ca2+ ATPase activity caused cytosolic Ca2+ efflux,
that the Ca2+ influx occurred through the Ca2+-channels, and that
increasing the cytosolic Ca2+ concentration might benefit the stability
and the integrity of the cell membrane and cell wall and sequentially
alleviate the injury of oil sunflowers against sodic stress. Wang et al. [7]
conducted a pot experiment to study the union response of sunflower
biological indicators (height, leaf area and dry matter weight), physio-
logical indicators (photosynthesis rate,transpiration rate and stomata
conductance) and yield to soil water content, soil salinity and soil
J. Wang, P. Yang Renewable and Sustainable Energy Reviews 82 (2018) 1969–1978

Table 5
Effects of FGD gypsum on growth and yield, and the sources of soil nutrients.

Plants Application rate Effects on growth and yield Sources of soil nutrients References

Alfalfa 75.2 Mg ha−1 Increase B Chen et al. [45]

67 Mg ha−1 Increase S Chen et al. [98]
2.5–10% Increase Ca, S, Mg, B and Mn Clark and Baligar [93], Clark and Baligar [101]
28 g kg−1 Increase Ca, Mg and S Stehouwer et al. [50]
18 Mg ha−1 Increase Ca Stout and Priddy [95]
Bean 1–1.5 Mg ha−1 Increase N and S Ivanoca and Pelovski [96]
Canola 22 kg S ha−1 Increase S Desutter et al. [99]
Citrus tree 4.48 Mg ha−1 Increase Ca Alva et al. [92]
Fescue 30–120 g kg−1 Increase Ca, Mg and S Stehouwer et al. [50], Stehouwer et al. [94]
2.5–10% Increase Ca, S, Mg, B and Mn Clark and Baligar [93], Clark and Baligar [101]
Maize 33 kg S ha−1 Increase S Chen et al. [5]
23 Mg ha−1 Increase B Chun et al. [40]
5 g kg−1 Increase B Clark et al. [100]
1–10% Increase B, Se and Mo Knox et al. [105]
20 Mg ha−1 Increase Ca and S Kost et al. [91]
Orchardgrass Saturated aqueous solution Increase Mg Feldhake and Ritchey [103]
Potato 1.5 Mg ha−1 Increase Ca and S Wang and Shi [106]
Soybean 67 Mg ha−1 Increase S Chen et al. [98]
Rice 1.125 Mg ha−1 Increase P, K, Ca, Mg and Si He and Shi [104]
wheat 22.4 Mg ha−1 No effect —— DeSutter et al. [23]
8.8 Mg ha−1 No effect —— Lee et al. [42]
White clover 2.5–10% Increase Ca, S, Mg, B and Mn Clark and Baligar [93], Clark and Baligar [101]

sodicity, and found that crop growth is simultaneously affected by soil
water content, soil salinity and soil sodicity in the process of soil
reclamation. Biological indicators and the yield of sunflowers decreased
with the increase of soil water content, soil salinity and soil sodicity.
The sunflower photosynthesis rate, transpiration rate and stomata
conductance increased with the increase of soil moisture and decreased
with the increase of soil salinity and soil sodicity. Soil salinity is the
dominant factor affecting sunflower yield and biological indicators, and
the effects of soil water content on the sunflower physiological
indicators were more clear than those of the other two factors [7].
5. Risk associated with FGDG application
5.1. Accumulation of toxic trace elements in plants
The effect of FGDG on the uptake/enrichment of toxic trace
elements (As, B, Cd, Cr, Cu, Hg, Mn, Mo, Ni, Pb, Se, Zn) in various
crops have been investigated with the safe uses of crop produced for
human consumption [19,109]. Concentrations of toxic trace elements
added to land, regardless of the source, should be monitored and be
within established standard limits. The changes in concentrations of
trace elements found in plants are listed in Table 6.
FGDG with a large amount of available Si may increase Si content in
roots and reduce the root absorption of heavy metals. It was reported
that the deposition of Si in the vicinity of the root endodermis might
partially physically block the apoplast bypass flow across the roots [110].
The heavy metal sequestration and detoxification are attributed to the
chemical and physical effects of Si on forming co-precipitation with
heavy metals and blocking the metal transfer in plants [111].
Concentrations of B, Se and As did not accumulate significantly in all
of the plant species tested (cotton, corn, soybean and radish crops) in a
greenhouse-based pot study and a large scale mesocosm experiment
[112,113]. No significant difference in the concentrations of Mo, Zn, Pb,
Ni, Cd, Mn, Cr, and Cu in corn leaves was observed between the FGDG
addition and the control [40]. The contents of almost all of the metals (B,
Cr, Mn, Ni, Cu, As, Cd, Pb) in the corn grains in the FGDG plots were
almost the same or lower than those in the control plot [39]. The
concentrations of Cr, Pb, Cd, As, and Hg in the seeds of corn and alfalfa
grown in China were far below the tolerance limits regulated by National
Food Standards of China [24]. After applying FGDG, the concentrations
of Cd, Cr, Cu, Pb, and As in sweet potato were reduced by 31.34%,
70.57%, 22.17%, 79.49%, and 100%, respectively [105]. Tissue Mn, Cu,
Ni, and Zn concentrations decreased from near phytotoxic levels to
normal levels after applying FGDG in mined soils [114].

Table 6
Effect of FGD gypsum on accumulation of toxic trace elements in various plants.

Plants Toxic trace elements References

B As Cd Cr Cu Hg Mn Mo Ni Pb Se Zn

Alfalfa ↑ — — — — — — ↑ — — — — Sloan et al. [115]

— N N N — N — — — N — — Wang et al. [24]
Bean — — — — — N — — — — — — Briggs et al. [118]
Cotton N N — — — — — — — — N — Punshon et al. [112], Punshon et al. [113]
Fescue — — — — ↓ — ↓ — ↓ — — ↓ Bigham et al. [114]
Maize N — N N N — N — N N — N Chun et al. [40]
— ↑ — — — — — ↑ — — — — Knox et al. [105]
N N — — — — — — — — N — Punshon et al. [112,113]
N N N N N — N — — N — — Sakai et al. [39]
— N N N — N — — — N — — Wang et al. [24]
Potato — ↓ ↓ ↓ ↓ — — — — ↓ — — Wang and Shi [105]
Radish N N — — — — — — — — N — Punshon et al. [112,113]
Soybean N N — — — — — — — — N — Punshon et al. [112,113]

Note: ↑ represents increasing the accumulation of the toxic trace elment in plant; ↓ represents decreasing the accumulation of the toxic trace elment in plant; N represents FGD gypsum
having no effect on the accumulation of the toxic trace elment in plant; — represents making no analysis on the accumulation of the toxic trace elment in plant.

1974
J. Wang, P. Yang
However, some studies also showed that the application of FGDG
could increase the accumulation of toxic metals, and using FGDG as a
soil amendment for the purpose of growing agronomic and horticul-
tural crops was not recommended. The elemental concentration of the
maize tissues indicated a characteristic elevation of B, As, Se and Mo
[105]. Alfalfa yields were unaffected by these rates of residue applica-
tions, but shoot concentrations of B in the second cutting and B, Mo in
the third cutting were increased by FGDG applications [115]. Cheng
et al. [116] evaluated the environmental impact associated with the
land application of FGDG by considering the overall mass balance of an
element in a life cycle starting from the coal combustion process to the
stage of land application. The author believed that considering only the
amounts of trace element uptake in surface vegetation may under-
estimate the overall release of the trace elements from FGDG and that
the mobility of trace elements varies when FGDG produced from
different processes were used.
5.2. Accumulation of heavy metals in soils
Although FGDG has become an effective soil amendment for soil
reclamation, it might deposit extra heavy metals into the soil environ-
ment. Some studies showed that FGDG does not contain significant
quantities of heavy metals and that the application of FGDG does not
cause soil contamination [117]. Briggs et al. [118] reported that total
Hg concentrations measured were similar for reclaimed and unclaimed
soils after FGDG application. Chen et al. [26] reported that As and Hg
concentrations in the soils were found to be positively correlated with
FGDG added. Yang et al. [119] conducted a soil column leaching
experiment to analyze the changes in heavy metals from reclaimed tidal
flat soil that used FGDG and found that the highest removal rates of Cd
and Pb in the upper soil layers (0–30 cm) were 52.7% and 30.5%,
respectively. The application of FGDG (two times) and the extension of
the leaching interval time to 20 days increased the heavy metal removal
rate in the upper soil layers. The heavy metals desorbed from the upper
soil layers were re-adsorbed and fixed in the 30–70 cm soil layers
[119]. Although there might be a slight increase in heavy metals, the
concentrations of Cr, Pb, Cd, As, and Hg in the treated soils are far
below the background values stipulated by the Environmental Quality
Standard for Soils (GB 15618-1995) [27,120]. Chen et al. [45] reported
that No soil contamination problems were observed even at high
application FGDG rates and that it can be safely applied to agricultural
soils. Chun et al. [40] also reported that no significant differences in the
concentrations of Mo, Zn, Pb, Ni, Cd, Mn, Cr, Cu, and Al in sodic soils
were observed between the FGDG addition and the control. Chen et al.
[48] found that compared to the conventional reclamation, Ca, S, B,
and Zn concentrations at 0–20 cm depth were generally increased by
the treatments with FGDG at a 280 Mg ha−1 application rate in an
abandoned surface coal mine in Ohio, while other trace metals
measured were generally not increased in short or long term measure-
ments.
As FGDG brings significant amounts of Ca2+ and SO42− to the soil, it
could affect the Pb sorption by Ferrihydrite and humic acid in soil.
Therefore, FGDG has the potential use as an in situ Pb stabilizer in
contaminated soils. The previous study showed that FGDG effectively
reduced the Pb leaching in two contaminated soils under leaching
conditions [121].
5.3. Effects of toxic trace elements on water quality
There are growing concerns regarding the effects of toxic trace
elements on water quality when FGDG is applied to agricultural fields.
Applying FGDG into acid forest soils has the potential to provide
growth benefits to a commercially important tree species (red oak), but
care would need to be taken to avoid the release of toxic levels of B.
Crews and Dick [9] reported that S concentration increased from less
than 10 mg l−1 to 234 mg l−1 in the leachate in four months after the
1975
Renewable and Sustainable Energy Reviews 82 (2018) 1969–1978
application of FGDG and that B also approached toxicity concentra-
tions (≈ l mg l−1) in the leachate from the soil treated during the initial
leaching but that the concentrations tended to decline with time.
Punshon et al. [113] conducted a greenhouse-based pot study and a
large scale mesocosm experiment and found that leachate pH was
unaffected by FGDG but that salinity rose sharply with increasing
application rates of FGDG. Moreover, leachates contained higher
concentrations of B with small increases in Se and As. While concerns
about heavy metal leaching are not without basis, concentrations of B,
Se and As do not exceed drinking water standards [112,122].
For the effects on surface water, Chen et al. [76] reported that the
concentrations of Ca, S and B in surface runoff generally increased by
the treatments with FGDG in both short- and long-term measurements
in a field plot experiment and that the concentrations of the trace
elements were generally not statistically increased in surface runoff
over the 20-year period. Stehouwer et al. [49] reported that leachate
pH, EC, dissolved organic C, Ca, Mg, and S tended to increase with the
increasing application rate of FGDG in a leaching experiment of mine
soils, and with FGDG of 120 g kg−1 or less, leachate concentrations of
most elements of environmental concern were less than the levels
mandated by drinking water standards. The amount of FGDG that can
be applied to mined soils is probably limited by soluble salts and
initially high pH levels rather than by the trace element loading of soil
or water [49]. Jenkins et al. [123] reported that FGDG applications
may be a management practice that reduces microbial contamination
of surface waters from manure applied to agricultural fields in the
southeastern United States. Salmonella was not detected in the runoff,
and after 3 years of FGDG applications, the highest rate of FGDG
resulted in decreased flow-weighted concentrations and total loads of
Escherichia coli. Torbert and Watts [124] carried out a rainfall
simulation to examine the impact of FGDG application on runoff
nutrient losses and found that a maximum of 61% reduction in soluble
reactive P concentration in runoff with the application of 8.9 Mg ha−1
FGDG and the concentrations of heavy metals in runoff were all found
to be below detection limits.
6. Conclusions
Annual production of FGDG will increase considerably as more
coal-fired power plants come online and as SO2 scrubbers are added to
existing power plants to comply with the rules on clean air. The
potential of FGDG as a resource material in agriculture is now a well-
established fact. In view of the fear of significant harm to the mind,
such as the presence of toxic heavy metals in FGDG and leaching
problems, it is necessary to involve FGDG more effectively in agricul-
ture to exploit its various physical and chemical properties fully, which
are beneficial for soil and crop health. According to the above
discussion, the key points from this comprehensive review can be
summarized as follows:
(1) Advantages and benefits
(i) The potentiality of FGDG for its utilization in agriculture is
becoming popular because it contains a large number of essential
nutrients for plant growth, i.e., macronutrients including Ca, S,
Fe, Mg and K and micronutrients such as Se, Mn, Zn, Cu, B and
Mo.
(ii) FGDG can effectively reclaim degraded soils, including saline and
sodic soil, acid soil and mined soil; however, it cannot be a
substitute for chemical fertilizers or organic manure. Applying
FGDG can improve physicochemical properties of degraded soils,
promote plant growth and improve crop quality.
(iii) The use of FGDG as a soil ameliorant can reduce net CO2 and SO2
emissions and thereby improve environmental quality and reduce
global warming. Moreover, applying FGDG can reduce the move-
ment of sediment, nutrients, and agricultural chemicals to surface
J. Wang, P. Yang
water and improve water quality. FGDG seems to have the
greatest promise of providing agricultural benefits with minimal
negative impacts on the environment.
(2) Disadvantages and risks
(i) In spite of some advantages of using FGDG in agriculture, many
should be concerned due to its heavy metal content even if studies
have proven that it is safe if FGDG is being applied in regular
quantities and be allowed for the distribution of heavy metals in
different release pathways (i.e., air emission, uptake in grass, and
soil leachate).
(ii) As is the case with fertilizers and any other agricultural inputs, the
amount, time and method of FGDG application vary with the type
of soil, the crop to be grown, the prevailing agro-climatic condi-
tion and the type of FGDG available. However, relative research
on these aspects is lacking and need to find a more effective
utilization of FGDG.
(iii) Although FGDG contains some beneficial trace elements for plant
growth, the accumulation of trace elements also causes toxicity,
and the excessive application of FGDG may lead to the accumula-
tion of salts and thus affect the plant growth.
(3) Outlook and suggestions
(i) There are significant areas of degraded soils in the world that
could benefit from the application of FGDG. Therefore, the
application of FGDG in agriculture has a vast range of prospects.
However, the benefits and risks for specific agricultural uses of
FGDG will need to be determined, and some guidelines should be
formulated for these specific uses developed.
(ii) In the future, attention should be given to some important areas
related to FGDG utilization, such as the proper handling of FGDG
in plants as well as in fields, the effective duration under different
application conditions, long-term studies of the impact of FGDG
on soil health, crop quality, and continuous monitoring of the
characteristics of soil as well as FGDG.
(iii) FGDG has its own limitations; combining application with other
materials, i.e., fly ash, microbial inoculum, organic acid and so on
should be considered. Moreover, the application field in agricul-
ture should also be expanded to reduce the amount of FGDG that
need to be disposed of or sequestered long-term in landfills.
Acknowledgments
This research was supported by National Natural Science
Foundation of China (50749032) and the Fundamental Research
Funds for the Central Universities of China (2652015179,
2652015336).
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