Materials Science in Semiconductor Processing 120 (2020) 105256

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Materials Science in Semiconductor Processing

journal homepage: http://www.elsevier.com/locate/mssp

Review

Recent development on BN-based photocatalysis: A review

Xinyu Gao, Yuan Yao, Xiangchao Meng *
Key Laboratory of Marine Chemistry Theory and Technology (Ministry of Education), College of Chemistry & Chemical Engineering, Ocean University of China, Qingdao,
Shandong, 266100, China

A R T I C L E I N F O A B S T R A C T

Keywords: As a variety of graphene analogue, boron nitride (BN) semiconductor has attracted widespread attention due to
BN its unique physiochemical properties. Among various applications of BN, photocatalysis has become a focus of
Graphene research. In essence, BN contains a wide band gap (~5.5 eV), which makes it extremely challenging to achieve
Photocatalysis
direct activation by light photons. Instead, BN could serve as a co-catalyst, as it has the capability to promote the
Two-dimensional materials
photocatalytic activity of the support. In general, the low quantum yield caused by the high recombination rate
of photogenerated charge carriers presents a tough challenge to the commercialization of photocatalysis. BN-
enhanced photocatalysis provides a flexible solution to the above-mentioned problem. Moreover, there have
been a variety of different BN-based composites reported and applied in photocatalysis, which is part of the
review conducted in this paper. In addition, the properties of BN, the approaches to experimental preparation of
BN as well as the recommendation for future work are also indicated and discussed.

1. Introduction outstanding thermal conductivity, high thermal stability, excellent

Recently, the exploration of alternative, sustainable energy sources
and environmental remedies has become a significant subject of dis­
cussion around the world [1,2]. Semiconductor photocatalysis repre­
sents a technology applied to make full use of solar energy while solving
environmental crisis [3–8]. When the energy of a light photon exceeds
the semiconductor band-gap value, valence electron can be activated
and transferred to the conduction band, thus resulting in the separation
of electron-hole [9]. The migration of these charge carriers from the bulk
to the surface of the photocatalyst can further trigger a string of redox
reactions [10,11]. As for the extensive applications of photocatalysis, a
major constraint is the high photon-energy required for the activation
and low quantum yield, which results from the large band gap of a
semiconductor and the high recombination of photogenerated charge
carriers, respectively [12,13]. In order to address these issues, the for­
mation of heterojunctions has been validated as an effective solution.
Among these reported works, hexagonal boron nitride (h-BN) has been
applied in photocatalysis to enhance the photocatalytic activity, which
attracts increasing attention.
Hexagonal boron nitride (h-BN) is known as a two-dimensional non-
metal material with a similar structure to graphite, as a result of which it
is also named as ‘white graphene’. Besides, h-BN exhibits such advan­
tages as a high degree of mechanical strength, massive surface area,
electrical conductivity, lubricity and high adsorption capacity [10,
14–17]. Due to its wide band gap of 5.5 eV, the application of h-BN in
photocatalysis is restricted to the UV irradiation with a wavelength of
less than 310 nm [15,18]. However, there have been some studies
suggesting that the coupling of BN with other semiconductors is effec­
tive in obtaining the composites with higher photocatalytic activity,
which could improve the degradation rate of organic pollutants
[19–22]. In this paper, systematic introduction and summary are made
of BN-enhanced photocatalysis. Moreover, the future directions are
indicated for the further research focusing on this field.
2. Properties of BN
With regard to crystal structure, BN shows a high level of similarity
to carbon and has four typical types, which are graphite-analogue hex­
agonal BN (h-BN), diamond-analogue cubic BN (c-BN), rhombohedral
BN (r-BN) and wurtzite BN (w-BN). Among them, c-BN and w-BN exhibit
a low-density phase with sp3 hybridized B–N bonds. By contrast, h-BN
and r-BN display a high-density phase with sp2 hybridized B–N bonds
[23]. Based on these types, the crystal structure of boron nitride is
illustrated in Fig. 1.
In comparison with the other three types of crystal structure, h-BN
has drawn most attention. The B–N bonds in BN layers are even stronger

* Corresponding author.
E-mail address: mengxiangchao@ouc.edu.cn (X. Meng).

https://doi.org/10.1016/j.mssp.2020.105256
Received 9 February 2020; Received in revised form 29 May 2020; Accepted 6 June 2020
Available online 12 July 2020
1369-8001/© 2020 Elsevier Ltd. All rights reserved.
X. Gao et al.
Fig. 1. Structures of the sp3-bonded phases c-BN and w-BN, and the sp2-bonded
phases h-BN and r-BN (Adapted from Ref. [24]).
than the C–C bonds in graphene, which make BN has high hardness
(15–24 kg mm 2), high conductivity (~6600 W m K 1), remarkable
mechanical strength, good elasticity, high thermal stability, high
chemical stability and anti-oxidation under high temperature [25,26].
Compared with other traditional materials such as silicon nitride and
Fig. 2. Optical image of an array of graphene transistors with device schematic (Adapted from Refs. [30]).
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Materials Science in Semiconductor Processing 120 (2020) 105256
aluminum nitride, BN exhibits good electrical insulation. This property
of BN allows some electrical leakage phenomena to be effectively
avoided [27]. In addition, the high specific surface area and special edge
structure of BN also make it appealing in wide range of applications such
as nanoelectronic, optoelectronic and nanocomposites [25].
By taking advantage of the large specific surface area and high
adsorption capacity of BN, Lei et al. prepared boron nitride nanosheets
with a porous structure [28]. The nanosheets of this kind proves effec­
tive in removing oil, organic solvents and dyes from water. The
adsorption capacity of BN nanosheets is even superior to those
commonly-used commercial and state-of-the-art adsorbents. Due to the
super-high hydrophobicity, porous BN nanosheets are capable of selec­
tively decomposing oil, organic solvents and dyes, which allows for its
extensive applications in such fields as water purification and treatment.
Zhi et al. made a discovery in their study that the composite of BN
nanosheets and PMMA has the capability of improving the thermal
expansion coefficient and enhancing the tensile properties of the ma­
terial. It was speculated that this phenomenon is attributed to the
combined effects of the flake topology caused by the peeling distortion
and the polarized surface formed between the two materials. In addi­
tion, some organic functional groups which are potentially presented on
the surface of BN nanosheets may also play a role in promoting the
interaction between BN and other material interfaces. Therefore, BN
nanosheets are supposed to be applied in the fabrication of optoelec­
tronic devices, composite optical windows and heat-releasing materials
through composite modification [29].
The interfacial properties of graphene/h-BN are extraordinary, and
the regions with different atomic compositions may coexist in contin­
uous films, which allows it to have the potential of exhibiting electrical
properties. Levendorf et al. applied the patterned regrowth technique to
prepare the layered materials which can go beyond h-BN and graphene
and can be applied in atomic thin circuits, as shown in Fig. 2. The
atomic-level electrical components in design could be manipulated to
form complex devices at the ultimate thickness limit after stacking [30].
Kubota et al. synthesized BN crystals with deep ultraviolet light­
–emitting properties under atmospheric pressure successfully, which
X. Gao et al.
Fig. 3. (a) Electronic band structures of BN and several materials (Adapted from Ref. [36]); (b)Energy band structure of several two-dimensional materials (Adapted
from Ref. [26,37]).
have also been commonly used in such fields as information storage,
environmental preservation and medical treatment [31].
In addition, due to the possibility of two-dimensional (2D) [26,32]
h-BN being either wrapped up into BN fullerenes (0D) [33] or rolled into
BN nanotubes (BNNTs, 1D) [34], h-BN is considered as promising to
enhance photocatalytic activity [23].
3. BN in photocatalysis
3.1. Light responsivity
As for the inherent properties, BN can be regarded as a semi­
conductor for applying in photocatalysis. However, the band gap width
of BN is excessively wide (5.0–6.0 eV) [26], as a result of which the
activation of BN can only be achieved by the light with a wavelength of
less than 310 nm [35]. Fig. 3 shows the electronic band structure of BN
and the bandwidth comparison between h-BN and several typical pho­
tocatalytic materials [26,36]. Due to the high levels of oxidation resis­
tance, chemical inertness, high thermal conductivity, high melting point
and massive specific surface area, h-BN is expected to be applied as an
excellent co-catalyst for improved photocatalytic activity of the support
[15]. Table 1 indicates some of the reported semiconductor/BN com­
posite catalysts and their applications. In addition, the characteristics of
several commonly-used semiconductor photocatalysts with BN modifi­
cation would be discussed in detail.
3.2. Modulation of energy band to improve the visible-light sensitivity of
BN
3.2.1. Modulation of energy band by sculpting of external electric fields
As reported, the band gap width of BN can be reduced by applying an
electric field [76]. The band structures of BN with either a positive or a
negative electric field were simulated, as shown in Fig. 4. Within the
positive electric field, the energy band of the first layer is bent down­
ward while the second layer remains unchanged basically. This phe­
nomenon ended up leading to a narrowed band gap, suggesting that the
largest valence band shows N-pz features from the second BN layer,
while the smallest conduction band displays the first layer B-pz features.
Similar results were also obtained from BN when negative electric fields
were imposed, which indicates that the applied electric field was
capable to adjust the band gap of the BN bilayer film. In the process of
applying electric field that changed from 0 a.u. (atomic units, 1 a.u. ¼
5.14225 � 1011 V/m) to 0.015 a.u., the band gap of the BN double-layer
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Materials Science in Semiconductor Processing 120 (2020) 105256
film was reduced from 4.45 eV to 0.3 eV. In addition, it was speculated
that the highest valence band and the lowest conduction band of the
double-layer membrane were comprised of N-pz and B-pz from the two
layers, respectively, which suggests that the electron-hole pairs were
well separated in photocatalysis. Also, it was suspected that this phe­
nomenon was attributed to the change in band structure, which resulted
from the potential difference under the electric field applied [76].
3.2.2. Modulation of band gap by doping
Heteroatom doping is considered as one of most effective methods of
modification to improve photocatalytic activity. The introduction of
heteroatoms is equivalent to adding a new energy band into the original
band gap. The impurity energy band can be viewed as either the top of
the valence band or the bottom of the conduction band, thus reducing
the band gap energy [77]. So far, a variety of heteroatoms (such as O, N,
B, S, etc.) have been successfully doped into graphene. Compared to
single element doping, the doping of two or more different elements can
lead to the generation of a unique electronic structure between different
heteroatoms. Due to the synergistic coupling effect, it is possible for the
photocatalytic ability of the material to be further improved [78].
Focusing on the properties of BN-doped graphene, Li et al. synthe­
sized the graphene decorated with in-plane h-BN domains (denoted as
BN-G), B and N singly doped graphene (denoted as B-G and N-G,
respectively) and B & N co-doped graphene (denoted as B, N-G), where
G refers to graphene. As shown in Fig. 5, this doping effect can reduce
the band gap width significantly [78].
Chen et al. proposed BCN-melamine borate, BCN-melamine phos­
phate borate, BCN-boric acid and BCN-boron oxide and discovered that
the doped materials could perform better in photocatalytic activity. As
being revealed by the experimental results, the band gap energies of
these four materials reached 1.54 eV, 1.99 eV, 1.09 eV and 1.01 eV,
respectively [79]. Feng et al. conducted investigation into the impact of
different reaction times on the performance of doped semiconductors by
doping sulfur (S) into BN. In the prepared S-BN, the smallest band gap
energy amounted to 2.77 eV [80]. In the process of doping the BCN
nanosheets with metal, Ri et al. denoted the samples as xGlu-Me, where
x refers to the weight percentage of glucose (Glu) and boron oxide while
Me represents alkaline earth metal. The result was obtained to suggest
that the band gap energies of xGlu-Ca (x ¼ 20, 30, 40) samples reached
2.85 eV, 2.53eV and 1.91 eV and those of 20 Glu-Me (Me ¼ Mg, Sr, Ba)
samples amounted to 2.70 eV, 2.75eV and 2.83 eV [81]. By doping a
variety of non-metallic elements into BN, Wang et al. achieved the
modification to its electronic structure. Concerning weakly
X. Gao et al. Materials Science in Semiconductor Processing 120 (2020) 105256

Table 1
Overview of application of BN modified semiconductor photocatalyst.
Photocatalyst Application Light type Efficiency Irradiation time Ref.

BN-TiO2 Degradation of Rhodamine B (RhB) and UV light 91.2% & 72.1% 20 min [38]
methylene blue (MB)
Degradation of MB Visible light 79% 200 min [39]
Degradation of methyl orange (MO) UV light 99% 75 min [40]
Degradation of RhB Visible light 99% 360 min [35]
Degradation of Reactive Yellow 161 (RY161) Simulated sunlight 100% (hydrolyzed) 160 min [41]
(300–800 nm)
Degradation of RhB and MB UV light 98% & 92% 50 min [42]
Degradation of ibuprofen UV light 98% 180 min [43]
Degradation of Lanaset Red 2B (LR2B) and Simulated sunlight 82.5% & 38.4% 180 min [14]
hexavalent chromium (Cr (VI))
1
Photocatalytic oxidations of acetic acid and Visible light About 2.9 μmol h & 0.08 μmol / [44]
crystal violet (CV) h 1
TiO2-xNx/BN Degradation of RhB Visible light 97.8% 40 min [45]
BN3–Ag3/TiO2 Degradation of MB Visible light 85% 80 min [46]
BN5–Ag3/TiO2 Degradation of MB Visible light 98% 80min [46]
Au/TiO2/BN Degradation of CV Visible light 10.3 μmol h 1 / [47]
Boron carbon nitride tubes Catalyse hydrogen evolution from water Visible light 2.8 μmol h 1 / [48]
(BCNTs)
Carbon nitride modified BN Degradation of enrofloxacin (ENFX, ENR) Visible light Observed Kinetic rate constant / [15]
(CMBN) (Kobs) ¼ 0.095 min 1
The ternary 2D h-BCN Convert benzene into phenol Visible light 14% (selectivity 88.3%) 120 min [49]
nanosheets
0.9% g-BN/g-C3N4 Degradation of bisphenol A (BPA) Visible light 91.9% 150 min [50]
BN/CN Degradation of RhB and MO Visible light Kinetic rate constant (K) ¼ 2.09 180 min [51]
h 1 & 1.19 h 1
CN–CNB-25 Degradation of MO and phenol Visible light 93% & 57% 120 min [52]
BCN–F Conversion of CO2 into CO Visible light 155 μmolg 1h 1 / [53]
CN/BN Production of H2 and H2O2 UV light 14.5 μmol & 2.8 mM 240 min [16]
B–SSCN Photocatalytic hydrogen generation Visible light 9.1 μmol h 1 / [54]
g-C3N4/PDI-BN-rGO Production of H2O2 Visible light The apparent quantum yields (ΦAQY) 120 min [36]
¼ 7.3%
h-BCN Dehydrogenation of N-heterocycles Visible light 79% (in H2O) 720 min [55]
h-BN/g-C3N4 Degradation of antibiotic tetracycline (TC) and Visible light 79.7% & 99.5% 60 min& 40 min [56]
RhB
BCN Degradation of RhB and MB Visible light 99.3% & 98.9% 90 min [57]
B-doped g-C3N4 Degradation of RhB and MO Visible light 98%& 80% 40 min & 300 min [58]
BCN nanocomposites Degradation of RhB UV light & visible light 97% & 95% 120 min [18]
BCN Benzyl alcohol oxidation Visible light ~70% (selectivity ~88.3%) 240 min [59]
BN/BiOBr Degradation of colorless antibiotic agent Visible light 81.5%, ~70% & 99% 80 min, 80 min & [60]
ciprofloxacin (CIP), TC and RhB 30 min
BN/oxygen vacancies- Degradation of RhB and BPA Visible light 58%& 72% 30 min& 140 min [61]
BiOCl
BN-Bi2MoO6 Degradation of RhB Visible light Almost 100% 120 min [62]
BN-BiOI Degradation of MO Visible light 86% 180 min [19]
h-BN/Bi4O5Br2-LMs Degradation of 4-tert-Butylphenol (PTBP), Visible light 97%, 50% & 90% 150 min, 180 min & [63]
Acetaminophen (paracetamol, 5 min
N-acetyl-para-aminophenol [APAP]) and
Norfloxacin (NOR)
BN/Bi4O5I2 Degradation of BPA Visible light 97% 20 min [21]
BN/BiPO4 Degradation of ENR UV light 91.5% 120 min [20]
BN/BiOCl Cr (VI) photoreduction Visible light 91.7% 140 min [64]
BN/Bi2WO6 Degradation of RhB Visible light 98.2% 100 min [17]
BN/BiOI Degradation of RhB Visible light 93% 100 min [65]
BN/BiOBr Degradation of RhB Visible light ~100% 60 min [66]
BN/Ag2CO3 Degradation of RhB Visible light 96.5% 60 min [67]
Ag3PO4/h-BN Oxygen evolution reaction Visible light ~28 μmol/L 35 min [68]
h-BN/Ag3VO4 Degradation of RhB Visible light 96.3% 90 min [69]
AgI-BN Degradation of RhB Simulated sunlight 96.17% 70 min [70]
BN/Ag3PO4 Degradation of RhB Visible light 97% 12 min [71]
BN/AgBr Degradation of MO Visible light 80.24% 15 min [22]
AgI/AgBr/h-BN Degradation of RhB and MO Visible light 97.4% & 95.1% 6 min [72]
Ag2CrO4/FBNNS Degradation of RhB Visible light 96.7% 120 min [73]
SnS2/FBNNS Degradation of RhB Visible light 93.7% 210 min [74]
h-BN/ZnO Degradation of RhB and MB UV light 82% & 60% 20 min [75]

electronegative elements, the band gap energies of Si-BN, P-BN and
C-BN declined to 4.51 eV, 3.45 eV and 3.69 eV, respectively. As for the
elements with a higher level of electronegativity, the band gap energies
of Cl-BN, O-BN and F-BN can be reduced to as low as 2.09 eV, 2.49 eV
and 2.21 eV, while the change can reach above 2 eV [82]. After pre­
paring S-doped h-BN nanosheets, Zhao et al. found out that the band gap
energy of S-boron nitride nanosheets (BNNS) was 4.13 eV, which is more
than 1 eV lower than that of BNNS alone (5.36 eV). Therefore, the effect
of doping on the band structure is self-evident [83].
3.2.3. Modulation of energy band by sculpting of h-BN fragments
Du et al. conducted study on h-BN monolayer materials by removing
a single B or N atom, which led to the findings that the three N–N po­
sitions at the B-type vacancies were asymmetric, the distance was

4
X. Gao et al.
Fig. 4. Band structures of the BN bilayer under an external electric field: (a) for
positive electric field, (b) for negative electric field (Adapted from Ref. [76]).
greater than that in pure h-BN, while the B–B position was symmetrical,
the distance was smaller than that in pure h-BN. In addition, B-type and
N-type vacancies were both ferromagnetic with a magnetic moment of 1
μB. As indicated by the Spin-resolved density of them, their magnetic
charge density is clearly concentrated on the vacancy edges.
Based on the magnetic moment enhancement and spin filtering po­
tential caused by the vacancy defects to this h-BN single-layer material, a
further study was conducted on it, which led to a discovery that trian­
gular nanopores of different types were conducive to enhancing mag­
netic moment. Such a strong magnetism can be attributable to the
dangling bonds of the atoms at the zigzag edges. Then, a further inves­
tigation was conducted into the properties of h-BN with regularly spaced
triangular vacancy defects. It was found out that this sort of antidot
super lattice structure exhibited not only a high lattice compression ratio
but also various geometric optimization properties. As shown in their
plots of the spin-resolved density of states (DOS), the formation of such
triangular vacancies can effectively reduce the band gap of the material
(as shown in Fig. 6). Therefore, the etching of h-BN nanosheet provides a
potential solution to adjust its band gap [84].
3.2.4. Modulation of energy band by controlling the morphology of the h-
BN
Wang et al. achieved a success in the fabrication of hexagonal boron
nitride submicro-boxes (BNMB), the size of which usually ranges from
0.5 to 1.4 μm. As shown in Fig. 7, the prepared BNMB presents itself as a
Fig. 5. (a) Total and partial electronic density of states (TDOS and PDOS, respectively) of BN-G (The Fermi level is set at 0 eV); (b) Calculated band gaps of G, B-G, N-
G, B,N-G, BN-G and h-BN (Adapted from Ref. [78]).
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Materials Science in Semiconductor Processing 120 (2020) 105256
polycrystalline hollow microbox [85]. The specific surface area of BNMB
is roughly 86.9 m2/g, which is larger than that of commercial h-BN
(~25.3 m2/g). Besides, the SnO2/BNMB material combined with SnO2
displays a superior performance in visible light response and less band
gap energy compared to single SnO2 and SnO2/Al2O3, as shown in Fig. 8.
Moreover, the photocatalysis test for the degradation of MO reveals that
this h-BN with an exceptional morphology could show an enhancement
of catalytic activity [85].
3.3. Co-catalyst to enhance photocatalytic activity
Co-catalyst loading is effective to improve the photocatalytic activity
of photocatalysts [86–92]. With the loading, the separation efficiency of
photogenerated charge carriers, the number of exposed active sites and
the light harvesting capacity could be greatly enhanced [93]. BN as a
co-catalyst exhibits excellences to enhance photocatalytic activity. Fig. 9
lists several mechanisms of promoting photocatalytic activity when BN
is used as a co-catalyst [17,38,45,63]. These situations may exist alone,
or they may cooperate to enhance the photocatalytic performance.
3.3.1. TiO2-BN
Due to such advantages as high optical, biological, electronic prop­
erties, chemical inertness, stability, nontoxicity, environmental friend­
liness, low cost and commercial availability, Titanium dioxide (TiO2)
has been commonly applied as semiconductor in photocatalysis [42,43,
46,47,94–96]. TiO2-based semiconductor as one of the most typical
composite photocatalysts ha been met with widespread applications for
example, environmental remediation and solar energy conversion [38,
39]. To be specific, they play an active role in dye-sensitized solar cells,
gas sensors, biofuel cells, biomaterials and the removal of toxic organic
compounds from waste water [45,97–100]. Nevertheless, pure TiO2
manifests itself as a wide band gap (Eg ¼ 3.2 eV [45]) semiconductor and
can be excited only through UV irradiation, which accounts for merely
3–4% of the solar light. Therefore, it is very difficult to realize its
application in direct sunlight. In addition, the high rate of excited
electron-hole recombination of TiO2 imposes a major restriction on its
photocatalytic reaction efficiency [39,45,101]. To solve the aforemen­
tioned problems, TiO2 semiconductors are normally used in combina­
tion with other semiconductor materials. Recently, the research
conducted on TiO2/graphene nanosheet composite materials has pro­
vided inspiration for the development of TiO2-BN composites [14].
Compared to graphene, hexagonal boron nitride (h-BN) sheets not only
show similar characteristic structure and lattice parameters to graphene,
but also exhibit unique properties due to their massive surface area and
reactive edge structure. In this study, it was suggested that the intro­
duction of BN nanosheets could improve the separation of electron-hole
X. Gao et al.
Fig. 6. Spin-resolved total density of states corresponding to (a) a perfect 10 �
10 h-BN monolayer; (b) B-terminated antidot super lattice; (c) the N-terminated
antidot super lattice (Adapted from Ref. [84]).
(e -hþ) pairs of TiO2. Fu et al. proposed that the ball-milled BN nano­
tubes with poor conductivity exhibited negative chargeability. Recom­
bining them with TiO2 can effectively move the holes inside TiO2 to
surface and improve the catalytic efficiency [38]. In addition, in the
TiO2-BN composite, the B–O–Ti–O bonds can also reduce the band gap
(Eg ¼ 2.95 eV) to enhance its photocatalytic performance. Up to now, BN
has already been proven as an excellent support for TiO2 [35,41]. There
have been reports on the degradation of MO using TiO2-BN composites.
In this paper, the degradation of MO is exemplified, as shown in Fig. 10,
which reveals that the composites are more capable of photocatalytic
activity than TiO2 alone or even P25 semiconductor materials under UV
light [40]. In addition, the application of TiO2-BN composite materials
in the photocatalytic degradation of dyes (Rhodamine B [38], methylene
blue [39], RY161 [41] and methyl orange [40], etc.) and heavy metals
(Cr (VI) [14]) has been reported as well.
3.3.2. C3N4-BN
Non-metallic graphite carbon nitride (g-C3N4) has attracted a great
deal of attention for research as a novel type of photocatalyst, due to its
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Materials Science in Semiconductor Processing 120 (2020) 105256
highly desirable properties such as stable chemical properties, non-
toxicity, abundance, cheap affordability and environmental friendli­
ness [102]. Apart from that, g-C3N4 is capable to be prepared through
the polycondensation of various nitrogen-rich organic precursors, for
example, cyanamide, dicyandiamide, melamine, urea and thiourea
[103–106]). It displays an approximate band gap (about 2.7 eV) and the
capability to absorb light when the wavelength is below 460 nm [15].
The g-C3N4 has demonstrated excellent photocatalytic activity in the
splitting of environmental remediation wand water [15,50,51,56,107].
Similar to most organic semiconductors, however, g-C3N4 shows such
drawbacks as a narrow range of visible light response, small surface
area, slow-paced charge transfer and high recombination rate of
photo-generated electron-hole pairs, which severely restricts its photo­
catalytic performance [50]. At present, there have been reported that
the coupling with other co-catalysts (such as Ag2O and BiOI [108,109])
to construct semiconductor heterojunctions is one of the effective ways
of improving the separation of photogenerated electron-hole pairs for
enhancing catalytic activity. In spite of this, these composite materials
remain possible to cause detrimental metal emissions in practice [15,50,
52].
Recently, BN has been applied as an electron transfer channel to
promote the separation of photo-induced charge carriers [110–113]. In
particular, due to the similarity in size and the chemical properties of
carbon atoms, the modified g-C3N4 is effective in acting as a replacement
for carbon atoms in the CN skeleton with boron. The combined ternary
non-metallic materials are known as boron carbon nitride (BCN) [16,51,
53,54,56,58,114].
This sort of BCN material has displayed the advantages of both
graphene and h-BN, in addition to exhibiting an adjustable band gap
(0–2.45 eV, depending on the stoichiometry [58]) due to the formation
of heterojunctions and excellent visible light response, which makes it
widely applicable in various fields, for instance, electronics, lumines­
cence and hydrogen storage. Jiang et al. found that the metal-free het­
erojunction formed between h-BN and g-C3N4. The formation of
heterojunction promoted the separation of photogenerated charge car­
riers [56]. Ternary BCN compounds can be prepared with various
morphologies, such as nanotubes [115], nanosheets [116], nanopore
structures [117] and fibers [28]. Fig. 11 shows BCN with a variety of
different microstructures. As a novel type of light harvester for the
sustainable utilization of solar energy, BCN has been suggested for the
research on not only photocatalytic hydrogen production but also the
decomposition of organic pollutants [18,48,49,53,59]. For example,
Zheng et al. applied BCN to conduct the dehydrogenation of N-hetero­
cycles under visible light in H2O. After 720 min of irradiation, the
removal rate reached 79% [55]. Kofuji et al. employed g-C3N4/ pyro­
mellitic diimide (PDI)-BN-reduced graphene oxide (rGO) to photosyn­
thesize H2O2 under visible light, which led to a 7.3% yield of apparent
quantum for the generation of H2O2 through irradiation of mono­
chromated 420 nm light [36].
Nevertheless, the preparation of the existing boron-modified g-C3N4
remains subject to some constraints, including complicated reaction
process, high calcination temperature (>500 � C), difficulty to control
the reaction process etc. Therefore, it is imperative to find a simple,
feasible and energy-efficient method to address these issues.
3.3.3. Bi-BN
Bismuth-based semiconductor (BBS) is a variety of promising pho­
tocatalytic semiconductor to enhance photocatalysis [77,118–126]. As a
significant part of BBS, bismuth oxyhalides (BiOX, X ¼ Cl, Br or I) exhibit
excellent visible light catalytic activity, which is attributed to their high
specific surface area, suitable energy band positions, high photocatalytic
activity, remarkable chemical stability and environmental-friendliness
[60,65,66]. BBS could be present in various forms like mesoporous,
nanospheres and nanoflakes [66]. The structure of [Bi2O2]2þ slabs is
intertwined with double slabs of halogen atoms, which could lead to the
generation of the self-built internal static electric fields, thus promoting
X. Gao et al. Materials Science in Semiconductor Processing 120 (2020) 105256

Fig. 7. (a) TEM image of a microbox; (b) SEM image of a microbox; (c) HRTEM image and SAED image of a part of a microbox; (d) Low magnification SEM and TEM
image of a microbox group; (e) SEM image of the broken hollow microbox after sonication (Adapted from Ref. [85]).

the photogenerated electron-hole pairs in an efficient way. Moreover,
this structure displays highly desirable anisotropic electrical, magnetic
and optical properties [63]. Among these BiOX photocatalysts, BiOI
exhibits the most satisfactory capability of light absorption due to the
minimum band gap (1.7–1.8 eV) [65]. In addition, bismuth-based oxy­
acid-type photocatalyst (such as BiPO4 [20], Bi2MoO6 [62] and BiWO6
[17]) exhibits strong photocatalytic activity and excellent chemical
stability. Among them, Bi2MoO6 has a suitable band gap (~2.6 eV) for
visible light-responsive (VLR) photocatalysis [62]. In many cases,
however, the above-mentioned BBSs encounter such problems as low
light absorption efficiency, low response and low adsorption capacity
under visible light irradiation. The band gaps of some BBS are exces­
sively narrow to the extent that it is impractical to improve the sepa­
ration of photogenerated charges carriers, which restricts its practical

7
X. Gao et al. Materials Science in Semiconductor Processing 120 (2020) 105256

adaptation and build intimate heterojunctions to reduce electron

transfer barriers and finally accelerate charge transfer. This phenome­
non also enhances the photocatalytic activity of the composite material
[63].
In addition to this, Liu et al. applied BN-BiOI to achieve the degra­
dation of RhB under visible light. After 100 min of irradiation, the
degradation rate reached 93% [65]. In the degradation experiment
conducted on ENR under UV light, Chen et al. applied BN-BiPO4 as the
photocatalyst, which led to a 91.5% rate of ENR removal for as long as
120 min [20]. These results prove that the combination with BN is
effective in improving the performance of BBS.

3.3.4. Ag compound-BN
Silver-based semiconductor (such as AgI [22], Ag3PO4 [71], Ag2CO3

Fig. 8. The UV–Vis diffuse reflectance spectra of the SnO2/BNMB and the plots
of (ahν)1/2 versus the energy of light (hν) (Adapted from Ref. [85]).

applications [21,60,61].
In consideration of this, a number of commonly-used modification
methods which have been applied to improve the photocatalytic activity
of BBS are reported. Besides, allowing for the superiority of BBS and BN
materials, combining these two materials into a composite may provide
a feasible way to further improve photocatalytic activity. In this sense,
Bi2MoO6 is considered as exemplary. There are reports where the
transient photocurrent response of pure Bi2MoO6 and BN-Bi2MoO6
composites are described. In Fig. 12, the photocurrent of the two sam­
ples suggests the stability of the as-prepared electrode, and the photo­
current intensity of the BN-Bi2MoO6 composite is shown to be more than
twice higher than that of pure Bi2MoO6, which conforms to the photo­
catalytic degradation of organic pollutants [62]. Graphene-analogue BN Fig. 10. Photodegradation of MO by P25, TiO2 nanofibers and BN/TiO2 com­
and BiOBr have similar layered structures, which can minimize lattice posites under UV light (Adapted from Ref. [40]).

Fig. 9. Several mechanisms of BN enhancing photo­

catalytic activity. (a) BN forms a heterostructure with
other catalysts, reducing the band gap energy and
improving the response to visible light. (b) The
negatively charged BN prepared in certain ways (such
as ball milled) causes the photo-generated holes in
other photocatalysts to migrate to the surface through
electrostatic action, which promotes the reaction. (c)
The photogenerated electrons in other photocatalysts
migrate to the surface of BN, which promotes the
separation of electron-hole pairs and improves
quantum efficiency. (d) The adsorption of organics by
large specific surface area BN promotes the occur­
rence of redox reactions.

8
X. Gao et al.
Fig. 11. SEM image of BCN with various microstructures ((a)adapted from Ref. [57], (b)adapted from Refs. [50], (c)adapted from Ref. [49] and (d)adapted
from Ref. [48]).
Fig. 12. The photocurrent of BN-Bi2MoO6 (Adapted from Refs. [62]).
[67], Ag3VO4 [69], etc.) materials have also been extensively applied as
promising photocatalysts in both the degradation of organic pollutants
and the splitting of water [69]. They exhibit strong photocatalytic ac­
tivity and the suitable level of band gap energy. For example, the band
gap energy of AgBr is roughly 2.58 eV [22]. However, a majority of
silver-based semiconductors lack stability under light irradiation. For
example, pure AgX (X ¼ Cl, Br or I) can be photoreduced by visible light
photons [22]. In addition, the rapid electron-hole recombination is also
significantly restrictive on its further applications [68]. Therefore, some
studies have been carried out to explore how to improve light stability
and the efficiency of carrier separation for silver-based photocatalysis. It
was found that such strategies as the formation of silver-based semi­
conductors with carbon materials, can inhibit the recombination of
charge carriers while enhancing both photocatalytic activity and sta­
bility [70]. Moreover, the silver halides/silver composite photocatalysts
with the cube shapes also shows their superiority to the conventional
silver-based photocatalysts regarding photocatalytic activity [72]. Due
to the extraordinary electronic structure, h-BN has been recognized as
9
Materials Science in Semiconductor Processing 120 (2020) 105256
Fig. 13. Cycling runs for photocatalytic degradation of RhB over graphene-
analogue BN/Ag3PO4 composite (adapted from Ref. [71]).
an important material for hole acceptors, as it is capable of promoting
the separation of electrons and holes [68]. Since BN has been proven to
form heterojunctions with various semiconductor materials such as TiO2
to enhance its photocatalytic activity, researchers consider combining it
with Ag-based materials to develop its wide applications [67].
Lv et al. conducted study on the photocatalytic performance of h-BN/
Ag3VO4 hybrid nanocomposite to degrade RhB under visible light. In
contrast with pure Ag3VO4, the h-BN/Ag3VO4 photocatalysts exhibited
stronger photocurrent responses, enhanced absorbance intensity, as well
as significantly enhanced photocatalytic activity and stability. After 90
min of irradiation, as much as 96.3% of RhB was removed [69]. Wu et al.
studied the degradation of RhB under visible light with Ag2CrO4/few
layer boron nitride nanosheets (FBNNS). The band gap energy of the
Ag2CrO4/FBNNS reached 1.60 eV, which is lower than 1.64 eV of pure
Ag2CrO4. After 120 min of irradiation, the degradation rate reached
96.7% [73]. Song et al. conducted investigation into the
graphene-analogue BN/Ag3PO4 and applied it to degrade RhB for five
repeated cycles under visible light, and the experiment results presented
in Fig. 13, which reveals that the photocatalytic efficiency is still capable
X. Gao et al. Materials Science in Semiconductor Processing 120 (2020) 105256

activity in the water splitting, further studies were still required [127].

3.3.6. ZnO-BN
ZnO is considered as an ideal photocatalyst, due to its relatively
cheap affordability. The wide band gap makes it possible for ZnO to
provide a wide range of holes with strong oxidation properties [128,
129]. Unfortunately, ZnO is prone to photocorrosion under UV light and
shows sensitivity to dissolution at an extreme level of pH values. Such
defects are adverse to broadening the practical applications of ZnO
[130]. As revealed by some studies, most of the photocorrosion pro­
cesses related to semiconductor could be induced by the transfer of
retarded hþ. In order to improve the efficiency of transferring semi­
conductor photo-generated carrier, plenty of work has been done. It is
worth pointing out that most of the work focuses on the transfer of e ,
but making improvement to the transfer efficiency of hþ with the
reduced characteristic recombination time may be an effective approach
Fig. 14. EIS spectra of the samples: (a) pure SnS2 and (b) the SnS2/FBNNS
to improve the catalytic performance of ZnO [75]. One potential solu­
composites (adapted from Ref. [74]).
tion to achieve this goal is to load some hole transfer promoters (such as
RuO2 [131], IrO2 [132] and iridium-based complexes [133]) into the
of reaching around 94% after five cycles, indicating that the stability of
ZnO semiconductor. However, most accelerators are based on precious
Ag3PO4 was significantly improved after the formation of a complex
metals and their applications are severely limited. Therefore, it is
with BN [71].
necessary to develop new affordable hole promoters.
In view of the fact that h-BN has been applied to study the photo­
3.3.5. SnS2-BN
catalytic promotion of TiO2, some researchers have started to use ball
SnS2 is a semiconductor with an extremely narrow band gap (Eg ¼
milling h-BN for the modification made to ZnO. Fu et al. applied the h-
2.18–2.44 eV [127]). The VB and CB energy levels (0.77 eV and 0.28 eV)
BN/ZnO sample as prepared using the ball milling approach to study the
of SnS2 are almost ideal placed for water splitting, which is an advantage
degradation of negatively charged dyes RhB and MB under UV light. The
[127]. Compared to those traditional semiconductors, SnS2 demon­
temporal UV–vis spectral changes of RhB and MB aqueous solution in
strates higher catalytic activity in the visible region and even in the
the presence of h-BN/ZnO as a function of irradiation time are shown in
near-infrared region. Due to its wide-area light-response performance,
Fig. 15. After 20 min of irradiation, there was as much as 82% of RhB
non-toxicity and environmental friendliness, it has been identified as
and 60% of MB removed. In the meantime, a small hypsochromic shift
having a massive potential of application as a photocatalyst. The major
was achieved [75]. But at the same time, they found that h-BN/ZnO
barriers to its extensive applications is its low photocatalytic activity and
exhibited negligible effect in the decomposition of negatively charged
instability [74]. Wu et al. conducted synthesis of SnS2/FBNNS composite
dyes such as CR and MO. Therefore, they speculate that negatively
material using a one-step hydrothermal method, and carried out eval­
charged ball-milled h-BN mainly promotes the reaction by inducing
uation of its photocatalytic activity through a experiment conducted on
electrostatic attraction in this system [75].
the degradation of RhB under visible light. Fig. 14 shows EIS of pure
SnS2 and SnS2/FBNNS. It can be seen from the figure that the hybrid
4. Future work and concluding remarks
sample has a smaller Nyquist circle diameter than pure SnS2, indicating
that the hybrid product has a lower charge transfer resistance. It is thus
BN demonstrates unique physiochemical characteristics in photo­
inferred that the composites with BN could help accelerate the interfa­
catalysis, and the photocatalyst obtained by compounding with other
cial charge process, thus improving the efficiency of electron-hole pair
semiconductors displays excellent photocatalytic activity. In this article,
separation. It is also observed from the figure that this composite ma­
a review was conducted of several BN composite photocatalysts that are
terial could degrade as high as 93.7% of RhB after 210 min of irradia­
currently being studied and a summary was made of several modifica­
tion, which is significantly higher compared to pure SnS2 [74]. Despite
tion schemes to address the typical photocatalyst defects. However, the
this SnS2/FBNNS composite material exhibited high photocatalytic

Fig. 15. The temporal UV–vis spectral changes of (a) RhB and (b) MB aqueous solution in the presence of h-BN/ZnO as a function of irradiation time (Adapted
from Ref. [75]).

10
X. Gao et al.
Table 2
Properties of BN applied in photocatalysis.
Advantages Disadvantages
BN applied Excellent physicochemical Wide band gap;
photocatalysis property; Visible-light
Large specific surface area; irresponsive
Layered structure;
Excellent electrochemical
conductivity
high electron-hole pair recombination rate, large forbidden bandwidth
and poor stability remain the main challenges facing its practical ap­
plications (Table 2).
In order for further research, the attention can be focused on the
following areas for future works:
1) Continue in-depth research on surface modification, doping,
morphology control and other approaches to find the best way of
improving photo-generated carrier separation.
2) Collaborate with other fields such as electrochemistry and mem­
brane technology to broaden the scope of potential applications for
BN.
3) Expand the BN-based photocatalytic system, work out the design of
photocatalytic reactor and assess the feasibility of its practical
application.
Despite preexisting reports on the BN-based semiconductors that
exhibit high catalytic activity under visible light, there remains a long
way to go before it can be demonstrated that they are photocatalysts
with a massive potential.
Declaration of competing interest
There are no conflicts to declare.
Acknowledgements
X.M. acknowledges the financial supports from the Key Laboratory of
Marine Chemistry Theory and Technology (Ministry of Education,
Ocean University of China) and Taishan Scholar Foundation of Shan­
dong province (No.: tsqn201909058).
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