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Engineering    2017, Vol. 3 Issue (3) : 365-378     https://doi.org/10.1016/J.ENG.2017.03.019
Research |
钽基氮氧化物——窄带隙光催化剂用于太阳能制氢
肖慕,王松灿,Thaweesak Supphasin,罗彬,王连洲()
Nanomaterials Center, School of Chemical Engineering, and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD 4072, Australia
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摘要 

光催化分解水可以将太阳能直接转化为氢能,是一种有效利用太阳能的途径。开发用于太阳能制氢的高效且稳定的光催化剂是光催化研究领域的重要目标之一。钽基氮氧化物具有窄的带隙宽度,并且光生电子和空穴的势能足够用来分解水,因此该类光催化剂最有可能实现太阳能制氢。到目前为止,全世界的研究小组对钽基氮氧化物光催化剂进行了系统而深入的研究,取得了大量的成果。然而,钽基氮氧化物的太阳能制氢效率还远远低于理论值。如何更好地设计这些材料进而提高其太阳能制氢效率这一命题是十分重要和有意义的。本文总结了钽基氮氧化物用于光催化制氢的研究和发展过程,着重分析了用于提高光催化分解水效率的各种方法。最后,探讨了窄带隙钽基氮氧化物光催化分解水研究领域的未来发展趋势。

关键词 钽基光催化剂窄带隙分解水    
Abstract

Photocatalytic water splitting, which directly converts solar energy into hydrogen, is one of the most desirable solar-energy-conversion approaches. The ultimate target of photocatalysis is to explore efficient and stable photocatalysts for solar water splitting. Tantalum (oxy)nitride-based materials are a class of the most promising photocatalysts for solar water splitting because of their narrow bandgaps and sufficient band energy potentials for water splitting. Tantalum (oxy)nitride-based photocatalysts have experienced intensive exploration, and encouraging progress has been achieved over the past years. However, the solar-to-hydrogen (STH) conversion efficiency is still very far from its theoretical value. The question of how to better design these materials in order to further improve their water-splitting capability is of interest and importance. This review summarizes the development of tantalum (oxy)nitride-based photocatalysts for solar water spitting. Special interest is paid to important strategies for improving photocatalytic water-splitting efficiency. This paper also proposes future trends to explore in the research area of tantalum-based narrow bandgap photocatalysts for solar water splitting.

Keywords Tantalum-based photocatalyst      Narrow bandgap      Water splitting      Hydrogen     
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通讯作者: 王连洲     E-mail: l.wang@uq.edu.au
最新录用日期:    发布日期: 2017-06-30
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Mu Xiao
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引用本文:   
Mu Xiao,Songcan Wang,Supphasin Thaweesak, et al. Tantalum (Oxy)Nitride: Narrow Bandgap Photocatalysts for Solar Hydrogen Generation[J]. Engineering, 2017, 3(3): 365-378.
网址:  
http://engineering.org.cn/EN/10.1016/J.ENG.2017.03.019     OR     http://engineering.org.cn/EN/Y2017/V3/I3/365
Fig.1  Main scheme of photocatalytic water splitting. CB: conduction band; VB: valence band.
Fig.2  Scheme of water splitting using semiconductors.
Compound Crystal structure Absorption edge (nm) Bandgap (eV)
Ta3N5 Anosovite 600 2.1
TaON Baddelyite 510 2.4
LaTaON2 Perovskite 640 1.9
CaTaO2N Perovskite 510 2.4
SrTaO2N Perovskite 570 2.2
BaTaO2N Perovskite 660 1.9
Tab.1  Representative tantalum (oxy)nitride-based photocatalysts [49].
Fig.3  Schematic band structures of Ta2O5, TaON, and Ta3N5 [54]. (Copyright 2003, American Chemical Society)
Fig.4  Bandgap diagrams of tantalum-based oxynitride perovskite [55]. EF: Femi lever; EVAC: vacuum lever. (Copyright 2013, American Chemical Society)
Fig.5  UV-Vis light absorption spectra of Ta3N5 prepared at 850 °C, 900 °C, 950 °C, and 1000 °C in NH3 gas collected in different mode: (a) transmission mode and (b) integrating sphere. Pictures inset in (b) show the gray tint in the sample treated at 950 °C and 1000 °C [62]. (Copyright 2014, American Chemical Society)
Fig.6  UV-Vis light diffuse reflectance spectra of Ta3N5. (a) Pristine Ta3N5; (b–e) samples treated at 823 K for 5 h with (b) 10 MPa of N2, (c) 10 MPa of NH3, (d) 50 MPa of NH3, and (e) 100 MPa of NH3 [64]. (Copyright 2012, Elsevier)
Fig.7  Scanning electron microscope (SEM) images of Ta3N5 prepared by various flux-assisted nitridation methods. (a) Ta2O5-NaCl (850 °C for 10 h); (b) Ta3N5-NaCl (850 °C for 10 h); (c) TaCl5-NaCl (800 °C for 10 h); and (d) TaCl5-Zn (800 °C for 10 h) [69]. (Copyright 2011, American Chemical Society)
Fig.8  (a) Time courses for photocatalytic H2 production on Ta3N5 variants separately replaced with different amounts of Mg, Zr, or Mg+Zr: (i) undoped; (ii) 25 at% Mg; (iii) 40 at% Mg; (iv) 25 at% Zr; (v) 40 at% Zr; (vi) 25 at% Mg+Zr; (vii) 40 at% Mg+Zr. (b) Band structure diagram of Ta3N5 and Ta3N5:Mg+ Zr [81]. Efb: flat band energy. (Copyright 2015, American Chemical Society)
Fig.9  (a) (F(R))1/2 versus the energy curve of LaMgxTa1–xO1+3xN2–3x derived from UV-Vis light diffuse reflectance spectra. (b) Band levels of LaMgxTa1–xO1+3xN2–3x (x = 0 and 0.33) obtained by PESA and theoretical calculations (CAL) [82]. (Copyright 2016, The Royal Society of Chemistry)
Fig.10  (a) Transmission electron microscope (TEM) image of mesoporous Ta3N5 [84] (Copyright 2010, American Chemical Society); (b) SEM image of Ta3N5 nanoparticles prepared using the reverse homogeneous precipitation (RHP) method [85] (Copyright 2009, Elsevier); (c) TEM image of Ta3N5 particles prepared by adopting mesoporous C3N4 as the template [86] (Copyright 2010, The Royal Society of Chemistry); (d) SEM image of macroporous Ta3N5 [87] (Copyright 2012, Wiley-VCH).
Fig.11  SEM images of: (a–d) u-Ta2O5, (e) γ/β-TaON(u), and (f) u-Ta3N5. (g) Scheme of the formation of hollow urchin-like u-Ta2O5 hierarchical nanostructures and the subsequent thermal nitridation, successively forming γ-TaON, β-TaON, and u-Ta3N5 [90]. (Copyright 2013, The Royal Society of Chemistry)
Fig.12  (a, c) SEM and (b, d) TEM images (top right insets: electron diffraction) of (a, b) Ta3N5 nanoplates and (c, d) Ta3N5 octahedra. (e) Diffuse reflectance spectra and (f) time-dependent H2 evolution reaction of different Ta3N5 samples [92]. (Copyright 2016, The Royal Society of Chemistry)
Fig.13  (a) UV-Vis diffuse reflectance spectra (inset: Tauc plot) and (b) band position of CaTaO2N as determined by calculation. Time courses of gas evolution during water splitting on titanium-oxyhydroxide-deposited RhCrOy/CaTaO2N under (c) UV+ Visible light (λ≥300 nm) and (d) visible light (λ≥420 nm) [51]. (Copyright 2015, The Royal Society of Chemistry)
Fig.14  Field emission scanning electron microscope (FESEM) images of (a) Pt/Ta3N5 and (b) Pt/MgO(in)-Ta3N5 [97] (Copyright 2016, Elsevier); (c) time course of visible-light H2 evolution with 0.5 wt% Pt/Ba(0.3)-Ta3N5; (d) relative band positions of the Ta3N5/BaTaO2N heterostructure [98] (Copyright 2017, The Royal Society of Chemistry).
Fig.15  (a) Scheme illustration of two separated co-catalysts used to decorate Ta3N5 hollow spheres to create an effective photocatalyst for water splitting. (b,c) SEM images of (b) Ta3N5/Pt/SiO2 spheres and (c) Ta3N5/Pt hollow spheres. The scale bar is 500 nm. (d) Time course of H2 evolution on Ta3N5 photocatalysts with and without spatially separated co-catalysts [40]. TPS: Ta3N5/Pt/SiO2; TS: Ta3N5/SiO2. (Copyright 2013, Wiley-VCH)
Fig.16  (a) Scheme of the mechanism of overall water splitting on an IrO2/Cr2O3/RuOx/ZrO2/TaON photocatalyst. (b) Time course of gas evolution using IrO2/Cr2O3/RuOx/TaON under visible light (λ>400 nm) [18]. (Copyright 2013, Wiley-VCH)
Fig.17  (a) A TEM image of Au nanoparticles; (b) high-angle annular dark-field scanning transmission electron microscope (STEM) image of nano Au/Ta3N5; (c) the UV-Vis diffuse reflectance spectra of nano Au/Ta3N5; (d) the time course of H2 generation for the nano Au/Ta3N5 composites [119]. (Copyright 2014, The Royal Society of Chemistry)
Fig.18  Relative bandgap positions and charge transfer mechanism (Z-scheme) in Bi2O3 and Ta3N5 under visible-light irradiation [121]. (Copyright 2015, The Royal Society of Chemistry)
Fig.19  (a) Scheme of the Z-scheme overall water splitting on a RuO2/TaON and Pt/TaON mixture with an I O 3 /I redox mediator [ 122] (Copyright 2008, The CSJ Journals); (b) Scheme of two-step water splitting on a Pt/ZrO2/TaON and Ir/R-TiO2/Ta3N5 mixture with an I O 3 /I redox mediator [ 123] (Copyright 2010, American Chemical Society).
Photocatalysts Morphology Co-catalyst
(Amount, wt%)
Light source Reaction solution Activity
(µmol·(g·h)−1)
Ref.
H2 O2
Ta3N5 Microparticles Pt (3.0) 300 W Xe (λ>420 nm) Methanol 9.0 NA [43]
Ta3N5 Nanoparticles Pt (0.5) 300 W Xe (λ>420 nm) Methanol 10.5 NA [85]
Ta3N5 Mesoporous Pt (3.0) 300 W Xe (λ>420 nm) Methanol 17.0 NA [84]
Ta3N5 Microparticles Pt (0.5) 300 W Xe (λ>420 nm) Methanol 110.0 NA [65]
Ta3N5 Nanoparticles Pt (0.5) 450 W Hg (λ>400 nm) Methanol 136.0 NA [86]
Ta3N5 Ordered porous Pt (3.0) 300 W Xe (λ>420 nm) Methanol 18.0 NA [91]
Ta3N5 Microparticles Pt (0.5) 70 W halide (λ>380 nm) Methanol 72.0 NA [64]
Ta3N5 Hollow structure Pt (0.1) 300 W Xe (λ>420 nm) Methanol 425.0 NA [90]
Ta3N5 Hollow spheres Pt (1) IrO2 (0.025) 300 W Xe (λ>420 nm) Methanol 206.3 NA [40]
Ta3N5 Nanoplates Pt (3.0) 300 W Xe (λ>400 nm) Methanol 26.5 NA [92]
Ta3N5 Macroporous NA 300 W Xe Methanol 82.5 NA [87]
Mg-Ta3N5 Microparticles Pt (0.3) 300 W Xe (λ>420 nm) Methanol 70.4 NA [81]
Zr-Ta3N5 Microparticles Pt (0.3) 300 W Xe (λ>420 nm) Methanol 80.6 NA [81]
(Mg+ Zr)-Ta3N5 Microparticles Pt (0.3) 300 W Xe (λ>420 nm) Methanol 60.8 NA [81]
SiO2/Ta3N5 Core/shell Pt (3.0) 300 W Xe (λ>420 nm) Methanol 83.3 NA [118]
ZrO2/Ta3N5 Microparticles Pt (0.5) 300 W Xe (λ>420 nm) Methanol 27.4 NA [96]
MgO/Ta3N5 Microparticles Pt (2.0) 300 W Xe (λ>420 nm) Methanol 149.3 NA [97]
BaTaO2N/Ta3N5 Microparticles Pt (0.5) 300 W Xe (λ>420 nm) Methanol 201.3 NA [98]
Au/Ta3N5 Nanoparticles Pt (1.0) 300 W Xe (λ>420 nm) Methanol 150.0 NA [119]
ZrO2/TaON Nanoparticles IrO2/Cr2O3/RuOx (3.0) 450 W Hg (λ>400 nm) Water 15.0 6.70 [18]
LaMg1/3Ta2/3ON Nanoparticles RhCrOy (0.5) 300 W Xe (λ>420 nm) Water 5.0 2.50 [21]
CaTaO2N Nanoparticles RhCrOy 300 W Xe (λ>420 nm) Water 0.7 0.35 [51]
Tab.2  Tantalum (oxy)nitride-based photocatalysts for water splitting.
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