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摘要

钙钛矿材料可以分为 ABO ₃氧化物和 ABX ₃( X= Cl, Br或I)卤化物两大类, 它们都具有丰富的物理性质和优异的光电性能, 比如铁电性和光催化性能. 本文介绍了BiFeO ₃和 MAPbI ₃等铁电半导体光催化材料和异质结的制备方法, 总结了它们在光电催化方面的研究进展. 目前研究者已经针对氧化物光催化材料做了各种研究, 包括: 降低吸光层铁电材料的带隙, 制备铁电/窄带半导体吸光层异质结, 制备比表面积很大的纳米片、纳米棒或者其他纳米结构, 以便吸收更多可见光; 让铁电极化及其退极化场垂直于光催化工作电极表面, 通过铁电/半导体异质结能带弯曲提供内电场, 通过外电场进行光电催化, 从而通过内、外电场高效分离光生-电子空穴对; 通过光催化或者光电催化降解染料、分解水制氢、将CO ₂转换为燃料; 通过铁电、热释电和压电协同效应提高催化效应和能量转换效率. MAPbI ₃等卤素钙钛矿具有优异的半导体性质, 其铁电性可能是引起超长的少数载流子寿命和载流子扩散长度的原因. 通过优化光催化多层膜结构并添加防止电解液渗透的封装层可以避免 MAPbI ₃被电解液分解, 从而制备了具有很高能量转换效率的光电催化结构. 最后, 我们分析和比较了这些钙钛矿铁电半导体在光电催化领域面临的挑战, 并展望了其应用前景.

关键词:

Abstract

There are two types of perovskites, i.e. ABO ₃-type oxides and ABX ₃-type ( X= F, Cl, Br and I) halides. Both of them exhibit rich physical properties and excellent photoelectric properties, such as ferroelectric and photocatalytic properties. In this paper we introduce the methods of preparing the ferroelectric semiconductors (i.e. BiFeO ₃and MAPbI ₃) and their heterogeneous junctions for photocatalytic applications, and summarizes the research progress and applications of photocatalytic devices. Various researches about oxide photocatalytic devices have been carried out. At first, several methods have been developed to absorb more visible light, such as reducing the band gap of ferroelectric materials, preparing junction composed of ferroelectric layer and light absorption layer with narrow-bandgap semiconductor, and growing nanosheet, nanorods or other nanostructures with large specific surface areas. Second, some electric fields are introduced to effectively separate light activated electron-holes pairs. In addition to the external electric field, an inner electric field can be introduced through the ferroelectric polarization perpendicular to the surface and/or the energy band bending at the ferroelectric/semiconductor interface. Thirdly, the degradation of dyes, the decomposition of water into hydrogen and the conversion of CO ₂into fuel have been realized in many photocatalytic or photoelectrocatalytic devices. Fourthly, the synergies of ferroelectric, pyroelectric and piezoelectric effects can largely increase the photocatalytic efficiency and the energy conversion efficiency. Furthermore, MAPbI ₃and other halogen perovskites show excellent semiconductor properties, such as the long carrier diffusion length and long minority carrier lifetime which may originate from ferroelectric dipoles. The MAPbI ₃can be applied to photocatalytic devices with a high energy conversion efficiency by optimizing the photocatalytic multi-layer structure and adding a package layer that prevents electrolyte for decomposing the MAPbI ₃. Finally, we analyze the challenges of the high-efficiency photocatalytic devices and look forward to their application prospects.

Keywords:

作者及机构信息

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通信作者:袁国亮,yuanguoliang@njust.edu.cn

基金项目:国家级-国家自然科学基金(51790492、51431006、51902159 、61874055)

Authors and contacts

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2.

Corresponding author:Yuan Guo-Liang,yuanguoliang@njust.edu.cn

文章全文: translate this paragraph

参考文献

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施引文献

下载: 全尺寸图片幻灯片

材料及结构 (铁电材料为粗体)	铁电	带隙/eV	激励源	催化降解物	催化活性	污染性	稳定性(性能/时间)	文献
BiFeO₃纳米粉体	强	2.18	紫外可见光	甲基橙	8 h降解90%	中	—	[14]
FTO玻璃/BiVO₄/BiFeO₃/CuInS₂	强	2.1—2.7	可见光	对硝基苯酚	K_obs= 0.02 min^–1	中	相对稳定/5次循环	[56]
NaNbO₃纳米棒	强	3.3	光+超声振动	甲基蓝	—	弱	98%/3次循环	[42]
BaTiO₃@Ag纳米颗粒	强	3.2	光	罗丹明B	K_obs= 0.087 min^–1	弱		[43]
BaTiO₃/MoO₃	强	3.2	紫外-可见光	罗丹明B	60 min降解86%	弱	95%/5次循环	[44]
BaTiO₃/Ag₂O纳米棒	强	3.2	紫外光+ 超声振动	罗丹明B (c= 15 mg·L^–1)	K_obs= 0.031 min^–1	弱	50%/5次循环	[18]
BaTiO₃@非晶BaTiO_3–_x	强	3.2	可见光	甲基蓝	5 h降解62.4%	弱	97%/5次循环	[45]
PbTiO₃/TiO₂纳米片	强	3.6	氙灯可见光	甲基蓝	K_obs= 0.057 min^–1 132.6 μmol·h^–1·g^–1产H₂	强	—	[46]
KNbO₃/g-C₃N₄	强	3.28	氙灯可见光	—	180 μmol·h^–1·g^–1产H₂	弱	95%/4次循环	[47]
{001} Bi₃TiNbO₉纳米片	—	3.3	氙灯可见光	—	342.6 μmol·h^–1·g^–1产H₂	中	—	[48]
KNbO₃颗粒	强	3.28	光	罗丹明B	K_obs= 0.317 min^–1	弱	—	[49]
KNbO₃纳米片	强	3.07	可见光+超声振动	罗丹明B	K_obs= 0.022 min^–12 h降解92.6%	弱	—	[50]
FTO玻璃/ZnSnO₃纳米线	弱	3.7	光+压力	甲基蓝	K_obs= 0.007 min^–1	弱	90%/1 h	[51]
FTO/ZnSnO_3–_x纳米线	弱	2.4—3.7	光、超声振动、光和超声振动	—	3562, 3453, 3882 μmol·h^–1·g^–1产H₂	弱	在振动下相对稳定/7 h	[52]
FTO/Zn_1–_xSnO₃纳米线	弱	2.4—3.7	紫外光+振动	甲基蓝	K_obs= 0.015 min^–1	弱	—	[53]
PZT@TiO₂核壳结构	强	3.6	光+搅拌	罗丹明B	80 min完全降解	强	—	[54]
BiOI-BaTiO₃纳米粒子	强	3.2	可见光	甲基橙	90 min降解95.4%	弱	—	[55]
ZnO纳米线	压电	3.37	光+摇摆	甲基蓝	K_obs= 0.025 min^–1	弱	99%/3次循环	[57]
ZnO纳米片/TiO₂纳米颗粒	压电	3.37	可见光	甲基橙	K_obs= 0.038 min^–1	弱	相对稳定/11 h	[58]
Ag-ZnO纳米线	压电	3.37	光+弯折	罗丹明B	K_obs= 0.052 min^–1	弱	90%/8次循环	[59]

下载: 导出CSV

材料和结构 (铁电材料为粗体)	铁电	PCE/%	带隙/eV	电解液	光源	工作电极电势	光电流密度/ mA·cm^–2	污染性	稳定性 (性能/时间)	文献
ITO/BiFeO₃/Au	强	—	2.16—2.7	0.1 mol/L KCl	AM1.5G	0 V vs.Ag/AgCl	0.05	弱	—	[60]
SrTiO₃/SrRuO₃/(111)BiFeO₃	强	—	2.16—2.7	0.5 mol/L Na₂SO₄	AM1.5G	0 V vs. Ag/AgCl	0.08	弱	100%/700 s	[61]
SrTiO₃/CaRuO₃/(111) Bi₂FeCrO₆	强	—	1.9—2.1	1 mol/L Na₂SO₄	AM1.5G	0 V vs. Ag/AgCl	–2.02	弱	—	[15]
SrTiO₃/SrRuO₃/Bi₂FeCrO₆/ NiO	强	—	1.8— –2.7	1 mol/L Na₂SO₄	AM1.5G	1.2 V vs. RHE	0.9	弱	95%/7 h	[62]
TiO₂@PbTiO₃核壳结构	强	—	3.6	—	氙灯100 mW·cm^–2	—	132 μmol·g^–1H₂	强	—	[63]
FTO/NaNbO₃	强	—	3.37	0.5 mol/L Na₂SO₄	AM1.5G	1 V vs. Ag/AgCl	0.51	弱	—	[64]
ITO/KNbO₃纳米片	强	—	2.86	0.5 mol/L Na₂SO₄	AM1.5G	0 V vs. Ag/AgCl	0.82	弱	—	[50]
(001) LiNbO₃单晶	强	—	3.26	mol/LK₃PO₄	AM1.5G	1.23 V vs. RHE	0.15	弱	—	[65]
FTO/TiO₂@BaTiO₃/Ag₂O	强	—	3.2	1 mol/LNaOH	AM1.5G	0.8 V vs. Ag/AgCl	1.8	弱	97%/1 h	[66]
FTO/TiO₂@SrTiO₃ (10 nm四方铁电相)	弱	—	3.2	1 mol/LNaOH	AM1.5G	1.23 V vs. RHE	1.43	弱	—	[67]
Glass/FTO/m-TiO₂/CH₃NH₃PbI₃/ Spiro-MeOTAD/Au/Ni	弱	14.4	1.5	—	AM1.5G	1.0 V vs. SHE	17.4	强	66%/1 h	[68]
FTO/PEDOT:PSS/CH₃NH₃PbI₃/ PCBM/PEIE/Ag/FM	弱	7.7	1.5	—	AM1.5G	1.2 V vs. RHE	15.0	强	80%/1 h	[69]
ITO/NiO/CH₃NH₃PbI₃/ PCBM/Ag/Ti/Pt	弱	16.1	1.5	0.5 mol/L H₂SO₄	AM1.5G	1.2 V vs. RHE	18	强	70%/12 h	[70]
CH₃NH₃PbI₃solar cells, a cell for H₂O splitting	弱	15.7	1.5	—	AM1.5G	—	10	强	75%/10 h	[71]
FTO/BiVO₄/black-phosphorene/ NiOOH	无	—	2.4—2.5	0.5 mol/L KH₂PO₄K₂HPO₄	AM1.5G	1.23 V vs. RHE	4.48	强	99%/60 h	[72]
FTO/H:TiO₂	无	1.63	3.2	1 mol/LNaOH	AM1.5G	–0.6 V vs. Ag/AgCl	1.97	弱	94%/28 h	[73]

下载: 导出CSV

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