金属卤化物钙钛矿光催化的研究进展

doi:10.6023/A19080292

摘要/Abstract

太阳能驱动光催化反应降解污染物、制备化学燃料或其他高附加值产品是绿色化学和可再生能源研究的重要方向.近年来，在传统的金属氧化物半导体材料之外，金属卤化物钙钛矿类化合物凭借其优异的光电特性也被逐步应用于高效光催化反应中.这篇文章综述了以铅卤钙钛矿为主的金属卤化物钙钛矿材料近年来在光催化领域的研究进展，总结了金属卤化物钙钛矿材料在光（电）催化产氢、CO₂还原反应和有机物高附加值转化反应中的应用与反应机制及其关键挑战，最后展望了高效稳定的金属卤化物钙钛矿光催化剂的发展方向和前景.

关键词: 金属卤化物钙钛矿, 光催化, 光催化产氢, 光催化CO₂还原, 光催化合成

photocatalytic pollutant degradation and the synthesis of chemical fuels or other high value-added products via photocatalysis have drawn plenty of attentions in green chemistry and renewable energy research. In recent years, metal-halide perovskites with superior photoelectric properties are successfully utilized into high-efficiency photocatalytic reactions in addition to conventional metal oxide semiconductor materials. In this paper, we reviewed the recent advances of metal-halide perovskite based photocatalyst, especially lead-halide perovskites in photocatalytic hydrogen production, photocatalytic degradation and CO₂ reduction. The reaction mechanisms and key challenges for metal halide perovskites photocatalyst are discussed and we prospect the further development of highly efficient and stable metal halide perovskite photocatalysis in the future.

Key words: metal halide perovskites, photocatalysis, photocatalytic hydrogen production, photocatalytic CO₂ reduction, photocatalytic synthesis

引用此文

李鑫, 张太阳, 王甜, 赵一新. 金属卤化物钙钛矿光催化的研究进展[J]. 化学学报, 2019, 77(11): 1075-1088.

Li Xin, Zhang Taiyang, Wang Tian, Zhao Yixin. Recent Progress of Photocatalysis Based on Metal Halide Perovskites[J]. Acta Chimica Sinica, 2019, 77(11): 1075-1088.

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图/表 10

图 1. ABX3铅卤钙钛矿晶体结构示意图[22]

Figure 1. Schematic representation of the typical ABX3 crystal structure of halide perovskites. Reprinted with permission from ref. [22]. Copyright (2019) Royal Society of Chemistry.

图 2. (a) 自然界光合作用机理示意图; (b)人工光合作用机理示意图[82]

Figure 2. Schematic illustration for natural (a) and artificial (b) photosynthesis. Reprinted with permission from ref. [82]. Copyright (2019) American Chemical Society.

图 3. (a) 以Ni金属层钝化的MAPbI3基光电阳极为工作电极, 使用标准三电极体系进行光电化学测试的示意图(左下图为光电阳极的截面SEM图)以及(b)各功能层的能带示意图[87]; (c)以Pt负载Ti金属层钝化的MAPbI3基光电阴极为工作电极, 使用标准三电极体系进行光电化学测试的示意图(左下图为光电阴极的截面SEM图)以及(d)各功能层的能带示意图[88]

Figure 3. (a) Schematic illustration of photoelectrochemical test of a Ni-coated perovskite photoanode in a PEC cell using standard three-electrode system. The photoanode is back illuminated from the FTO side. (b) Schematic energy diagram of TiO2, CH3NH3PbI3, spiro-MeOTAD, Au, and Ni. The energy levels of each material are given in eV. Reprinted with permission from ref. [87]. Copyright (2015) American Chemical Society. (c) Schematic illustration of the sandwich-like CH3NH3PbI3 photocathode for PEC H2 evolution in a standard three-electrode system. The photocathode is back illuminated from the ITO side. (d) Schematic energy diagram of each component in inverted CH3NH3PbI3 solar cell. Reprinted with permission from ref. [88]. Copyright (2018) John Wiley and Sons.

图 4. (a) MAPbI3在HI饱和溶液中沉淀-溶解平衡示意图; (b)不同浓度H+和I－时HI溶液中稳定的沉淀相情况[97]; (c)两步法铅活化-胺辅助的PbAAA反应机理示意图[98]

Figure 4. (a) Schematic illustration of the MAPbI3 powder in dynamic equilibrium with a saturated HI solution. (b) Constructed phase map as a function of [I?] and [H+]. Reprinted by permission from ref. [97]. Copyright (2016) Springer Nature. (c) Pb-Activated amine-assisted (PbAAA) reaction pathway for H2 generation on MAPbI3 surface in acidic solvent. Reprinted by permission from ref. [98]. Copyright (2018) American Chemical Society.

图 5. (a) 引入Pt/Ta2O5和PEDOT:PSS分别作为电子传输材料和空穴传输材料的MAPbBr3基产氢光催化剂的反应机理示意图; (b) HBr分解反应中MAPbBr3, Ta2O5和PEDOT:PSS的能级分布示意图[102]

Figure 5. (a) Schematic illustration of the reaction mechanism for MAPbBr3 with Pt/Ta2O5 and PEDOT:PSS as the electron- and hole-transporting motifs, respectively. (b) Schematic energy level diagrams of MAPbBr3, Ta2O5, and PEDOT:PSS for HBr splitting reaction. Reprinted by permission from ref. [102]. Copyright (2019) American Chemical Society.

图 6. (a) CsPbBr3 NC/MRGO二元结构和(b) CsPbBr3 NC/BZNW/ MRGO三元结构在可见光作用下光催化还原CO2的机理示意图[108]

Figure 6. Schematic illustration of the energy band structure and possible transfer process of photo-induced carriers: (a) CsPbBr3 NC/MRGO and (b) CsPbBr3 NC/BZNW/MRGO hybrids under visible light irradiation. Reprinted by permission from ref. [108]. Copyright (2019) Royal Society of Chemistry.

图 7. 使用纯组分CsPbBr3、Co掺杂CsPbBr3和Fe掺杂CsPbBr3时CO2还原最佳路径的自由能谱, 标注为每种情况下速控步的ΔG [109]

Figure 7. The free energy diagrams of the most favored paths of CO2 reduction on pristine, Co-doped and Fe-doped cases. The ΔG of the rate-determining step for each case is listed. Reprinted by permission from ref. [109]. Copyright (2019) Royal Society of Chemistry.

图 8. LED白光作用下利用CsPbBr3光催化聚合苯乙烯的机理示意图[116]

Figure 8. Proposed reaction mechanism of the perovskite photoactivated polymerization of styrene. Reprinted with permission from ref. [116]. Copyright (2019) John Wiley and Sons.

图 9. (a) CsSnBr3光催化降解结晶紫染料的机理示意图[125]; (b) Cs3Bi2Br9光催化环氧化合物开环反应的机理示意图[59]

Figure 9. (a) Scheme of the photocatalysis mechanism proposed. Reprinted with permission from ref. [125]. Copyright (2018) John Wiley and Sons. (b) Proposed photocatalytic cycle for epoxide alcoholysis reaction over Cs3Bi2Br9 with proper Lewis acids sites on surface. Reprinted with permission from ref. [59]. Copyright (2019) John Wiley and Sons.

图 10. (a) 立方晶相Cs2AgBiBr6的晶体结构; (b) Cs2AgBiBr6光催化还原CO2的机理示意图[62]

Figure 10. (a) Crystal structure of cubic Cs2AgBiBr6. (b) Schematic diagram of the photoreduction of CO2 on the surface of Cs2AgBiBr6 NCs. Reprinted with permission from ref. [62]. Copyright (2018) John Wiley and Sons.

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