Research progress of photocatalytic CO2 reduction based on CsPbBr3 perovskite
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摘要: 探索绿色发展、解决能源危机已成为近年来商业发展的趋势。金属卤化物钙钛矿因其独特的光催化性能而备受关注。其中，CsPbBr3钙钛矿具有较高的光催化活性和优异的稳定性，在光催化CO2还原方面发展迅速。在能源发展趋势下，减少碳排放和催化还原CO2作为燃料是研究热点和主要途径。然而，纯CsPbBr3较差的CO2吸附还原能力、严重的电荷复合和较低的电荷效率严重阻碍了钙钛矿光催化的商业化。为了解决纯CsPbBr3材料光催化中的一系列问题，对CsPbBr3钙钛矿进行表面改性或构建多组分复合材料是目前最经济、最有前景的解决方案。本文讨论了CsPbBr3钙钛矿的光催化反应原理及所面临稳定性和还原能力的阻碍，对CsPbBr3钙钛矿及其复合物的光催化CO2还原研究进行了系统的回顾。最后对构建更加稳定、高效及可持续性的CO2还原光催化剂新的探索方向进行了展望。Abstract: Exploring green development and solving the energy crisis has become a trend of commercial development in recent years. Metal halide perovskites have attracted great attentions due to their unique photocatalytic properties. Among them, CsPbBr3 perovskite has high photocatalytic activity and excellent stability, and has developed rapidly in photocatalytic CO2 reduction. Under the trend of energy development, reducing carbon emissions and catalytic reduction of CO2 as fuels are research hotspots and main approaches. However, the poor CO2 adsorption capacity, severe charge recombination, and low charge efficiency of pure CsPbBr3 seriously hinder the commercialization of perovskite photocatalysis. In order to solve a series of problems in photocatalysis of pure CsPbBr3 materials, surface modification the of CsPbBr3 perovskite or construct on of multicomponent composites is currently the most economical and promising solution. In this review, we systematically review the latest research on photocatalytic CO2 reduction of CsPbBr3 perovskites and their composites, discuss the photocatalytic reaction mechanism of CsPbBr3 perovskites, and then propose obstacles to development. Finally, we expect this review to provide new exploration directions for building more stable, efficient and sustainable photocatalysts for CO2 emission reduction.
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Key words:
- photocatalytic CO2 reduction /
- perovskites /
- catalysts /
- surface modification /
- composite material /
- CsPbBr3
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图 1 CsPbBr3全无机钙钛矿的一般晶体结构
Figure 1. General crystal structure of CsPbBr3 all-inorganic perovskite
图 2 CsPbBr3钙钛矿光催化原理
Figure 2. Schematic diagram of CsPbBr3 perovskite photocatalysis
VB—Valence band; CB—Conduction band
图 3 不同样品的CO产量(a)和 CH4产量(b)图作为反应时间的函数；(c) CsPbBr3/沸石咪唑酯骨架结构材料 (ZIFs) 的制备过程和CO2光还原过程的示意图[45]；(d) 钴掺杂CsPbBr3@石墨二炔 (GDY)的合成及其光氧化还原反应示意图[47]
Figure 3. CO yield (a) and CH4 yield (b) plots of different samples as the function of reaction time; (c) Schematic illustration of the fabrication process and CO2 photoreduction process of CsPbBr3/zeolite imidazolate framework (ZIFs)[45]; (d) Illustration of the synthesis of cobalt doped CsPbBr3@graphdiyne (GDY) and its photoredox reactions[47]
2-Hmim—2-Methylimidazole; Eg—Electronic transition
图 4 (a) 模拟阳光下CsPbBr3-Cu-还原氧化石墨烯(RGO)纳米复合材料CO2还原电荷分离与转移机制示意图[55]；(b) Cu/CsPbBr3-Cs4PbBr6合成过程示意图；(c)原位转化、嵌入和掺杂过程的原子结构转换示意图[56]
Figure 4. (a) Schematic diagram for the charge separation and transfer mechanism of CO2 reduction on CsPbBr3-Cu-reduced graphene oxide (RGO) nanocomposites under simulated sunlight[55]; (b) Schematic diagram of Cu/CsPbBr3-Cs4PbBr6 synthesis process; (c) Schematic atomic structures conversion for in-situ transformation, embedding and doping processes[56]
NHE—Normal hydrogen electrode; Cu(acac)2—Cupric(II) acetylacetonate; TOPO—Trioctylphosphine oxide; 1-ODE—1-octadecene; E—Potential
图 5 (a) CsPbBr3-Au纳米复合材料的制备示意图[60]；(b) 块体CsPbBr3、三维有序大孔(3DOM) CsPbBr3和3DOM Au-CsPbBr3的XRD图谱及CsPbBr3和Au的标准PDF卡；(c) 3DOM Au-CsPbBr3光催化剂的合成过程示意图；(d) 光催化反应过程中可能的电荷转移途径[61]；(e) Fe掺杂CsPbBr3和未掺杂CsPbBr3纳米晶光催化剂的示意图[63]
Figure 5. (a) Sketch of the fabrication of CsPbBr3-Au nanocomposites[60]; (b) XRD patterns of bulk CsPbBr3, 3DOM CsPbBr3 and 3DOM Au-CsPbBr3 and the standard PDF cards of CsPbBr3 and Au; (c) Illustration of the synthesis process of three dimensional ordered macropore (3DOM) Au-CsPbBr3 photocatalyst; (d) Possible charge transfer route during the photocatalytic reaction[61]; (e) Schematic presentation of Fe-doped CsPbBr3 and undoped CsPbBr3 nanocrystal photocatalysts[63]
NPs—Nanoparticles; NCs—Nanocrystallines; MPA—3-mercaptopropionic acid; λ—Wavelength
图 6 (a) TiO2/CsPbBr3异质结示意图：内电场(IEF)诱导的电荷转移、分离和在紫外可见光照射下形成S型异质结用于CO2光还原[77]；(b) 静电自组装制备的2D/2D CsPbBr3/Bi2WO6异质结示意图[78]；(c) α-Fe2O3/Amine-RGO/CsPbBr3制备过程示意图-固态Z型光催化剂[79]；(d) 三元WO3/CsPbBr3/ZIF-67异质结构制备过程示意图[80]
Figure 6. (a) Schematic illustration of TiO2/CsPbBr3 heterojunction: Internal electric field (IEF)-induced charge transfer, separation, and the formation of S-scheme heterojunction under UV-visible-light irradiation for CO2 photoreduction[77]; (b) Schematic diagram of 2D/2D CsPbBr3/Bi2WO6 heterojunction prepared via electrostatic self-assembly process[78]; (c) Schematic illustration of the fabrication procedure of α-Fe2O3/Amine-RGO/CsPbBr3 all-solid-state Z-scheme photocatalyst[79]; (d) Schematic illustration of the preparation process of the ternary WO3/CsPbBr3/ZIF-67 heterostructure[80]
EF—Electric potential; NS—Nanosheets; IPA—Isopropanol; [BMIM]BF4—1-butyl-3-methylimidazolium tetrafluoroborate; E—Potential
图 8 CsPbBr3 QDs (BZA & BA)和CsPbBr3 QDs (BZA & BA)/BP NSs ((a), (b))、CsPbBr3 QDs (OA & OAm)和CsPbBr3 QDs (OA & OAm)/BP NSs ((c), (d))、CsPbBr3 QDs (APS) (e)和CsPbBr3 QDs (APS)/BP NSs (f)的PL图谱和时间分辨PL图谱[86]
Figure 8. PL spectra and time-resolved PL spectra of CsPbBr3 QDs (BZA & BA) and CsPbBr3 QDs (BZA & BA)/BP NSs ((a), (b)), CsPbBr3 QDs (OA & OAm) and CsPbBr3 QDs (OA & OAm)/BP NSs ((c), (d)), CsPbBr3 QDs (APS) (e) and CsPbBr3 QDs (APS)/BP NSs (f)[86]
OA—Oleic acid; OAm—Oleylamine; APS—Modified ligand 3-aminopropyltriethoxysilane with glutaric anhydride; T1-T3—Time; A1, A2—Charge transfer contribution
图 9 (a) CsPbBr3 钙钛矿量子点 (PQDs) 和CsPbBr3/聚苯胺 (PANI)复合电极在Na2SO4水溶液(0.1 mol/L，pH=6.8)中的瞬态光电流响应；(b) CsPbBr3 PQDs和CsPbBr3/PANI复合材料的电化学阻抗谱(EIS)[90]；(c) 电流测量电流密度-时间曲线；(d) EIS奈奎斯特图[93]
Figure 9. (a) Transient photocurrent responses of CsPbBr3 perovskite quantum dots (PQDs) and CsPbBr3/polyaniline (PANI) composite electrodes in Na2SO4 aqueous solution (0.1 mol/L, pH=6.8); (b) Electrochemical impedance spectra (EIS) of CsPbBr3 PQDs and the CsPbBr3/PANI composite[90]; (c) Amperometric current density-time curves; (d) EIS Nyquist plots[93]
P3 HT—Poly(3-hexylthiophene-2,5-diyl); Z''—Imaginary reactance of impedance Z; Z'—Real part resistance of impedance Z
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