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化学进展 2021, Vol. 33 Issue (8): 1331-1343 DOI: 10.7536/PC201236 前一篇   后一篇

• 综述 •

钼酸铋光催化剂的结构缺陷调控

赵依凡1, 毛琦云1, 翟晓雅1, 张国英1,2,3,*()   

  1. 1 天津师范大学化学学院 天津市功能分子结构与性能重点实验室 天津 300387
    2 山东师范大学 分子与纳米探针教育部重点实验室 济南 250014
    3 南开大学先进能源材料化学教育部重点实验室 天津 300071
  • 收稿日期:2020-12-21 修回日期:2021-02-08 出版日期:2021-08-20 发布日期:2021-03-04
  • 通讯作者: 张国英
  • 基金资助:
    山东师范大学分子与纳米探针教育部重点实验室开放基金(2018KLMNP05); 南开大学先进能源材料化学教育部重点实验室开放基金; 天津市研究生科研创新项目(2020YJSS049)
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Structural Defects Regulation of Bismuth Molybdate Photocatalyst

Yifan Zhao1, Qiyun Mao1, Xiaoya Zhai1, Guoying Zhang1,2,3()   

  1. 1 Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University,Tianjin 300387, China
    2 Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Normal University,Jinan 250014, China
    3 Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
  • Received:2020-12-21 Revised:2021-02-08 Online:2021-08-20 Published:2021-03-04
  • Contact: Guoying Zhang
  • Supported by:
    Open Foundation of Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Normal University(2018KLMNP05); Open Foundation of Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education); College of Chemistry, Nankai University and the Postgraduate and Doctoral Innovation Project of Tianjin(2020YJSS049)

钼酸铋(Bi2MoO6)作为一种新型层状光催化材料,具有成本低廉、清洁高效、带隙较窄和可见光响应等优点,在降解水体污染物、净化空气、抑菌、光解水、二氧化碳还原及固氮等领域具有广泛的应用前景,是一种极具发展潜力的Bi(Ⅲ)基半导体光催化剂。然而该材料在实际应用中还存在太阳光吸收效率较低、光生载流子复合速率较快等亟待解决的瓶颈问题。针对上述科学问题,对Bi2MoO6光催化剂进行结构缺陷调控已证明是行之有效的解决策略,本文系统阐述了近年来Bi2MoO6晶体结构缺陷工程的研究进展,主要包括各类元素掺杂、氧空位引入以及二者的伴生协同作用等,分别从制备方法和催化性能改善等角度对Bi2MoO6的缺陷研究和发展动态进行了归纳,并对其在相关应用领域的构-效关系及作用机制进行了深入探讨和总结。最后,分析了缺陷型Bi2MoO6光催化剂目前所存在的不足,并对未来的发展方向和前景进行了展望。

关键词： 钼酸铋, 缺陷调控, 离子掺杂, 氧空位, 协同效应, 光催化

As a novel type of Bi(Ⅲ)-based semiconductor photocatalyst, bismuth molybdate(Bi2MoO6) possesses the advantages of layered structure, low cost, cleanness and efficiency, narrow band gap and visible light response, etc. Resultantly, it exhibits widely potential applications in various photocatalytic areas such as degradation of water pollutants, air purification, antibacterial, water splitting, carbon dioxide reduction and nitrogen fixation. However, there are still two main bottleneck problems which would restrict the practical applications of Bi2MoO6 and needs to be addressed urgently. One is the low absorption efficiency for solar energy and the other is the fast recombination rate of photogenerated electron-hole pairs. Introduction and regulation of structure defects in Bi2MoO6 have been proved to be effective strategies to resolve the above problems. In the paper, the research progress of Bi2MoO6 defect engineering in recent years is comprehensively reviewed, including elemental doping, oxygen vacancy, synergistic effects, etc. The different methods to construct defects in Bi2MoO6 and the corresponding photocatalytic properties are extensively summarized. Also, the structure-activity relationship and action mechanism of the structural defects in different research fields are in-depth discussed and concluded. Finally, the present shortcomings of defective Bi2MoO6 photocatalyst are analyzed and the development direction and prospects in future are prospected.

Contents

1 Introduction

2 Elemental doping defect of bismuth molybdate

2.1 Rare earth ion doping

2.2 Transition metal ion doping

2.3 Non-metal ion doping

2.4 Ion co-doping strategy

3 Oxygen vacancy defect of bismuth molybdate

3.1 Ion doping associated oxygen vacancy

3.2 Individual oxygen vacancy

3.3 Oxygen vacancy synergy

4 Conclusion and outlook

Key words: bismuth molybdate, defect modulation, ion doping, oxygen vacancy, synergistic effect, photocatalysis
()
图1 (a)BMO的Aurivillius型结构[24];(b)BMO的完整及局部DOS图[26]
Fig. 1 (a) Aurivillius structure of BMO[24];(b) Complete and partial DOS diagram of BMO[26]. Copyright 2020, Elsevier; Copyright 2012, Elsevier
图2 (a)La-BMO可见光催化降解RhB的效率,(b)其从棒状向薄片结构的转变[46];(c)Sm-BMO的电子结构随掺杂量的变化[51]
Fig. 2 (a) The visible light photocatalytic efficiency of La-BMO for RhB degradation,(b) transition from rod-like to lamellar structure[46];(c) changes in the electronic structure of Sm-BMO with doping content[51]. Copyright 2018, Springer Nature; Copyright 2016, American Chemical Society.
表1 BMO的过渡金属离子掺杂研究汇总
Table 1 Summary of transition metal ions doped BMO
Ion Synthetic method Application Activity Light condition Ref.
Ti4+ Sonochemical MB/MG 90 min 99%/45min 92% 150 W Xe lamp(Visible) 58
Mn2+ Sonochemical MB/MG 90 min 70%/45 min 72% 150 W Xe lamp(Visible) 58
Cu2+ Sonochemical MB/MG 90 min 78%/45 min 90% 150 W Xe lamp(Visible) 58
Zn2+ Sonochemical MB/MG 90 min 80%/45 min 99% 150 W Xe lamp(Visible) 58
Zn2+ Hydrothermal RhB 30 min, 98.9% 240 W Xe lamp(UV-Visible) 59
Fe3+ Solvothermal N2 fixation/Cr(Ⅵ) 106.5 μmol·g-1·h-1/20 min 100% 300 W Xe lamp(Visible) 60
Fe3+ Solvothermal PE of H2O/Na2SO3 0.021%/0.018% AM 1.5(UV-Visible) 61
W6+ Solvothermal PE of H2O/Na2SO3 0.023%/0.021% AM 1.5(UV-Visible) 61
W6+ Hydrothermal RhB 140 min, 100% Xe lamp(Visible) 62
Co2+ Solvothermal RhB 120 min, 99.7% 500 W Xe lamp(Visible) 63
Pd2+ Photo-reduction Phenol 300 min, 22% 300 W halogen tungsten lamp(310~800 nm) 64
Bi3+ Hydrothermal NO removal 40 min, 55% 30 W LEDs(Visible) 65
Ru3+ Theoretical calculation 24
图3 BMO及0.5% Fe-BMO的(a)产NH3能力对比,(b)能带结构变化及(c,d)相对功函数图[60]
Fig. 3 (a) Comparison of NH3 production capacity,(b) energy band structure change and(c,d) relative work function diagrams of BMO and 0.5% Fe-BMO, respectively[60]. Copyright 2019, Elsevier
图4 BOC及Br-BOC的(a)态密度图和(b)阻抗图[19];C-BMO体系中(c)·O2-和(d)·OH的电子自旋共振(ESR)信号峰[69]
Fig. 4 (a) Density of states and(b) EIS Nyquist curves of BOC and Br-BOC[19]; ESR peaks of(c) ·O2-and(d) ·OH in C-BMO[69]. Copyright 2019, Elsevier; Copyright 2017, Wiley
图5 (a)Tb/Eu、Dy/Sm及Er/Nd的 4f电子补偿性分配示意图[83];(b)Gd/Er/Lu三掺杂BMO的光催化降解机理[84]
Fig. 5 (a) Schematic diagram of compensated distribution of 4f electrons of Tb/Eu, Dy/Sm and Er/Nd[83];(b) photocatalytic degradation mechanism over Gd/Er/Lu triple-doped BMO[84]. Copyright 2017, Elsevier; Copyright 2019, Elsevier
图6 (a)Ce掺杂 BMO体系中缺陷的形成过程示意图,(b)Ce-Vo-BMO样品的ESR光谱,(c)可见光催化降解甲基对氧磷的活性,(d)金黄色葡萄球菌的抑菌效率[99]
Fig. 6 (a) Illustration of the possible formation process of crystal defects in Ce-doped BMO structure,(b) the ESR signal of Ce-Vo-defects in Ce-doped BMO structure,(c) visible light photocatalytic degradation of methyl paraoxon, and(d) photocatalytic disinfection efficiency of staphylococcus aureus[99]. Copyright 2016, American Chemical Society
表2 单一Vo-BMO体系的构筑方法及应用领域汇总
Table 2 Summary of the construction and application of individual Vo-BMO system
Synthetic method Synthetic condition Application Ref.
solvothermal CTAB, 180 ℃,3 h Selective oxidation of BA 101
Br- induction CTAB,140 ℃,72 h,pH=6 NO removal 102
Atmosphere calcination 450 ℃,in air,2 h TC 103
Atmosphere calcination 250 ℃,in air,1 h RhB 104
Atmosphere calcination 250 ℃,in air,2 h Phenol 105
Atmosphere calcination 375 ℃,in air,2 h Phenol/4-NP 106
Chemical reduction NaBH4 + PVP,1 h NO removal 107
Chemical reduction NaBH4,pH=5 RhB/MO/Phenol 108
Reduction-reoxidation CaH2,140 ℃,12 h;250 ℃,5 h Phenol/MB 109
NaOH etching 0.05 M NaOH,20 h SMX/E. coli 110
Template direction BiOBr + Na2MoO4,50 ℃,48 h CO2 reduction/O2 evolution 111
图7 (a)水热法制备Vo-BMO分级超结构,(b)富Vo的BMO在吸附苯甲醇前后的原位FTIR光谱[101],(c)Vo-BMO超薄纳米片和BMO块体的EPR谱,(d)原子分辨率STEMI-ADF图像[111]
Fig. 7 (a) Diagram of hierarchical Vo-BMO architectures,(b) in situ FTIR spectra of Vo-rich BMO before and after benzyl alcohol adsorption[101],(c) EPR spectra of Vo-BMO ultrathin nanosheets and bulk BMO,(d) atomic resolution STEMI-ADF images[111]. Copyright 2019, Elsevier; Copyright 2019, Elsevier
图8 BMO基系列样品的(a)紫外-可见漫反射光谱,(b)瞬态光电流响应[104];Fe(Ⅲ)-Vo-BMO体系的(c)HRTEM图像,(d)光催化降解有机污染物的机理示意图[105]
Fig. 8 (a) UV-vis diffuse reflectance spectra, and(b) transient photocurrent response of BMO-based samples[104];(c) HRTEM image and(d) schematic diagram of photocatalytic degradation mechanism for organic pollutants of Fe(Ⅲ)-Vo-BMO[105]. Copyright 2018, Elsevier; Copyright 2019, Elsevier
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摘要

钼酸铋光催化剂的结构缺陷调控