基于超薄纳米结构的光催化二氧化碳选择性转化

doi:10.15541/jim20210368

无机材料学报 ›› 2022, Vol. 37 ›› Issue (1): 3-14.DOI: 10.15541/jim20210368

所属专题：【能源环境】CO2绿色转换； 2022年度中国知网高下载论文

基于超薄纳米结构的光催化二氧化碳选择性转化

高娃¹(), 熊宇杰², 吴聪萍¹^,³^,⁴(), 周勇¹^,³(), 邹志刚¹^,³^,⁴

1.南京大学物理学院, 南京 210093
2.中国科学技术大学化学与材料科学学院, 合肥 230026
3.昆山创新研究院, 昆山 215300
4.江苏延长桑莱特新能源有限公司, 昆山 215300

收稿日期:2021-06-10 修回日期:2021-07-30 出版日期:2022-01-20 网络出版日期:2021-07-20
通讯作者: 周勇, 教授. E-mail: zhouyong1999@nju.edu.cn; 吴聪萍, 高级工程师. E-mail: cpwu@nju.edu.cn
作者简介:高娃(1994-), 女, 博士研究生. E-mail: dz1622007@smail.nju.edu.cn
基金资助:
科技部国家重点研发计划国家自然科学基金重点项目(2018YFE0208500);国家自然科学基金(51972164);国家自然科学基金(21972065);国家自然科学基金(21773114);先进能源科学与技术广东省实验室佛山仙湖实验项目(XHD2020-002);中国科学技术大学合肥微尺度物质科学国家研究中心开放课题(KF2020006)

Recent Progress on Photocatalytic CO₂ Reduction with Ultrathin Nanostructures

GAO Wa¹(), XIONG Yujie², WU Congping¹^,³^,⁴(), ZHOU Yong¹^,³(), ZOU Zhigang¹^,³^,⁴

1. School of Physics, Nanjing University, Nanjing 210093, China
2. School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China
3. Kunshan Institute of Innovation, Kunshan 215300, China
4. Jiangsu Yanchang Sunlaite Group, Kunshan 215300, China

Received:2021-06-10 Revised:2021-07-30 Published:2022-01-20 Online:2021-07-20
Contact: ZHOU Yong, professor. E-mail: zhouyong1999@nju.edu.cn; WU Congping, senior engineer. E-mail: cpwu@nju.edu.cn
About author:GAO Wa (1994-), female, PhD candidate. E-mail: dz1622007@smail.nju.edu.cn
Supported by:
National Key Research and Development Program of the Ministry of Science and Technology of China(2018YFE0208500);National Natural Science Foundation of China(51972164);National Natural Science Foundation of China(21972065);National Natural Science Foundation of China(21773114);Foshan Xianhu Experiment Project of Guangdong Laboratory of Advanced Energy Science and Technology(XHD2020-002);Hefei National Laboratory for Physical Sciences at the Microscale(KF2020006)

摘要/Abstract

摘要：

21世纪以来, 能源短缺和环境污染一直是人类面临的重大挑战｡光催化二氧化碳(CO₂)还原, 通过半导体捕获光能, 获得碳氢化合物太阳能燃料是解决能源危机并推动碳循环的有前景的策略之一｡然而, 活性低､产物选择性差又极大地限制了这一技术的实际应用｡因此, 调控产物选择性并提高光催化效率、加深对CO₂还原反应机理的理解具有重要意义｡近年来, 超薄材料以其较高的比表面积, 丰富的不饱和配位的表面原子, 较短的电荷从内部到表面的迁移路径, 以及可裁剪的能带结构受到了广泛关注, 并在光催化CO₂还原领域取得了可喜的成果｡本文在总结光催化CO₂还原反应机理的基础上, 介绍了通过构建异质结构、设计Z型系统、引入助催化剂以及缺陷工程等策略促进超薄纳米结构电子空穴分离和调控其电荷迁移路径的研究成果, 并指出了提高光催化CO₂还原效率和优化产物选择性的发展前景与挑战｡

关键词: 光催化CO₂还原, 超薄异质结构, 助催化剂, 反应机理, 综述

Abstract:

Since the beginning of the 21st century, energy shortage and environmental pollution have been the major challenges faced by human beings. Photocatalytic carbon dioxide (CO₂) reduction is one of the promising strategies to solve the energy crisis and promote the carbon cycle, in which semiconductor captures solar energy to obtain hydrocarbon fuel. However, the low activity and poor selectivity of the products greatly limit the practical application of this technology. Thus, it is of great significance to regulate product selectivity, improve photocatalytic efficiency, and deeply understand the mechanism of CO₂ reduction reaction. In recent years, ultrathin materials have attracted extensive attention from researchers due to their high specific surface area, abundant unsaturated coordination surface atoms, shortened charge migration path from inside to surface, and tailorable energy band structure, and have achieved promising results in the field of photocatalytic CO₂ reduction. In this paper, the reaction mechanism of photocatalytic CO₂ reduction is firstly summarized. Next, the research results of promoting electron hole separation and regulating charge transport path of ultrathin nanostructures by constructing heterostructures, designing Z-scheme systems, introducing co-catalysts, and defect engineering are introduced. Finally, the prospect and challenge of improving the efficiency of photocatalytic CO₂ reduction and optimizing the product selectivity are pointed out.

Key words: photocatalytic CO₂ reduction, ultrathin heterostructures, cocatalysts, reaction mechanism, review

中图分类号:

TQ174

高娃, 熊宇杰, 吴聪萍, 周勇, 邹志刚. 基于超薄纳米结构的光催化二氧化碳选择性转化[J]. 无机材料学报, 2022, 37(1): 3-14.

GAO Wa, XIONG Yujie, WU Congping, ZHOU Yong, ZOU Zhigang. Recent Progress on Photocatalytic CO₂ Reduction with Ultrathin Nanostructures[J]. Journal of Inorganic Materials, 2022, 37(1): 3-14.

图/表 12

图1 CO2吸附在光催化剂表面的不同模式[4]

Fig. 1 Different CO2 adsorption modes on the surface of photocatalysts[4]

表1 在标准条件下(1.01×105 Pa和25 ℃)将水溶液中的CO2转化为各种C1和C2产物的标准电位[34]

Table 1 Standard potentials of convert CO2 to various C1 and C2 products in aqueous solutions at standard conditions (1.01×105 Pa and 25 ℃) [34]

Half electrochemical thermodynamic reactions	Standard potential /V (vs SHE)
CO₂(g) + 2H⁺ + 2e^- = HCOOH(1)	-0.250
CO₂(g) + 2H⁺ + 2e^- = CO(g)+ H₂O (1)	-0.106
2CO₂(g) + 2H⁺ + 2e^- = H₂C₂O₄(aq)	-0.500
2CO₂(g) + 2e^- = C₂O₄^2-(aq)	-0.590
CO₂(g) + 4H⁺ + 4e^- = C(s) + 2H₂O(1)	0.210
CO₂(g) + 4H⁺ + 4e^- = CH₂O(1) + H₂O(1)	-0.070
CO₂(g) + 6H⁺ + 6e^- = CH₃OH(1) + H₂O(1)	0.016
CO₂(g) + 8H⁺ + 8e^- = CH₄(g) + 2H₂O(1)	0.169
2CO₂(g) + 12H⁺ + 12e^- = CH₂CH₂(g) + 4H₂O(1)	0.064
2CO₂(g) + 12H⁺ + 12e^- = CH₃CH₂OH(1) + 3H₂O(1)	0.084

图2 CO2还原为HCHO、CH3OH和CH4的可能反应路线[35,36]

Fig. 2 Possible reaction paths for CO2 reduction to produce HCHO, CH3OH, and CH4[35,36] (A) A thermodynamic analysis; (B) A combined thermodynamic and kinetic analysis; (C) Glyoxal route

图3 CO2还原为C2H4、CH3CHO和C2H5OH的可能反应路线[35]

Fig. 3 Possible reaction paths for CO2 reduction to produce C2H4, CH3CHO, and C2H5OH[35] (A) Coupling of two *CH2 species or CO insertion in a Fischer-Tropsch-like step; (B) *CO dimerization

图4 (a)计算的WO3纳米片和商用WO3粉末相对于CO2/CH4氧化还原电位的能带位置, (b)可见光照射下WO3纳米片和商品粉末的CH4产量随时间的变化(λ≥420 nm)[38]

Fig. 4 (a) Calculated band positions of the WO3 nanosheet and commercial WO3, relative to the redox potential of CO2/CH4 in the presence of water, and (b) CH4 generation over the nanosheet and commercial powder as a function of visible light irradiation time (λ≥420 nm)[38]

图5 (a)原子薄的InVO4纳米片, (b)InVO4纳米立方体, 和(c)固相烧结InVO4样品的高度图像; (a’)、(b’)和(c’)中的表面光电压图像是光照条件下和暗态下图像之间的差值图像; (d)表面光电压变化, 由暗条件下的电势减去光照条件下的电势(ΔCPD = CPDdark - CPDlight)[13]

Fig. 5 Height images of (a) atomically thin InVO4 nanosheet, (b) nanocube, and (c) bulk materials obtained by conventional solid-state reaction, surface photovoltage spectroscopy (SPV) images in (a′), (b′), and (c′) displaying differential images between potential images under light and in the dark, and (d) surface photovoltage change by subtracting the potential under dark conditions from that under illumination (SPV, ΔCPD = CPDdark - CPDlight)[13]

图6 PCMT@In2O3/ZIS的能带结构[47]

Fig. 6 Band structures of PCMT@In2O3/ZIS[47]

图7 光催化(a)CO和(b)CH4的产量随光照时间的变化; (c)不同样品的光催化活性比较; (d)ZnIn2S4/BiVO4纳米复合材料光催化CO2还原示意图; (e)Z型电子/空穴转移机制示意图; (f)光辐照下异质结型电子空穴转移机制[50]

Fig. 7 Photocatalytic (a) CO and (b) CH4 output changing with light irradiation time, (c) comparison of photocatalytic activity over different samples, (d)schematic illustration of the photocatalytic CO2 reduction for ZnIn2S4/BiVO4 nanocomposite, schematic representation of (e) Z-scheme electron-hole transfer mechanisms, and (f) heterojunction-type electron-hole transfer mechanisms under light irradiation[50]

图8 (a, b)聚甲基丙烯酸甲酯球包覆(PEI/Ti0.91O2/PEI/GO)5, (c, d)(G-Ti0.91O2)5空心球的TEM照片, (e)产物产率的比较[53]

Fig. 8 TEM images of (a, b) poly(methylmethacrylate) spheres coated with (protonic polyethylenimine (PEI)/Ti0.91O2/ PEI/GO)5, (c, d) (G-Ti0.91O2)5 hollow spheres, and (e)comparation of the average product formation rates[53]

图9 (a, b)高倍率下InVO4/Ti3C2Tx的SEM照片, (c)InVO4/ Ti3C2Tx的HRTEM照片, (d)InVO4/Ti3C2Tx杂化体系中, CO2光催化还原过程中的空间电荷分离和传输方案, (e)InVO4/ Ti3C2Tx的能级结构[56]

Fig. 9 (a, b) SEM images of InVO4/Ti3C2Tx at higher magnification, (c) HRTEM images of InVO4/Ti3C2Tx, (d)scheme for spatial charge separation and transport during the photocatalytic reduction of CO2 over hierarchical InVO4/Ti3C2Tx heterosystem, and (e)energy level alignment of InVO4/Ti3C2Tx hybrid[56]

图10 (a) Au-TiO2复合材料的制备过程示意图, (b) Au-TiO2体系中电荷分离和转移及CO2光还原成不同产物的示意图[57]

Fig. 10 Schematic illustration of the preparation procedure of the Au-TiO2 composites (b), schematic illustration of charge separation and transfer in the Au-TiO2 system and photoreduction of CO2 into different products[57]

图11 (a)富氧空位WO3原子层和WO3原子层的电子能带结构示意图和(b)富氧空位WO3原子层的原位红外光谱[60]

Fig. 11 (a) Scheme of the electronic band structures of Vo-rich WO3 atomic layers and WO3 atomic layers, and (b) in situ FT-IR spectra for the IR light-driven CO2 reduction process on the Vo-rich WO3 atomic layers[60]

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基于超薄纳米结构的光催化二氧化碳选择性转化

Recent Progress on Photocatalytic CO₂ Reduction with Ultrathin Nanostructures

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基于超薄纳米结构的光催化二氧化碳选择性转化

Recent Progress on Photocatalytic CO2 Reduction with Ultrathin Nanostructures

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Recent Progress on Photocatalytic CO₂ Reduction with Ultrathin Nanostructures