基于立方烷结构的分子催化剂在光催化水氧化中的研究进展

引用本文: 孙万军, 林军奇, 梁向明, 杨峻懿, 马宝春, 丁勇. 基于立方烷结构的分子催化剂在光催化水氧化中的研究进展[J]. 物理化学学报, 2020, 36(3): 1905025-0. doi: 10.3866/PKU.WHXB201905025 shu

Citation: Sun Wanjun, Lin Junqi, Liang Xiangming, Yang Junyi, Ma Baochun, Ding Yong. Recent Advances in Catalysts Based on Molecular Cubanes for Visible Light-Driven Water Oxidation[J]. Acta Physico-Chimica Sinica, 2020, 36(3): 1905025-0. doi: 10.3866/PKU.WHXB201905025 shu

基于立方烷结构的分子催化剂在光催化水氧化中的研究进展

孙万军 ^1,3, ,
林军奇 ^1, ,
梁向明 ^1, ,
杨峻懿 ^1, ,
马宝春 ^1, ,
丁勇 ^{1,2,
,}

1.
兰州大学化学化工学院，兰州 730000
2.
中国科学院兰州化学物理研究所，羰基合成与选择氧化国家重点实验室，兰州 730000
3.
甘肃民族师范学院化学与生命科学系，甘肃合作 747000

作者简介:

丁勇，教授，博士生导师，甘肃省飞天学者特聘教授。主要从事光催化以及光电催化水的氧化和水的还原以及多酸催化化学。2004年12月于中国科学院兰州化学物理研究所获得博士学位，之后加盟兰州大学化学化工学院。2009年12月至2011年01月在美国埃默里大学化学系访学。现任Chinese Journal of Catalysis青年编委，中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室客座研究员。至今在SCI学术刊物上发表研究论文100余篇;

通讯作者: 丁勇, dingyong1@lzu.edu.cn

基金项目:

国家自然科学基金(21773096, 21572084), 兰州大学中央高校基本科研业务费(lzujbky-2018-k08), 甘肃省自然科学基金(17JR5RA186)和甘肃省高等学校科学研究(2018A-123)项目资助

摘要: 随着化石燃料大量使用带来的气候变化和环境污染问题日趋严重，寻找清洁高效的可再生能源用做传统化石燃料的替代品，已经成为当前的研究热点。光驱动的水分解反应被认为是太阳能制氢的可行途径。水的全分解包括两个半反应-水的氧化和质子还原。其中水的氧化反应是一个涉及四个电子和四个质子转移的复杂过程，需要很高的活化能，被认为是全分解水反应的瓶颈步骤。因此，开发高效、稳定、廉价丰产的水氧化催化剂是人工光合作用突破的关键因素。立方烷具有类似自然界光合作用酶光系统Ⅱ(PSⅡ)活性中心Mn₄CaO₅簇的结构，世界各国的科学家受自然界光合作用的启发，开发出了许多基于过渡金属的立方烷结构的催化剂，常见的有锰、钴和铜等立方烷催化剂。本文简要地综述了近年来立方烷分子催化剂在光催化水氧化中的研究进展。首先介绍了立方烷基光催化水氧化反应历程，继而详细介绍了基于有机配体的立方烷配合物和全无机的多金属氧酸盐立方烷水氧化催化剂，其次是半导体(BiVO₄或聚合的氮化碳(PCN))为捕光材料复合立方烷分子催化剂的水氧化体系最新研究进展。最后总结并展望了该领域所面临的挑战及其前景。

关键词:

English

Recent Advances in Catalysts Based on Molecular Cubanes for Visible Light-Driven Water Oxidation

1.
College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, P. R. China
2.
State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, P. R. China
3.
Department of Chemistry and Life Science, Gansu Normal University for Nationalities, Hezuo 747000, Gansu Province, P. R. China

Corresponding author: Yong Ding, Email: dingyong1@lzu.edu.cn; Tel.: +86-931-8912585

Received Date: 06 May 2019
Accepted Date: 20 June 2019
Revised Date: 11 June 2019
Available Online: 15 March 2020
Fund Project:

The project was supported by the Natural Science Foundation of China (21773096, 21572084), Fundamental Research Funds for the Central Universities (lzujbky-2018-k08), Natural Science Foundation of Gansu (17JR5RA186) and Higher Education Institution Research Project of Gansu Province (2018A-123)

Abstract: Increasing climate change and environmental pollution caused by the excessive use of fossil fuels have prompted intensive research into clean and efficient renewable sources as a substitute for traditional fossil fuels. A very promising approach is to mimic the water splitting process that occurs in plants during photosynthesis, in order to convert solar energy into chemical energy. A successful water splitting reaction, which comprises two half reactions (water oxidation and the reduction of protons), can generate H₂ and O₂ from water. Hydrogen is a promising renewable energy carrier because of its clean combustion and high calorific value. Light-driven water splitting is considered to be a feasible way to transform water and solar energy into hydrogen energy. However, water oxidation is considered to be the bottleneck process of water splitting because it advances in a thermodynamically uphill manner with the involvement of 4e⁻ and 4H⁺. Inspired by the nature of Mn₄CaO₅ in photosystem Ⅱ (PS Ⅱ), the comprehensive understanding of its key features for use in active molecular water oxidation catalysts (WOCs) remains challenging. Extensive effort has been devoted to researching and manufacturing the structure and biomimicking the catalytic activity of Mn₄CaO₅ clusters that contain the Mn₃CaO₄ cubane structure, for the construction of low-cost and robust WOCs. WOCs can be divided into heterogeneous and homogeneous catalysts. Although heterogeneous WOCs are convenient for recycling and are easily prepared on a large scale, homogeneous WOCs, especially complexes based on organic ligands or polyoxometalates (POMs), have more advantages owing to their catalytic efficiency, structural modifications, and mechanistic understanding. Thus, recently, some molecules with an M₄O₄ (M = transition metals, mainly Mn, Co, Ni, and Cu) cubic structure have been reportedly used as photocatalytic WOCs. In this review, we present an overview of the most important and recent advances based on M₄O₄ cubic WOCs that contain first-row transition metal cubanes for visible light-driven water oxidation. Our main focus is on the structure of cubane catalysts, including metal complexes, POMs, and a system containing BiVO₄ or polymeric carbon nitride (PCN) as a photosensitizer, and cubic complexes as WOCs. Results have shown that the activity and stability of the catalyst can be tuned by the ligand stability, metal center, coordination environment, and other factors. This review will be helpful for designing new cubane catalysts for photocatalytic water oxidation that are highly efficient and stable.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

基于立方烷结构的分子催化剂在光催化水氧化中的研究进展

通讯作者: 丁勇, dingyong1@lzu.edu.cn

English

Recent Advances in Catalysts Based on Molecular Cubanes for Visible Light-Driven Water Oxidation

Corresponding author: Yong Ding, Email: dingyong1@lzu.edu.cn; Tel.: +86-931-8912585

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