g-C3N4光催化材料的第一性原理研究

郄佳; 李明; 刘利; 梁英华; 崔文权*

doi:10.7536/PC160623

化学进展 ›› 2016, Vol. 28 ›› Issue (10) :1569-1577 DOI: 10.7536/PC160623

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g-C₃N₄光催化材料的第一性原理研究

郄佳, 李明, 刘利, 梁英华, 崔文权*

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Research of Photocatalyst g-C₃N₄ Using First Principles

Qie Jia, Li Ming, Liu Li, Liang Yinghua, Cui Wenquan*

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摘要

能源短缺和环境恶化是人类社会快速发展面临的重大难题。太阳能作为一种清洁无污染的理想新型能源，具有取之不尽、用之不竭的特点，是实现可持续发展的最佳能源选择。半导体光催化可以直接利用太阳光进行催化反应，得到了广泛关注。作为一种低成本无金属光催化剂，g-C₃N₄具有独特的电子能带结构、优良的化学稳定性和热力学稳定性，在光催化领域如分解水制氢制氧、降解有机污染物、CO₂还原、抗菌和有机官能团选择性转换等方面表现出巨大的应用前景。目前g-C₃N₄光催化剂存在着如比表面积小、可见光利用率低、量子产率低和光生载流子易复合等问题，制约了其在光催化领域的应用。因此，提升g-C₃N₄光催化性能是光催化研究领域的重要课题。第一性原理具有半经验方法不可比拟的优势，已成为光催化研究领域计算和模拟的重要基础。基于密度泛函理论的第一性原理在光催化领域的广泛应用，为有效迅速地探求能够改善g-C₃N₄光催化性能的方法提供了明确的研究手段。本文从理论计算的角度综述了近年来在g-C₃N₄改性方面所取得的一些重要研究进展，主要包括元素掺杂、复合和形貌调控等改性手段。本文以g-C₃N₄改性光催化剂为研究对象，从电子性质、能带结构、光学性质和缺陷形成能的角度阐述了各种改性手段提高光催化活性的微观机理。最后，在总结前文所述各类改性研究的基础上，对g-C₃N₄改性光催化剂未来的发展趋势作出了展望。

Abstract

Energy shortage and environmental deterioration are the difficult problems now confronting us in the development of human society. As one of the best and new type energy which is clean, renewable and zero-pollution, solar energy is the best choice to achieve sustainable development, because it is an inexhaustible energy source. The issue that semiconductor photocatalysis can use solar light directly to conduct the photocatalytic reaction has aroused widely public concern. As a kind of low cost and non-metal photocatalyst, graphitic carbon nitride (g-C₃N₄) shows great application prospects in decomposition of water into hydrogen and oxygen, photocatalytic degradation of organic pollutants, carbon dioxide reduction, antibacterial, selective conversion of organic functional groups, as well as other fields, for its unique electronic band structure, thermal and chemical stability. But at present, g-C₃N₄ photocatalyst still exists some problems such as small specific surface area, low visible light utilization rate, low light quantum yield, and easy recombination of photo-generated carriers which restrict its application in the field of photocatalysis. Therefore, it has become a key subject in the field of photocatalytic research to improve the photocatalytic activity of g-C₃N₄. The first principles have the incomparable advantages over semi empirical method, which have become an important basis for the calculation and simulation in the field of photocatalytic research. The wide application of first principles based on density functional theory in the field of photocatalysis provides a clear research means to explore the method to improve the photocatalytic activity of g-C₃N₄ effectively and quickly. In this review, some important research progress in g-C₃N₄ modification in recent years is reviewed from the theoretical point of view, including element doping modification, composite modification, morphology control modification and other means of modification. The microscopic mechanism of improved photocatalytic activity of g-C₃N₄ modified photocatalyst is studied, from the point of view of electronic properties, band structure, optical properties and defect formation energy. Finally, on the basis of summarizing various of the modification research mentioned above, the future development trend of g-C₃N₄ modified photocatalyst is discussed.

Contents
1 Introduction
2 Molecular model and band structure of g-C₃N₄
2.1 Molecular model of g-C₃N₄
2.2 Band structure of g-C₃N₄
3 Modification research of g-C₃N₄
3.1 Doping modification
3.2 Composite modification
3.3 Morphology control modification
3.4 Other modification research
4 Conclusion

Graphical abstract

关键词

光催化 / g-C₃N₄ / 密度泛函理论 / 第一性原理

Key words

photocatalytic / g-C₃N₄ / density functional theory / first principles

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郄佳, 李明, 刘利, 梁英华, 崔文权*. g-C₃N₄光催化材料的第一性原理研究[J]. 化学进展, 2016, 28(10): 1569-1577 DOI:10.7536/PC160623

Qie Jia, Li Ming, Liu Li, Liang Yinghua, Cui Wenquan*. Research of Photocatalyst g-C₃N₄ Using First Principles[J]. Progress in Chemistry, 2016, 28(10): 1569-1577 DOI:10.7536/PC160623

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