Progress and Prospects of Non-Metal Doped Graphitic Carbon Nitride for Improved Photocatalytic Performances

Citation: Wang Yiqing, Shen Shaohua. Progress and Prospects of Non-Metal Doped Graphitic Carbon Nitride for Improved Photocatalytic Performances[J]. Acta Physico-Chimica Sinica, 2020, 36(3): 1905080-0. doi: 10.3866/PKU.WHXB201905080 shu

非金属掺杂石墨相氮化碳光催化的研究进展与展望

王亦清 ,
沈少华 ^,

.
西安交通大学，动力工程多相流国家重点实验室，国际可再生能源研究中心，西安710049

作者简介:
Shaohua Shen is currently a full professor at Xi'an Jiaotong University, China. He obtained his Ph.D. degree in thermal engineering in 2010 from Xi'an Jiaotong University. During 2008–2009 and 2011–2012, he worked as a guest researcher at Lawrence Berkeley National Laboratory and a postdoctoral researcher at the University of California at Berkeley. His research interests include photocatalytic and photoelectrochemical solar energy conversion;

通讯作者: 沈少华, shshen_xjtu@mail.xjtu.edu.cn

基金项目:
国家自然科学基金 21875183

国家自然科学基金 51672210

国家自然科学基金(21875183, 51672210, 51888103)资助项目

国家自然科学基金 51888103

摘要: 自从Fujishima和Honda利用TiO₂光阳极和Pt电极成功实现太阳能光电化学分解水之后，光催化被认为是解决环境污染和能源短缺两大问题最有前景的方法之一，因为该技术可以有效的利用太阳能这种地球上最丰富的能源来驱动多种不同的催化反应实现能源生产和环境净化，比如：水分解、CO₂还原、有机污染物降解和有机合成等。除了金属氧化物、金属硫化物和金属氮氧化物等多类金属化合物半导体光催化剂，近几年，石墨相氮化碳(g-C₃N₄)因其原料来源广泛、无毒、稳定以及相对较窄的带隙(2.7 eV)而具备可见光响应等特点，在光催化领域获得了广泛的重视。然而，g-C₃N₄对太阳光谱中可见光的吸收效率较低且光生电子和空穴复合严重，导致其光催化活性处于较低水平。至今，研究人员已经开发出多种提高g-C₃N₄光催化活性的方法，如元素掺杂、微纳结构和异质结构设计和助催化剂修饰等。元素掺杂被证明是调节g-C₃N₄独特电子结构和分子结构的有效方法，可以大幅扩展其光响应范围，并促进光生电荷分离。特别地是，非金属元素掺杂以提高g-C₃N₄的光催化活性已经得到很好的研究。通常用于掺杂g-C₃N₄的非金属元素是氧(O)、磷(P)、硫(S)、硼(B)、卤素(F、Cl、Br、I)和其他非金属元素(如碳(C)和氮(N)自掺杂)，因为这些非金属元素有着易于获取的原材料并可以较为简单的引入g-C₃N₄骨架结构中。在这篇综述文章中，作者首先介绍了g-C₃N₄的结构和光学性质，接着简要介绍了光催化剂的g-C₃N₄的改性；然后详细回顾了非金属掺杂改善g-C₃N₄光催化活性的进展，同时总结了光催化机理以期更好地理解光催化的本质并指导新型g-C₃N₄光催化剂的开发。最后，对g-C₃N₄光催化剂的后续研究进行了展望。

关键词:

English

Progress and Prospects of Non-Metal Doped Graphitic Carbon Nitride for Improved Photocatalytic Performances

Wang Yiqing ,
Shen Shaohua ^,

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an 710049, P. R. China

Author Bio: Shaohua Shen is currently a full professor at Xi'an Jiaotong University, China. He obtained his Ph.D. degree in thermal engineering in 2010 from Xi'an Jiaotong University. During 2008–2009 and 2011–2012, he worked as a guest researcher at Lawrence Berkeley National Laboratory and a postdoctoral researcher at the University of California at Berkeley. His research interests include photocatalytic and photoelectrochemical solar energy conversion;

Corresponding author: Shen Shaohua, shshen_xjtu@mail.xjtu.edu.cn

Received Date: 28 May 2019
Accepted Date: 15 July 2019
Revised Date: 15 July 2019
Available Online: 15 March 2020
Fund Project:
the National Natural Science Foundation of China 21875183

the National Natural Science Foundation of China 51672210

The project was supported by the National Natural Science Foundation of China (21875183, 51672210, 51888103)

the National Natural Science Foundation of China 51888103

Abstract: Since Fujishima and Honda demonstrated the photoelectrochemical water splitting on TiO₂ photoanode and Pt counter electrode, photocatalysis has been considered as one of the most promising technologies for solving both the problems of environmental pollution and energy shortage. This process can effectively use solar energy, the most abundant energy resource on the earth, to drive various catalytic reactions, such as water splitting, CO₂ reduction, organic pollutant degradation, and organic synthesis, for energy generation and environmental purification. Except for the various metal-based semiconductors, such as metal oxides, metal sulfides, and metal oxynitrides, developed for photocatalysis, graphitic carbon nitride (g-C₃N₄) has attracted significant attention in the recent years because of its earth abundancy, non-toxicity, good stability, and relatively narrow band gap (2.7 eV) for visible light response. However, g-C₃N₄ suffers from insufficient absorption of visible light in the solar spectrum and rapid recombination of photogenerated electrons and holes, thus resulting in low photocatalytic activity. Until now, various strategies have been developed to enhance the photocatalytic activity of g-C₃N₄, including element doping, nanostructure and heterostructure design, and co-catalyst decoration. Among these methods, element doping has been found to be very effective for adjusting the unique electronic and molecular structures of g-C₃N₄, which could significantly expand the range of photoresponse under visible light and improve the charge separation. Especially, non-metal doping has been well investigated frequently to improve the photocatalytic activity of g-C₃N₄. The non-metal dopants commonly used for the doping of g-C₃N₄ include oxygen (O), phosphorus (P), sulfur (S), boron (B), and halogen (F, Cl, Br, I) and also carbon (C) and nitrogen (N) (for self-doping), as they are easily accessible and can be introduced into the g-C₃N₄ framework through different physical and chemical synthetic methods. In this review article, the structural and optical properties of g-C₃N₄ is introduced first, followed by a brief introduction to the modification of g-C₃N₄ as photocatalysts. Then, the progress in the non-metal doped g-C₃N₄ with improved photocatalytic activity is reviewed in detail, with the photocatalytic mechanisms presented for easy understanding of the fundamentals of photocatalysis and for guiding in the design of novel g-C₃N₄ photocatalysts. Finally, the prospects of the modification of g-C₃N₄ for further advances in photocatalysis is presented.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

非金属掺杂石墨相氮化碳光催化的研究进展与展望

通讯作者: 沈少华, shshen_xjtu@mail.xjtu.edu.cn

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Progress and Prospects of Non-Metal Doped Graphitic Carbon Nitride for Improved Photocatalytic Performances

Corresponding author: Shen Shaohua, shshen_xjtu@mail.xjtu.edu.cn

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