用于人工光合作用和环境修复的基于石墨化氮化碳（gC <sub>3</sub> N <sub>4</sub>）的光催化剂：我们是否更接近实现可持续性？,Chemical Reviews

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用于人工光合作用和环境修复的基于石墨化氮化碳（gC ₃ N ₄）的光催化剂：我们是否更接近实现可持续性？
Chemical Reviews ( IF 51.4 ) Pub Date : 2016-05-20 00:00:00 , DOI: 10.1021/acs.chemrev.6b00075
Wee-Jun Ong ₁ , Lling-Lling Tan ₁ , Yun Hau Ng ₂ , Siek-Ting Yong ₁ , Siang-Piao Chai ₁

Affiliation

作为一种令人着迷的共轭聚合物，石墨碳氮化物（gC ₃ N ₄）已成为新的研究热点，并在太阳能转化和环境修复领域作为无金属和可见光响应的光催化剂受到了跨学科的关注。这是由于其引人注目的电子带结构，较高的理化稳定性和“丰富的地球”性质。这篇重要的评论总结了有关基于原始gC ₃ N ₄和基于gC ₃ N ₄的纳米复合材料的设计和构建的最新进展的全景，包括（1）裸gC ₃ N ₄的纳米体系结构设计，例如硬和软模板方法，超分子预组装，剥离和无模板合成路线；（2）gC ₃ N ₄在原子级（元素掺杂）和分子级（共聚合）的功能化；以及（3）用另一种半导体或金属作为助催化剂的能级非常匹配的方法对gC ₃ N ₄进行修饰，以形成异质结纳米结构。将严格审查异质结体系每个分类的结构和特征，即金属-gC ₃ N ₄，半导体-gC ₃ N ₄，同型gC ₃ N ₄ / gC₃ N ₄，石墨碳-gC ₃ N ₄，导电聚合物-gC ₃ N ₄，敏化剂-gC ₃ N ₄和多组分异质结。基于第一原理密度泛函理论（DFT）的计算，理论上还将讨论基于gC ₃ N ₄的异质结构纳米杂化物的能带结构，电子性质，光吸收和界面电荷转移，从而提供有关电荷载流子动力学的深刻见解。除此之外，多功能光氧化还原技术在人工光合作用（CO _2的水分解和光固定化）方面的进展），环境净化和细菌消毒将被详细介绍。最后但并非最不重要的一点是，本文将对本研究平台最前沿的挑战和未来方向进行总结并提出一些令人振奋的观点，从而对本次综述进行总结。可以预期，本综述可以通过利用出色的结构，电子和光学特性，为可持续发展的未来发展而又不损害环境，激发新的研究途径，以促进具有改进性能的下一代基于gC ₃ N ₄的光催化剂。

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Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

As a fascinating conjugated polymer, graphitic carbon nitride (g-C₃N₄) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C₃N₄ and g-C₃N₄-based nanocomposites, including (1) nanoarchitecture design of bare g-C₃N₄, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C₃N₄ at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C₃N₄ with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The construction and characteristics of each classification of the heterojunction system will be critically reviewed, namely metal-g-C₃N₄, semiconductor-g-C₃N₄, isotype g-C₃N₄/g-C₃N₄, graphitic carbon-g-C₃N₄, conducting polymer-g-C₃N₄, sensitizer-g-C₃N₄, and multicomponent heterojunctions. The band structures, electronic properties, optical absorption, and interfacial charge transfer of g-C₃N₄-based heterostructured nanohybrids will also be theoretically discussed based on the first-principles density functional theory (DFT) calculations to provide insightful outlooks on the charge carrier dynamics. Apart from that, the advancement of the versatile photoredox applications toward artificial photosynthesis (water splitting and photofixation of CO₂), environmental decontamination, and bacteria disinfection will be presented in detail. Last but not least, this comprehensive review will conclude with a summary and some invigorating perspectives on the challenges and future directions at the forefront of this research platform. It is anticipated that this review can stimulate a new research doorway to facilitate the next generation of g-C₃N₄-based photocatalysts with ameliorated performances by harnessing the outstanding structural, electronic, and optical properties for the development of a sustainable future without environmental detriment.

更新日期：2016-05-20

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