Recent Advances in Graphitic Carbon Nitride Supported Single-Atom Catalysts for Energy Conversion
Recent Advances in Graphitic Carbon Nitride Supported Single-Atom Catalysts for Energy Conversion
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石墨碳氮化物负载单原子能量转换催化剂的最新进展
DOI：
10.1002/cctc.202001517
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发表时间：
2021
期刊：
影响因子：
4.5
通讯作者：
Zhang Hongjie
中科院分区：
文献类型：
--
作者：
Zhao Meng;Feng Jing;Yang Weiting;Song Shuyan;Zhang Hongjie
单原子催化剂是催化领域最具活力的前沿研究领域之一，由于独特的配位环境、高原子利用率、高活性和选择性，在多种化学反应中表现出独特的性能。然而，催化剂颗粒尺寸的减小伴随着表面能的急剧增加，因此超小的颗粒很容易形成纳米团簇的聚集，无法保持原子级的分散性。保护催化位点的关键因素是调控单原子与底物之间的相互作用。作为最有前途的稳定孤立金属原子的二维载体之一，石墨碳氮化物因其存在丰富的吡啶类氮原子来牢固锚定金属中心以及源自碳与邻近氮原子之间相互作用引起的电子重排的独特结构而被广泛研究。在这篇综述中，我们系统地概括了石墨氮化碳负载的孤立单原子催化剂的可控合成、理论计算、表征和应用，最后根据当前的实验和计算工作，总结了这一新兴领域的前景和挑战。
Single‐atom catalysts are one of the most energetic frontier research fields of catalysis, which exhibit distinctive performance for diverse chemical reactions due to the unique coordination environment, high atomic utilization, high activity and selectivity. Nevertheless, the size decrease of catalyst particles is accompanied with the sharply increased surface energy, thus ultra‐small particles are easy to form aggregation of nanoclusters and cannot maintain the atomic level dispersion. The key factor to protect catalytic sites is to regulate and control the interaction between single atoms and the substrate. As one of the most promising two‐dimensional supports to stabilize the isolated metal atoms, graphitic carbon nitride has been widely studied owing to the existence of abundant pyridine‐like nitrogen atoms for strongly anchoring metal centers and the distinct structure originating from electron rearrangement caused by the interaction between carbon and neighbor nitrogen atoms. In this review, we systematically generalize the controllable syntheses, theoretical calculations, characterizations and applications of graphitic carbon nitride supported isolated single‐atom catalysts, and finally, the prospects and challenges in this emergent field are featured on the basis of current experimental and computational efforts.