Spatially separating redox centers on 2D carbon nitride with cobalt single atom for photocatalytic H2O2 production
Spatially separating redox centers on 2D carbon nitride with cobalt single atom for photocatalytic H2O2 production
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DOI：
10.1073/pnas.1913403117
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发表时间：
2020-03-24
影响因子：
11.1
通讯作者：
Kim, Jae-Hong
中科院分区：
文献类型：
--
作者：
Chu, Chiheng;Zhu, Qianhong;Kim, Jae-Hong
氧化还原助催化剂在光合反应中起着至关重要的作用，但同时负载氧化和还原助催化剂往往会导致增强的电荷重组，这是有害的光合作用。本研究介绍了一种方法，同时负载两个氧化还原助催化剂，原子分散的钴，以提高氧化活性和蒽醌，以提高还原选择性，到石墨氮化碳（C3 N4）纳米片光催化H2 O2的生产。在二维光催化剂上实现了氧化性和还原性助催化剂的空间分离，通过将钴单原子配位在C3 N4的空中心上方并将蒽醌锚定在C3 N4纳米片的边缘。这种空间分离，实验证实和计算模拟，被认为是关键的，以提高表面电荷分离，实现高效的过氧化氢生产。这种用于助催化剂的空间分离的中心/边缘策略可以应用于在光合反应中越来越多地研究的其他2D光催化剂。
Redox cocatalysts play crucial roles in photosynthetic reactions, yet simultaneous loading of oxidative and reductive cocatalysts often leads to enhanced charge recombination that is detrimental to photosynthesis. This study introduces an approach to simultaneously load two redox cocatalysts, atomically dispersed cobalt for improving oxidation activity and anthraquinone for improving reduction selectivity, onto graphitic carbon nitride (C3N4) nanosheets for photocatalytic H2O2 production. Spatial separation of oxidative and reductive cocatalysts was achieved on a two-dimensional (2D) photocatalyst, by coordinating cobalt single atom above the void center of C3N4 and anchoring anthraquinone at the edges of C3N4 nanosheets. Such spatial separation, experimentally confirmed and computationally simulated, was found to be critical for enhancing surface charge separation and achieving efficient H2O2 production. This center/edge strategy for spatial separation of cocatalysts may be applied on other 2D photo-catalysts that are increasingly studied in photosynthetic reactions.