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Promoting Dinuclear-Type Catalysis in Cu1–C3N4 Single-Atom Catalysts
Advanced Materials ( IF 27.4 ) Pub Date : 2022-06-24 , DOI: 10.1002/adma.202204638 Jingting Song 1, 2 , Zhongxin Chen 2 , Xiangbin Cai 3 , Xin Zhou 2 , Gaolei Zhan 2 , Runlai Li 2 , Pingping Wei 1, 4 , Ning Yan 1, 4 , Shibo Xi 5 , Kian Ping Loh 1, 2
Advanced Materials ( IF 27.4 ) Pub Date : 2022-06-24 , DOI: 10.1002/adma.202204638 Jingting Song 1, 2 , Zhongxin Chen 2 , Xiangbin Cai 3 , Xin Zhou 2 , Gaolei Zhan 2 , Runlai Li 2 , Pingping Wei 1, 4 , Ning Yan 1, 4 , Shibo Xi 5 , Kian Ping Loh 1, 2
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Reducing particle size in supported metal catalysts to single-atom level isolates the active metal sites and maximizes the atomic utilization efficiency. However, the large inter-atom distance, particularly in low-loading single-atom catalyst (SAC), is not favorable for a complex reaction where two (or more) reactants have to be activated. A key question is how to control the inter-atom distances to promote dinuclear-type coactivation at the adjacent metal sites. Here, it is reported that reducing the average inter-atom distance of copper SACs supported on carbon nitride (C3N4) to 0.74 ± 0.13 nm allows these catalysts to exhibit a dinuclear-type catalytic mechanism in the nitrile–azide cycloaddition. Operando X-ray absorption fine structure study reveals a dynamic ligand exchange process between nitrile and azide, followed by their coactivation on dinuclear Cu SAC sites to form the tetrazole product. This work highlights that reducing the nearest-neighbor distance of SAC allows the mechanistic pathway to diversify from single-site to multisite catalysis.
中文翻译：
促进 Cu1–C3N4 单原子催化剂中的双核型催化
将负载型金属催化剂中的粒径减小到单原子水平可以隔离活性金属位点并最大限度地提高原子利用效率。然而，大的原子间距离，特别是在低负载单原子催化剂 (SAC) 中，不利于必须活化两种（或多种）反应物的复杂反应。一个关键问题是如何控制原子间距离以促进相邻金属位点的双核型共活化。在这里，据报道，减少了负载在氮化碳（C 3 N 4 ）上的铜 SAC 的平均原子间距离) 到 0.74 ± 0.13 nm 允许这些催化剂在腈-叠氮化物环加成中表现出双核型催化机制。Operando X 射线吸收精细结构研究揭示了腈和叠氮化物之间的动态配体交换过程，然后它们在双核 Cu SAC 位点上共活化形成四唑产物。这项工作强调，减少 SAC 的最近邻距离可以使机理途径从单位点催化多样化到多位点催化。
更新日期：2022-06-24
中文翻译：
促进 Cu1–C3N4 单原子催化剂中的双核型催化
将负载型金属催化剂中的粒径减小到单原子水平可以隔离活性金属位点并最大限度地提高原子利用效率。然而，大的原子间距离，特别是在低负载单原子催化剂 (SAC) 中，不利于必须活化两种（或多种）反应物的复杂反应。一个关键问题是如何控制原子间距离以促进相邻金属位点的双核型共活化。在这里，据报道，减少了负载在氮化碳（C 3 N 4 ）上的铜 SAC 的平均原子间距离) 到 0.74 ± 0.13 nm 允许这些催化剂在腈-叠氮化物环加成中表现出双核型催化机制。Operando X 射线吸收精细结构研究揭示了腈和叠氮化物之间的动态配体交换过程，然后它们在双核 Cu SAC 位点上共活化形成四唑产物。这项工作强调，减少 SAC 的最近邻距离可以使机理途径从单位点催化多样化到多位点催化。
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