Isolating Single Sn Atoms in CuO Mesocrystal to Form Ordered Atomic Interfaces: An Effective Strategy for Designing Highly Efficient Mesocrystal Catalysts.
Isolating Single Sn Atoms in CuO Mesocrystal to Form Ordered Atomic Interfaces: An Effective Strategy for Designing Highly Efficient Mesocrystal Catalysts.
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DOI：
10.1002/smll.202203658
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发表时间：
2022-09
期刊：
影响因子：
13.3
通讯作者：
Yongjun Ji;Huiyang Zhou;Shaomian Liu;Ting Kang;Yu Zhang-;Wenxing Chen;Dongxing Fu;Z. Zhong;
中科院分区：
文献类型：
--
作者：
Yongjun Ji;Huiyang Zhou;Shaomian Liu;Ting Kang;Yu Zhang-;Wenxing Chen;Dongxing Fu;Z. Zhong;
在原子水平上调节介晶的电子结构是获得前所未有的性能的有效途径。在这里，晶格限制的策略，以获得孤立的单位点锡原子在氧化铜介晶，以提高催化性能的报告。Sn/CuO介晶复合材料（Sn/CuOMC）具有有序的Sn-O-Cu原子界面，这源于CuO介晶本身的长程有序。X射线吸收精细结构测试证实，Sn/CuO MC中带正电荷的Sn原子对Cu原子的电子结构有一定的调节作用，这与传统的单原子Sn修饰的CuO纳米颗粒和纳米SnO 2修饰的CuO介晶催化剂中的电子结构有很大不同.在硅氢氯化反应制备三氯氢硅的实验中，Sn/CuO MC表现出明显优于上述两种催化剂的性能。理论计算进一步揭示了活性Cu组分的电子修饰和诱导的HCl吸附的改善，从而提高催化剂的性能。这项工作演示了如何设计有效的金属氧化物介晶催化剂，通过电子结构修饰的方法。
Tuning the electronic structures of mesocrystals at the atomic level is an effective approach to obtaining unprecedented properties. Here, a lattice-confined strategy to obtain isolated single-site Sn atoms in CuO mesocrystals to improve catalytic performance is reported. The Sn/CuO mesocrystal composite (Sn/CuO MC) has ordered Sn-O-Cu atomic interfaces originated from the long-range ordering of the CuO mesocrystal itself. X-ray absorption fine structure measurements confirm that the positively charged Sn atoms can tune the electronic structure of the Cu atoms to some extent in Sn/CuO MC, quite different from that in the conventional single-atom Sn-modified CuO nanoparticles and nanoparticulate SnO2 -modified CuO mesocrystal catalysts. When tested for the Si hydrochlorination reaction to produce trichlorosilane, Sn/CuO MC exhibits significantly better performances than the above two catalysts. Theoretical calculations further reveal the electronic modification to the active Cu component and the induced improvement in HCl adsorption, and thus enhance the catalytic performance. This work demonstrates how to design efficient metal oxide mesocrystal catalysts through an electronic structure modification approach.