Isolating Single Sn Atoms in CuO Mesocrystal to Form Ordered Atomic Interfaces: An Effective Strategy for Designing Highly Efficient Mesocrystal Catalysts

TY - JOUR

T1 - Isolating Single Sn Atoms in CuO Mesocrystal to Form Ordered Atomic Interfaces: An Effective Strategy for Designing Highly Efficient Mesocrystal Catalysts

AU - Ji, Yongjun

AU - Zhou, Hui

AU - Liu, Shaomian

AU - Kang, Ting

AU - Zhang, Yu

AU - Chen, Wenxing

AU - Fu, Dongxing

AU - Zhong, Ziyi

AU - Xu, Guangwen

AU - Gong, Xue‐Qing

AU - Su, Fabing

PY - 2022/9/26

Y1 - 2022/9/26

N2 - 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.

AB - 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.

KW - electron transfer

KW - high-efficiency catalysts

KW - metal oxide mesocrystals

KW - ordered atomic interfaces

KW - single atoms

U2 - 10.1002/smll.202203658

DO - 10.1002/smll.202203658

M3 - 文章

C2 - 36161498

SN - 1613-6810

JO - Small

JF - Small

ER -