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Experimental and theoretical investigation of the tuning of electronic structure in SnO2via Co doping for enhanced styrene epoxidation catalysis

机译：SNO2VIA CO中电子结构调整的实验和理论研究，以增强苯乙烯环氧催化催化

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摘要

Exploiting new heterogeneous catalysts composed of earth-abundant elements for various organic transformations under moderate reaction conditions is of vital importance in modern synthetic chemistry. Herein, we report an effective strategy for the tuning of electronic structure in SnO2, which leads to a huge boost in the styrene epoxidation reaction (SER) performance. Combined experimental and theoretical analyses highlight the validity of Co doping strategy in the manipulation of the electronic structure of SnO2 to achieve the decrease of oxygen vacancy (OV) formation energy, modulation of Sn valence state and adjustment of Sn–O interactions. The Sn2+–OV–Co–O species are proposed as the active sites, contributing to the activation of tert-butyl hydroperoxide and coordination of styrene. This work serves as a guideline for the performance enhancement of selective oxidation of aromatics via introducing hetero-atom doping strategy in the metal oxide catalyst system.
机译：在中等反应条件下，利用由地球的各种有机转化组成的新的异质催化剂在现代合成化学中至关重要。 在此，我们报告了SNO2中电子结构调整的有效策略，这导致了苯乙烯环氧反应（SER）的巨大提升。 合并的实验和理论分析突出了CO掺杂策略在操纵SNO2电子结构方面的有效性，以实现氧气空位（OV）形成能量的降低，SN价状态的调节和SN -O相互作用的调整。 SN2+–OV – Co-O物种被提出为活性位点，有助于丁基氢过氧化物的激活和苯乙烯的协调。 这项工作是通过在金属氧化物催化剂系统中引入异质原子掺杂策略来增强芳香族剂选择性氧化的指南。

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