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钌/二氧化钛上的抑制性强金属-载体相互作用促进了甲烷光驱动光热 CO 还原。

Suppressive Strong Metal-Support Interactions on Ruthenium/TiO Promote Light-Driven Photothermal CO Reduction with Methane.

机构信息

Xiamen Key Laboratory of Materials for Gaseous Pollutant Control, Institute of Urban Environment, Chinese Academy of Sciences, 361021, Xiamen, China.

CAS Center for Excellence in Regional Atmospheric Environment, Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of Sciences, 361021, Xiamen, China.

出版信息

Angew Chem Int Ed Engl. 2023 May 2;62(19):e202300129. doi: 10.1002/anie.202300129. Epub 2023 Mar 29.

DOI:10.1002/anie.202300129
PMID:36896935
Abstract

Strong metal-support interactions (SMSI) have gained great attention in the heterogeneous catalysis field, but its negative role in regulating light-induced electron transfer is rarely explored. Herein, we describe how SMSI significantly restrains the activity of Ru/TiO in light-driven CO reduction by CH due to the photo-induced transfer of electrons from TiO to Ru. In contrast, on suppression of SMSI Ru/TiO -H achieves a 46-fold CO conversion rate compared to Ru/TiO . For Ru/TiO -H , a considerable number of photo-excited hot electrons from Ru nanoparticles (NPs) migrate to oxygen vacancies (OVs) and facilitate CO activation under illumination, simultaneously rendering Ru electron deficient and better able to accelerate CH decomposition. Consequently, photothermal catalysis over Ru/TiO -H lowers the activation energy and overcomes the limitations of a purely thermal system. This work offers a novel strategy for designing efficient photothermal catalysts by regulating two-phase interactions.

摘要

强金属-载体相互作用(SMSI)在多相催化领域引起了广泛关注,但它在调节光致电子转移方面的负面作用却很少被探索。在此,我们描述了 SMSI 如何通过 TiO 向 Ru 的光致电子转移,显著抑制 Ru/TiO 在光驱动 CO 还原反应中 CH 的活性。相比之下,通过抑制 SMSI,Ru/TiO -H 的 CO 转化率比 Ru/TiO 提高了 46 倍。对于 Ru/TiO -H ,大量来自 Ru 纳米粒子(NPs)的光激发热电子迁移到氧空位(OVs)并在光照下促进 CO 的活化,同时使 Ru 电子不足,并能够更好地加速 CH 的分解。因此,Ru/TiO -H 的光热催化降低了活化能,并克服了纯热系统的限制。这项工作为通过调节两相相互作用设计高效光热催化剂提供了一种新策略。

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