论文成果

Single Mo Atoms Stabilized on High-Entropy Perovskite Oxide: A Frontier for Aerobic Oxidative Desulfurization

摘要:The design and preparation of catalysts with both excellentstabilityand maximum exposure of catalytic active sites is highly desirable;however, it remains challenging in heterogeneous catalysis. Herein,a entropy-stabilized single-site Mo catalyst via a high-entropy perovskiteoxide LaMn0.2Fe0.2Co0.2Ni0.2Cu0.2O3 (HEPO) with abundant mesoporous structureswas initiated by a sacrificial-template strategy. The presence ofelectrostatic interaction between graphene oxide and metal precursorseffectively inhibits the agglomeration of precursor nanoparticlesin a high-temperature calcination process, thereby endowing the atomicallydispersed Mo6+ coordinated with four O atoms on the defectivesites of HEPO. The unique structure of single-site Mo atoms'random distribution with an atomic scale greatly enriches the oxygenvacancy and increases surface exposure of the catalytic active siteson the Mo/HEPO-SAC catalyst. As a result, the obtained Mo/HEPO-SACexhibits robust recycling stability and ultra-high oxidation activity(turnover frequency = 3.28 x 10(-2)) for thecatalytic removal of dibenzothiophene (DBT) with air as the oxidant,which represents the top level and is strikingly higher than the state-of-the-artoxidation desulfurization catalysts reported previously under thesame or similar reaction conditions. Therefore, the finding here forthe first time expands the application of single-atom Mo-supportedHEPO materials into the field of ultra-deep oxidative desulfurization. A single-site Mo-supported HEPO LaMn0.2Fe0.2Co0.2Ni0.2Cu0.2O3 with abundant mesoporous structures was initiated bya sacrificial-templatesynthesis protocol, which exhibits robust recycling stability andexceptional activity for the catalytic oxidation of DBT and its derivatives.

ISSN号:0020-1669

卷、期、页:卷62期28:11044-11055

发表日期:2023-07-06

影响因子:0.000000

期刊分区(SCI为中科院分区):二区

收录情况:SCI(科学引文索引印刷版),EI(工程索引),SCIE(科学引文索引网络版)

发表期刊名称:INORGANIC CHEMISTRY

参与作者:Liu, Jixing,Deng, Chang,Liu, Xiangqi,Shao, Shijia,Zheng, Peng,Chen, Linlin,Wu, Peiwen,Li, Huaming,Ji, Hongbing

第一作者:朱文帅

论文类型:期刊论文

论文概要:Liu, Jixing,Deng, Chang,Liu, Xiangqi,Shao, Shijia,Zheng, Peng,Chen, Linlin,Wu, Peiwen,Li, Huaming,Ji, Hongbing,朱文帅,Single Mo Atoms Stabilized on High-Entropy Perovskite Oxide: A Frontier for Aerobic Oxidative Desulfurization,INORGANIC CHEMISTRY,2023,卷62期28:11044-11055

论文题目:Single Mo Atoms Stabilized on High-Entropy Perovskite Oxide: A Frontier for Aerobic Oxidative Desulfurization