文献类型：期刊文献

英文题名：Rational Design of Precious-Metal Single-Atom Catalysts for Methane Combustion

作者：Pu, Tiancheng[1];Ding, Jiaqi[1];Tang, Xuan[2];Yang, Kewu[1];Wang, Ke[1];Huang, Bei[1];Dai, Sheng[1,2];He, Yi[3,4];Shi, Yao[1];Xie, Pengfei[1]

机构：[1]Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]Univ Washington, Dept Chem Engn, Seattle, WA 98195 USA;[4]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2022

卷号：14

期号：38

起止页码：43141

外文期刊名：ACS APPLIED MATERIALS & INTERFACES

收录：;EI(收录号：20224112851321);WOS:【SCI-EXPANDED(收录号:WOS:000861805600001)】；

基金：This work was supported by the Natural Science Foundation of Zhejiang Province (No. LR22B060002), the National Natural Science Foundation of China (No. 22178299), the Fundamental Research Funds for the Central Universities, Shanxi-Zheda Insititute of Advanced Materials and Chemical Engineering (2021ST-AT-002), Shanghai Rising-star Program (No. 20QA1402400), and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning.

语种：英文

外文关键词：single-atom catalyst; methane combustion; density functional theory; C-H activation; oxygen vacancy formation

摘要：Supported precious-metal single-atom catalysts (PM SACs) have emerged as a new frontier of high-performance catalytic material with 100% atom utilization efficiency. However, the rational design of such material with guidance from fundamental understandings of the structure-activity relationship remains challenging. Here, we report the synthesis, characterizations, and mechanistic investigation of various PM SACs supported on nanoceria for CH4 combustion. Using density functional theory, two descriptors as the d-band center of PMs and oxygen vacancy formation energy are established, which jointly govern the reactivity for CH4 combustion. These descriptors are thus applied to predict a dual SAC consisting of proximate Pd and Rh sites, demonstrating a remarkable improvement versus Pd or Rh catalyst, respectively. Our results reveal the general strategy of integrating experimental and computational efforts for investigation of various PM SACs in methane combustion, thus paving the way for the next generation of advanced catalytic materials.