文献类型：期刊文献

英文题名：Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane

作者：Zhang, Pu[1,2];Li, Junwei[3];Huang, Haowei[11];Sui, Xiaoyu[1];Zeng, Haihua[1];Lu, Haijiao[4,5];Wang, Ying[1];Jia, Yanyan[9,10];Steele, Julian A.[6,7];Ao, Yanhui[2];Roeffaers, Maarten B. J.[8];Dai, Sheng[9,10];Zhang, Zizhong[1];Wang, Lianzhou[4,5];Fu, Xianzhi[1];Long, Jinlin[1]

机构：[1]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China;[2]Hohai Univ, Coll Environm, Minist Educ, Key Lab Integrated Regulat & Resource Dev Shallow, Nanjing 210098, Peoples R China;[3]Katholieke Univ Leuven, Dept Chem Engn, B-3001 Leuven, Belgium;[4]Univ Queensland, Nanomat Ctr, Sch Chem Engn, St Lucia, Qld 4072, Australia;[5]Univ Queensland, Australian Inst Bioengn & Nanotechnol, St Lucia, Qld 4072, Australia;[6]Univ Queensland, Australian Inst Bioengn & Nanotechnol, Brisbane, Qld 4072, Australia;[7]Univ Queensland, Sch Math & Phys, Brisbane, Qld 4072, Australia;[8]Katholieke Univ Leuven, Ctr Membrane Separat Adsorpt Catalysis & Spect Sus, B-3001 Leuven, Belgium;[9]East China Univ Sci & Technol, Inst Fine Chem, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[10]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[11]Southeast Univ, Sch Energy & Environm, Nanjing 210096, Peoples R China

年份：2024

卷号：146

期号：34

起止页码：24150

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20243416901303);WOS:【SCI-EXPANDED(收录号:WOS:001291768800001)】；

基金：This work is supported by the National Natural Science Foundation of China (Grants nos. 22072022, 22202046, and 22302038) and the Natural Science Foundation of Fujian Province (2021L3003). The authors wish to acknowledge the resources provided by the X-ray absorption spectroscopy beamline at the Australian Synchrotron, part of ANSTO (Grant no. M20481). J.A.S. is thankful for the financial support provided by the Australian Research Council (ARC) through the Discovery Fellowship grant (DE230100173).

语种：英文

外文关键词：Activation energy - Photocatalytic activity

摘要：This work introduces a new strategy of a single-atom nest catalyst, whereby several single atoms are positioned closely, aiming to achieve the dual benefits of high atom-utilization efficiency while avoiding the steric hindrance in the coupling reaction. As a proof of concept, Pt single-atom nests, where the adjacent Pt single atoms are approximately 4 & Aring; apart, are precisely engineered on the TiO2 photocatalyst for photocatalytic non-oxidative coupling of methane. The Pt single-atom nest photocatalyst demonstrates remarkable activity, achieving a C2H6 yield and turnover frequency of 251.6 mu mol g(cat)(-1) h(-1) and 20 h(-1), respectively, representing a 3.2-fold improvement compared to the Pt single-atom photocatalyst. Density functional theory calculations reveal that the Pt single-atom nest can significantly decrease the energy barrier for the activation of both CH4 molecules in the coupling process.