Stable anchoring of single rhodium atoms by indium in zeolite alkane dehydrogenation catalysts

• 成果类型: Article
• 署名作者: Zeng, Lei; Cheng, Kang; Sun, Fanfei; Fan, Qiyuan; Li, Laiyang; Zhang, Qinghong; Wei, Yao; Zhou, Wei; Kang, Jincan; Zhang, Qiuyue; Chen, Mingshu; Liu, Qiunan; Zhang, Liqiang; Huang, Jianyu; Cheng, Jun; Jiang, Zheng; Fu, Gang; Wang, Ye
• 署名单位: Xiamen University; Chinese Academy of Sciences; Shanghai Institute of Applied Physics, CAS; Shanxi University; Yanshan University
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-12673
• DOI: 10.1126/science.adk5195
• 发表日期: 2024-03-01
• 页码: 998-1004
• 关键词: total-energy calculations; driven migration; light alkanes; propane; metal; DYNAMICS; clusters; rh; pseudopotentials; alloys

摘要

Maintaining the stability of single-atom catalysts in high-temperature reactions remains extremely challenging because of the migration of metal atoms under these conditions. We present a strategy for designing stable single-atom catalysts by harnessing a second metal to anchor the noble metal atom inside zeolite channels. A single-atom rhodium-indium cluster catalyst is formed inside zeolite silicalite-1 through in situ migration of indium during alkane dehydrogenation. This catalyst demonstrates exceptional stability against coke formation for 5500 hours in continuous pure propane dehydrogenation with 99% propylene selectivity and propane conversions close to the thermodynamic equilibrium value at 550(degrees)C. Our catalyst also operated stably at 600(degrees)C, offering propane conversions of >60% and propylene selectivity of >95%.