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
State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201210, China.
Science. 2024 Mar;383(6686):998-1004. doi: 10.1126/science.adk5195. Epub 2024 Feb 29.
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°C. Our catalyst also operated stably at 600°C, offering propane conversions of >60% and propylene selectivity of >95%.
由于在高温反应条件下金属原子会发生迁移，因此保持单原子催化剂的稳定性极具挑战性。我们提出了一种设计稳定单原子催化剂的策略，即利用第二种金属将贵金属原子锚定在沸石通道内。通过在烷烃脱氢过程中铟的原位迁移，在沸石硅铝酸盐-1内部形成了单原子铑-铟簇催化剂。在550℃下连续纯丙烷脱氢反应中，该催化剂在5500小时内对积炭表现出卓越的稳定性，丙烯选择性达99%，丙烷转化率接近热力学平衡值。我们的催化剂在600℃下也能稳定运行，丙烷转化率>60%，丙烯选择性>95%。
