Dealuminated Beta zeolite reverses Ostwald ripening for durable copper nanoparticle catalysts
成果类型：
Article
署名作者：
Liu, Lujie; Lu, Jiaye; Yang, Yahui; Ruettinger, Wolfgang; Gao, Xinhua; Wang, Ming; Lou, Hao; Wang, Zhandong; Liu, Yifeng; Tao, Xin; Li, Lina; Wang, Yong; Li, Hangjie; Zhou, Hang; Wang, Chengtao; Luo, Qingsong; Wu, Huixin; Zhang, Kaidi; Ma, Jiabi; Cao, Xiaoming; Wang, Liang; Xiao, Feng-Shou
署名单位：
Zhejiang University; East China University of Science & Technology; BASF; Ningxia University; Beijing Institute of Technology; Chinese Academy of Sciences; University of Science & Technology of China, CAS; Zhejiang University; Chinese Academy of Sciences; Shanghai Institute of Applied Physics, CAS; Zhejiang University; Zhejiang University; Shanghai Jiao Tong University; Beijing University of Chemical Technology
刊物名称：
SCIENCE
ISSN/ISSBN：
0036-9002
DOI：
10.1126/science.adj1962
发表日期：
2024-01-05
页码：
94-101
关键词：
metal-support interactions
total-energy calculations
cu/sio2 catalyst
dimethyl oxalate
deactivation mechanism
methanol
ethylene
hydrogenation
conversion
DECOMPOSITION
摘要：
Copper nanoparticle-based catalysts have been extensively applied in industry, but the nanoparticles tend to sinter into larger ones in the chemical atmospheres, which is detrimental to catalyst performance. In this work, we used dealuminated Beta zeolite to support copper nanoparticles (Cu/Beta-deAl) and showed that these particles become smaller in methanol vapor at 200 degrees C, decreasing from similar to 5.6 to similar to 2.4 nanometers in diameter, which is opposite to the general sintering phenomenon. A reverse ripening process was discovered, whereby migratable copper sites activated by methanol were trapped by silanol nests and the copper species in the nests acted as new nucleation sites for the formation of small nanoparticles. This feature reversed the general sintering channel, resulting in robust catalysts for dimethyl oxalate hydrogenation performed with supported copper nanoparticles for use in industry.