二甲醚
甲醇
催化作用
高分辨率透射电子显微镜
X射线光电子能谱
X射线吸收精细结构
选择性
铜
介孔材料
化学工程
化学
无机化学
材料科学
透射电子显微镜
纳米技术
光谱学
有机化学
工程类
量子力学
物理
作者
Xiaojing Cui,Wenjun Yan,Huanhuan Yang,Ying Shi,Yanfeng Xue,He Zhang,Yulan Niu,Weibin Fan,Tiansheng Deng
出处
期刊:ACS Sustainable Chemistry & Engineering
[American Chemical Society]
日期:2021-02-10
卷期号:9 (7): 2661-2672
被引量:35
标识
DOI:10.1021/acssuschemeng.0c07258
摘要
It is of importance but highly challenging for copper (Cu)-based catalysts to maintain the structure of active Cu sites under working conditions. Herein, the commercial Cu/ZnO/Al2O3 catalyst was confined in the mesoporous SiO2–Al2O3 shell via hydrothermal synthesis (CZAS@SA) for selective hydrogenation of CO2 to dimethyl ether (DME) and methanol. CZAS@SA catalysts exhibited higher intrinsic activity for the formation of DME and methanol and much lower intrinsic activity for CO formation than Cu/ZnO/Al2O3. Thus, the total selectivity of DME and methanol was enhanced from 9.1 to 63.3 mol %. In situ X-ray photoelectron spectroscopy/X-ray absorption fine structure/high-resolution transmission electron microscopy (XPS/XAFS/HRTEM) results and catalytic measurements indicated that the metallic Cu(Cu0)–ZnO interface was the active site for methanol formation. Commercial Cu/ZnO/Al2O3 underwent a separation of Cu0 and ZnO phases during the reaction, and this phase separation caused agglomeration of Cu0 and shrinking of the active Cu0–ZnO interface, which aggregated CO formation. The active Cu0–ZnO interface in CZAS@SA was preserved due to the confinement effect of the shell, which improved methanol selectivity.
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