催化作用
双金属片
格式化
介孔材料
材料科学
介孔二氧化硅
甲酸
化学工程
金属
无机化学
化学
有机化学
工程类
冶金
作者
Jiafu Qu,Songqi Li,Zhiyuan Deng,Jundie Hu,Xiaogang Yang,Yahui Cai,Feng Du,Bailing Zhong,Chang Ming Li,Qiming Sun
标识
DOI:10.1016/j.cej.2023.143405
摘要
Converting CO2 to formic acid/formate is a considerably significant pathway for future energy storage and utilization; however, it is critical to tailor high-performance catalysts for realizing the process. Herein, highly dispersed Pd-Ni(OH)2 hybrids were immobilized in ordered mesoporous silica SBA-15 via a facile impregnation method. The prepared SBA-15-supported Pd-Ni(OH)2 catalyst exhibited extraordinarily high catalytic performance and stability during the hydrogenation of CO2 toward formate. Significantly, Pd5Ni5/SBA-15, an optimized Pd5Ni5/SBA-15 catalyst afforded a superior formate generation rate of 150.5 molformate moltotalPd-1h−1 at a low temperature (40 °C), which was about 3-fold higher than that of monometallic Pd counterpart. Such a catalytic activity outperforms most of the previously reported catalysts because of its charge polarization action and synergy between bimetallic components as well as ultrasmall and well-dispersed metal species with increased accessible active sites. The relevant experimental observations were well supported by density functional theory (DFT) calculations. In addition, the catalytic activity of SBA-15-supported metal catalysts remained unchanged even after the 5th cycle, demonstrating excellent cycling durability due to the confinement effect of mesoporous silica. The facile synthesis strategy and excellent catalytic performance hold great potential applications of the prepared catalysts in CO2 hydrogenation to formate.
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