CO 2 -Assisted Two-Step Pyrolysis Fabrication of Hierarchical Porous Ni/ZrO 2 Catalyst for Low-Temperature Dry Reforming of Methane

作     者：Xinrong He Bang Xu Sanli Tang Xiaoguang Liu Qibin Liu Zongguo Wen Maohong Fan 

作者机构：Beijing Key Laboratory for Green Catalysis and Separation Department of Materials Science and Engineering Beijing University of Technology Beijing 100124 China Institute of Engineering Thermophysics Chinese Academy of Sciences Beijing 100190 China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai 200092 China School of Environment Tsinghua University Beijing 100084 China College of Engineering and Physical Sciences School of Energy Resources University of Wyoming Laramie WY 82071 USA College of Engineering Georgia Institute of Technology Atlanta Georgia 30332 USA 

出 版 物：《Journal of Environmental Sciences》 

年 卷 期：2025年

学科分类：0830[工学-环境科学与工程（可授工学、理学、农学学位）] 08[工学] 

摘      要：A new strategy for preparing highly dispersed, richer oxygen vacancies Ni/ZrO 2 catalysts derived from UiO-66-NH 2 is reported via pyrolysis-calcination removal of the ligands under N 2 , CO 2 , and Air atmospheres followed by loading Ni with 5 wt.% via wet impregnation method. Subsequently, the low-temperature dry reforming of methane (DRM) reaction over the obtained Ni/ZrO 2 catalysts was preliminarily investigated. The results indicated that the Ni/ZrO 2 -C catalyst, obtained by two-step pyrolysis in CO 2 , contained smaller Ni particles with a size of only 5-7 nm and possessed a hierarchical porous structure, as well as richer oxygen vacancies and basic active sites compared to the other two catalysts. Its catalytic activity in the DRM reaction presented the highest initial conversion of CH 4 (35 %) and CO 2 (26 %) at 600 °C, which was 5 % higher than that of the Ni/ZrO 2 -N and Ni/ZrO 2 -O catalysts obtained by two-step pyrolysis under an N 2 atmosphere and one-step pyrolysis under an air atmosphere, respectively. Meanwhile, an in-situ DRIFTS experiment revealed that Ni/ZrO 2 -C could enhance the adsorption and activation of CO 2 by promoting the formation of formate as an intermediate of CO hydrogenation and reverse water-gas shift (RWGS) reactions, which in turn facilitates the decomposition of CH 4 .