文献类型：期刊文献

英文题名：Zr-regulated Ni/SiO2-fumed catalysts with enhanced Ni-ZrOx interfacial interaction and promoted formate-related pathway for low-temperature CO2 methanation

作者：Liu, Jundi[1];Fang, Yuan[1];Ju, Ziying[1];Liu, Naiwang[1];Meng, Xuan[1]

机构：[1]East China Univ Sci & Technol, Int Joint Res Ctr Green Energy Chem Engn, Shanghai 200237, Peoples R China

年份：2026

卷号：726

外文期刊名：APPLIED CATALYSIS A-GENERAL

收录：;EI(收录号：20263421348295);Scopus(收录号：2-s2.0-105047939816);WOS:【SCI-EXPANDED(收录号:WOS:001856049300001)】；

语种：英文

外文关键词：Ni based catalysts; Zr incorporation; SiO2-Fumed support; Formate-related pathway; CO2 methanation

摘要：In this work, Ni/ZrxSi1-x catalysts were prepared on commercial SiO2-Fumed by a citric acid complexation method, and the effects of Zr/Si ratio and preparation method on CO2 methanation were investigated. Compared with impregnation-derived samples, the complexation-derived catalysts showed smaller and more uniformly distributed metal-containing domains and a more homogeneous spatial association between Ni and Zr-containing species. H2-TPR revealed distinct NiO reduction environments, while H2-TPD, CO2-TPD, and XPS showed differences in apparent Ni dispersion, hydrogen adsorption, medium-strength basic sites, and the near-surface electronic environment. The physical-mixture control exhibited CO2 conversion below 8%, a dominant low-temperature NiO reduction feature, and a limited contribution from medium-strength basic sites, indicating that simple coexistence of Ni and ZrOx is insufficient to reproduce the promotional effect of the integrated catalyst. In situ DRIFTS showed that Zr incorporation suppressed CO-related intermediates and promoted carbonate-and formate-related species. Ni/Zr0.6Si0.4 achieved CO2 conversions of 66.49% and 90.37% at 250 and 300 degrees C, respectively, with nearly 100% CH4 selectivity. During a 30 h test at 250 degrees C, conversion decreased from approximately 66-60%, while CH4 selectivity remained near 100%. These results associate the improved performance with the combined regulation of accessible Ni sites, surface basicity, and close Ni-ZrOx spatial contact.