Performance regulation of acetic acid auto-thermal reforming reaction: Oxygen vacancy defects and active sites controlled by V species

作者：Xianghua Zhang, Mao Gan, Yali Tan, Ying Su, Jinbo Liu, Wenjing Sun, Lihong Huang · 发表于：Colloids and Surfaces A Physicochemical and Engineering Aspects · 年份：2025 · DOI：10.1016/j.colsurfa.2025.139332 · 被引用次数：2 · 研究领域：Catalysts for Methane Reforming、Chemical Looping and Thermochemical Processes、Catalytic Processes in Materials Science

Hydrogen can be produced from acetic acid (HAc) via auto-thermal reforming (ATR). Ni-based catalysts are widely used in ATR of HAc, but suffer from deactivation due to coke deposition, sintering, and oxidation. To address these issues, Ni-Sm-V-O catalysts were prepared via sol-gel method by incorporating vanadium and samarium. Results showed that V incorporation promoted formation of SmVO 3 perovskite, which orchestrated a synergistic promotion mechanism. Specifically, the perovskite structure simultaneously modulated the electronic and geometric properties of the catalyst. On one hand, charge transfer from the V-doped support created electron-rich Ni sites, which enhanced the metallic Ni 0 stability and facilitated the activation of C–H/C–C bonds in acetic acid. On the other hand, the lattice distortion induced abundant oxygen vacancies, which served as activation centers for oxidants (H 2 O/O 2 ). These factors reinforced each other during the reaction: the carbonaceous intermediates generated on the highly dispersed active Ni sites were instantly gasified by the mobile active oxygen species (O*) migrating from the adjacent vacancies. This cooperative “cracking-gasification” cycle effectively suppressed coke deposition while maintaining high activity. Notably, no deactivation was observed during the 50-h testing, which is fundamentally attributed to the synergistic suppression of coke deposition via V-induced electronic modulation and oxygen vacancy engineering. This work r...