Pt/Cr 2 O 3 Catalysts for the Reverse Water–Gas Shift Reaction: Unraveling Crucial Roles of Interfacial Synergy and Oxygen Vacancies

作者：Chen Zhu, Xiaowei Wang, Shaorong Deng, Xiuzhong Fang, Xianglan Xu, Xiang Wang · 发表于：Inorganic Chemistry · 年份：2025 · DOI：10.1021/acs.inorgchem.5c00487 · 被引用次数：12 · 研究领域：Catalytic Processes in Materials Science、Catalysts for Methane Reforming、Catalysis and Hydrodesulfurization Studies

The development of high-efficiency platinum-based catalysts and the clarification of reaction pathways are fundamental challenges for a reverse water–gas shift (RWGS) reaction. Herein, we prepare a Pt/Cr 2 O 3 catalyst with a 1% Pt weight loading using an impregnation method for the low-temperature RWGS reaction. This catalyst achieved high activity, selectivity, and long-term stability. At 350 °C and a space velocity of 24,000 mL h –1 g cat –1, the catalyst achieved approximately 33.2% CO 2 conversion, nearing equilibrium conversion and much higher than Pt/Al 2 O 3 and Pt/SiO 2 . Pt species were highly dispersed on Pt/Cr 2 O 3, existing in both Pt 0 and Pt n + states, while the Cr species of the support primarily existed as Cr 3+ . Combined in situ experiments and density functional theory calculations revealed that the RWGS reaction on the Pt/Cr 2 O 3 catalyst followed the carboxyl (COOH*) route: adsorbed CO 2 is hydrogenated through its O-end to produce trans -COOH*, which then converts to cis -COOH*, followed by the formation of CO via the dissociation of cis -COOH. The high activity of the Pt/Cr 2 O 3 catalyst can be attributed to the interfacial synergy between Pt and Cr 2 O 3 and the presence of oxygen vacancies. This work provides valuable insights into the design of high-performance catalysts for the RWGS reaction.