Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, Central China Normal University, Wuhan 430079, P. R. China.
Environ Sci Technol. 2024 Oct 8;58(40):18020-18032. doi: 10.1021/acs.est.4c04946. Epub 2024 Sep 26.
The effects of sulfur dioxide (SO) in the catalytic purification of short-chain hydrocarbons are still controversial, and the exact role of SO on adsorption and reaction pathways during the catalytic oxidation of different volatile organic compounds (VOCs) remains unclear. Herein, a three-dimensional ordered macroporous CeZrO supported Pt nanoparticle monolithic catalyst (Pt/OM CZO) was synthesized to investigate these effects. Our findings uncover the diverse effects of SO: Upon SO treatment, the coupling between the S 3p and Pt 5d orbitals promotes the Pt-O-SO structure in situ formed on the catalyst surface. The propene (CH) molecule readily binds with the oxygen atom in Pt-O-SO, resulting in the accumulation of acetone and carbon deposition, thereby hindering CH oxidation. Conversely, a cleaved oxygen atom within the Pt-O-SO structure enhances propane (CH) adsorption and activates the C-H bond, facilitating CH oxidation. These insights are pivotal for advancing the frontier of sulfur-tolerant catalysts, addressing both economic and environmental challenges.
二氧化硫（SO）在短链烃类催化净化中的作用仍存在争议，SO 在不同挥发性有机化合物（VOCs）的催化氧化过程中对吸附和反应途径的确切作用尚不清楚。在此，我们合成了一种三维有序大孔 CeZrO 负载 Pt 纳米颗粒整体式催化剂（Pt/OM CZO）来研究这些影响。我们的研究结果揭示了 SO 的多种作用：SO 处理后，S 3p 和 Pt 5d 轨道之间的耦合促进了催化剂表面原位形成的 Pt-O-SO 结构。丙烯（CH）分子容易与 Pt-O-SO 中的氧原子结合，导致丙酮的积累和积碳，从而阻碍 CH 的氧化。相反，Pt-O-SO 结构中的一个断裂氧原子增强了丙烷（CH）的吸附并激活了 C-H 键，促进了 CH 的氧化。这些见解对于推进耐硫催化剂的前沿具有重要意义，同时解决了经济和环境方面的挑战。
