铑
催化作用
甲烷
动力学
拉曼光谱
化学
碳纤维
二氧化碳重整
光谱学
光化学
无机化学
材料科学
化学工程
合成气
有机化学
复合数
物理
工程类
量子力学
光学
复合材料
作者
Riccardo Colombo,Gianluca Moroni,Chiara Negri,Guusje Delen,Matteo Monai,Alessandro Donazzi,Bert M. Weckhuysen,Matteo Maestri
标识
DOI:10.1002/anie.202408668
摘要
Abstract A mechanism for carbon deposition and its impact on the reaction kinetics of Methane Dry Reforming (MDR) using Rhodium‐based catalysts is presented. By integrating Raman spectroscopy with kinetic analysis in an operando‐annular chemical reactor under strict chemical conditions, we discovered that carbon deposition on a Rh/α‐Al 2 O 3 catalyst follows a nucleation‐growth mechanism. The dynamics of carbon aggregates at the surface is found to be ruled by the CO 2 /CH 4 ratio and the inlet CH 4 concentration. The findings elucidate the spatiotemporal development of carbon aggregates on the catalyst surface and their effects on catalytic performance. Furthermore, the proposed mechanism for carbon formation shows that the influence of CO 2 on MDR kinetics is an indirect result of carbon accumulation over time frames exceeding the turnover frequency, thus reconciling conflicting reports in the literature regarding CO 2 ′s kinetic role in MDR.
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