Monitoring the influence of steam on highly-active rhodium catalyst during the combined reforming of biogas by transient and steady-state operando spectroscopic studies

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-06-17 DOI:10.1039/d4cy00236a
Victoria Garcilaso , Rubén Blay-Roger , Miriam González-Castaño , Luis F. Bobadilla , Miguel A. Centeno , José A. Odriozola
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Abstract

The impact derived from incorporating water into CH4/CO2 biogas stream for the generation of syngas was investigated over the Rh/MgAl2O4 catalyst using operando steady-state and transient DRIFT spectroscopy coupled with MS. The incorporation of steam resulted in improved CH4 conversion rates and attained syngas streams with higher H2/CO ratios. It was demonstrated that in the presence of steam, the generation of CHxO species through the reaction of CO* with active *OH species is favored at the metal support surface. Besides, the enhanced resistance delivered by water molecules towards deactivating the coking phenomena was associated with easier carbonaceous decomposition and the exposition of the very active Rh (100) surfaces for methane decomposition. The Rh/MgAl2O4 catalyst was demonstrated to be an effective catalyst for the production of H2-rich syngas streams. More importantly, the insights reported herein provide new evidences regarding the impact of steam on biogas reforming reactions.

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通过瞬态和稳态操作光谱研究监测沼气联合转化过程中蒸汽对高活性铑催化剂的影响
使用操作稳态和瞬态 DRIFT 光谱及 MS,研究了在 Rh/MgAl2O4 催化剂上将水加入 CH4/CO2 生物气流以生成合成气所产生的影响。蒸汽的加入提高了 CH4 转化率,并获得了 H2/CO 比率更高的合成气流。研究表明,在有蒸汽存在的情况下,CO*与活性 *OH 物种的反应有利于在金属支撑表面生成 CHxO 物种。此外,水分子在使结焦现象失活方面的阻力增大与碳质分解更容易以及非常活跃的 Rh (100) 表面暴露于甲烷分解有关。事实证明,Rh/MgAl2O4 催化剂是生产富含 H2- 的合成气流的有效催化剂。更重要的是,本文报告的见解为蒸汽对沼气重整反应的影响提供了新的证据。
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
期刊最新文献
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