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Surface Carbon Formation and its Impact on Methane Dry Reforming Kinetics on Rhodium-Based Catalysts by Operando Raman Spectroscopy.
Colombo, Riccardo; Moroni, Gianluca; Negri, Chiara; Delen, Guusje; Monai, Matteo; Donazzi, Alessandro; Weckhuysen, Bert M; Maestri, Matteo.
Afiliação
  • Colombo R; Laboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa 34, 20156, Milano, Italy.
  • Moroni G; Laboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa 34, 20156, Milano, Italy.
  • Negri C; Laboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa 34, 20156, Milano, Italy.
  • Delen G; Inorganic Chemistry and Catalysis Group, Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.
  • Monai M; Inorganic Chemistry and Catalysis Group, Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.
  • Donazzi A; Laboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa 34, 20156, Milano, Italy.
  • Weckhuysen BM; Inorganic Chemistry and Catalysis Group, Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.
  • Maestri M; Laboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa 34, 20156, Milano, Italy.
Angew Chem Int Ed Engl ; : e202408668, 2024 Jul 03.
Article em En | MEDLINE | ID: mdl-38958601
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-Al2O3 catalyst follows a nucleation-growth mechanism. The dynamics of carbon aggregates at the surface is found to be ruled by the CO2/CH4 ratio and the inlet CH4 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 CO2 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 CO2's kinetic role in MDR.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article