Low temperature reforming of methane with CO2over Pt/CeO2, Ni/CeO2and Pt–Ni/CeO2catalysts prepared by a solution-combustion methodElectronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d3cy00600j

Autor: Khatun, Rubina, Siddiqui, Nazia, Pal, Rohan Singh, Bhandari, Sonu, Khan, Tuhin Suvra, Singh, Shivani, Poddar, Mukesh Kumar, Samanta, Chanchal, Bal, Rajaram
Zdroj: Catalysis Science & Technology; 2023, Vol. 13 Issue: 22 p6431-6445, 15p
Abstrakt: This study investigates the low temperature reforming of methane with CO2over mono-metallic (Pt/CeO2and Ni/CeO2) and bi-metallic (Pt–Ni/CeO2) solid solution catalysts prepared by using a one-pot solution-combustion method. Various analytical techniques were employed to analyze the synthesized catalysts in order to correlate their physicochemical properties to their catalytic activity. Solid solution formation was confirmed by the lattice parameter shifting and Rietveld refinement analysis. Solid-solution formation enhanced the defective oxygen species. The TPR and TPDsstudies showed that the synergy between Pt and Ni enhanced the active oxygen species and metal–support interaction of the Pt–Ni/CeO2catalyst, which are beneficial for the higher adsorption of CH4and CO2. Pt–Ni/CeO2catalysts have a higher amount of O22−, O2−species and AD/AF2gratio followed by the NC and PC catalysts, as confirmed by the O2-TPD, XPS and RAMAN analysis. Pt-based catalysts start the DRM reaction at 350 °C, whereas Ni/CeO2activates at a temperature 100 °C higher than Pt–Ni/CeO2and Pt/CeO2. At 675 °C, Pt–Ni/CeO2showed ∼86% conversion of CO2and CH4with 100% selectivity of synthesis gas with a H2/CO ratio of ∼1, while Pt/CeO2and Ni/CeO2shows ∼46.2 and ∼59.8% conversion, respectively. DFT calculations showed that the Pt–Ni/CeO2catalyst required lower activation energy than the monometallic catalyst to activate CH4and CO2. We believe that the synergy between Ni and Pt enhanced the structural and electronic properties of Pt–Ni/CeO2, which is responsible for its excellent performance at low temperature.
Databáze: Supplemental Index