文献类型：期刊文献

英文题名：Realization of High-Pressure Dry Methane Reforming by Suppressing Coke Deposition with Co-Rh Intermetallic Clusters

作者：Zhu, Kake[1]; Liu, Qing[1]; Liu, Yang[2]; Zhou, Ning[1]; Zhang, Penghao[1]; Liu, Zhicheng[3]; Vovk, Evgeny I.[2]; Zhu, Yi-An[1]; Yang, Yong[2]

机构：[1] UNILAB, State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China; [2] School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201203, China; [3] Shanghai Research Institute of Petrochemical Technology, Shanghai, 201208, China

年份：2023

外文期刊名：SSRN

收录：EI(收录号：20230171134)

语种：英文

外文关键词：Binary alloys - Catalysis - Catalysts - Cobalt alloys - Density functional theory - Intermetallics - Methane - Reaction intermediates - Surface segregation

摘要：It is economical to perform methane and carbon dioxide reforming under high-pressure and temperature conditions, but the harsh operation condition poses a grand challenge for coke-resistant catalyst design. We report herein that surface-segregation-free Co1Rh3 clusters are stable catalysts under 20 bars at 850 oC. Microkinetic analysis discloses that balanced and lowered surface coverages of C* and O* constitute the most abundant reaction intermediates on Co1Rh3 cluster at elevated pressures, with respect to that of the monometallic ones, thus avoiding surface carbon accumulation or surface oxidative deactivation. Moreover, density functional theory calculations of carbon atom nucleation discloses that adsorbed carbon transformation to refractory, graphene-like carbon is suppressed on Co1Rh3 cluster surface, owing to increased energetic barrier and ensemble size, hence, only CO2 gasifiable soft carbon could form. The revelation of the electronic/geometric features of Co1Rh3 is regarded to provide a guidance for future coke-resistant catalyst design. ? 2023, The Authors. All rights reserved.