低碳化学与化工2025,Vol.50Issue(6):25-33,9.DOI:10.12434/j.issn.2097-2547.20240380
镍-镧双金属催化剂CO2-CH4重整制合成气催化性能研究
Study on catalytic performance of Ni-La bimetallic catalyst for CO2-CH4 reforming to syngas
摘要
Abstract
The catalytic dry reforming of CO2 and CH4 holds significant importance.On one hand,it enables the recycling of two major greenhouse gases.On the other hand,its reaction products,H2 and CO,serve as critical feedstocks for Fischer-Tropsch synthesis.Nickel-based catalysts have attracted widespread attention due to their high catalytic activity and low cost.La2NiO4/MCM-41 serials bimetallic catalysts were prepared using the sol-gel method,with MCM-41 as the support.The effects of calcination temperature,Ni content(mass fraction,the same below),n(La)/n(Ni),and reaction temperature on its CH4-CO2 catalytic reforming performance were investigated.The catalysts before/after reaction were characterized using BET,SEM-EDX,XRD,H2-TPR,TG-DSC,Raman,and TPO techniques.The results show that spinel La2NiO4 is the primary form of nickel in the catalyst and exhibites good dispersion.As the Ni content increases,the specific surface area and pore volume of the catalysts decrease rapidly.Ni content and reaction temperature are found to have the most significant impact on the catalytic performance of bimetallic catalysts.Under reaction conditions of 700℃,0.10 MPa and 18000 mL/(h·g),the conversion rates of CH4 and CO2 after 100 h reaction show varying degrees of decline compared to the initial values.However,their equilibrium conversion rates still reach 72.89%and 81.08%,respectively.Post-reaction characterization reveals significant carbon deposition on the catalyst surface,primarily in the form of carbon nanotubes.The size of these carbon nanotubes increases as the reaction time prolongs,eventually covering the active Ni sites on the catalyst surface and leading to catalyst deactivation.关键词
Ni-La双金属催化剂/La2NiO4/MCM-41/CO2-CH4/干重整Key words
Ni-La bimetallic catalyst/La2NiO4/MCM-41/CO2-CH4/dry reforming分类
化学工程引用本文复制引用
张国佩,王聪,张肖阳,李兆敏..镍-镧双金属催化剂CO2-CH4重整制合成气催化性能研究[J].低碳化学与化工,2025,50(6):25-33,9.基金项目
山东省青年基金项目(ZR2022QE111) (ZR2022QE111)
天池人才支持计划(CZ000401). (CZ000401)