Abstract
Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted significant attention,but the effect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO2 nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our findings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the inter-action between Ru sites and N dopants increases the Ru0/Ruδ+ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst's overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO2@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C5+time yield of 219.4 molCO/(molRu·h)and C5+selectivity of 85.5％.
基金项目
国家重点研发计划(2022YFB4101800)
国家自然科学基金(22278298)
Program for Introducing Talents of Discipline to Universities of China(BP0618007)
万方数据