燃料化学学报(中英文)2024,Vol.52Issue(1):19-28,10.DOI:10.1016/S1872-5813(23)60378-0
Fe/g-C3N4表面改性及其对CO加氢产物分布的影响
Effect of surface modification of Fe/g-C3N4 catalyst on the product distribution in CO hydrogenation
摘要
Abstract
Carbon nitride(g-C3N4)prepared using thermal condensation of urea was pretreated by H2O2/NH3·H2O and used as support to obtain Fe/g-C3N4 catalyst via impregnation method.The catalytic performance of the catalysts both before and after modification was investigated in CO hydrogenation.Combining detailed characterizations,such as XRD,SEM,TEM,FT-IR,TG,CO2-TPD,CO-TPD,H2-TPR,contact angle measurement,and N2 physical adsorption and desorption,we investigated the effects of surface pretreatment on the texture properties of Fe/g-C3N4 catalysts and the product distribution of CO hydrogenation.The results demonstrate that various pretreatment techniques have significant influences on the textural properties and catalytic performance of the catalysts.The prepared g-C3N4 with a typical honeycomb structure has strong interaction with highly dispersed Fe.Both before and after modification,the materials are hydrophilic,and the hydrophilicity is increased after treatment with H2O2 and NH3·H2O.Treatment with H2O2 enhances surface hydroxyl groups.NH3·H2O treatment improves surface amino groups,promotes CO adsorption,and facilitates the formation of Fe(NCN)phase.The surface basicity of all pretreated catalysts is enhanced.The water gas shift(WGS)reaction activity of the two-step modified catalyst Fe/AM-g-C3N4 was lower,and the CO2 selectivity in CO hydrogenation was reduced to 11.61%.Due to the enhanced basicity of Fe/AM-g-C3N4,the secondary hydrogenation ability of olefins was inhibited to obtain higher olefin selectivity with C2=-C4 s of 32.37%and an O/P value of 3.23.关键词
CO加氢/表面改性/Fe/g-C3N4催化剂/产物分布Key words
CO hydrogenation/surface modification/Fe/g-C3N4 catalyst/product distribution分类
化学化工引用本文复制引用
孙禹,高新华,马清祥,范素兵,赵天生,张建利..Fe/g-C3N4表面改性及其对CO加氢产物分布的影响[J].燃料化学学报(中英文),2024,52(1):19-28,10.基金项目
The project was supported by the National Natural Science Foundation of China(21968025)and the Key Project of Ningxia Natural Science Foundation(2022AAC02002).国家自然科学基金(21968025)和宁夏自然科学基金重点项目(2022AAC02002)资助 (21968025)