低碳化学与化工2025，Vol.50Issue(8)：123-132,10.DOI:10.12434/j.issn.2097-2547.20250140
焙烧温度对Pd/LDH催化剂上CH4-CO2两步梯阶转化合成乙酸的影响
Effects of calcination temperatures on CH4-CO2 two stepwise conversion to acetic acid over Pd/LDH catalysts
摘要
Abstract
The direct conversion of CH4 and CO2 to acetic acid is a 100%atom-economical reaction,but its reaction conditions are harsh.The hydrotalcite(LDH)has good application prospects in the field of CH4-CO2 catalytic conversion due to its advantages of large specific surface area,good dispersion for active components and adjustable acid-base properties.MgAl-LDH with n(Mg)/n(Al)of 5 was used as the support,and palladium(Pd)with mass fraction of 5%was loaded as the active component by ion-exchange method,and a series of Pd/LDH-X catalysts(X represents the calcination temperature)were prepared by calcinating the resultant precursors at different temperatures.The structures of catalysts were characterized by XRD,FT-IR,SEM,etc.,and the catalytic performances of the catalysts were investigated in two-step stepwise conversion of CH4-CO2 to acetic acid.The results show that the catalytic performance of Pd/LDH-150 obtained under calcination temperature of 150℃is the best under the CH4-CO2 two-step stepwise conversion reaction conditions set in this study for 30 min,with acetic acid spatiotemporal yield of 61.8 μmol/(g·h),which is significantly greater than acetic acid spatiotemporal yield(2.4 μmol/(g·h))under the CH4-CO2 cofeeding conditions,and acetic acid is the only liquid product.The structural integrity of LDH is a key factor affecting the catalytic performance of the catalyst,and the presence of more medium-strong acidic sites and medium-strong basic sites on the surface of catalyst is favorable for the synthesis of acetic acid.Excessively high calcination temperature can lead to the collapse of the layered structure of LDH,resulting in the decrease of the number of medium-strong acidic sites and medium-strong basic sites on the surface,which can adversely affect the catalytic performance of the catalyst.关键词
CH4-CO2两步阶梯转化/MgAl水滑石/Pd催化剂/乙酸/焙烧温度Key words
CH4-CO2 two stepwise conversion/MgAl hydrotalcite/Pd catalysts/acetic acid/calcination temperatures分类
化学化工引用本文复制引用
王小双,吴怡枭,王菲,张凯玮,刘勇军,黄伟..焙烧温度对Pd/LDH催化剂上CH4-CO2两步梯阶转化合成乙酸的影响[J].低碳化学与化工,2025,50(8):123-132,10.基金项目
国家自然科学基金(22479105,21908157) （22479105,21908157）
新疆维吾尔自治区自然科学基金(2024D01A130) （2024D01A130）
山西省基础研究计划(202403021221040) （202403021221040）
榆林学院-中国科学院洁净能源创新研究院联合基金(YLU-DNL2023002). （YLU-DNL2023002）
