低碳化学与化工2025,Vol.50Issue(10):36-46,99,12.DOI:10.12434/j.issn.2097-2547.20250026
Nd掺杂对Ce基催化剂用于CO2与CH3OH直接合成DMC的影响
Effects of Nd doping on direct synthesis of DMC with CO2 and CH3OH catalyzed by Ce-based catalysts
摘要
Abstract
The direct synthesis of dimethyl carbonate(DMC)with carbon dioxide(CO2)and methanol(CH3OH)is currently one of the most environmentally advantageous methods for DMC production.Ce based catalysts are commonly used in direct synthesis of DMC with CO2 and CH3OH,but CeO2 suffers from issues such as insufficient thermal stability and limited active sites.Using neodymium nitrate hexahydrate(NdN3O9·6H2O)as the promoter,a series of Nd-doped Ce-based catalysts were prepared by co-precipitation method.The structures of catalysts were characterized by ICP-OES,XRD,HR-TEM,and XPS,etc.,and their catalytic performances were investigated.The results show that the appropriate Nd doping amount(mass fraction,the same below)can positively optimize the catalyst's specific surface area,oxygen vacancy density and the number of acid-base sites.Among them,the catalyst with Nd doping amount of 5%(5%Nd2O3-CeO2)has the highest oxygen vacancy density,more medium-strong acid sites,and the most weak base sites.Under the reaction conditions of CH3OH dosage of 23.74 g,2-cyanopyridine dosage of 36.44 g,5%Nd2O3-CeO2 dosage of 200 mg,temperature of 140 ℃ and pressure of 1.2 MPa,5%the CH3OH conversion rate is 27.35%,DMC selectivity is 77.72%and DMC yield is 392.90 mmol/g catalyzed by 5%Nd2O3-CeO2 after reacting for 2 h.After four cycles under the conditions of temperature of 140℃,pressure of 1.2 MPa,CH3OH dosage of 23.74 g,5%Nd2O3-CeO2 dosage of 200 mg and reaction time of 2 h,the catalytic performance of 5%Nd2O3-CeO2 remains superior to that of CeO2.关键词
碳酸二甲酯/直接合成/Nd掺杂/Ce基催化剂/二氧化碳/甲醇Key words
dimethyl carbonate/direct synthesis/Nd doping/Ce-based catalysts/carbon dioxide/methanol分类
化学化工引用本文复制引用
沈怡婷,张海涛,马宏方,钱炜鑫,应卫勇..Nd掺杂对Ce基催化剂用于CO2与CH3OH直接合成DMC的影响[J].低碳化学与化工,2025,50(10):36-46,99,12.基金项目
国家自然科学基金(22178113) (22178113)
中央高校基本科研业务费专项资金(JKA01231712,JKCA1241202). (JKA01231712,JKCA1241202)