利用3-氨丙基三甲氧基硅烷(APTMS)对氧化石墨烯(GO)进行功能化改性得到GO-NH₂,再通过水热还原法制备高分散Pd/GO-NH₂催化剂,用于肉桂醛(CAL)选择性加氢制氢化肉桂醛(HCAL)。结果表明,APTMS的接枝量对CAL选择性加氢性能具有较大影响,当APTMS与GO的质量比[m(APTMS)/m(GO)]≤10时,随着m(APTMS)/m(GO)的增大Pickering乳液液滴尺寸逐渐减小,CAL的选择性加氢性能增强;当m(APTMS)/m(GO)>10时,由于含氧官能团数量有限,接枝量基本保持不变。因此,Pd/GO-NH₂-10表现出最高的CAL转化率(99.8%)、HCAL选择性(85.8%)和优异的CAL选择性加氢稳定性。

GO-NH₂ is obtained through modifying graphene oxide (GO) by 3-aminopropyltrimethoxysilane (APTMS),and then highly dispersed Pd/ GO-NH₂ catalysts are prepared via hydrothermal method,and applied to selective hydrogenation of cinnamaldehyde (CAL) in aqueous solution.The result suggests that the grafting amount of APTMS affects the performance of the catalysts in selective hydrogenation of CAL.As the mass ratio of APTMS to GO [m(APTMS)/m(GO)] is not more than 10,an increase of [m(APTMS)/m(GO)] in Pd/GO-NH₂ catalyst leads to a decrease in the size of Pickering emulsion,which enhances the amount of CAL adsorbed on the catalyst,thereby promoting the selective hydrogenation of CAL.As [m(APTMS)/m(GO)] is greater than 10,the grafting amount of APTMS on GO has hardly changed due to the limited number of oxygen-containing functional groups.Therefore,Pd/GO-NH₂-10 exhibits the highest CAL conversion of 99.8%,delivering a HCAL selectivity of 85.8%,as well as excellent stability in selective hydrogenation of CAL.

文成龙(1993-),男,博士,讲师,研究方向为催化加氢,wenchenglong@cczu.edu.cn;鲁墨弘(1978-),男,博士,教授,研究方向为催化加氢,通讯联系人,mlu@cczu.edu.cn。