摘要
以葡萄糖为碳源、硫脲为氮源,合成了氮掺杂碳载体(N-C),利用掺杂的氮原子作为作用位点与贵金属钯纳米粒子(Pd NPs)相互作用,得到了负载Pd纳米粒子的N-C(Pd/N-C)催化剂,将其用于硅烷与醇的脱氢偶联反应,并推测了其催化硅烷和醇脱氢偶联反应的可能机理。采用XRD、XPS、SEM、TEM、ICP-OES和GC-MS对催化剂进行了结构和性能表征。结果表明,负载在载体上的Pd NPs分散均匀,粒径大小为(4.87±1.10)nm;Pd/N-C中的N与Pd NPs相互作用能有效分散并稳定Pd NPs。与Pd/C催化剂相比,Pd/N-C催化剂具有良好的催化效果,N-C载体对Pd催化剂的催化性能具有显著的促进作用,在Pd/N-C催化二苯基硅烷与甲醇的脱氢偶联反应1 h的条件下,二苯基硅烷转化率和二苯基二甲氧基硅烷的选择性均可达到99%以上,催化剂循环使用6次后二苯基硅烷转化率仍达92%以上,二苯基二甲氧基硅烷选择性达到99%以上;此外,Pd/N-C催化剂还具有优异的底物普适性。
Nitrogen-doped carbon carrier(N-C)was synthesized using glucose as carbon source and thiourea as nitrogen source,of which the doped nitrogen atom interacted with palladium nanoparticles(Pd NPs)to obtain Pd/N-C catalyst.The Pd/N-C catalyst,characterized by XRD,XPS,SEM,TEM,ICP-OES,and GC-MS,was used in the dehydrogenation coupling reaction of silanes and alcohols,and the underlying mechanism was speculated.The results indicated that the Pd NPs,with a particle size of(4.87±1.10)nm,were uniformly dispersed on the carrier.The interaction between N in the N-C carrier and Pd NPs effectively dispersed and stabilized the Pd NPs.Compared with Pd/C catalyst,Pd/N-C catalyst displayed better catalytic performance,with N-C carrier exhibiting significant promotional effect on the catalytic performance of Pd catalyst.The Pd/N-C catalyst achieved a diphenylsilane conversion and diphenyldimethoxysilane selectivity of over 99%after 1 h for the dehydrogenative coupling reaction of diphenylsilane with methanol.The catalyst retained a conversion rate of over 92%after six cycles,and the final product,diphenyldimethoxysilane,achieved a selectivity of over 99%.In addition,Pd/N-C catalyst showed substrate versatility.
作者
曾蓉
钟燚超
张慧颖
那兵
王和荣
丁顺民
ZENG Rong;ZHONG Yichao;ZHANG Huiying;NA Bing;WANG Herong;DING Shunmin(Jiangxi Province Key Laboratory of Polymer Micro/Nano Manufacturing and Devices,School of Materials and Chemistry Science,East China University of Science and Technology,Nanchang 330013,Jiangxi,China;Key Laboratory of Jiangxi Province for Environment and Energy Catalysis,School of Chemistry and Chemical Engineering,Nanchang University,Nanchang 330031,Jiangxi,China)
出处
《精细化工》
北大核心
2025年第9期2022-2028,共7页
Fine Chemicals
基金
国家自然科学基金项目(22002056,22262022)
江西省自然科学基金-面上项目(20232BAB203013,20232BAB203016)
江西省教育厅科学技术研究项目(GJJ210707)
江西省聚合物微纳制造与器件重点实验室开放基金项目(PMND202110)
东华理工大学博士科研启动基金项目(DHBK2019113)。
关键词
氮掺杂碳
负载钯催化剂
脱氢偶联反应
硅烷
醇
催化技术
nitrogen-doped carbon
supported palladium catalysts
dehydrogenation coupling reaction
silanes
alcohols
catalysis technology
