氮掺杂多孔碳负载纳米钯银合金催化剂的制备及催化脱氢性能研究  

Preparation of Nitrogen-doped Porous Carbon Supported Palladium-Silver Alloy Nano-catalysts and Their Catalytic Dehydrogenation Performance

作　　者：陈晓敏 白雪峰[1] CHEN Xiao-min;BAI Xue-feng(Institute of Petrochemistry,Heilongjiang Academy of Sciences,Harbin 150040,China)

机构地区：[1]黑龙江省科学院石油化学研究院,黑龙江哈尔滨150040

出　　处：《化学与粘合》2021年第5期323-329,共7页Chemistry and Adhesion

基　　金：黑龙江省科学院基金项目(编号:KY2020SH01)。

摘　　要：为了减少Pd的用量,在不加任何保护剂的条件下,以乙醇为还原剂,在碱性环境下制备了氮掺杂多孔碳(NC)负载纳米钯银合金催化剂(Pd-Ag/NC),并应用于催化全氢化N-乙基咔唑(12H-NEC)脱氢反应。采用XRD,XPS和TEM对Pd-Ag/NC的结构、组成和形貌进行了表征。表征与催化实验结果表明:纳米Pd与Ag以合金的形式存在,粒径范围在2.24~4.85nm,平均粒径为3.65nm,均匀分散在NC表面。Pd与Ag以及合金与掺氮碳之间发生电子转移,两者的协同作用可以提高催化剂的催化活性。在180℃、Pd/12H-NEC物质的量比为0.4%下,脱氢反应10h时,12H-NEC转化率可达99.72%,脱氢效率达到93.26%,释氢量为5.40wt%。In order to reduce the amount of Pd, the nitrogen-doped porous carbon(NC)supported palladium-silver alloy nano-catalysts(Pd-Ag/NC) are prepared with the ethanol as a reducing agent without adding any protective agents in an alkaline environment. And the catalytic dehydro-genation of dodecahydro-N-ethylcarbazole(12 H-NEC)is carried out over the Pd-Ag/NC. The structure, composition and morphology of the prepared Pd-Ag/NC catalysts are characterized with the XRD, XPS and TEM. The characterization and catalysis experiments show that the nano-Pd and Ag ex-ists in the form of alloys with a particle size range of 2.24~4.85 nm and an average particle size of 3.65 nm, they uniformly disperse on the surface of the NC. The electron transfer occurs between Pd and Ag and between the alloy and nitrogen-doped carbon, and their synergistic effect can improve the catalytic activity of the catalysts. When the dehydrogenation reaction carries out for 10 h under the conditions of 180 °C and a Pd/12 H-NEC molar ratio of 0.4%, the conversion rate of 12 H-NEC and dehydrogenation efficiency can reach 99.72% and 93.26%, respectively. The hydrogen release amount is 5.40 wt%.

关 键 词：氮掺杂多孔碳 钯银合金催化剂 全氢化N-乙基咔唑 脱氢反应 

分 类 号：TQ426.82[化学工程]