多孔掺氮石墨化碳负载纳米钯催化剂催化十二氢N-乙基咔唑脱氢反应  

Catalytic Dehydrogenation of Dodecahydro-N-ethylcarbazole over Porous Nitrogen-doped Partially Graphitized Carbon Supported Palladium Nanocatalysts

作　　者：唐晨溪 吴绵园 白雪峰[1,2] TANG Chenxi;WU Mianyuan;BAI Xuefeng(School of Chemistry and Material Sciences,Heilongjiang University,Harbin 150080,China;Institute of Petrochemistry,Heilongjiang Academy of Sciences,Harbin 150040,China)

机构地区：[1]黑龙江大学化学化工与材料学院,黑龙江哈尔滨150080 [2]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》2024年第1期6-9,15,共5页Chemistry and Adhesion

基　　金：黑龙江省科学院基金项目(编号:STYZ2022SH01)。

摘　　要：采用湿法浸渍-化学还原法,制备了ZIF-67衍生的氮掺杂部分石墨化碳(NpGC)负载纳米钯催化剂(Pd/NpGC)。通过XRD、XPS、TEM、Raman、N_(2)物理吸附脱附等手段,对钯纳米颗粒(PdNPs)的结构、形貌和组成以及载体NpGC石墨化程度和掺氮情况进行了分析和表征。PdNPs均匀分散在NpGC表面,平均粒径为9.39 nm。载体中出现的部分石墨化和氮掺杂有利于电荷传输和反应物吸附。在常压180℃条件下,Pd/NpGC-800催化十二氢N-乙基咔唑(H12-NEC)脱氢实验结果表明:反应10 h的释氢量为5.66%(wt),脱氢率可达97.92%,同时具有较好的催化稳定性。Nitrogen doped partially graphitized carbon(NpGC)derived from ZIF-67 supported palladium nanocatalysts(Pd/NpGC)are prepared by wet impregnation-NaBH4 reduction method.The structure,morphology,composition of palladium nanoparticles(PdNPs)and the graphitization degree,nitrogen doping properties of NpGC carrier are analyzed and characterized with XRD,XPS,TEM,Raman and N_(2) physical adsorption&desorption methods.The PdNPs are uniformly dispersed on the surface of NpGC with an average particle size of 9.39 nm.The partial graphitization and nitrogen doping of carrier is beneficial to the charge transfer and adsorption of reactant.Under atmospheric pressure and 180°C,the experimental results of dehydrogenation of dodecahydro-N-ethylcarbazole(H12-NEC)catalyzed by Pd/NpGC-S show that the hydrogen release for 10 h is 5.66%(wt),and the dehydrogenation efficiency can reach 97.92%.The catalyst has a good catalytic stability.

关 键 词：ZIF-67衍生碳 氮掺杂 石墨化 脱氢反应 负载纳米钯催化剂 十二氢-N-乙基咔唑 

分 类 号：O643.38[理学—物理化学]