当前位置: X-MOL 学术React. Kinet. Mech. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Relationship between the structure and dehydrogenation of alcohols/hydrogenation of nitroarenes and base catalysis performance of Co–N–C catalyst
Reaction Kinetics, Mechanisms and Catalysis ( IF 1.8 ) Pub Date : 2020-02-03 , DOI: 10.1007/s11144-020-01737-4
Minjie Liu , Hao Zhang , Junyan Wang , Guoming Zhao , Di Liu

A Co–N–C catalyst was fabricated via pyrolysis–reduction process. Dehydrogenation/hydrogenation and base catalysis performances of the Co–N–C catalyst were investigated by using the reductive coupling of nitroarenes with alcohols and aldol condensation as probe reactions. Various characterizations were performed to explore effects of reduction and pyrolysis temperature on the structure/composition and basicity of the Co–N–C catalyst, and the relationship between structure-dehydrogenation/hydrogenation and base catalysis performance was discussed accordingly. Two different structures of Co–N–C catalyst (Co–N–C/C3N4 and Co–N–C/CNT) were obtained in different pyrolysis temperature. Co–N–C-600 with C3N4 exhibits very weak catalytic performance owe to its poor pore system and active phase. Dehydrogenation/hydrogenation behaviors of Co–N–C/CNT depend on the amount of Co–N, graphitic N in Co–N–C, while the basicity of Co–N–C is closely related to the content of N species, particularly pyrrolic N and pyridinic N. The appropriate pyrolysis temperature benefits the formation of active species, developed pore organization and strong basicity. And, the H2 reduction improve dehydrogenation/hydrogenation activity of Co–N–C/CNT because reduction can destroy carbon coating layers to expose more Co–N species and promote the transformation of N species to graphitic N. Meanwhile, H2 reduction increases the contents of graphitic N and reduces the content of pyrrolic N and pyridinic N, thus weakening catalyst basicity and consequently reducing base catalytic activity of Co–N–C/CNT.



中文翻译:

醇的结构与脱氢/硝基芳烃的加氢与Co–N–C催化剂的碱催化性能之间的关系

通过热解-还原过程制备了Co-N-C催化剂。通过使用硝基芳烃与醇的还原偶联和醇醛缩合反应作为探针反应,研究了Co–N–C催化剂的脱氢/加氢和碱催化性能。进行了各种表征,以探讨还原和热解温度对Co-N-C催化剂的结构/组成和碱度的影响,并据此讨论了结构-脱氢/加氢与碱催化性能之间的关系。在不同的热解温度下获得了两种不同的Co–N–C催化剂结构(Co–N–C / C 3 N 4和Co–N–C / CNT)。Co–N–C-600与C 3 N 4由于其较差的孔隙系统和活性相,其催化性能非常弱。Co–N–C / CNT的脱氢/氢化行为取决于Co–N–C中Co–N,石墨态氮的含量,而Co–N–C的碱度与N种类的含量密切相关,特别是适当的热解温度有利于活性物种的形成,发达的孔组织和强碱性。而且,H 2还原可提高Co–N–C / CNT的脱氢/氢化活性,因为还原会破坏碳涂层,从而暴露更多的Co–N物种,并促进N物种向石墨N的转化。同时,H 2 还原会增加石墨态氮的含量,并减少吡咯氮和吡啶二氮的含量,从而削弱了催化剂的碱性,因此降低了Co–N–C / CNT的碱催化活性。

更新日期:2020-04-22
down
wechat
bug