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典型文献
Non-contact biomimetic mechanism for selective hydrogenation of nitroaromatics on heterogeneous metal nanocatalysts
文献摘要:
While the enzymatic reduction of unsaturated compounds usually has high specificity,highly selective reduction processes are hardly realized by heterogeneous industrial catalysts,which is critical for the green production of many fine chemicals.Here,we report an unexpected discovery of a biomimetic behavior of dicyandiamide(DICY)-modified Pt nanocatalysts for the green hydrogenation of a wide range of nitroaromatics.We demonstrate that the surface modification by DICY not only prevents the direct contact of nitroaromatic reactants with Pt surface but also induces an effective non-contact hydrogenation mechanism mediated by protons and electrons.In such a process,the DICY layer serves as a"semi-permeable membrane"to allow the permeation of H2 molecules for being activated into electrons and protons at the Pt-DICY interface.With the generation of separated protons and electrons,the nitro group with strong electrophilic properties can be hydrogenated through the electron transfer followed by the proton transfer,which is facilitated by the hydrogen bonding network formed by protonated DICY.The unique mechanism makes it highly directional toward the hydrogenation of nitro groups without side reactions.Owing to its capability to largely eliminate the waste generation,the developed Pt-DICY catalysts have been successfully applied for the green industrial production of many important aniline intermediates.
文献关键词:
作者姓名:
Wenting Zhou;Laiyang Li;Ruixuan Qin;Jiaxin Zhu;Shengjie Liu;Shiguang Mo;Zaifa Shi;Huihuang Fang;Pengpeng Ruan;Jun Cheng;Gang Fu;Nanfeng Zheng
作者机构:
State Key Laboratory for Physical Chemistry of Solid Surfaces,Collaborative Innovation Center of Chemistry for Energy Materials,and Department of Chemistry,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China;Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM),Xiamen 361005,China
引用格式:
[1]Wenting Zhou;Laiyang Li;Ruixuan Qin;Jiaxin Zhu;Shengjie Liu;Shiguang Mo;Zaifa Shi;Huihuang Fang;Pengpeng Ruan;Jun Cheng;Gang Fu;Nanfeng Zheng-.Non-contact biomimetic mechanism for selective hydrogenation of nitroaromatics on heterogeneous metal nanocatalysts)[J].中国科学:化学(英文版),2022(04):726-732
A类:
dicyandiamide,DICY,nitroaromatic
B类:
Non,contact,biomimetic,mechanism,selective,hydrogenation,nitroaromatics,heterogeneous,metal,nanocatalysts,While,enzymatic,reduction,unsaturated,compounds,usually,has,specificity,highly,processes,are,hardly,realized,by,industrial,which,critical,green,production,many,fine,chemicals,Here,report,unexpected,discovery,behavior,modified,Pt,wide,range,We,demonstrate,that,surface,modification,not,only,prevents,reactants,but,also,induces,effective,mediated,protons,electrons,In,such,layer,serves,semi,permeable,membrane,allow,permeation,H2,molecules,being,activated,into,interface,With,generation,separated,strong,electrophilic,properties,can,hydrogenated,through,transfer,followed,facilitated,bonding,network,formed,protonated,unique,makes,directional,toward,groups,without,side,reactions,Owing,its,capability,largely,eliminate,waste,developed,have,been,successfully,applied,important,aniline,intermediates
AB值:
0.550466
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