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Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene

查看全文 作  者:Yu [1,2]Xiong;Wenming [3]Sun;Yunhu [4]Han;Pingyu [2]Xin;Xusheng [5]Zheng;Wensheng [5]Yan;Juncai [6]Dong;Jian [2]Zhang;Dingsheng [2]Wang;Yadong [2]Li 高影响力作者 机构地区:[1]Department of Chemistry and Chemical Engineering,Central South University,Changsha 410083,China;[2]Department of Chemistry,Tsinghua University,Beijing 100084,China;[3]China College of Science,China Agricultural University,Beijing 100193,China;[4]Institute of Flexible Electronics,Northwestern Polytechnical University,Xi’an 710072,China;[5]National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China;[6]Beijing Synchrotron Radiation Facility,Institute of High Energy Physics,Chinese Academy of Sciences,Beijing 100084,China高影响力机构 出  处:《Nano Research》索引2021年第14卷第7期,共6页高影响力期刊 基  金:This work was supported by the National Key R&D Program of China(Nos.2018YFA0702003 and 2016YFA0202801);the National Natural Science Foundation of China(Nos.21890383,21671117,21871159,and 21901135);Science and Technology Key Project of Guangdong Province of China(No.2020B010188002);Beijing Municipal Science&Technology Commission(No.Z191100007219003);China Postdoctoral Science Foundation(No.2018M640114). 摘  要:The oxidation of hydrocarbons to produce high value-added compounds(ketones or alcohols)using oxygen in air as the only oxidant is an efficient synthetic strategy from both environmental and economic views.Herein,we successfully synthesized cobalt single atom site catalysts(Co SACs)with high metal loading of 23.58 wt.%supported on carbon nitride(CN),which showed excellent catalytic properties for oxidation of ethylbenzene in air.Moreover,Co SACs show a much higher turn-over frequency(19.6 h^(−1))than other reported non-noble catalysts under the same condition.Comparatively,the as-obtained nanosized or homogenous Co catalysts are inert to this reaction.Co SACs also exhibit high selectivity(97%)and stability(unchanged after five runs)in this reaction.DFT calculations reveal that Co SACs show a low energy barrier in the first elementary step and a high resistance to water,which result in the robust catalytic performance for this reaction. 关 键 词:single atom site high-loading catalysts heterogeneous catalysts ethylbenzene oxidation
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