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Uniform single atomic Cu_(1)-C_(4)sites anchored in graphdiyne for hydroxylation of benzene to phenol

查看全文 作　　者：Jia [1,2]Yu;Changyan [1,2]Cao;Hongqiang [1,2]Jin;Weiming [1,2]Chen;Qikai [1,2]Shen;Peipei [1,2]Li;Lirong [3]Zheng;Feng [4]He;Weiguo [1,2]Song;Yuliang [2,4]Li 高影响力作者 机构地区：[1]Beijing National Laboratory for Molecular Sciences,CAS Research,Education Center for Excellence in Molecular Sciences,Key Laboratory of Molecular Nanostructures and Nanotechnology,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China;[2]University of Chinese Academy of Sciences,Beijing 100049,China;[3]Beijing Synchrotron Radiation Facility(BSRF),Institute of High Energy Physics,Chinese Academy of Sciences,Beijing 100049,China;[4]Beijing National Laboratory for Molecular Sciences,CAS Research,Education Center for Excellence in Molecular Sciences,Laboratory of Organic Solids,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China高影响力机构 出　　处：《National Science Review》索引2022年第9卷第9期,共8页高影响力期刊 基　　金：supported by the National Key R&D Program of China(2018YFA0703503 and 2018YFA0208504);the National Natural Science Foundation of China(21932006);the Youth Innovation Promotion Association of CAS。 摘　　要：For single-atom catalysts(SACs),the catalyst supports are not only anchors for single atoms,but also modulators for geometric and electronic structures,which determine their catalytic performance.Selecting an appropriate support to prepare SACs with uniform coordination environments is critical for achieving optimal performance and clarifying the relationship between the structure and the property of SACs.Approaching such a goal is still a significant challenge.Taking advantage of the strong d-πinteraction between Cu atoms and diacetylenic in a graphdiyne(GDY)support,we present an efficient and simple strategy for fabricating Cu single atoms anchored on GDY(Cu_(1)/GDY)with uniform Cu_(1)-C_(4)single sites under mild conditions.The Cu atomic structure was confirmed by combining synchrotron radiation X-ray absorption spectroscopy,X-ray photoele ctron spectroscopy and density functional theory(DFT)calculations.The as-prepared Cu1/GDY exhibits much higher activity than state-of-the-art SACs in direct benzene oxidation to phenol with H_(2)O_(2)reaction,with turnover frequency values of 251 h^(-1)at room temperature and 1889 h^(-1)at 60℃,respectively.Furthermore,even with a high benzene conversion of86%,high phenol sele ctivity(96%)is maintaine d,which can be ascribed to the hydrophobic and oleophyllic surface nature of Cu1/GDY for benzene adsorption and phenol desorption.Both experiments and DFT calculations indicate that Cu_(1)-C_(4)single sites are more effective at activating H_(2)O_(2)to form Cu=O bonds,which are important active intermediates for benzene oxidation to phenol. 关 键 词：single-atom catalysis graphdiyne copper benzene oxidation PHENOL
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