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Optimizing geometric configuration of single Zn-N_(4) sites for boosting reciprocal transformation between aromatic alcohols and aldehydes

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摘要 It is significant to optimize geometric configuration of metal catalytic sites and boost their catalytic activity.Herein,we synthesized isolated single Zn-N_(4)sites on N-doped carbon(Zn-CN)by pyrolyzing zeolite imidazole framework-8(ZIF-8)at different temperatures.For the reciprocal transformation between benzyl alcohol and benzaldehyde,the catalytic activities of Zn-CN catalysts exhibited a volcano-like trend as the pyrolysis temperatures increased.The optimal catalyst was Zn-CN-900,with outstanding catalytic activity exceeding commercial 20 wt.%Pd/C and 20 wt.%Pt/C,promising to substitute the noble metalbased catalysts.X-ray absorption near-edge structure(XANES)measurements and density functional theory(DFT)calculation revealed the gradual transformation from tetrahedral ZnN_(4)sites of ZIF-8 into planar ZnN_(4)sites above 700℃,with the maximum planar ZnN_(4)sites in Zn-CN-900.The stronger adsorption between reactants and planar ZnN_(4)sites facilitated the activation of reactants compared with tetrahedral ZnN_(4)sites.This work will provide valuable insight into rational design of efficient catalysts by optimizing geometric configuration of catalytic sites.
出处 《Nano Research》 SCIE EI CSCD 2023年第7期9132-9141,共10页 纳米研究(英文版)
基金 This work was supported by the National Postdoctoral Program for Innovative Talents(No.BX20220159) the National Natural Science Foundation of China(No.21890383)。
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