Bi_(2)O_(2)CO_(3)/ZnIn_(2)S_(4)上活性氧物种和光活性电荷的协同作用实现5-羟甲基糠醛的选择性光氧化转化  

Customizing the synergy of reactive oxygen species and photoactive charges on Bi_(2)O_(2)CO_(3)/ZnIn_(2)S_(4) for the selective photooxidation transformation of 5-hydroxymethylfurfural

作　　者：杨碧霞 朱孟瑶 江兴朋 邵文磊 王智琦 颜家伟 郑艳婷 庄赞勇 于岩 Bixia Yang;Mengyao Zhu;Xingpeng Jiang;Wenlei Shao;Zhiqi Wang;Jiawei Yan;Yanting Zheng;Zanyong Zhuang;Yan Yu(College of Materials Science and Engineering,Fuzhou University,Fuzhou 350108,China;Key Laboratory of Advanced Materials Technologies,Fuzhou University,Fuzhou 350108,China)

机构地区：[1]College of Materials Science and Engineering,Fuzhou University,Fuzhou 350108,China [2]Key Laboratory of Advanced Materials Technologies,Fuzhou University,Fuzhou 350108,China

出　　处：《Science China Materials》2024年第1期162-169,共8页中国科学（材料科学）（英文版）

基　　金：financially supported by the National Key Research and Development Program/Key Scientific Issues of Transformative Technology (2020YFA0710303);the National Natural Science Foundation of China (U1905215 and 52072076);Fujian Science Foundation Grant (2022J01554);the Key Project of Science and Technology Innovation of Fujian Provincial Department of Education (2022G02002)。

摘　　要：光氧化转化可再生生物质衍生物为高附加值的化学品具有重要意义,但由于在控制氧化物种和理想的反应途径方面存在挑战,其选择性通常较低.本工作报道了利用CO_(2)气体介导的固固相变法制备Bi_(2)O_(2)CO_(3)/ZnIn_(2)S_(4)异质结构,用于光氧化转化生物质衍生的5-羟甲基糠醛(HMF)生成2,5-二甲酰基呋喃(DFF),其选择性高达98.1%,产率达882.6μmol g^(-1)h^(-1).金属碳酸盐/氧化物异质界面诱导了光活性电子和空穴的有效转移,优化了表面氧的活化,促进了·OOH和空穴的协同作用,进而可以选择性地将HMF转化为DFF.本工作表明异质界面上电子-空穴对和活性氧物种的调控有助于利用可再生原料实现可持续发展.The photooxidation of renewable bioderivatives into value-added chemicals is highly significant;however,it typically exhibits low selectivity owing to the challenges in controlling the oxidative species and managing the desirable reaction pathways.In this work,we used the Bi2O_(2)CO_(3)/ZnIn_(2)S_(4) heterostructure,prepared by a CO_(2)-mediated solid-solid phase transition,to catalyze the photooxidation of bio-derived 5-hydroxymethylfurfural(HMF)into 2,5-di-formylfuran(DFF)with a high selectivity of 98.1%and a yield rate of 882.6μmol g^(-1)h^(-1).The metal carbonate/oxide hetero-interface enables the effective transfer of photoactive electrons and holes,optimizes surface oxygen activation,and facilitates the synergy of·OOH and holes to selectively convert HMF into DFF.The findings unravel how the tailoring and coupling of the electron-hole pairs and reactive oxygen species on het-erostructured materials can promote the usage of renewable feedstocks for sustainable development.

关 键 词：光活性 可再生原料 可再生生物质 活性氧物种 光氧化 反应途径 异质结构 表面氧 

分 类 号：O626[理学—有机化学]