MOF衍生Co3O4/ZrO2介孔八面体:优化电荷转移和中间体转化用于高效CO2光还原

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中文摘要：调控电荷转移和反应路径是促进光催化CO2还原的两种有效策略.本研究通过热解UIO-66@ZIF-67核壳八面体,合成了Co3O4/ZrO2介孔八面体.该介孔八面体由高度分散的小尺寸纳米颗粒组装而成,平均颗粒尺寸为13 nm,平均孔径为5.8 nm,比表面积为43.11 m2g-1.受益于活性位点设计,电荷转移动力学和CO2吸附得以增强.此外,密度泛函理论计算结果显示,ZrO2能够有效调控CO2还原的反应路径,包括促进CO2活化为*CO2、中间体(*COOH和*CO)的形成、以及减小限速步(*CO→CO)的能垒.因此,Co3O4/ZrO2介孔八面体的周转率高达28.82,是纯Co3O4的16.95倍.

外文标题：MOF-derived Co3O4/ZrO2 mesoporous octahedrons with optimized charge transfer and intermediate conversion for efficient CO2 photoreduction

外文摘要：Regulating charge transfer and reaction path-ways are effective strategies for boosting photocatalytic CO2 reduction.Herein,Co3O4/ZrO2 mesoporous octahedrons are synthesized through facile pyrolysis of UIO-66@ZIF-67 core/shell octahedrons.The as-obtained Co3O4/ZrO2 mesoporous octahedrons are assembled by highly dispersive and small-sized nanoparticles,with 13 nm average particle size and 5.8 nm pore width,leading to a high specific surface area of 43.11 m2g-1.Benefiting from active-site engineering,the charge-transfer kinetics and CO2 adsorption are successfully enhanced.In addition,density functional theory calculations reveal that ZrO2 tailors the reaction pathway of CO2 reduction by promoting CO2 activation to*CO2 and intermediate for-mation(*COOH and*CO),as well as decreasing the energy barrier of the rate-limiting step(*CO→CO).Thus,the Co3O4/ZrO2 mesoporous octahedrons afford a turnover frequency of 28.82 h-1,16.95-fold larger than pure Co3O4.

外文关键词：

metal-organic frameworksmesoporousoxidesphotocatalysisCO2 reduction

作者：

刘海兵、邱衍滨、甘文秀、庄国鑫、陈飞飞、杨程凯、于岩

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作者单位：

Key Laboratory of Advanced Materials Technologies,International(HongKong Macao and Taiwan)Joint Laboratory on Advanced Materials Technologies,College of Materials Science and Engineering,Fuzhou University,Fuzhou 350108,China

Scientific Research and Experiment Center,Fujian Police College,Fuzhou 350007,China

关键词：

metal-organic frameworks mesoporous oxides photocatalysis CO2 reduction

基金：

National Key Research and Development Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNatural Science Foundation of Fujian ProvinceNatural Science Foundation of Fujian Province

项目编号：

2020YFA071030352002072U1905215520720762021J015892023J05082

出版年：

2024

DOI：

10.1007/s40843-023-2707-3

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(2)

参考文献量70