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

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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Abstract

Regulating charge transfer and reaction pathways 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 m2 g−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 formation (*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.

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 m2 g−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.

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Acknowledgements

This work was supported by the National Key Research and Development Program of China (2020YFA0710303), the National Natural Science Foundation of China (52002072, U1905215, and 52072076), and the Natural Science Foundation of Fujian Province (2021J01589 and 2023J05082).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. 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

    Haibing Liu  (刘海兵), Yanbin Qiu  (邱衍滨), Wenxiu Gan  (甘文秀), Fei-Fei Chen  (陈飞飞), Chengkai Yang  (杨程凯) & Yan Yu  (于岩)

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

    Guoxin Zhuang  (庄国鑫)

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  1. Haibing Liu  (刘海兵)
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Contributions

Author contributions Liu H performed the experiments and wrote the draft; Gan W contributed to sample synthesis; Zhuang G contributed to the data analysis; Qiu Y and Yang C contributed to the theoretical analysis; Chen FF and Yu Y conceived the ideal and revised the manuscript. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Fei-Fei Chen  (陈飞飞), Chengkai Yang  (杨程凯) or Yan Yu  (于岩).

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Conflict of interest The authors declare that they have no conflict of interest.

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Supplementary information Supporting data are available in the online version of the paper.

Haibing Liu received his Bachelor’s degree from Nanchang Hangkong University in 2020 and his Master’s degree from Fuzhou University in 2023. His research interest is the synthesis of advanced catalysts using MOF precursors for CO2 photoreduction.

Yanbin Qiu received his Bachelor’s degree from Fujian Normal University in 2021. Currently, he is a graduate student at Fuzhou University. His research focuses on building structure–performance relationships based on DFT calculations.

Fei-Fei Chen received his Bachelor’s degree from Xiamen University in 2014, and Doctor’s degree from Shanghai Institute of Ceramics, Chinese Academy of Sciences in 2019. Currently, he is an associate professor at Fuzhou University. His research interest is the development of ecological materials for water and air purification.

Chengkai Yang received his Bachelor’s degree from Tianjin University, and Doctor’s degree from Peking University in 2019. Currently, he is an associate professor at Fuzhou University. His research interests include energy materials, the electrochemistry of zinc-ion/lithium-ion/lithium–sulfur batteries, and material calculations.

Yan Yu received her Bachelor’s, Master’s, and Doctor’s degrees from Fuzhou University. She was a postdoctoral fellow at Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, in 2010–2013. Currently, she is a professor at Fuzhou University. Her research interests include water purification, utilization of solid waste, ecological materials, and photocatalytic CO2 reduction and H2 production.

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

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Liu, H., Qiu, Y., Gan, W. et al. MOF-derived Co3O4/ZrO2 mesoporous octahedrons with optimized charge transfer and intermediate conversion for efficient CO2 photoreduction. Sci. China Mater. 67, 588–597 (2024). https://doi.org/10.1007/s40843-023-2707-3

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