ZIF-67-derived Co3O4@CN-assisted g-C3N4 for efficient photocatalytic hydrogen peroxide production

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-09-28 DOI:10.1016/j.mcat.2024.114584
Heng Chen, Longhui Nie, Yiqiong Yang, Caihong Fang, Xingru Chen, Xueling Li
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Abstract

The conversion of solar energy into chemical energy can be realized by photocatalytic technology, which is also used for hydrogen peroxide (H2O2) production because of its clean and eco-friendly properties. Here, g-C3N4 (GCN) was coupled with the ZIF-67 derivate (Co3O4@CN) by a thermal treatment to obtain the ZCN-X (X = 5, 10, 15 mg of ZIF-67) composite photocatalyst for H2O2 production for the first time. ZCN-10 showed the optimal photocatalytic H2O2 production efficiency of 531.1 μM (or 2655.3 µmol⋅g-1⋅h-1) in one hour, which was 3.49 times that of GCN (152.0 μM). ZCN-10 also showed relatively good stability of photocatalytic H2O2 production with a slight decrease after five cycles. The introduction of Co3O4@CN on GCN increases the catalyst's specific surface area, visible light adsorption, surface-adsorbed oxygen content, and separation efficiency of photogenerated carriers, which jointly cause a large increase in photocatalytic H2O2 production. The mechanism for H2O2 production was proved to be a two-step one-electron oxygen reduction reaction (ORR) pathway. This work would shed light on the fabrication of g-C3N4-based photocatalysts with high performance for H2O2 production.

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ZIF-67 衍生 Co3O4@CN 辅助 g-C3N4 用于高效光催化过氧化氢生产
光催化技术可将太阳能转化为化学能,由于其清洁环保的特性,也可用于生产过氧化氢(H2O2)。在这里,g-C3N4(GCN)与 ZIF-67 衍生物(Co3O4@CN)通过热处理耦合,首次获得了用于生产 H2O2 的 ZCN-X(X = 5、10、15 毫克 ZIF-67)复合光催化剂。ZCN-10 在一小时内的最佳光催化 H2O2 生成效率为 531.1 μM(或 2655.3 µmol-g-1-h-1),是 GCN(152.0 μM)的 3.49 倍。ZCN-10 在光催化产生 H2O2 方面也表现出较好的稳定性,但在五个周期后略有下降。在 GCN 上引入 Co3O4@CN 增加了催化剂的比表面积、可见光吸附量、表面吸附氧含量和光生载流子的分离效率,共同导致光催化 H2O2 产率的大幅提高。H2O2 生成的机理被证明是两步单电子氧还原反应(ORR)途径。这项工作将为制备高性能的 g-C3N4 基光催化剂提供启示。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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