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A green edge-hosted zinc single-site heterogeneous catalyst for superior Fenton-like activity.

ABSTRACT: Developing green heterogeneous catalysts with excellent Fenton-like activity is critical for water remediation technologies. However, current catalysts often rely on toxic transitional metals, and their catalytic performance is far from satisfactory as alternatives of homogeneous Fenton-like catalysts. In this study, a green catalyst based on Zn single-atom was prepared in an ammonium atmosphere using ZIF-8 as a precursor. Multiple characterization analyses provided evidence that abundant intrinsic defects due to the edge sites were created, leading to the formation of a thermally stable edge-hosted Zn-N₄ single-atom catalyst (ZnN₄-Edge). Density functional theory calculations revealed that the edge sites equipped the single-atom Zn with a super catalytic performance, which not only promoted decomposition of peroxide molecule (HSO₅^-) but also greatly lowered the activation barrier for ^•OH generation. Consequently, the as-prepared ZnN₄-Edge exhibited extremely high Fenton-like performance in oxidation and mineralization of phenol as a representative organic contaminant in a wide range of pH, realizing its quick detoxification. The atom-utilization efficiency of the ZnN₄-Edge was ~10⁴ higher than an equivalent amount of the control sample without edge sites (ZnN₄), and the turnover frequency was ~10³ times of the typical benchmark of homogeneous catalyst (Co²⁺). This study opens up a revolutionary way to rationally design and optimize heterogeneous catalysts to homogeneous catalytic performance for Fenton-like application.

SUBMITTER: Yu X

PROVIDER: S-EPMC10450848 | biostudies-literature | 2023 Aug

REPOSITORIES: biostudies-literature

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A green edge-hosted zinc single-site heterogeneous catalyst for superior Fenton-like activity.

Yu Xiaoyong X Liu Hongzhi H Huang Yixuan Y Li Changlin C Kuang Liuning L Zhong Jinyu J Zhu Shuo S Gou Yating Y Wang Yunhang Y Zhang Yinqing Y Shan Guoqiang G Lv Zhengxin Z Zhang Shuo S Zhu Lingyan L

Proceedings of the National Academy of Sciences of the United States of America 20230817 34

Developing green heterogeneous catalysts with excellent Fenton-like activity is critical for water remediation technologies. However, current catalysts often rely on toxic transitional metals, and their catalytic performance is far from satisfactory as alternatives of homogeneous Fenton-like catalysts. In this study, a green catalyst based on Zn single-atom was prepared in an ammonium atmosphere using ZIF-8 as a precursor. Multiple characterization analyses provided evidence that abundant intrin ...[more]

PMID: 37590415

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Project description:The development of a heterogeneous catalyst for use in environmental remediation remains a challenging and attractive research endeavor. Specifically, for Fenton reactions, most research approaches have focused on the preparation of iron-containing heterostructures as photo-Fenton catalysts that utilize visible light for enhancing the degradation efficiency. Herein, the synthesis and novel application of C,N-doped iron borates are demonstrated as single-component heterogeneous photo-Fenton catalysts with high Fenton activity under visible light. Under the optimal conditions, 10 mg of the catalyst is shown to achieve effective degradation of 10 ppm methylene blue (MB) dye, Rhodamine B (RhB) dye, and tetracycline (TC) under simulated solar irradiation with a first-order rate constant of k = 0.218 min-1, 0.177 min-1, and 0.116 min-1, respectively. Using MB as a model system, the C,N-doped iron borate exhibits 10- and 26-fold increases in catalytic activity relative to that of the 50 nm hematite nanoparticles and that of the non-doped iron borate, respectively, in the presence of H2O2 under the simulated solar irradiation. Furthermore, the optimum reaction conditions used only 320 equivalents of H2O2 with respect to the concentration of dye, rather than the several thousand equivalents of H2O2 used in conventional heterogeneous Fenton catalysts. In addition, the as-prepared C,N-doped iron borate achieves 75% MB degradation after 20 min in the dark, thus enabling the continuous degradation of pollutants at night and in areas with poor light exposure. The stability and recyclability of C,N-doped iron borate for the oxidation of MB was demonstrated over three cycles with insignificant loss in photo-Fenton activity. The high Fenton activity of the C,N-doped iron borate is considered to be due to the synergistic action between the negatively-charged borate ligands and the metal center in promoting the Fenton reaction. Moreover, carbon and nitrogen doping are shown to be critical in modifying the electronic structure and increasing the conductivity of the catalyst. In view of its synthetic simplicity, high efficiency, low cost of reagents, and minimal cost of operation (driven by natural sunlight), the as-prepared heterogeneous single-component metal borate catalyst has potential application in the industrial treatment of wastewater.

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A green edge-hosted zinc single-site heterogeneous catalyst for superior Fenton-like activity.

Publications

A green edge-hosted zinc single-site heterogeneous catalyst for superior Fenton-like activity.

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