A green edge-hosted zinc single-site heterogeneous catalyst for superior Fenton-like activity
Xiao-Yong Yu, Hong‐Zhi Liu, Yixuan Huang, Changlin Li, Liuning Kuang, Jinyu Zhong, Shuo Zhu, Yating Gou, Yunhang Wang, Yinqing Zhang, Guoqiang Shan, Zhengxin Lv, Shuo Zhang, Lingyan Zhu
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−N 4 single-atom catalyst (ZnN 4 −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 (HSO 5 − ) but also greatly lowered the activation barrier for • OH generation. Consequently, the as-prepared ZnN 4 −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 ZnN 4 −Edge was ~10 4 higher than an equivalent amount of the control sample without edge sites (ZnN 4 ), and the turnover frequency was ~10 3 times of the typical benchmark of homogeneous catalyst (Co 2+ ). This study opens up a revolutionary way to rationally design and optimize heterogeneous catalysts to homogeneous catalytic performance for Fenton-like application.