中性介质高性能氧还原合成过氧化氢碳基催化电极研究

本项目针对中性介质中电化学催化氧气还原制备过氧化氢过程中存在的催化剂活性低、反应过电位过高及电极稳定性差等问题，以构建中性介质中活性好及耐久性高的催化电极为目标，拟开展基于金属Zn和Al的M-O-C或M-S-C金属单原子调控碳材料活性并发展相应催化剂的自支撑、超亲气结构电极等。研究内容主要包括以不同配体的金属有机框架材料为前驱体制备不同配位原子支持的金属单原子掺杂的碳材料；探索碳材料组成与活性的构效关系；并发展相应活性的自支撑、超亲气碳材料电极，完成高活性、高过氧化氢产量碳基电极的制备。从实践和理论研究两方面探究中性介质中碳基材料电极高效催化氧气还原制备过氧化氢的关键问题。通过本项目的研究，能够在中性介质中快速生产过氧化氢，降低生活污水及湖泊污水的处理成本。

Electrochemical oxygen reduction reaction via a two-electron pathway in neutral medium offers an attractive route for low-concentration on-site H2O2 generation, which can be directly used in wastewater treatment, pulp bleaching and family disinfection. Compared with the acidic or alkaline conditions, the mechanism of 2e- ORR in neutral medium, such as the catalytically active site and the reaction pathway, remains elusive. The carbon-based materials have been found to be efficient in 2-e ORR. However, the most common non-noble metal single-atomic-site catalysts, including Fe, Co, Ni et al, possess active 4e ORR performance. .Herein, the applicant plans to develop Al or Zn single-atomic-site doped carbon materials. Firstly, the Metal-Organic Frameworks (MOFs) with different ligands (BDC/BTC/ H2DMBDC) are synthesized as the precursors. Then the Al and Zn single-atom-site doped carbon materials will be collected after the MOFs materials carbonized under high temperature and leached by alkaline. Then the structure characterization and reaction mechanism will reveal the relationship between the structure and properties. Finally, self-standing electrode will be prepared by using ZnO nanoarrays as the template, and through introducing target metal precursors while the conversion of ZnO to MOFs. After the carbonization, a self-standing carbon-based electrode will be completed, then a superaerophilic process will be carried out by using the PTFE modification. This project will provide insight into the development of Al and Zn single-atomic-site doped carbon-based materials and high performance of 2e-ORR.