Wang Nan, Ma Shaobo, Zhang Ruiyong, Wang Lifei, Wang Yanan, Yang Lihui, Li Jianhua, Guan Fang, Duan Jizhou, Hou Baorong
CAS Key Laboratory of Marine Environmental Corrosion and Bio-Fouling, Institute of Oceanology, Chinese Academy of Sciences, 7 Nanhai Road, Qingdao, 266071, China.
Science Center for Material Creation and Energy Conversion, Institute of Frontier and Interdisciplinary Science, Shandong University, Qingdao, 266237, China.
Adv Sci (Weinh). 2023 Nov;10(31):e2302446. doi: 10.1002/advs.202302446. Epub 2023 Sep 28.
Electrochemical oxygen reduction reaction (ORR) is an attractive and alternative route for the on-site production of hydrogen peroxide (H O ). The electrochemical synthesis of H O in neutral electrolyte is in early studying stage and promising in ocean-energy application. Herein, N-doped carbon materials (N-C ) with different N types are prepared through the pyrolysis of zeolitic imidazolate frameworks. The N-C catalysts, especially N-C , exhibit an attracting 2e ORR catalytic activity, corresponding to a high H O selectivity (≈95%) and preferable stability in 0.5 m NaCl solution. Additionally, the N-C possesses an attractive H O production amount up to 631.2 mmol g h and high Faraday efficiency (79.8%) in H-type cell. The remarkable 2e ORR electrocatalytic performance of N-C catalysts is associated with the N species and N content in the materials. Density functional theory calculations suggest carbon atoms adjacent to graphitic N are the main catalytic sites and exhibit a smaller activation energy, which are more responsible than those in pyridinic N and pyrrolic N doped carbon materials. Furthermore, the N-C catalyst demonstrates an effective antibacterial performance for marine bacteria in simulated seawater. This work provides a new insight for electro-generation of H O in neutral electrolyte and triggers a great promise in ocean-energy application.
电化学氧还原反应(ORR)是一种颇具吸引力的现场生产过氧化氢(H₂O₂)的替代途径。在中性电解质中电化学合成H₂O₂尚处于早期研究阶段,在海洋能源应用方面前景广阔。在此,通过沸石咪唑酯骨架的热解制备了具有不同N类型的N掺杂碳材料(N-C)。N-C催化剂,尤其是N-C₂,表现出引人注目的2e ORR催化活性,对应于高H₂O₂选择性(约95%)以及在0.5 m NaCl溶液中的良好稳定性。此外,N-C₂在H型电池中具有高达631.2 mmol g⁻¹ h⁻¹的可观H₂O₂产量和高法拉第效率(79.8%)。N-C催化剂显著的2e ORR电催化性能与材料中的N物种和N含量有关。密度泛函理论计算表明,与石墨N相邻的碳原子是主要催化位点,且具有较小的活化能,比吡啶型N和吡咯型N掺杂碳材料中的那些碳原子更具催化活性。此外,N-C₂催化剂在模拟海水中对海洋细菌表现出有效的抗菌性能。这项工作为在中性电解质中电生成H₂O₂提供了新的见解,并在海洋能源应用方面展现出巨大潜力。