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调控氮掺杂碳电催化剂中的N物种以在模拟海水中高效合成过氧化氢

Regulating N Species in N-Doped Carbon Electro-Catalysts for High-Efficiency Synthesis of Hydrogen Peroxide in Simulated Seawater.

作者信息

Wang Nan, Ma Shaobo, Zhang Ruiyong, Wang Lifei, Wang Yanan, Yang Lihui, Li Jianhua, Guan Fang, Duan Jizhou, Hou Baorong

机构信息

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.

出版信息

Adv Sci (Weinh). 2023 Nov;10(31):e2302446. doi: 10.1002/advs.202302446. Epub 2023 Sep 28.

Abstract

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.

摘要

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。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/19c6/10625060/9cd5333a26c2/ADVS-10-2302446-g006.jpg

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