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通过在介孔碳骨架上引入多种掺杂剂同时改善氧还原和催化剂锚定用于柔性铝空气电池

Simultaneous Improvement of Oxygen Reduction and Catalyst Anchoring via Multiple Dopants on Mesoporous Carbon Frameworks for Flexible Al-Air Batteries.

作者信息

Hu Kailong, Wang Xudong, Hu Yixuan, Hu Haolin, Lin Xiaorong, Reddy Kolan Madhav, Luo Min, Qiu Hua-Jun, Lin Xi

机构信息

School of Materials Science and Engineering, and Institute of Materials Genome & Big Data, Harbin Institute of Technology Shenzhen, Shenzhen 518055, P. R. China.

State Key Laboratory of Advanced Welding and Joining, Harbin Institute of Technology, Harbin 150001, P. R. China.

出版信息

ACS Nano. 2022 Nov 22;16(11):19165-19173. doi: 10.1021/acsnano.2c08332. Epub 2022 Nov 10.

Abstract

Mesoporous carbon supported non-noble metals, as promising catalysts for boosting the oxygen reduction reaction (ORR) in metal-air batteries, usually face challenges of low activity and performance degradation caused by the catalyst detachment from carbon substrates. Herein, a one-stone-two-birds strategy is reported to simultaneously improve the ORR activity and anchor nanosized MnS catalysts on a mesoporous carbon framework via nitrogen (N) and sulfur (S) dopants (MnS/NS-C). Synchrotron-based X-ray absorption spectroscopy (XAS) confirms the existence of Mn-N and Mn-S bonds, which firmly anchor active MnS nanoparticles. Density functional theory (DFT) calculations reveal that the N, S codoping lowers the d-band center of Mn and optimizes ORR intermediate adsorption. An excellent ORR performance (the onset and half-wave potential of 1.07 and 0.91 V) and long-term durability are achieved for MnS/NS-C in alkaline media. The flexible Al-air battery, using MnS/NS-C as the cathode catalyst, shows a power density of 134.6 mW cm in comparison to the Pt/C-based counterpart of 106.2 mW cm. This study constructs a stable interaction with non-noble catalysts and carbon substrates for enhancing catalytic activity and durability in metal-air batteries.

摘要

介孔碳负载的非贵金属作为金属空气电池中促进氧还原反应(ORR)的有前景的催化剂,通常面临活性低以及催化剂从碳载体上脱离导致性能下降的挑战。在此,报道了一种一石二鸟的策略,通过氮(N)和硫(S)掺杂剂(MnS/NS-C)同时提高ORR活性并将纳米级MnS催化剂锚定在介孔碳框架上。基于同步加速器的X射线吸收光谱(XAS)证实了Mn-N键和Mn-S键的存在,它们牢固地锚定了活性MnS纳米颗粒。密度泛函理论(DFT)计算表明,N、S共掺杂降低了Mn的d带中心并优化了ORR中间体吸附。MnS/NS-C在碱性介质中实现了优异的ORR性能(起始电位和半波电位分别为1.07和0.91 V)以及长期耐久性。使用MnS/NS-C作为阴极催化剂的柔性铝空气电池,其功率密度为134.6 mW/cm²,而基于Pt/C的对照电池为106.2 mW/cm²。本研究构建了非贵金属催化剂与碳载体之间的稳定相互作用,以提高金属空气电池的催化活性和耐久性。

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