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单原子与硫空位协同作用用于先进的多硫化物-碘化物氧化还原液流电池

Synergy of single atoms and sulfur vacancies for advanced polysulfide-iodide redox flow battery.

作者信息

Wang Zhigui, Lu Guolong, Wei Tianran, Meng Ge, Cai Haoxiang, Feng Yanhong, Chu Ke, Luo Jun, Hu Guangzhi, Wang Dingsheng, Liu Xijun

机构信息

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035, China.

Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, Guangxi, China.

出版信息

Nat Commun. 2025 Mar 25;16(1):2885. doi: 10.1038/s41467-025-58273-9.

DOI:10.1038/s41467-025-58273-9
PMID:40133276
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11937296/
Abstract

Aqueous redox flow batteries (RFBs) incorporating polysulfide/iodide chemistries have received considerable attention due to their safety, high scalability, and cost-effectiveness. However, the sluggish redox kinetics restricted their output energy efficiency and power density. Here we designed a defective MoS nanosheets supported Co single-atom catalyst that accelerated the transformation of S/S and I/I redox couples, hence endow the derived polysulfide-iodide RFB with an initial energy efficiency (EE) of 87.9% and an overpotential of 113 mV with an average EE 80.4% at 20 mA cm and 50% state-of-charge for 50 cycles, and a maximal power density of 95.7 mW cm for an extended cycling life exceeding 850 cycles at 10 mA cm and 10% state-of-charge. In situ experimental and theoretical analyses elucidate that Co single atoms induce the generation of abundant sulfur vacancies in MoS via a phase transition process, which synergistically contributed to the enhanced adsorption of reactants and key reaction intermediates and improved charge transfer, resulting in the enhanced RFB performance.

摘要

包含多硫化物/碘化物化学体系的水系氧化还原液流电池(RFBs)因其安全性、高可扩展性和成本效益而受到了广泛关注。然而,缓慢的氧化还原动力学限制了它们的输出能量效率和功率密度。在此,我们设计了一种缺陷型MoS纳米片负载的Co单原子催化剂,该催化剂加速了S/S和I/I氧化还原对的转化,从而赋予所制备的多硫化物-碘化物RFB在20 mA cm、50%充电状态下50个循环的初始能量效率(EE)为87.9%、过电位为113 mV且平均EE为80.4%,以及在10 mA cm、10%充电状态下超过850个循环的延长循环寿命时最大功率密度为95.7 mW cm。原位实验和理论分析表明,Co单原子通过相变过程诱导MoS中产生大量硫空位,这协同促进了反应物和关键反应中间体的增强吸附以及电荷转移的改善,从而提高了RFB的性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/50cacb9b2d1d/41467_2025_58273_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/f0852794eff5/41467_2025_58273_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/df3eaa141287/41467_2025_58273_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/06f1ca78fd83/41467_2025_58273_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/240dbdbb497e/41467_2025_58273_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/50cacb9b2d1d/41467_2025_58273_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/f0852794eff5/41467_2025_58273_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/df3eaa141287/41467_2025_58273_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/06f1ca78fd83/41467_2025_58273_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/240dbdbb497e/41467_2025_58273_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b82c/11937296/50cacb9b2d1d/41467_2025_58273_Fig5_HTML.jpg

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