首页|d-Orbital steered FeN4 moiety through N,S dual-site adjustation for zinc-air flow battery

d-Orbital steered FeN4 moiety through N,S dual-site adjustation for zinc-air flow battery

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The implementation of pristine covalent organic polymer(COP)with well-defined structure as air elec-trode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains chal-lenges in synergistically regulating their electronic states and structural porosity for the great device performance.Here,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron pathway.Meanwhile,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive substances.Benefiting from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E1/2=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@COP cat-alyst demonstrate exceptional power density(163.8 mW cm-2)and continuous charge and discharge for approximately 140 h at 10 mA cm-2,outperforming the noble-metal benchmarks.

Nitrogen/sulfur dual sitesMetal-coordinated nitrogen sitesCovalent organic polymerOxygen reduction reactionZn-air flow battery

Chunzhu Bao、Mingwei Tong、Xueli Li、Zhonghua Xiang

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State Key Laboratory of Organic-Inorganic Composites,Beijing University of Chemical Technology,Beijing 100029,China

National Key Research and Development Program of ChinaNatural Science Foundation of ChinaBeijing Natural Science Foundation"Double-First-Class"construction projects"Double-First-Class"construction projectsChina Postdoctoral Science FoundationDostdoctoral Fellowship Program of CPSF

2022YFB380750022220102003JL23003XK180301XK1804-022023TQ0020GZC20230199

2024

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子:0.654
ISSN:2095-4956
年,卷(期):2024.92(5)