Daijie Deng, Junchao Qian, Suqin Wu, Wei Zhang*, Erjin Zhang, Henan Li* and Li Xu*,
{"title":"准固态锌-空气电池中Mn-Nx位与丰富缺陷碳的耦合增强氧电还原","authors":"Daijie Deng, Junchao Qian, Suqin Wu, Wei Zhang*, Erjin Zhang, Henan Li* and Li Xu*, ","doi":"10.1021/acssuschemeng.5c04630","DOIUrl":null,"url":null,"abstract":"<p >The integration of Mn–N<sub><i>x</i></sub> sites with defective carbon can significantly enhance the oxygen reduction reaction (ORR) activity of carbon-based catalysts. Herein, wheat straw is molecularly assembled with Mn source and nitrogen-rich compounds to generate a macromolecular precursor through hydrogen bonding and promote the dispersion of Mn-related species. The Mn–N<sub><i>x</i></sub> sites anchored on wheat straw-derived porous carbon can be synthesized during high-temperature pyrolysis. Meanwhile, the macromolecular precursor can produce nitrogen-related and carbon-related gases to form defective carbon (r-Mn/N-WSPC). Rich Mn–N<sub><i>x</i></sub> sites can serve as effective ORR sites on r-Mn/N-WSPC. Abundant defective carbon can optimize the electronic structure of Mn–N<sub><i>x</i></sub> sites, adjust O<sub>2</sub> adsorption energy to a moderate state, and reduce the energy barrier. The r-Mn/N-WSPC exhibits a large specific surface area of 1667.53 m<sup>2</sup> g<sup>–1</sup> and an ORR half-wave potential of 0.921 V (vs RHE). With r-Mn/N-WSPC as the cathode catalyst, the excellent performance of quasi-solid-state zinc-air batteries (ZABs) with a specific capacity of 639.74 mA h g<sup>–1</sup>, a power density of 36.16 mW cm<sup>–2</sup>, and a long-term charge–discharge cycle stability of about 28 h can be obtained. The performance exploration of r-Mn/N-WSPC contributes to the efficient development and applications of wheat straw-derived carbon in quasi-solid-state ZABs.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 35","pages":"14472–14482"},"PeriodicalIF":7.3000,"publicationDate":"2025-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Coupling of Mn–Nx Sites with Abundant Defective Carbon for Enhanced Oxygen Electroreduction in Quasi-Solid-State Zinc–Air Batteries\",\"authors\":\"Daijie Deng, Junchao Qian, Suqin Wu, Wei Zhang*, Erjin Zhang, Henan Li* and Li Xu*, \",\"doi\":\"10.1021/acssuschemeng.5c04630\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The integration of Mn–N<sub><i>x</i></sub> sites with defective carbon can significantly enhance the oxygen reduction reaction (ORR) activity of carbon-based catalysts. 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引用次数: 0
摘要
Mn-Nx位点与缺陷碳的整合可以显著提高碳基催化剂的氧还原反应(ORR)活性。本文将麦秆与Mn源和富氮化合物进行分子组装,通过氢键生成大分子前体,促进Mn相关物种的分散。在高温热解过程中,可以合成锚定在麦秆衍生多孔碳上的Mn-Nx位点。同时,大分子前驱体可以产生氮相关气体和碳相关气体,形成缺陷碳(r-Mn/N-WSPC)。富Mn-Nx位点可作为r-Mn/N-WSPC的有效ORR位点。丰富的缺陷碳可以优化Mn-Nx位的电子结构,将O2吸附能调节到一个适中的状态,降低能垒。r-Mn/N-WSPC的比表面积为1667.53 m2 g-1, ORR半波电位为0.921 V(相对于RHE)。以r-Mn/N-WSPC为阴极催化剂,准固态锌空气电池(ZABs)具有优异的性能,比容量为639.74 mA h g-1,功率密度为36.16 mW cm-2,长期充放电循环稳定性约为28 h。研究r-Mn/N-WSPC的性能有助于麦秸碳在准固态ZABs中的高效开发和应用。
Coupling of Mn–Nx Sites with Abundant Defective Carbon for Enhanced Oxygen Electroreduction in Quasi-Solid-State Zinc–Air Batteries
The integration of Mn–Nx sites with defective carbon can significantly enhance the oxygen reduction reaction (ORR) activity of carbon-based catalysts. Herein, wheat straw is molecularly assembled with Mn source and nitrogen-rich compounds to generate a macromolecular precursor through hydrogen bonding and promote the dispersion of Mn-related species. The Mn–Nx sites anchored on wheat straw-derived porous carbon can be synthesized during high-temperature pyrolysis. Meanwhile, the macromolecular precursor can produce nitrogen-related and carbon-related gases to form defective carbon (r-Mn/N-WSPC). Rich Mn–Nx sites can serve as effective ORR sites on r-Mn/N-WSPC. Abundant defective carbon can optimize the electronic structure of Mn–Nx sites, adjust O2 adsorption energy to a moderate state, and reduce the energy barrier. The r-Mn/N-WSPC exhibits a large specific surface area of 1667.53 m2 g–1 and an ORR half-wave potential of 0.921 V (vs RHE). With r-Mn/N-WSPC as the cathode catalyst, the excellent performance of quasi-solid-state zinc-air batteries (ZABs) with a specific capacity of 639.74 mA h g–1, a power density of 36.16 mW cm–2, and a long-term charge–discharge cycle stability of about 28 h can be obtained. The performance exploration of r-Mn/N-WSPC contributes to the efficient development and applications of wheat straw-derived carbon in quasi-solid-state ZABs.
期刊介绍:
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