{"title":"焦耳加热合成的无碘氮金属纳米纤维用于H2O2电合成的微环境调节策略。","authors":"Yao Hu, Haihui Lan, Qinyuan Hu, Jiaxuan Gong, Liuhong Yang, Zhaoyu Wang, Tianyi Han, Xingchen Jiao, Dongjian Shi, Mingqing Chen, Baochun Guo, Mingliang Du","doi":"10.1021/acs.nanolett.5c02227","DOIUrl":null,"url":null,"abstract":"<p><p>The increasing demand for hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) necessitates greener production methods. In response, we developed an iodine-nitrogen-codoped metal-free carbon catalyst using the coordination microstructure regulation strategy, combined with rapid Joule heating for precise iodine and nitrogen doping. This approach allows precise control over the formation of active iodine-nitrogen coordination sites, significantly enhancing the catalytic performance for H<sub>2</sub>O<sub>2</sub> production via the two-electron oxygen reduction reaction. Among the synthesized catalysts, I-N<sub>4</sub> demonstrated superior catalytic activity, achieving a high H<sub>2</sub>O<sub>2</sub> selectivity of 90-96% and a production rate of 1265 mg L<sup>-1</sup> h<sup>-1</sup> at -0.4 V vs reversible hydrogen electrode. Operando Raman spectroscopy confirmed the dynamic evolution of intermediates during the reaction, while chronoamperometric tests showed long-term stability. This scalable, energy-efficient synthesis method offers significant potential for sustainable energy and environmental applications.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":"11266-11274"},"PeriodicalIF":9.1000,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Joule-Heating-Synthesized Iodine-Nitrogen Metal-Free Nanofiber for H<sub>2</sub>O<sub>2</sub> Electroproduction via a Coordination Microenvironment Regulation Strategy.\",\"authors\":\"Yao Hu, Haihui Lan, Qinyuan Hu, Jiaxuan Gong, Liuhong Yang, Zhaoyu Wang, Tianyi Han, Xingchen Jiao, Dongjian Shi, Mingqing Chen, Baochun Guo, Mingliang Du\",\"doi\":\"10.1021/acs.nanolett.5c02227\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The increasing demand for hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) necessitates greener production methods. In response, we developed an iodine-nitrogen-codoped metal-free carbon catalyst using the coordination microstructure regulation strategy, combined with rapid Joule heating for precise iodine and nitrogen doping. This approach allows precise control over the formation of active iodine-nitrogen coordination sites, significantly enhancing the catalytic performance for H<sub>2</sub>O<sub>2</sub> production via the two-electron oxygen reduction reaction. Among the synthesized catalysts, I-N<sub>4</sub> demonstrated superior catalytic activity, achieving a high H<sub>2</sub>O<sub>2</sub> selectivity of 90-96% and a production rate of 1265 mg L<sup>-1</sup> h<sup>-1</sup> at -0.4 V vs reversible hydrogen electrode. Operando Raman spectroscopy confirmed the dynamic evolution of intermediates during the reaction, while chronoamperometric tests showed long-term stability. This scalable, energy-efficient synthesis method offers significant potential for sustainable energy and environmental applications.</p>\",\"PeriodicalId\":53,\"journal\":{\"name\":\"Nano Letters\",\"volume\":\" \",\"pages\":\"11266-11274\"},\"PeriodicalIF\":9.1000,\"publicationDate\":\"2025-07-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nano Letters\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.nanolett.5c02227\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/7/11 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nano Letters","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acs.nanolett.5c02227","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/7/11 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
对过氧化氢(H2O2)的需求不断增加,需要更环保的生产方法。为此,我们利用配位微观结构调控策略,结合快速焦耳加热技术,开发了一种碘氮共掺杂无金属碳催化剂。这种方法可以精确控制活性碘氮配位位点的形成,显著提高了通过双电子氧还原反应生成H2O2的催化性能。在所合成的催化剂中,I-N4表现出优异的催化活性,在-0.4 V vs可逆氢电极下,对H2O2的选择性达到90-96%,产率达到1265 mg L-1 h-1。Operando拉曼光谱证实了反应过程中中间体的动态演变,而计时安培测试显示了长期稳定性。这种可扩展的、节能的合成方法为可持续能源和环境应用提供了巨大的潜力。
Joule-Heating-Synthesized Iodine-Nitrogen Metal-Free Nanofiber for H2O2 Electroproduction via a Coordination Microenvironment Regulation Strategy.
The increasing demand for hydrogen peroxide (H2O2) necessitates greener production methods. In response, we developed an iodine-nitrogen-codoped metal-free carbon catalyst using the coordination microstructure regulation strategy, combined with rapid Joule heating for precise iodine and nitrogen doping. This approach allows precise control over the formation of active iodine-nitrogen coordination sites, significantly enhancing the catalytic performance for H2O2 production via the two-electron oxygen reduction reaction. Among the synthesized catalysts, I-N4 demonstrated superior catalytic activity, achieving a high H2O2 selectivity of 90-96% and a production rate of 1265 mg L-1 h-1 at -0.4 V vs reversible hydrogen electrode. Operando Raman spectroscopy confirmed the dynamic evolution of intermediates during the reaction, while chronoamperometric tests showed long-term stability. This scalable, energy-efficient synthesis method offers significant potential for sustainable energy and environmental applications.
期刊介绍:
Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including:
- Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale
- Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies
- Modeling and simulation of synthetic, assembly, and interaction processes
- Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance
- Applications of nanoscale materials in living and environmental systems
Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.