均相分子氧化还原介质的电化学氨氧化研究

IF 7.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chemical Science Pub Date : 2025-07-02 DOI:10.1039/d5sc00730e

Tarisha Gupta, Sanyam ., Shivani Saraswat, Anirban Mondal, Biswajit Mondal

{"title":"均相分子氧化还原介质的电化学氨氧化研究","authors":"Tarisha Gupta, Sanyam ., Shivani Saraswat, Anirban Mondal, Biswajit Mondal","doi":"10.1039/d5sc00730e","DOIUrl":null,"url":null,"abstract":"Ammonia (NH₃) is a promising carbon-free energy carrier due to its high energy density and hydrogen storage capacity. Its utilization in energy systems relies on the ammonia oxidation reaction (AOR), which is critical for direct ammonia fuel cells (DAFCs) and hydrogen production. Herein, we explore a robust and inexpensive Ferrocene-based molecular electrochemical mediator, N-pyridylferrocenecarboxamide (Fcpy), for AOR. The Fcpy-mediated AOR exhibits the N2 Faradaic efficiency (FE) of 94.7 %, along with the concomitant production of H2 (FE = 87.3 %). Mechanistic studies reveal the crucial role of H-bonding through the pyridyl moiety of Fcpy in facilitating N–H bond activation. Computational analysis further corroborates the observed reaction pathways, providing deeper insights. This work highlights the potential of molecular catalysts to advance ammonia oxidation and underscores their role in sustainable energy systems.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"287 1","pages":""},"PeriodicalIF":7.4000,"publicationDate":"2025-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electrochemical Ammonia Oxidation with a Homogeneous Molecular Redox Mediator\",\"authors\":\"Tarisha Gupta, Sanyam ., Shivani Saraswat, Anirban Mondal, Biswajit Mondal\",\"doi\":\"10.1039/d5sc00730e\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Ammonia (NH₃) is a promising carbon-free energy carrier due to its high energy density and hydrogen storage capacity. Its utilization in energy systems relies on the ammonia oxidation reaction (AOR), which is critical for direct ammonia fuel cells (DAFCs) and hydrogen production. Herein, we explore a robust and inexpensive Ferrocene-based molecular electrochemical mediator, N-pyridylferrocenecarboxamide (Fcpy), for AOR. The Fcpy-mediated AOR exhibits the N2 Faradaic efficiency (FE) of 94.7 %, along with the concomitant production of H2 (FE = 87.3 %). Mechanistic studies reveal the crucial role of H-bonding through the pyridyl moiety of Fcpy in facilitating N–H bond activation. Computational analysis further corroborates the observed reaction pathways, providing deeper insights. This work highlights the potential of molecular catalysts to advance ammonia oxidation and underscores their role in sustainable energy systems.\",\"PeriodicalId\":9909,\"journal\":{\"name\":\"Chemical Science\",\"volume\":\"287 1\",\"pages\":\"\"},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2025-07-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Science\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1039/d5sc00730e\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Science","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d5sc00730e","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

摘要

氨（NH₃）是一种很有前途的无碳能源载体，因为它具有高能量密度和储氢能力。它在能源系统中的利用依赖于氨氧化反应（AOR），这对直接氨燃料电池（DAFCs）和制氢至关重要。在此，我们探索了一种坚固且廉价的基于二茂铁的分子电化学介质，n -吡啶基二茂铁甲酰胺（Fcpy），用于AOR。fcpy介导的AOR表现出94.7%的N2法拉第效率（FE），并伴随H2的生成（FE = 87.3%）。机制研究揭示了h键通过Fcpy的吡啶基部分在促进N-H键激活中的关键作用。计算分析进一步证实了观察到的反应途径，提供了更深入的见解。这项工作突出了分子催化剂推进氨氧化的潜力，并强调了它们在可持续能源系统中的作用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

Electrochemical Ammonia Oxidation with a Homogeneous Molecular Redox Mediator

Ammonia (NH₃) is a promising carbon-free energy carrier due to its high energy density and hydrogen storage capacity. Its utilization in energy systems relies on the ammonia oxidation reaction (AOR), which is critical for direct ammonia fuel cells (DAFCs) and hydrogen production. Herein, we explore a robust and inexpensive Ferrocene-based molecular electrochemical mediator, N-pyridylferrocenecarboxamide (Fcpy), for AOR. The Fcpy-mediated AOR exhibits the N2 Faradaic efficiency (FE) of 94.7 %, along with the concomitant production of H2 (FE = 87.3 %). Mechanistic studies reveal the crucial role of H-bonding through the pyridyl moiety of Fcpy in facilitating N–H bond activation. Computational analysis further corroborates the observed reaction pathways, providing deeper insights. This work highlights the potential of molecular catalysts to advance ammonia oxidation and underscores their role in sustainable energy systems.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Chemical Science CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

4.80%

发文量

1352

审稿时长

2.1 months

期刊介绍： Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.