低配位Co-Ru双原子通过解锁竞争性吸附限制实现环境氨氧化。

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-10-22 DOI:10.1038/s41467-025-64418-7

Jialin Yang,Zhecheng Fang,Zhiwei Sun,Wenhua Zhou,Bing Nan,Xiaolong Liu,Zixu Ma,Renfeng Nie,Jie Fu

{"title":"低配位Co-Ru双原子通过解锁竞争性吸附限制实现环境氨氧化。","authors":"Jialin Yang,Zhecheng Fang,Zhiwei Sun,Wenhua Zhou,Bing Nan,Xiaolong Liu,Zixu Ma,Renfeng Nie,Jie Fu","doi":"10.1038/s41467-025-64418-7","DOIUrl":null,"url":null,"abstract":"Direct ammoxidation of biomass-derived alcohols/aldehydes to nitriles faces challenges from N-species competitive adsorption, leading to low efficiency under harsh conditions. Herein, we report the rational design of a single-nitrogen-bridged Co-Ru dual-atom catalyst (CoRu-N-C) on nitrogen-doped carbon, enabling efficient ammoxidation at ambient conditions. At 35 °C and 1 bar air, CoRu-N-C achieved 98% yield of 2-furonitrile (FAN) with 73 mmol/g-metal/h productivity, representing a 3.5-fold enhancement compared to Co-N-C, and outperforming numerous reported noble/non-noble metal catalysts. Mechanistic studies reveal synergistic O2 and imine adsorption on low-coordinated CoN3 and RuN3 sites, mitigating imine-induced oxygen activation inhibition. Specifically, the strong O₂ adsorption on CoN3 forms superoxide radicals (O2-•) via electron transfer, driving a relay mechanism with proximally adsorbed imine to accelerate overall reaction kinetics. This work provides valuable insights for the design of stable and highly efficient ammoxidation catalysts operating under mild conditions.","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"58 1","pages":"9351"},"PeriodicalIF":15.7000,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Low-coordinated Co-Ru dual-atom enables ambient ammoxidation via unlocking competitive adsorption limitations.\",\"authors\":\"Jialin Yang,Zhecheng Fang,Zhiwei Sun,Wenhua Zhou,Bing Nan,Xiaolong Liu,Zixu Ma,Renfeng Nie,Jie Fu\",\"doi\":\"10.1038/s41467-025-64418-7\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Direct ammoxidation of biomass-derived alcohols/aldehydes to nitriles faces challenges from N-species competitive adsorption, leading to low efficiency under harsh conditions. Herein, we report the rational design of a single-nitrogen-bridged Co-Ru dual-atom catalyst (CoRu-N-C) on nitrogen-doped carbon, enabling efficient ammoxidation at ambient conditions. At 35 °C and 1 bar air, CoRu-N-C achieved 98% yield of 2-furonitrile (FAN) with 73 mmol/g-metal/h productivity, representing a 3.5-fold enhancement compared to Co-N-C, and outperforming numerous reported noble/non-noble metal catalysts. Mechanistic studies reveal synergistic O2 and imine adsorption on low-coordinated CoN3 and RuN3 sites, mitigating imine-induced oxygen activation inhibition. Specifically, the strong O₂ adsorption on CoN3 forms superoxide radicals (O2-•) via electron transfer, driving a relay mechanism with proximally adsorbed imine to accelerate overall reaction kinetics. This work provides valuable insights for the design of stable and highly efficient ammoxidation catalysts operating under mild conditions.\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":\"58 1\",\"pages\":\"9351\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2025-10-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-025-64418-7\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-64418-7","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}

引用次数: 0

摘要

生物质醇/醛直接氨氧化制腈面临n -物种竞争吸附的挑战，导致在恶劣条件下效率低。在此，我们报告了在氮掺杂碳上合理设计单氮桥接Co-Ru双原子催化剂（CoRu-N-C），实现了在环境条件下的高效氨氧化。在35°C和1 bar空气条件下，CoRu-N-C的2-呋喃（FAN）收率为98%，产率为73 mmol/g-metal/h，比Co-N-C提高了3.5倍，并且优于许多已报道的贵金属/非贵金属催化剂。机制研究表明，低配位的CoN3和RuN3位点协同O2和亚胺吸附，减轻亚胺诱导的氧活化抑制。具体来说，CoN3对O₂的强吸附通过电子转移形成超氧自由基（O2-•），驱动与近端吸附亚胺的接力机制，加速整体反应动力学。这项工作为设计在温和条件下运行的稳定高效的氨氧化催化剂提供了有价值的见解。

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

Low-coordinated Co-Ru dual-atom enables ambient ammoxidation via unlocking competitive adsorption limitations.

Direct ammoxidation of biomass-derived alcohols/aldehydes to nitriles faces challenges from N-species competitive adsorption, leading to low efficiency under harsh conditions. Herein, we report the rational design of a single-nitrogen-bridged Co-Ru dual-atom catalyst (CoRu-N-C) on nitrogen-doped carbon, enabling efficient ammoxidation at ambient conditions. At 35 °C and 1 bar air, CoRu-N-C achieved 98% yield of 2-furonitrile (FAN) with 73 mmol/g-metal/h productivity, representing a 3.5-fold enhancement compared to Co-N-C, and outperforming numerous reported noble/non-noble metal catalysts. Mechanistic studies reveal synergistic O2 and imine adsorption on low-coordinated CoN3 and RuN3 sites, mitigating imine-induced oxygen activation inhibition. Specifically, the strong O₂ adsorption on CoN3 forms superoxide radicals (O2-•) via electron transfer, driving a relay mechanism with proximally adsorbed imine to accelerate overall reaction kinetics. This work provides valuable insights for the design of stable and highly efficient ammoxidation catalysts operating under mild conditions.

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

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.