{"title":"通过定向蚀刻模板策略调节原子分散的 Ru 微环境以实现高效固氮","authors":"Zhiya Han*, Jiaxi Yuan, Gaijuan Guo, Yue Kang, Yixin Liu, Chunxia Zhou, Liping Tong, Binfeng Lu, Xiyang Liu, Quan Wang, Miaosen Yang, Senhe Huang, Boxu Feng* and Sheng Han*, ","doi":"10.1021/acsanm.4c02608","DOIUrl":null,"url":null,"abstract":"<p >The synthesis of ammonia (NH<sub>3</sub>) via the Haber–Bosch process is energy-intensive and environmentally challenging, necessitating the development of sustainable alternatives. Herein, we report a directed etch template strategy to create atomically dispersed Ru–N<sub>4</sub> active sites within layered porous carbon (NC@Ru) for efficient electrochemical nitrogen reduction reaction (NRR). The removal of the MgO template results in an interconnected carbon network with hierarchical porous structures, significantly enhancing the accessibility and mass transfer of the active sites. The NC@Ru catalyst demonstrated superior NRR performance, achieving an ammonia yield rate of 196.2 μg h<sup>–1</sup> mg<sub>cat.</sub><sup>–1</sup> and a Faradaic efficiency of 43.8%. In situ electrochemical mass spectrometry was employed to analyze NRR kinetics, while density functional theory calculations were utilized to elucidate the NRR mechanism and identify the rate-determining step. The work introduces a novel high-performance catalyst for electrocatalytic NRR and provides a practical strategy for optimizing active-site microenvironments, laying the groundwork for future commercial applications of electrocatalytic NRR.</p>","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.3000,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Modulation of Atomically Dispersed Ru Microenvironments by a Directed Etch Template Strategy for Efficient Nitrogen Fixation\",\"authors\":\"Zhiya Han*, Jiaxi Yuan, Gaijuan Guo, Yue Kang, Yixin Liu, Chunxia Zhou, Liping Tong, Binfeng Lu, Xiyang Liu, Quan Wang, Miaosen Yang, Senhe Huang, Boxu Feng* and Sheng Han*, \",\"doi\":\"10.1021/acsanm.4c02608\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The synthesis of ammonia (NH<sub>3</sub>) via the Haber–Bosch process is energy-intensive and environmentally challenging, necessitating the development of sustainable alternatives. Herein, we report a directed etch template strategy to create atomically dispersed Ru–N<sub>4</sub> active sites within layered porous carbon (NC@Ru) for efficient electrochemical nitrogen reduction reaction (NRR). The removal of the MgO template results in an interconnected carbon network with hierarchical porous structures, significantly enhancing the accessibility and mass transfer of the active sites. The NC@Ru catalyst demonstrated superior NRR performance, achieving an ammonia yield rate of 196.2 μg h<sup>–1</sup> mg<sub>cat.</sub><sup>–1</sup> and a Faradaic efficiency of 43.8%. In situ electrochemical mass spectrometry was employed to analyze NRR kinetics, while density functional theory calculations were utilized to elucidate the NRR mechanism and identify the rate-determining step. The work introduces a novel high-performance catalyst for electrocatalytic NRR and provides a practical strategy for optimizing active-site microenvironments, laying the groundwork for future commercial applications of electrocatalytic NRR.</p>\",\"PeriodicalId\":6,\"journal\":{\"name\":\"ACS Applied Nano Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-06-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Nano Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsanm.4c02608\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Nano Materials","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsanm.4c02608","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Modulation of Atomically Dispersed Ru Microenvironments by a Directed Etch Template Strategy for Efficient Nitrogen Fixation
The synthesis of ammonia (NH3) via the Haber–Bosch process is energy-intensive and environmentally challenging, necessitating the development of sustainable alternatives. Herein, we report a directed etch template strategy to create atomically dispersed Ru–N4 active sites within layered porous carbon (NC@Ru) for efficient electrochemical nitrogen reduction reaction (NRR). The removal of the MgO template results in an interconnected carbon network with hierarchical porous structures, significantly enhancing the accessibility and mass transfer of the active sites. The NC@Ru catalyst demonstrated superior NRR performance, achieving an ammonia yield rate of 196.2 μg h–1 mgcat.–1 and a Faradaic efficiency of 43.8%. In situ electrochemical mass spectrometry was employed to analyze NRR kinetics, while density functional theory calculations were utilized to elucidate the NRR mechanism and identify the rate-determining step. The work introduces a novel high-performance catalyst for electrocatalytic NRR and provides a practical strategy for optimizing active-site microenvironments, laying the groundwork for future commercial applications of electrocatalytic NRR.
期刊介绍:
ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.