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Hydrophobic Microenvironment Modulation of Ru Nanoparticles in Metal-Organic Frameworks for Enhanced Electrocatalytic N2 Reduction

文献类型：期刊论文

作者Wen, Lulu3; Liu, Xiaoshuo2; Li, Xinyang3; Zhang, Hanlin1,3; Zhong, Shichuan3; Zeng, Pan1,3; Shah, Syed Shoaib Ahmad5; Hu, Xiaoye3; Cai, Weiping3; Li, Yue3,4
刊名ADVANCED SCIENCE
出版日期2024-07-10
关键词d-band center electrocatalytic N-2 reduction hydrophobic microenvironment metal-organic frameworks Ru nanoparticles
DOI10.1002/advs.202405210
通讯作者Li, Yue(yueli@issp.ac.cn)
英文摘要The modulation of the chemical microenvironment surrounding metal nanoparticles (NPs) is an effective means to enhance the selectivity and activity of catalytic reactions. Herein, a post-synthetic modification strategy is developed to modulate the hydrophobic microenvironment of Ru nanoparticles encapsulated in a metal-organic framework (MOF), MIP-206, namely Ru@MIP-F-x (where x represents perfluoroalkyl chain lengths of 3, 5, 7, 11, and 15), in order to systematically explore the effect of the hydrophobic microenvironment on the electrocatalytic activity. The increase of perfluoroalkyl chain length can gradually enhance the hydrophobicity of the catalyst, which effectively suppresses the competitive hydrogen evolution reaction (HER). Moreover, the electrocatalytic production rate of ammonia and the corresponding Faraday efficiency display a volcano-like pattern with increasing hydrophobicity, with Ru@MIP-F-7 showing the highest activity. Theoretical calculations and experiments jointly show that modification of perfluoroalkyl chains of different lengths on MIP-206 modulates the electronic state of Ru nanoparticles and reduces the rate-determining step for the formation of the key intermediate of N2H2*, leading to superior electrocatalytic performance.
WOS关键词NITROGEN REDUCTION ; CATALYSTS ; FIXATION ; AMMONIA ; CATIONS ; MOFS
资助项目National Science Fund for Distinguished Young Scholars ; Natural Science Foundation of China[92263209] ; Natural Science Foundation of China[52201232] ; Scientific Instrument Developing Project of the Chinese Academy of Sciences[YJKYYQ20210009] ; China Postdoctoral Science Foundation[2023M733536] ; China Postdoctoral Science Foundation[2020M682891]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
语种英语
WOS记录号WOS:001268889500001
出版者WILEY
资助机构National Science Fund for Distinguished Young Scholars ; Natural Science Foundation of China ; Scientific Instrument Developing Project of the Chinese Academy of Sciences ; China Postdoctoral Science Foundation
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/137140]  
专题中国科学院合肥物质科学研究院
通讯作者Li, Yue
作者单位1.Univ Sci & Technol China, Hefei 230026, Peoples R China
2.Southeast Univ, Sch Energy & Environm, Key Lab Energy Thermal Convers & Control, Minist Educ, Nanjing 210096, Peoples R China
3.Chinese Acad Sci, Hefei Inst Phys Sci, Anhui Key Lab Nanomat & Nanotechnol, Key Lab Mat Phys,Inst Solid State Phys, Hefei 230031, Anhui, Peoples R China
4.Tiangong Univ, Sch Phys Sci & Technol, Tianjin 300387, Peoples R China
5.Natl Univ Sci & Technol, Sch Nat Sci, Dept Chem, Islamabad 44000, Pakistan
推荐引用方式
GB/T 7714		 Wen, Lulu,Liu, Xiaoshuo,Li, Xinyang,et al. Hydrophobic Microenvironment Modulation of Ru Nanoparticles in Metal-Organic Frameworks for Enhanced Electrocatalytic N2 Reduction[J]. ADVANCED SCIENCE,2024.
APA Wen, Lulu.,Liu, Xiaoshuo.,Li, Xinyang.,Zhang, Hanlin.,Zhong, Shichuan.,...&Li, Yue.(2024).Hydrophobic Microenvironment Modulation of Ru Nanoparticles in Metal-Organic Frameworks for Enhanced Electrocatalytic N2 Reduction.ADVANCED SCIENCE.
MLA Wen, Lulu,et al."Hydrophobic Microenvironment Modulation of Ru Nanoparticles in Metal-Organic Frameworks for Enhanced Electrocatalytic N2 Reduction".ADVANCED SCIENCE (2024).

入库方式： OAI收割

来源：合肥物质科学研究院

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