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Ambient Electrochemical Nitrogen Fixation over a Bifunctional Mo- (O-C-2)(4) Site Catalyst | |
Zhang, Shengbo1,2; Shi, Tongfei1; Li, Ke1; Sun, Qiao5; Lin, Yue3; Zheng, Li Rong4; Wang, Guozhong1; Zhang, Yunxia1; Yin, Huajie1; Zhang, Haimin1,2 | |
2022-01-10 | |
发表期刊 | JOURNAL OF PHYSICAL CHEMISTRY C |
ISSN | 1932-7447 |
通讯作者 | Li, Ke(kelee@mail.ustc.edu.cn) ; Sun, Qiao(sunqiao@suda.edu.cn) ; Zhang, Haimin(zhanghm@issp.ac.cn) |
摘要 | The electrochemical synthesis of NH3 and NO3- by the N-2 reduction reaction (NRR) and the N-2 oxidation reaction (NOR) under ambient conditions utilizing H2O as the hydrogen and oxygen source has aroused great attention. Here, we report the fabrication of oxygen-coordinated molybdenum (Mo) single atoms anchored on carbon (Mo-O-C) using bacterial cellulose (BC) as the impregnation regulator and carbon source. As a result, the as-synthesized Mo-O-C as an electrocatalyst exhibits superior bifunctional NRR and NOR activities with high stability. A superb NH3 yield rate of 248.6 +/- 12.9 mu g h(-1) mg(cat)(-1) and a faradaic efficiency (FE) of 43.8 +/- 2.3% can be obtained at -0.20 V (vs RHE) by the Mo-O-C-catalyzed NRR, and Mo-O-C can also afford a NO3- yield rate of 217.1 +/- 13.5 mu g h(-4) mg(cat)(-1) with a FE of 7.8 +/- 0.5% at 2.35 V (vs ) for the NOR The synchrotron-based X-ray absorption spectra and theoretical calculation results unveil that the O-coordinated molybdenum configuration of Mo-(O-C-2)(4) anchored on carbon is the most stable single-atom structure as the catalytic active sites for N-2 adsorption, activation, and bifunctional hydrogenation/oxidation reactions. |
DOI | 10.1021/acs.jpcc.1c10039 |
关键词[WOS] | SINGLE-ATOM CATALYSTS ; AMMONIA-SYNTHESIS ; CONVERSION ; EFFICIENT ; DIOXIDE |
收录类别 | SCI |
语种 | 英语 |
资助项目 | Natural Science Foundation of China[51872292] ; Natural Science Foundation of Anhui Province[2108085QB60] ; Natural Science Foundation of Anhui Province[2108085QB61] ; CASHIPS Director's Fund[YZJJ2021QN21] ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China |
项目资助者 | Natural Science Foundation of China ; Natural Science Foundation of Anhui Province ; CASHIPS Director's Fund ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China |
WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science |
WOS类目 | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
WOS记录号 | WOS:000743225400001 |
出版者 | AMER CHEMICAL SOC |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.hfcas.ac.cn:8080/handle/334002/127104 |
专题 | 中国科学院合肥物质科学研究院 |
通讯作者 | Li, Ke; Sun, Qiao; Zhang, Haimin |
作者单位 | 1.Chinese Acad Sci, Ctr Environm & Energy Nanomat, CAS Ctr Excellence Nanosci,Key Lab Mat Phys, Inst Solid State Phys,Anhui Key Lab Nanomat & Nan, Hefei 230031, Peoples R China 2.Univ Sci & Technol China, Hefei 230026, Peoples R China 3.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China 4.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China 5.Soochow Univ, Collaborat Innovat Ctr Radiat Med, Sch Radiol & Interdisciplinary Sci, State Key Lab Radiat Med & Protect,Jiangsu Higher, Suzhou 215123, Peoples R China |
推荐引用方式 GB/T 7714 | Zhang, Shengbo,Shi, Tongfei,Li, Ke,et al. Ambient Electrochemical Nitrogen Fixation over a Bifunctional Mo- (O-C-2)(4) Site Catalyst[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2022. |
APA | Zhang, Shengbo.,Shi, Tongfei.,Li, Ke.,Sun, Qiao.,Lin, Yue.,...&Zhang, Haimin.(2022).Ambient Electrochemical Nitrogen Fixation over a Bifunctional Mo- (O-C-2)(4) Site Catalyst.JOURNAL OF PHYSICAL CHEMISTRY C. |
MLA | Zhang, Shengbo,et al."Ambient Electrochemical Nitrogen Fixation over a Bifunctional Mo- (O-C-2)(4) Site Catalyst".JOURNAL OF PHYSICAL CHEMISTRY C (2022). |
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