{"title":"导电性介导的 CuOx 原位电化学重构,用于将硝酸盐还原为氨气","authors":"Hao Liang, Yinqiao Zhang, Xiaona Zhang, Zhao Erzhuo, Wendan Xue, Enguang Nie, Jianqiu Chen, Sijin Zuo, Minghua Zhou","doi":"10.1039/d4nr01625d","DOIUrl":null,"url":null,"abstract":"Electrocatalytic nitrate reduction reaction (NO3RR) is an ideal NH3 synthesis route with ease of operation, high energy efficiency, and low environmental detriment. The electrocatalytic cathodes play a dominant role in NO3RR. Herein, we constructed a carbon fiber paper-supported CuOx nanoarray catalyst (CP/CuOx) by an in situ electrochemical reconstruction method for NO3−-to-NH3 conversion. XRD, in situ Raman, and XPS characterizations unveil the CP/CuOx is a polycrystalline-faceted composite copper nanocatalyst with a valence composition containing Cu0, Cu+ and Cu2+. The CP/CuOx shows more efficient NO3−-to-NH3 conversion than CP/Cu and CP/Cu2O, which indicates the coexistence of various Cu valence states could play a dominant role. The CP/CuOx with suitable Cu2+ content that obtained by adjusting the conductivity during the in situ electrochemical reconstruction process exhibited more than 90% of Faradaic efficiencies for NO3RR in the broad range of -0.3 to -1.0 V vs. RHE, 28.65 mg cm-2 h-1 of peak ammonia yield, and stable NO3RR efficiencies for ten cycles. These findings suggest that the CP/CuOx with suitable copper valence states obtained by fine-tuning the conductivity of the electrochemical reconstruction may provide a competitive cathode catalyst for achieving excellent activity and selectivity of NO3−-to-NH3 conversion.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Conductivity-mediated in situ electrochemical reconstruction of CuOx for nitrate reduction to ammonia\",\"authors\":\"Hao Liang, Yinqiao Zhang, Xiaona Zhang, Zhao Erzhuo, Wendan Xue, Enguang Nie, Jianqiu Chen, Sijin Zuo, Minghua Zhou\",\"doi\":\"10.1039/d4nr01625d\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Electrocatalytic nitrate reduction reaction (NO3RR) is an ideal NH3 synthesis route with ease of operation, high energy efficiency, and low environmental detriment. The electrocatalytic cathodes play a dominant role in NO3RR. Herein, we constructed a carbon fiber paper-supported CuOx nanoarray catalyst (CP/CuOx) by an in situ electrochemical reconstruction method for NO3−-to-NH3 conversion. XRD, in situ Raman, and XPS characterizations unveil the CP/CuOx is a polycrystalline-faceted composite copper nanocatalyst with a valence composition containing Cu0, Cu+ and Cu2+. The CP/CuOx shows more efficient NO3−-to-NH3 conversion than CP/Cu and CP/Cu2O, which indicates the coexistence of various Cu valence states could play a dominant role. The CP/CuOx with suitable Cu2+ content that obtained by adjusting the conductivity during the in situ electrochemical reconstruction process exhibited more than 90% of Faradaic efficiencies for NO3RR in the broad range of -0.3 to -1.0 V vs. RHE, 28.65 mg cm-2 h-1 of peak ammonia yield, and stable NO3RR efficiencies for ten cycles. These findings suggest that the CP/CuOx with suitable copper valence states obtained by fine-tuning the conductivity of the electrochemical reconstruction may provide a competitive cathode catalyst for achieving excellent activity and selectivity of NO3−-to-NH3 conversion.\",\"PeriodicalId\":92,\"journal\":{\"name\":\"Nanoscale\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-06-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nanoscale\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d4nr01625d\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nanoscale","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4nr01625d","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Conductivity-mediated in situ electrochemical reconstruction of CuOx for nitrate reduction to ammonia
Electrocatalytic nitrate reduction reaction (NO3RR) is an ideal NH3 synthesis route with ease of operation, high energy efficiency, and low environmental detriment. The electrocatalytic cathodes play a dominant role in NO3RR. Herein, we constructed a carbon fiber paper-supported CuOx nanoarray catalyst (CP/CuOx) by an in situ electrochemical reconstruction method for NO3−-to-NH3 conversion. XRD, in situ Raman, and XPS characterizations unveil the CP/CuOx is a polycrystalline-faceted composite copper nanocatalyst with a valence composition containing Cu0, Cu+ and Cu2+. The CP/CuOx shows more efficient NO3−-to-NH3 conversion than CP/Cu and CP/Cu2O, which indicates the coexistence of various Cu valence states could play a dominant role. The CP/CuOx with suitable Cu2+ content that obtained by adjusting the conductivity during the in situ electrochemical reconstruction process exhibited more than 90% of Faradaic efficiencies for NO3RR in the broad range of -0.3 to -1.0 V vs. RHE, 28.65 mg cm-2 h-1 of peak ammonia yield, and stable NO3RR efficiencies for ten cycles. These findings suggest that the CP/CuOx with suitable copper valence states obtained by fine-tuning the conductivity of the electrochemical reconstruction may provide a competitive cathode catalyst for achieving excellent activity and selectivity of NO3−-to-NH3 conversion.
期刊介绍:
Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.