Weihui OU, Ying Guo, Jing Zhong, Fucong Lyu, Junda J. Shen, Hongkun Li, Shaoce Zhang, zebiao Li, Zhijian He, Jun He, Quanxi Mo, Chunyi Zhi, Yang Yang Li, Jian Lu
{"title":"在质子天线反应器催化剂上实现硝酸盐到氨的转化","authors":"Weihui OU, Ying Guo, Jing Zhong, Fucong Lyu, Junda J. Shen, Hongkun Li, Shaoce Zhang, zebiao Li, Zhijian He, Jun He, Quanxi Mo, Chunyi Zhi, Yang Yang Li, Jian Lu","doi":"10.1039/d4ee03678f","DOIUrl":null,"url":null,"abstract":"Electrochemical conversion of nitrate to ammonia is an appealing route to efficiently synthesizing ammonia at ambient conditions while reducing environmental nitrate pollutants. However, this approach is obstructed by the limited yield and selectivity of ammonia because the electrochemical nitrate-to-ammonia conversion involves multi-electron/proton transfer and faces competition from hydrogen evolution reaction. Here, we demonstrate a plasmon-assisted strategy to improve the performance of nitrate-to-ammonia electrochemical conversion by constructing plasmonic antenna-reactor catalysts, where Au and Pd nanoparticles/hydrogen substituted graphdiyne (Pd/HsGDY) work as light antenna and reaction site, respectively. Plasmonic excitation of Au-Pd/HsGDY catalysts can remarkably accelerate the nitrate reduction, with the yield rate, selectivity, and FE of ammonia respectively increased by 14.3, 2.1, and 1.8 times under optimal conditions. Mechanistic investigations unveil that Au plasmon-induced hot electrons facilitate nitrate-to-ammonia reaction by regulating the adsorption of reaction intermediates on Pd/HsGDY, wherein the rate-determining step was shifted from nitrate adsorption to *NH protonation and the overall apparent activation was reduced. Moreover, hot electrons suppress the competing hydrogen evolution by enlarging Gibbs free energy of hydrogen formation. These results open the avenue to develop a desirable catalyst for producing value-added ammonia from environmentally hazardous nitrate by a synergistic combination of electricity and light","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"193 1","pages":""},"PeriodicalIF":32.4000,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Nitrate-to-Ammonia Conversion at Plasmonic Antenna-Reactor Catalyst\",\"authors\":\"Weihui OU, Ying Guo, Jing Zhong, Fucong Lyu, Junda J. Shen, Hongkun Li, Shaoce Zhang, zebiao Li, Zhijian He, Jun He, Quanxi Mo, Chunyi Zhi, Yang Yang Li, Jian Lu\",\"doi\":\"10.1039/d4ee03678f\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Electrochemical conversion of nitrate to ammonia is an appealing route to efficiently synthesizing ammonia at ambient conditions while reducing environmental nitrate pollutants. However, this approach is obstructed by the limited yield and selectivity of ammonia because the electrochemical nitrate-to-ammonia conversion involves multi-electron/proton transfer and faces competition from hydrogen evolution reaction. Here, we demonstrate a plasmon-assisted strategy to improve the performance of nitrate-to-ammonia electrochemical conversion by constructing plasmonic antenna-reactor catalysts, where Au and Pd nanoparticles/hydrogen substituted graphdiyne (Pd/HsGDY) work as light antenna and reaction site, respectively. Plasmonic excitation of Au-Pd/HsGDY catalysts can remarkably accelerate the nitrate reduction, with the yield rate, selectivity, and FE of ammonia respectively increased by 14.3, 2.1, and 1.8 times under optimal conditions. Mechanistic investigations unveil that Au plasmon-induced hot electrons facilitate nitrate-to-ammonia reaction by regulating the adsorption of reaction intermediates on Pd/HsGDY, wherein the rate-determining step was shifted from nitrate adsorption to *NH protonation and the overall apparent activation was reduced. Moreover, hot electrons suppress the competing hydrogen evolution by enlarging Gibbs free energy of hydrogen formation. 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Nitrate-to-Ammonia Conversion at Plasmonic Antenna-Reactor Catalyst
Electrochemical conversion of nitrate to ammonia is an appealing route to efficiently synthesizing ammonia at ambient conditions while reducing environmental nitrate pollutants. However, this approach is obstructed by the limited yield and selectivity of ammonia because the electrochemical nitrate-to-ammonia conversion involves multi-electron/proton transfer and faces competition from hydrogen evolution reaction. Here, we demonstrate a plasmon-assisted strategy to improve the performance of nitrate-to-ammonia electrochemical conversion by constructing plasmonic antenna-reactor catalysts, where Au and Pd nanoparticles/hydrogen substituted graphdiyne (Pd/HsGDY) work as light antenna and reaction site, respectively. Plasmonic excitation of Au-Pd/HsGDY catalysts can remarkably accelerate the nitrate reduction, with the yield rate, selectivity, and FE of ammonia respectively increased by 14.3, 2.1, and 1.8 times under optimal conditions. Mechanistic investigations unveil that Au plasmon-induced hot electrons facilitate nitrate-to-ammonia reaction by regulating the adsorption of reaction intermediates on Pd/HsGDY, wherein the rate-determining step was shifted from nitrate adsorption to *NH protonation and the overall apparent activation was reduced. Moreover, hot electrons suppress the competing hydrogen evolution by enlarging Gibbs free energy of hydrogen formation. These results open the avenue to develop a desirable catalyst for producing value-added ammonia from environmentally hazardous nitrate by a synergistic combination of electricity and light
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).