Zheng Lv, Shuanglong Zhou, Liang Zhao, Ziyi Liu, Jiaxin Liu, Wenxia Xu, Lei Wang, Jianping Lai
{"title":"尿素电合成中多相反应物的共活化","authors":"Zheng Lv, Shuanglong Zhou, Liang Zhao, Ziyi Liu, Jiaxin Liu, Wenxia Xu, Lei Wang, Jianping Lai","doi":"10.1002/aenm.202300946","DOIUrl":null,"url":null,"abstract":"<p>N<sub>2</sub> and CO<sub>2</sub> fixation is an environmentally friendly waste-to-energy technology that can replace tedious and demanding industrial urea productive processes. Here, V<sub>N</sub>-Cu<sub>3</sub>N-300 catalysts with tip and vacancy structures are designed for the coactivation of multiphase reactants in the urea electrosynthesis process. Under environmental conditions, the urea yield is 81 µg h<sup>−1</sup> cm<sup>−2</sup>, this is the first report of high area active electrocatalyst, and the corresponding Faraday efficiency is able to reach 28.7%. The full-cell electrolysis exhibits good stability, providing a current density of 0.7 mA cm<sup>−2</sup> at 2.1 V. The electrolyte after continuous electrolysis for 48 h is subjected to being evaporated and recrystallized, and it is determined by <sup>1</sup>H NMR that the purity of urea can reach 100%. Comprehensive analysis shows that the local electric field formed by the tip effect can effectively promote the adsorption and activation of CO<sub>2</sub>. The presence of surface nitrogen vacancies promotes the formation of *NN* intermediates, ensuring C<span></span>N coupling, and also optimizing the dissociation process of water, providing a proton supply for the synthesis of urea. Thus, the rate-determining step is altered and the formation of urea is ensured.</p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4000,"publicationDate":"2023-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"1","resultStr":"{\"title\":\"Coactivation of Multiphase Reactants for the Electrosynthesis of Urea\",\"authors\":\"Zheng Lv, Shuanglong Zhou, Liang Zhao, Ziyi Liu, Jiaxin Liu, Wenxia Xu, Lei Wang, Jianping Lai\",\"doi\":\"10.1002/aenm.202300946\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>N<sub>2</sub> and CO<sub>2</sub> fixation is an environmentally friendly waste-to-energy technology that can replace tedious and demanding industrial urea productive processes. Here, V<sub>N</sub>-Cu<sub>3</sub>N-300 catalysts with tip and vacancy structures are designed for the coactivation of multiphase reactants in the urea electrosynthesis process. Under environmental conditions, the urea yield is 81 µg h<sup>−1</sup> cm<sup>−2</sup>, this is the first report of high area active electrocatalyst, and the corresponding Faraday efficiency is able to reach 28.7%. The full-cell electrolysis exhibits good stability, providing a current density of 0.7 mA cm<sup>−2</sup> at 2.1 V. The electrolyte after continuous electrolysis for 48 h is subjected to being evaporated and recrystallized, and it is determined by <sup>1</sup>H NMR that the purity of urea can reach 100%. Comprehensive analysis shows that the local electric field formed by the tip effect can effectively promote the adsorption and activation of CO<sub>2</sub>. The presence of surface nitrogen vacancies promotes the formation of *NN* intermediates, ensuring C<span></span>N coupling, and also optimizing the dissociation process of water, providing a proton supply for the synthesis of urea. Thus, the rate-determining step is altered and the formation of urea is ensured.</p>\",\"PeriodicalId\":111,\"journal\":{\"name\":\"Advanced Energy Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":24.4000,\"publicationDate\":\"2023-05-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"1\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/aenm.202300946\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/aenm.202300946","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Coactivation of Multiphase Reactants for the Electrosynthesis of Urea
N2 and CO2 fixation is an environmentally friendly waste-to-energy technology that can replace tedious and demanding industrial urea productive processes. Here, VN-Cu3N-300 catalysts with tip and vacancy structures are designed for the coactivation of multiphase reactants in the urea electrosynthesis process. Under environmental conditions, the urea yield is 81 µg h−1 cm−2, this is the first report of high area active electrocatalyst, and the corresponding Faraday efficiency is able to reach 28.7%. The full-cell electrolysis exhibits good stability, providing a current density of 0.7 mA cm−2 at 2.1 V. The electrolyte after continuous electrolysis for 48 h is subjected to being evaporated and recrystallized, and it is determined by 1H NMR that the purity of urea can reach 100%. Comprehensive analysis shows that the local electric field formed by the tip effect can effectively promote the adsorption and activation of CO2. The presence of surface nitrogen vacancies promotes the formation of *NN* intermediates, ensuring CN coupling, and also optimizing the dissociation process of water, providing a proton supply for the synthesis of urea. Thus, the rate-determining step is altered and the formation of urea is ensured.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.