Yini Mao, Qiao Gou, Yimin Jiang, Wei Shen, Ming Li, Rongxing He
{"title":"界面工程可增强路易斯酸度并激活惰性位点,从而共同促进硝酸盐还原成氨","authors":"Yini Mao, Qiao Gou, Yimin Jiang, Wei Shen, Ming Li, Rongxing He","doi":"10.1016/j.jhazmat.2024.136083","DOIUrl":null,"url":null,"abstract":"Electrocatalytic nitrate reduction to ammonia (NRA) has been considered a highly promising method for \"waste to treasure\". Herein, a heterogeneous catalyst FeP/Cu<sub>3</sub>P/CF enriched with Lewis acid sites was designed for efficient NRA. The faradaic efficiency and NH<sub>3</sub> yield are up to 95.61% and 0.2573<!-- --> <!-- -->mmol<!-- --> <!-- -->h<sup>−1</sup> cm<sup>−2</sup>, the NH<sub>3</sub>−N selectivity is 95.11%, and the NO<sub>3</sub><sup>–</sup>−N conversion is close to 100%. Experimental and theoretical studies verify that the formation of the interface activates the originally inert Fe site and makes it become the second active center in addition to Cu. The charge transfer greatly raises the positive charge density of Fe<sup>δ+</sup> and Cu<sup>δ+</sup> sites, leading to a significant increase in their Lewis acidity, which enables them to interact strongly with the Lewis base NO<sub>3</sub><sup>−</sup> and improves the NRA performance; meanwhile, the ability of P site with increased negative charge density to capture H enhances, which is beneficial for the subsequent hydrogenation of nitrate reduction. This work provides an approach for designing efficient NRA catalysts through interface engineering strategy.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":12.2000,"publicationDate":"2024-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Interface engineering enhances Lewis acidity and activates inert sites to jointly promote nitrate reduction to ammonia\",\"authors\":\"Yini Mao, Qiao Gou, Yimin Jiang, Wei Shen, Ming Li, Rongxing He\",\"doi\":\"10.1016/j.jhazmat.2024.136083\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Electrocatalytic nitrate reduction to ammonia (NRA) has been considered a highly promising method for \\\"waste to treasure\\\". Herein, a heterogeneous catalyst FeP/Cu<sub>3</sub>P/CF enriched with Lewis acid sites was designed for efficient NRA. The faradaic efficiency and NH<sub>3</sub> yield are up to 95.61% and 0.2573<!-- --> <!-- -->mmol<!-- --> <!-- -->h<sup>−1</sup> cm<sup>−2</sup>, the NH<sub>3</sub>−N selectivity is 95.11%, and the NO<sub>3</sub><sup>–</sup>−N conversion is close to 100%. Experimental and theoretical studies verify that the formation of the interface activates the originally inert Fe site and makes it become the second active center in addition to Cu. The charge transfer greatly raises the positive charge density of Fe<sup>δ+</sup> and Cu<sup>δ+</sup> sites, leading to a significant increase in their Lewis acidity, which enables them to interact strongly with the Lewis base NO<sub>3</sub><sup>−</sup> and improves the NRA performance; meanwhile, the ability of P site with increased negative charge density to capture H enhances, which is beneficial for the subsequent hydrogenation of nitrate reduction. This work provides an approach for designing efficient NRA catalysts through interface engineering strategy.\",\"PeriodicalId\":361,\"journal\":{\"name\":\"Journal of Hazardous Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":12.2000,\"publicationDate\":\"2024-10-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Hazardous Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jhazmat.2024.136083\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Hazardous Materials","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1016/j.jhazmat.2024.136083","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Interface engineering enhances Lewis acidity and activates inert sites to jointly promote nitrate reduction to ammonia
Electrocatalytic nitrate reduction to ammonia (NRA) has been considered a highly promising method for "waste to treasure". Herein, a heterogeneous catalyst FeP/Cu3P/CF enriched with Lewis acid sites was designed for efficient NRA. The faradaic efficiency and NH3 yield are up to 95.61% and 0.2573 mmol h−1 cm−2, the NH3−N selectivity is 95.11%, and the NO3–−N conversion is close to 100%. Experimental and theoretical studies verify that the formation of the interface activates the originally inert Fe site and makes it become the second active center in addition to Cu. The charge transfer greatly raises the positive charge density of Feδ+ and Cuδ+ sites, leading to a significant increase in their Lewis acidity, which enables them to interact strongly with the Lewis base NO3− and improves the NRA performance; meanwhile, the ability of P site with increased negative charge density to capture H enhances, which is beneficial for the subsequent hydrogenation of nitrate reduction. This work provides an approach for designing efficient NRA catalysts through interface engineering strategy.
期刊介绍:
The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.