Donghai Wu, Kai Chen, Peng Lv, Ziyu Ma, Ke Chu* and Dongwei Ma*,
{"title":"通过铁双原子催化剂将八电子 N2O 直接电还原为 NH3。","authors":"Donghai Wu, Kai Chen, Peng Lv, Ziyu Ma, Ke Chu* and Dongwei Ma*, ","doi":"10.1021/acs.nanolett.4c00576","DOIUrl":null,"url":null,"abstract":"<p >N<sub>2</sub>O is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of N<sub>2</sub>O has gained increasing attention to remove N<sub>2</sub>O, but its product is worthless N<sub>2</sub>. Here, we propose a direct eight-electron (8<i>e</i>) pathway to electrochemically convert N<sub>2</sub>O into NH<sub>3</sub>. As a proof of concept, using density functional theory calculation, an Fe<sub>2</sub> double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe<sub>2</sub>@NG) was screened out to be the most active and selective catalyst for N<sub>2</sub>O electroreduction toward NH<sub>3</sub> via the novel 8<i>e</i> pathway, which benefits from the unique bent N<sub>2</sub>O adsorption configuration. Guided by theoretical prediction, Fe<sub>2</sub>@NG DAC was fabricated experimentally, and it can achieve a high N<sub>2</sub>O-to-NH<sub>3</sub> Faradaic efficiency of 77.8% with a large NH<sub>3</sub> yield rate of 2.9 mg h<sup>–1</sup> cm<sup>–2</sup> at −0.6 V vs RHE in a neutral electrolyte. Our study offers a feasible strategy to synthesize NH<sub>3</sub> from pollutant N<sub>2</sub>O with simultaneous N<sub>2</sub>O removal.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Direct Eight-Electron N2O Electroreduction to NH3 Enabled by an Fe Double-Atom Catalyst\",\"authors\":\"Donghai Wu, Kai Chen, Peng Lv, Ziyu Ma, Ke Chu* and Dongwei Ma*, \",\"doi\":\"10.1021/acs.nanolett.4c00576\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >N<sub>2</sub>O is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of N<sub>2</sub>O has gained increasing attention to remove N<sub>2</sub>O, but its product is worthless N<sub>2</sub>. Here, we propose a direct eight-electron (8<i>e</i>) pathway to electrochemically convert N<sub>2</sub>O into NH<sub>3</sub>. As a proof of concept, using density functional theory calculation, an Fe<sub>2</sub> double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe<sub>2</sub>@NG) was screened out to be the most active and selective catalyst for N<sub>2</sub>O electroreduction toward NH<sub>3</sub> via the novel 8<i>e</i> pathway, which benefits from the unique bent N<sub>2</sub>O adsorption configuration. Guided by theoretical prediction, Fe<sub>2</sub>@NG DAC was fabricated experimentally, and it can achieve a high N<sub>2</sub>O-to-NH<sub>3</sub> Faradaic efficiency of 77.8% with a large NH<sub>3</sub> yield rate of 2.9 mg h<sup>–1</sup> cm<sup>–2</sup> at −0.6 V vs RHE in a neutral electrolyte. Our study offers a feasible strategy to synthesize NH<sub>3</sub> from pollutant N<sub>2</sub>O with simultaneous N<sub>2</sub>O removal.</p>\",\"PeriodicalId\":53,\"journal\":{\"name\":\"Nano Letters\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.6000,\"publicationDate\":\"2024-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nano Letters\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.nanolett.4c00576\",\"RegionNum\":1,\"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":"Nano Letters","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.nanolett.4c00576","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Direct Eight-Electron N2O Electroreduction to NH3 Enabled by an Fe Double-Atom Catalyst
N2O is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of N2O has gained increasing attention to remove N2O, but its product is worthless N2. Here, we propose a direct eight-electron (8e) pathway to electrochemically convert N2O into NH3. As a proof of concept, using density functional theory calculation, an Fe2 double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe2@NG) was screened out to be the most active and selective catalyst for N2O electroreduction toward NH3 via the novel 8e pathway, which benefits from the unique bent N2O adsorption configuration. Guided by theoretical prediction, Fe2@NG DAC was fabricated experimentally, and it can achieve a high N2O-to-NH3 Faradaic efficiency of 77.8% with a large NH3 yield rate of 2.9 mg h–1 cm–2 at −0.6 V vs RHE in a neutral electrolyte. Our study offers a feasible strategy to synthesize NH3 from pollutant N2O with simultaneous N2O removal.
期刊介绍:
Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including:
- Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale
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