Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang, Quan Li, Jia-Ping Tong, Wen-Tai Wang, Yu-Hua Fan, Feng Shao
{"title":"由双核-铜基团构建的二维 MOF,用于高性能电催化 NO 还原成 NH3。","authors":"Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang, Quan Li, Jia-Ping Tong, Wen-Tai Wang, Yu-Hua Fan, Feng Shao","doi":"10.1021/jacsau.4c00475","DOIUrl":null,"url":null,"abstract":"<p><p>Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH<sub>3</sub> synthesis. However, their complex kinetics and energy demands necessitate high-performance electrocatalysts to ensure effective and selective process outcomes. Herein, we report that a two-dimensional Cu-based metal-organic framework (MOF), {[Cu(HL)]·H<sub>2</sub>O} <sub><i>n</i></sub> , (<b>Cu-OUC</b>, H<sub>3</sub>L = 5-(2'-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH<sub>3</sub> conversion. Electrochemical experimental studies showed that in 0.1 M K<sub>2</sub>SO<sub>4</sub> solution, the as-prepared <b>Cu-OUC</b> achieved a peak Faradaic efficiency of 96.91% and a notable NH<sub>3</sub> yield as high as 3415.82 μg h<sup>-1</sup> mg<sup>-1</sup>. The Zn-NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm<sup>-2</sup> while simultaneously achieving an NH<sub>3</sub> yield of 616.92 μg h<sup>-1</sup> mg<sup>-1</sup>. Theoretical calculations revealed that the surface of <b>Cu-OUC</b> effectively facilitates NO activation through a two-way charge transfer mechanism of \"electron acceptance and donation\", with the *NO formation step being the potential-determining stage. The study pioneers the use of a MOF as an electrocatalyst for ambient NO-to-NH<sub>3</sub> conversion.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":null,"pages":null},"PeriodicalIF":8.5000,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11522898/pdf/","citationCount":"0","resultStr":"{\"title\":\"Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH<sub>3</sub>.\",\"authors\":\"Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang, Quan Li, Jia-Ping Tong, Wen-Tai Wang, Yu-Hua Fan, Feng Shao\",\"doi\":\"10.1021/jacsau.4c00475\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH<sub>3</sub> synthesis. However, their complex kinetics and energy demands necessitate high-performance electrocatalysts to ensure effective and selective process outcomes. Herein, we report that a two-dimensional Cu-based metal-organic framework (MOF), {[Cu(HL)]·H<sub>2</sub>O} <sub><i>n</i></sub> , (<b>Cu-OUC</b>, H<sub>3</sub>L = 5-(2'-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH<sub>3</sub> conversion. Electrochemical experimental studies showed that in 0.1 M K<sub>2</sub>SO<sub>4</sub> solution, the as-prepared <b>Cu-OUC</b> achieved a peak Faradaic efficiency of 96.91% and a notable NH<sub>3</sub> yield as high as 3415.82 μg h<sup>-1</sup> mg<sup>-1</sup>. The Zn-NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm<sup>-2</sup> while simultaneously achieving an NH<sub>3</sub> yield of 616.92 μg h<sup>-1</sup> mg<sup>-1</sup>. Theoretical calculations revealed that the surface of <b>Cu-OUC</b> effectively facilitates NO activation through a two-way charge transfer mechanism of \\\"electron acceptance and donation\\\", with the *NO formation step being the potential-determining stage. The study pioneers the use of a MOF as an electrocatalyst for ambient NO-to-NH<sub>3</sub> conversion.</p>\",\"PeriodicalId\":94060,\"journal\":{\"name\":\"JACS Au\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.5000,\"publicationDate\":\"2024-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11522898/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"JACS Au\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1021/jacsau.4c00475\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/10/28 0:00:00\",\"PubModel\":\"eCollection\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"JACS Au","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1021/jacsau.4c00475","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/10/28 0:00:00","PubModel":"eCollection","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH3.
Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH3 synthesis. However, their complex kinetics and energy demands necessitate high-performance electrocatalysts to ensure effective and selective process outcomes. Herein, we report that a two-dimensional Cu-based metal-organic framework (MOF), {[Cu(HL)]·H2O} n , (Cu-OUC, H3L = 5-(2'-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH3 conversion. Electrochemical experimental studies showed that in 0.1 M K2SO4 solution, the as-prepared Cu-OUC achieved a peak Faradaic efficiency of 96.91% and a notable NH3 yield as high as 3415.82 μg h-1 mg-1. The Zn-NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm-2 while simultaneously achieving an NH3 yield of 616.92 μg h-1 mg-1. Theoretical calculations revealed that the surface of Cu-OUC effectively facilitates NO activation through a two-way charge transfer mechanism of "electron acceptance and donation", with the *NO formation step being the potential-determining stage. The study pioneers the use of a MOF as an electrocatalyst for ambient NO-to-NH3 conversion.