Meng Zhang, Xuetao Cheng, Yun Duan, Junxiang Chen, Lei Wang, Yan-Qin Wang
{"title":"水合效应增强的活性氢促进硝酸盐还原的中性氨电合成","authors":"Meng Zhang, Xuetao Cheng, Yun Duan, Junxiang Chen, Lei Wang, Yan-Qin Wang","doi":"10.1002/adfm.202413070","DOIUrl":null,"url":null,"abstract":"Electrocatalytic nitrate reduction to ammonia (NO<sub>3</sub>RR) in a neutral medium is a green and effective strategy for treating nitrate pollution meanwhile producing ammonia. However, the insufficient active hydrogen (H<sup>*</sup>) on the catalyst surface resulting from the sluggish Volmer step (H<sub>2</sub>O → H<sup>+</sup> + OH<sup>−</sup>), and the competitive hydrogen evolution reaction (HER) caused by H<sup>*</sup> coupling severely restrict the enhancement of NO<sub>3</sub>RR activity. Herein, a hydration-effect boosted H<sup>*</sup>-rich strategy facilitating neutral ammonia electrosynthesis from nitrate reduction is proposed. The introduction of the hydration-effect-promoting element aluminum into the copper-based catalyst forming CuAlO<sub>2</sub>, which adjusts the electron density distribution in the catalyst system, and the resulting hydration-effect significantly promotes the H<sup>*</sup> generation in a neutral medium. Moreover, the rapid charge transfer at the CuO/CuAlO<sub>2</sub> interface facilitates the reaction kinetics and the H<sup>*</sup> diffusion. More importantly, the introduction of Al weakens the overly strong adsorption of intermediates by CuO, thereby accelerating the hydrogenation process and suppressing HER. Thus, under neutral conditions, CuO/CuAlO<sub>2</sub> reached a Faradaic efficiency and an ammonia yield as high as 97.81 ± 1.94% and 10.21 ± 0.64 mg h<sup>−1</sup> cm<sup>−2</sup> at −1.0 V versus RHE toward NO<sub>3</sub>RR.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":18.5000,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hydration-effect Boosted Active Hydrogen Facilitates Neutral Ammonia Electrosynthesis from Nitrate Reduction\",\"authors\":\"Meng Zhang, Xuetao Cheng, Yun Duan, Junxiang Chen, Lei Wang, Yan-Qin Wang\",\"doi\":\"10.1002/adfm.202413070\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Electrocatalytic nitrate reduction to ammonia (NO<sub>3</sub>RR) in a neutral medium is a green and effective strategy for treating nitrate pollution meanwhile producing ammonia. However, the insufficient active hydrogen (H<sup>*</sup>) on the catalyst surface resulting from the sluggish Volmer step (H<sub>2</sub>O → H<sup>+</sup> + OH<sup>−</sup>), and the competitive hydrogen evolution reaction (HER) caused by H<sup>*</sup> coupling severely restrict the enhancement of NO<sub>3</sub>RR activity. Herein, a hydration-effect boosted H<sup>*</sup>-rich strategy facilitating neutral ammonia electrosynthesis from nitrate reduction is proposed. The introduction of the hydration-effect-promoting element aluminum into the copper-based catalyst forming CuAlO<sub>2</sub>, which adjusts the electron density distribution in the catalyst system, and the resulting hydration-effect significantly promotes the H<sup>*</sup> generation in a neutral medium. Moreover, the rapid charge transfer at the CuO/CuAlO<sub>2</sub> interface facilitates the reaction kinetics and the H<sup>*</sup> diffusion. More importantly, the introduction of Al weakens the overly strong adsorption of intermediates by CuO, thereby accelerating the hydrogenation process and suppressing HER. Thus, under neutral conditions, CuO/CuAlO<sub>2</sub> reached a Faradaic efficiency and an ammonia yield as high as 97.81 ± 1.94% and 10.21 ± 0.64 mg h<sup>−1</sup> cm<sup>−2</sup> at −1.0 V versus RHE toward NO<sub>3</sub>RR.\",\"PeriodicalId\":112,\"journal\":{\"name\":\"Advanced Functional Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":18.5000,\"publicationDate\":\"2024-10-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Functional Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/adfm.202413070\",\"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":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adfm.202413070","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}
Hydration-effect Boosted Active Hydrogen Facilitates Neutral Ammonia Electrosynthesis from Nitrate Reduction
Electrocatalytic nitrate reduction to ammonia (NO3RR) in a neutral medium is a green and effective strategy for treating nitrate pollution meanwhile producing ammonia. However, the insufficient active hydrogen (H*) on the catalyst surface resulting from the sluggish Volmer step (H2O → H+ + OH−), and the competitive hydrogen evolution reaction (HER) caused by H* coupling severely restrict the enhancement of NO3RR activity. Herein, a hydration-effect boosted H*-rich strategy facilitating neutral ammonia electrosynthesis from nitrate reduction is proposed. The introduction of the hydration-effect-promoting element aluminum into the copper-based catalyst forming CuAlO2, which adjusts the electron density distribution in the catalyst system, and the resulting hydration-effect significantly promotes the H* generation in a neutral medium. Moreover, the rapid charge transfer at the CuO/CuAlO2 interface facilitates the reaction kinetics and the H* diffusion. More importantly, the introduction of Al weakens the overly strong adsorption of intermediates by CuO, thereby accelerating the hydrogenation process and suppressing HER. Thus, under neutral conditions, CuO/CuAlO2 reached a Faradaic efficiency and an ammonia yield as high as 97.81 ± 1.94% and 10.21 ± 0.64 mg h−1 cm−2 at −1.0 V versus RHE toward NO3RR.
期刊介绍:
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