{"title":"实现己二酸与氢高效共电解的镍铜合金阵列","authors":"Xuhui Ren , Qianyu Zhang , Yun Tong, Guorong Zhou, Cong Lin, Yanying Zhao, Pengzuo Chen","doi":"10.1016/j.jechem.2024.09.033","DOIUrl":null,"url":null,"abstract":"<div><div>Constructing electrocatalytic overall reaction technology to couple the electrosynthesis of adipic acid with energy-saving hydrogen production is of significant for sustainable energy systems. However, the development of highly-active bifunctional electrocatalysts remains a challenge. Herein, 3D hierarchical nickel-copper alloying arrays with dendritic morphology are manufactured by a simple electrodeposition process, standing for the excellent bifunctional electrocatalyst towards the co-production of adipic acid and H<sub>2</sub> from cyclohexanone and water. The membrane-free flow electrolyzer of Cu<sub>0.81</sub>Ni<sub>0.19</sub>/NF shows the superior electrooxidation performance of ketone-alcohol (KA) oil with high faradaic efficiencies of over 90% for adipic acid and H<sub>2</sub>, robust stability over 200 h as well as a high yield of 0.6 mmol h<sup>−1</sup> for adipic acid at 100 mA cm<sup>−2</sup>. In-situ spectroscopy indicates the Cu<sub>0.81</sub>Ni<sub>0.19</sub> alloy contributes to forming more active NiOOH species to involve in the conversion of cyclohexanone to adipic acid, while the proposed reaction pathway undergoes the 2-hydroxycyclohexanone and 2,7-oxepanedione intermediates. Moreover, the theoretical calculations confirm that the optimal electronic interaction, boosted reaction kinetics as well as improved adsorption free energy of reaction intermediates, synergistically endows Cu<sub>0.81</sub>Ni<sub>0.19</sub> alloy with superior bifunctional performance.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"101 ","pages":"Pages 7-15"},"PeriodicalIF":13.1000,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Nickel-copper alloying arrays realizing efficient co-electrosynthesis of adipic acid and hydrogen\",\"authors\":\"Xuhui Ren , Qianyu Zhang , Yun Tong, Guorong Zhou, Cong Lin, Yanying Zhao, Pengzuo Chen\",\"doi\":\"10.1016/j.jechem.2024.09.033\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Constructing electrocatalytic overall reaction technology to couple the electrosynthesis of adipic acid with energy-saving hydrogen production is of significant for sustainable energy systems. However, the development of highly-active bifunctional electrocatalysts remains a challenge. Herein, 3D hierarchical nickel-copper alloying arrays with dendritic morphology are manufactured by a simple electrodeposition process, standing for the excellent bifunctional electrocatalyst towards the co-production of adipic acid and H<sub>2</sub> from cyclohexanone and water. The membrane-free flow electrolyzer of Cu<sub>0.81</sub>Ni<sub>0.19</sub>/NF shows the superior electrooxidation performance of ketone-alcohol (KA) oil with high faradaic efficiencies of over 90% for adipic acid and H<sub>2</sub>, robust stability over 200 h as well as a high yield of 0.6 mmol h<sup>−1</sup> for adipic acid at 100 mA cm<sup>−2</sup>. In-situ spectroscopy indicates the Cu<sub>0.81</sub>Ni<sub>0.19</sub> alloy contributes to forming more active NiOOH species to involve in the conversion of cyclohexanone to adipic acid, while the proposed reaction pathway undergoes the 2-hydroxycyclohexanone and 2,7-oxepanedione intermediates. Moreover, the theoretical calculations confirm that the optimal electronic interaction, boosted reaction kinetics as well as improved adsorption free energy of reaction intermediates, synergistically endows Cu<sub>0.81</sub>Ni<sub>0.19</sub> alloy with superior bifunctional performance.</div></div>\",\"PeriodicalId\":15728,\"journal\":{\"name\":\"Journal of Energy Chemistry\",\"volume\":\"101 \",\"pages\":\"Pages 7-15\"},\"PeriodicalIF\":13.1000,\"publicationDate\":\"2024-09-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Energy Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2095495624006570\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"Energy\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Energy Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2095495624006570","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Energy","Score":null,"Total":0}
Nickel-copper alloying arrays realizing efficient co-electrosynthesis of adipic acid and hydrogen
Constructing electrocatalytic overall reaction technology to couple the electrosynthesis of adipic acid with energy-saving hydrogen production is of significant for sustainable energy systems. However, the development of highly-active bifunctional electrocatalysts remains a challenge. Herein, 3D hierarchical nickel-copper alloying arrays with dendritic morphology are manufactured by a simple electrodeposition process, standing for the excellent bifunctional electrocatalyst towards the co-production of adipic acid and H2 from cyclohexanone and water. The membrane-free flow electrolyzer of Cu0.81Ni0.19/NF shows the superior electrooxidation performance of ketone-alcohol (KA) oil with high faradaic efficiencies of over 90% for adipic acid and H2, robust stability over 200 h as well as a high yield of 0.6 mmol h−1 for adipic acid at 100 mA cm−2. In-situ spectroscopy indicates the Cu0.81Ni0.19 alloy contributes to forming more active NiOOH species to involve in the conversion of cyclohexanone to adipic acid, while the proposed reaction pathway undergoes the 2-hydroxycyclohexanone and 2,7-oxepanedione intermediates. Moreover, the theoretical calculations confirm that the optimal electronic interaction, boosted reaction kinetics as well as improved adsorption free energy of reaction intermediates, synergistically endows Cu0.81Ni0.19 alloy with superior bifunctional performance.
期刊介绍:
The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies.
This journal focuses on original research papers covering various topics within energy chemistry worldwide, including:
Optimized utilization of fossil energy
Hydrogen energy
Conversion and storage of electrochemical energy
Capture, storage, and chemical conversion of carbon dioxide
Materials and nanotechnologies for energy conversion and storage
Chemistry in biomass conversion
Chemistry in the utilization of solar energy