{"title":"氧化还原介导的解耦海水直接分裂制取 H2","authors":"Tao Liu, Cheng Lan, Min Tang, Mengxin Li, Yitao Xu, Hangrui Yang, Qingyue Deng, Wenchuan Jiang, Zhiyu Zhao, Yifan Wu, Heping Xie","doi":"10.1038/s41467-024-53335-w","DOIUrl":null,"url":null,"abstract":"<p>Seawater direct electrolysis (SDE) using renewable energy provides a sustainable pathway to harness abundant oceanic hydrogen resources. However, the side-reaction of the chlorine electro-oxidation reaction (ClOR) severely decreased direct electrolysis efficiency of seawater and gradually corrodes the anode. In this study, a redox-mediated strategy is introduced to suppress the ClOR, and a decoupled seawater direct electrolysis (DSDE) system incorporating a separate O<sub>2</sub> evolution reactor is established. Ferricyanide/ferrocyanide ([Fe(CN)<sub>6</sub>]<sup>3−/4−</sup>) serves as an electron-mediator between the cell and the reactor, thereby enabling a more dynamically favorable half-reaction to supplant the traditional oxygen evolution reaction (OER). This alteration involves a straightforward, single-electron-transfer anodic reaction without gas precipitation and effectively eliminates the generation of chlorine-containing byproducts. By operating at low voltages (~1.37 V at 10 mA cm<sup>−2</sup> and ~1.57 V at 100 mA cm<sup>−2</sup>) and maintaining stability even in a Cl<sup>−</sup>-saturated seawater electrolyte, this system has the potential of undergoing decoupled seawater electrolysis with zero chlorine emissions. Further improvements in the high-performance redox-mediators and catalysts can provide enhanced cost-effectiveness and sustainability of the DSDE system.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":null,"pages":null},"PeriodicalIF":14.7000,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Redox-mediated decoupled seawater direct splitting for H2 production\",\"authors\":\"Tao Liu, Cheng Lan, Min Tang, Mengxin Li, Yitao Xu, Hangrui Yang, Qingyue Deng, Wenchuan Jiang, Zhiyu Zhao, Yifan Wu, Heping Xie\",\"doi\":\"10.1038/s41467-024-53335-w\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Seawater direct electrolysis (SDE) using renewable energy provides a sustainable pathway to harness abundant oceanic hydrogen resources. However, the side-reaction of the chlorine electro-oxidation reaction (ClOR) severely decreased direct electrolysis efficiency of seawater and gradually corrodes the anode. In this study, a redox-mediated strategy is introduced to suppress the ClOR, and a decoupled seawater direct electrolysis (DSDE) system incorporating a separate O<sub>2</sub> evolution reactor is established. Ferricyanide/ferrocyanide ([Fe(CN)<sub>6</sub>]<sup>3−/4−</sup>) serves as an electron-mediator between the cell and the reactor, thereby enabling a more dynamically favorable half-reaction to supplant the traditional oxygen evolution reaction (OER). This alteration involves a straightforward, single-electron-transfer anodic reaction without gas precipitation and effectively eliminates the generation of chlorine-containing byproducts. By operating at low voltages (~1.37 V at 10 mA cm<sup>−2</sup> and ~1.57 V at 100 mA cm<sup>−2</sup>) and maintaining stability even in a Cl<sup>−</sup>-saturated seawater electrolyte, this system has the potential of undergoing decoupled seawater electrolysis with zero chlorine emissions. Further improvements in the high-performance redox-mediators and catalysts can provide enhanced cost-effectiveness and sustainability of the DSDE system.</p>\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.7000,\"publicationDate\":\"2024-10-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-024-53335-w\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-024-53335-w","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
摘要
利用可再生能源进行海水直接电解(SDE)为利用丰富的海洋氢资源提供了一条可持续发展的途径。然而,氯电氧化反应(ClOR)的副反应严重降低了海水直接电解的效率,并逐渐腐蚀阳极。本研究引入了一种氧化还原介导的策略来抑制 ClOR,并建立了一个包含独立氧气进化反应器的解耦海水直接电解(DSDE)系统。铁氰化物/铁氰化物([Fe(CN)6]3-/4-)作为电池和反应器之间的电子介质,从而实现了更有利的半反应,取代了传统的氧进化反应(OER)。这种改变是一种直接的单电子转移阳极反应,没有气体析出,并有效地消除了含氯副产物的产生。通过在低电压下运行(10 mA cm-2 时 ~1.37 V,100 mA cm-2 时 ~1.57 V)并在 Cl 饱和的海水电解质中保持稳定,该系统有可能在零氯排放的情况下进行解耦海水电解。进一步改进高性能氧化还原介质和催化剂可以提高 DSDE 系统的成本效益和可持续性。
Redox-mediated decoupled seawater direct splitting for H2 production
Seawater direct electrolysis (SDE) using renewable energy provides a sustainable pathway to harness abundant oceanic hydrogen resources. However, the side-reaction of the chlorine electro-oxidation reaction (ClOR) severely decreased direct electrolysis efficiency of seawater and gradually corrodes the anode. In this study, a redox-mediated strategy is introduced to suppress the ClOR, and a decoupled seawater direct electrolysis (DSDE) system incorporating a separate O2 evolution reactor is established. Ferricyanide/ferrocyanide ([Fe(CN)6]3−/4−) serves as an electron-mediator between the cell and the reactor, thereby enabling a more dynamically favorable half-reaction to supplant the traditional oxygen evolution reaction (OER). This alteration involves a straightforward, single-electron-transfer anodic reaction without gas precipitation and effectively eliminates the generation of chlorine-containing byproducts. By operating at low voltages (~1.37 V at 10 mA cm−2 and ~1.57 V at 100 mA cm−2) and maintaining stability even in a Cl−-saturated seawater electrolyte, this system has the potential of undergoing decoupled seawater electrolysis with zero chlorine emissions. Further improvements in the high-performance redox-mediators and catalysts can provide enhanced cost-effectiveness and sustainability of the DSDE system.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.