{"title":"用于酸性水分离的多熵高铱钌氧化物","authors":"Chun Hu, Kaihang Yue, Jiajia Han, Xiaozhi Liu, Lijia Liu, Qiunan Liu, Qingyu Kong, Chih-Wen Pao, Zhiwei Hu, Kazu Suenaga, Dong Su, Qiaobao Zhang, Xianying Wang, Yuanzhi Tan, Xiaoqing Huang","doi":"10.1126/sciadv.adf9144","DOIUrl":null,"url":null,"abstract":"<div >Designing an efficient catalyst for acidic oxygen evolution reaction (OER) is of critical importance in manipulating proton exchange membrane water electrolyzer (PEMWE) for hydrogen production. Here, we report a fast, nonequilibrium strategy to synthesize quinary high-entropy ruthenium iridium-based oxide (M-RuIrFeCoNiO<sub>2</sub>) with abundant grain boundaries (GB), which exhibits a low overpotential of 189 millivolts at 10 milliamperes per square centimeter for OER in 0.5 M H<sub>2</sub>SO<sub>4</sub>. Microstructural analyses, density functional calculations, and isotope-labeled differential electrochemical mass spectroscopy measurements collectively reveal that the integration of foreign metal elements and GB is responsible for the enhancement of activity and stability of RuO<sub>2</sub> toward OER. A PEMWE using M-RuIrFeCoNiO<sub>2</sub> catalyst can steadily operate at a large current density of 1 ampere per square centimeter for over 500 hours. This work demonstrates a pathway to design high-performance OER electrocatalysts by integrating the advantages of various components and GB, which breaks the limits of thermodynamic solubility for different metal elements.</div>","PeriodicalId":21609,"journal":{"name":"Science Advances","volume":"9 37","pages":""},"PeriodicalIF":11.7000,"publicationDate":"2023-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.science.org/doi/reader/10.1126/sciadv.adf9144","citationCount":"0","resultStr":"{\"title\":\"Misoriented high-entropy iridium ruthenium oxide for acidic water splitting\",\"authors\":\"Chun Hu, Kaihang Yue, Jiajia Han, Xiaozhi Liu, Lijia Liu, Qiunan Liu, Qingyu Kong, Chih-Wen Pao, Zhiwei Hu, Kazu Suenaga, Dong Su, Qiaobao Zhang, Xianying Wang, Yuanzhi Tan, Xiaoqing Huang\",\"doi\":\"10.1126/sciadv.adf9144\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div >Designing an efficient catalyst for acidic oxygen evolution reaction (OER) is of critical importance in manipulating proton exchange membrane water electrolyzer (PEMWE) for hydrogen production. Here, we report a fast, nonequilibrium strategy to synthesize quinary high-entropy ruthenium iridium-based oxide (M-RuIrFeCoNiO<sub>2</sub>) with abundant grain boundaries (GB), which exhibits a low overpotential of 189 millivolts at 10 milliamperes per square centimeter for OER in 0.5 M H<sub>2</sub>SO<sub>4</sub>. Microstructural analyses, density functional calculations, and isotope-labeled differential electrochemical mass spectroscopy measurements collectively reveal that the integration of foreign metal elements and GB is responsible for the enhancement of activity and stability of RuO<sub>2</sub> toward OER. A PEMWE using M-RuIrFeCoNiO<sub>2</sub> catalyst can steadily operate at a large current density of 1 ampere per square centimeter for over 500 hours. This work demonstrates a pathway to design high-performance OER electrocatalysts by integrating the advantages of various components and GB, which breaks the limits of thermodynamic solubility for different metal elements.</div>\",\"PeriodicalId\":21609,\"journal\":{\"name\":\"Science Advances\",\"volume\":\"9 37\",\"pages\":\"\"},\"PeriodicalIF\":11.7000,\"publicationDate\":\"2023-09-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.science.org/doi/reader/10.1126/sciadv.adf9144\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science Advances\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://www.science.org/doi/10.1126/sciadv.adf9144\",\"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":"Science Advances","FirstCategoryId":"103","ListUrlMain":"https://www.science.org/doi/10.1126/sciadv.adf9144","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
设计一种用于酸性氧进化反应(OER)的高效催化剂对于质子交换膜水电解槽(PEMWE)制氢至关重要。在此,我们报告了一种快速、非平衡策略,用于合成具有丰富晶界(GB)的二元高熵钌铱基氧化物(M-RuIrFeCoNiO2),该氧化物在 0.5 M H2SO4 中进行 OER 反应时,过电势较低,在 10 毫安/平方厘米时为 189 毫伏。微结构分析、密度泛函计算和同位素标记的差分电化学质谱测量共同揭示了外来金属元素与 GB 的结合是提高 RuO2 对 OER 的活性和稳定性的原因。使用 M-RuIrFeCoNiO2 催化剂的 PEMWE 可在每平方厘米 1 安培的大电流密度下稳定运行 500 小时以上。这项工作展示了通过整合各种成分和国标的优势来设计高性能 OER 电催化剂的途径,打破了不同金属元素热力学溶解度的限制。
Misoriented high-entropy iridium ruthenium oxide for acidic water splitting
Designing an efficient catalyst for acidic oxygen evolution reaction (OER) is of critical importance in manipulating proton exchange membrane water electrolyzer (PEMWE) for hydrogen production. Here, we report a fast, nonequilibrium strategy to synthesize quinary high-entropy ruthenium iridium-based oxide (M-RuIrFeCoNiO2) with abundant grain boundaries (GB), which exhibits a low overpotential of 189 millivolts at 10 milliamperes per square centimeter for OER in 0.5 M H2SO4. Microstructural analyses, density functional calculations, and isotope-labeled differential electrochemical mass spectroscopy measurements collectively reveal that the integration of foreign metal elements and GB is responsible for the enhancement of activity and stability of RuO2 toward OER. A PEMWE using M-RuIrFeCoNiO2 catalyst can steadily operate at a large current density of 1 ampere per square centimeter for over 500 hours. This work demonstrates a pathway to design high-performance OER electrocatalysts by integrating the advantages of various components and GB, which breaks the limits of thermodynamic solubility for different metal elements.
期刊介绍:
Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.