{"title":"高性能质子交换膜水电解中铱单原子催化剂的可控结构活化","authors":"Wonjae Ko, Jaehyuk Shim, Hyunsoo Ahn, Hee Jung Kwon, Kangjae Lee, Yoon Jung, Wytse Hooch Antink, Chan Woo Lee, Sungeun Heo, Seongbeom Lee, Junghwan Jang, Jiheon Kim, Hyeon Seok Lee, Sung-Pyo Cho, Byoung-Hoon Lee, Minho Kim, Yung-Eun Sung, Taeghwan Hyeon","doi":"10.1021/jacs.4c11442","DOIUrl":null,"url":null,"abstract":"Iridium single atom catalysts are promising oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane water electrolysis (PEMWE), as they can reduce the reliance on costly Ir in the OER catalysts. However, their practical application is hindered by their limited stability during PEMWE operation. Herein, we report on the activation of Ir-doped CoMn<sub>2</sub>O<sub>4</sub> in acidic electrolyte that leads to enhanced activity and stability in acidic OER for long-term PEMWE operation. In-depth material characterization combined with electrochemical analysis and theoretical calculations reveal that activating Ir-doped CoMn<sub>2</sub>O<sub>4</sub> induces controlled restructuring of Ir single atoms to IrO<sub><i>x</i></sub> nanoclusters, resulting in an optimized Ir configuration with outstanding mass activity of 3562 A g<sub>Ir</sub><sup>–1</sup> at 1.53 V (vs RHE) and enhanced OER stability. The PEMWE using activated Ir-doped CoMn<sub>2</sub>O<sub>4</sub> exhibited a stable operation for >1000 h at 250 mA cm<sup>–2</sup> with a low degradation rate of 0.013 mV h<sup>–1</sup>, demonstrating its practical applicability. Furthermore, it remained stable for more than 400 h at a high current density of 1000 mA cm<sup>–2</sup>, demonstrating long-term durability under practical operation conditions.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"217 1","pages":""},"PeriodicalIF":15.6000,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Controlled Structural Activation of Iridium Single Atom Catalyst for High-Performance Proton Exchange Membrane Water Electrolysis\",\"authors\":\"Wonjae Ko, Jaehyuk Shim, Hyunsoo Ahn, Hee Jung Kwon, Kangjae Lee, Yoon Jung, Wytse Hooch Antink, Chan Woo Lee, Sungeun Heo, Seongbeom Lee, Junghwan Jang, Jiheon Kim, Hyeon Seok Lee, Sung-Pyo Cho, Byoung-Hoon Lee, Minho Kim, Yung-Eun Sung, Taeghwan Hyeon\",\"doi\":\"10.1021/jacs.4c11442\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Iridium single atom catalysts are promising oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane water electrolysis (PEMWE), as they can reduce the reliance on costly Ir in the OER catalysts. However, their practical application is hindered by their limited stability during PEMWE operation. Herein, we report on the activation of Ir-doped CoMn<sub>2</sub>O<sub>4</sub> in acidic electrolyte that leads to enhanced activity and stability in acidic OER for long-term PEMWE operation. In-depth material characterization combined with electrochemical analysis and theoretical calculations reveal that activating Ir-doped CoMn<sub>2</sub>O<sub>4</sub> induces controlled restructuring of Ir single atoms to IrO<sub><i>x</i></sub> nanoclusters, resulting in an optimized Ir configuration with outstanding mass activity of 3562 A g<sub>Ir</sub><sup>–1</sup> at 1.53 V (vs RHE) and enhanced OER stability. The PEMWE using activated Ir-doped CoMn<sub>2</sub>O<sub>4</sub> exhibited a stable operation for >1000 h at 250 mA cm<sup>–2</sup> with a low degradation rate of 0.013 mV h<sup>–1</sup>, demonstrating its practical applicability. Furthermore, it remained stable for more than 400 h at a high current density of 1000 mA cm<sup>–2</sup>, demonstrating long-term durability under practical operation conditions.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"217 1\",\"pages\":\"\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-01-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.4c11442\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c11442","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
铱单原子催化剂是质子交换膜水电解(PEMWE)中很有前途的析氧反应(OER)电催化剂,因为它可以减少OER催化剂对昂贵的Ir的依赖。然而,它们在PEMWE运行过程中有限的稳定性阻碍了它们的实际应用。在此,我们报道了在酸性电解液中激活ir掺杂的CoMn2O4,从而提高了在酸性OER中长期运行的PEMWE的活性和稳定性。深入的材料表征结合电化学分析和理论计算表明,激活Ir掺杂的CoMn2O4可以诱导Ir单原子向IrOx纳米团簇的可控重组,从而优化了Ir结构,在1.53 V (vs RHE)下具有3562 A gIr-1的突出质量活性,并增强了OER稳定性。采用活化ir掺杂的CoMn2O4制备的PEMWE在250 mA cm-2下稳定工作1000 h,降解率为0.013 mV h - 1,具有较好的实用性。此外,它在1000 mA cm-2的高电流密度下保持稳定超过400小时,在实际操作条件下表现出长期耐用性。
Controlled Structural Activation of Iridium Single Atom Catalyst for High-Performance Proton Exchange Membrane Water Electrolysis
Iridium single atom catalysts are promising oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane water electrolysis (PEMWE), as they can reduce the reliance on costly Ir in the OER catalysts. However, their practical application is hindered by their limited stability during PEMWE operation. Herein, we report on the activation of Ir-doped CoMn2O4 in acidic electrolyte that leads to enhanced activity and stability in acidic OER for long-term PEMWE operation. In-depth material characterization combined with electrochemical analysis and theoretical calculations reveal that activating Ir-doped CoMn2O4 induces controlled restructuring of Ir single atoms to IrOx nanoclusters, resulting in an optimized Ir configuration with outstanding mass activity of 3562 A gIr–1 at 1.53 V (vs RHE) and enhanced OER stability. The PEMWE using activated Ir-doped CoMn2O4 exhibited a stable operation for >1000 h at 250 mA cm–2 with a low degradation rate of 0.013 mV h–1, demonstrating its practical applicability. Furthermore, it remained stable for more than 400 h at a high current density of 1000 mA cm–2, demonstrating long-term durability under practical operation conditions.
期刊介绍:
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