{"title":"原子分散的高价金属打破了质子交换膜电解中活性-稳定性的权衡","authors":"Jaehyuk Shim, Kangjae Lee, Yunjae Yu, Hyeon Seok Lee, Heejong Shin, Kug-Seung Lee, Megalamane S. Bootharaju, Sanghwi Han, Gyu Seong Yi, Hyojoo Ko, Sihwa Lee, Jaeyune Ryu, Minho Kim, Byoung-Hoon Lee, Taeghwan Hyeon, Yung-Eun Sung","doi":"10.1021/jacs.5c00936","DOIUrl":null,"url":null,"abstract":"Green hydrogen production via proton exchange membrane water electrolysis (PEMWE) faces economic feasibility challenges, primarily due to its reliance on noble metal catalysts. While cost-effective Ru-based catalysts show promise as alternatives to expensive Ir-based catalysts for an anodic oxygen evolution reaction, their long-term performance is compromised by overoxidation at high current densities. In addressing this challenge, we present a cooperative dual-site strategy for atomic-scale incorporation of high-valent d<sup>0</sup>-metal cations into RuO<sub>2</sub>. This synthesis results in uniformly distributed Ru–O–d<sup>0</sup>metal bonds, effectively reconciling the activity and stability trade-off. Leveraging these effects, our optimized Ta<sub>1</sub>/RuO<sub>2</sub> catalyst demonstrates exceptional performance, with a low overpotential of 164 ± 2 mV and stable operation for 1000 h at 100 mA cm<sup>–2</sup>. In practical PEMWE systems, Ta<sub>1</sub>/RuO<sub>2</sub> achieves 1.58 V at 2 A cm<sup>–2</sup>, surpassing the 2026 Department of Energy target, and maintains remarkable stability over 650 h at 500 mA cm<sup>–2</sup>. This breakthrough offers a highly active and durable PEMWE system suitable for industrial-scale applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"48 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Atomically Dispersed High-Valent d0-Metal Breaks the Activity–Stability Trade-Off in Proton Exchange Membrane Water Electrolysis\",\"authors\":\"Jaehyuk Shim, Kangjae Lee, Yunjae Yu, Hyeon Seok Lee, Heejong Shin, Kug-Seung Lee, Megalamane S. Bootharaju, Sanghwi Han, Gyu Seong Yi, Hyojoo Ko, Sihwa Lee, Jaeyune Ryu, Minho Kim, Byoung-Hoon Lee, Taeghwan Hyeon, Yung-Eun Sung\",\"doi\":\"10.1021/jacs.5c00936\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Green hydrogen production via proton exchange membrane water electrolysis (PEMWE) faces economic feasibility challenges, primarily due to its reliance on noble metal catalysts. While cost-effective Ru-based catalysts show promise as alternatives to expensive Ir-based catalysts for an anodic oxygen evolution reaction, their long-term performance is compromised by overoxidation at high current densities. In addressing this challenge, we present a cooperative dual-site strategy for atomic-scale incorporation of high-valent d<sup>0</sup>-metal cations into RuO<sub>2</sub>. This synthesis results in uniformly distributed Ru–O–d<sup>0</sup>metal bonds, effectively reconciling the activity and stability trade-off. Leveraging these effects, our optimized Ta<sub>1</sub>/RuO<sub>2</sub> catalyst demonstrates exceptional performance, with a low overpotential of 164 ± 2 mV and stable operation for 1000 h at 100 mA cm<sup>–2</sup>. In practical PEMWE systems, Ta<sub>1</sub>/RuO<sub>2</sub> achieves 1.58 V at 2 A cm<sup>–2</sup>, surpassing the 2026 Department of Energy target, and maintains remarkable stability over 650 h at 500 mA cm<sup>–2</sup>. This breakthrough offers a highly active and durable PEMWE system suitable for industrial-scale applications.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"48 1\",\"pages\":\"\"},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2025-05-01\",\"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.5c00936\",\"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.5c00936","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
通过质子交换膜电解(PEMWE)绿色制氢面临着经济可行性的挑战,主要是由于它对贵金属催化剂的依赖。虽然性价比高的ru基催化剂有望取代昂贵的ir基催化剂用于阳极析氧反应,但在高电流密度下,它们的长期性能会受到过氧化的影响。为了解决这一挑战,我们提出了一种合作的双位点策略,用于在原子尺度上将高价金属阳离子结合到RuO2中。这种合成的结果是均匀分布的ru -o - do金属键,有效地协调了活性和稳定性的权衡。利用这些效应,我们优化的Ta1/RuO2催化剂表现出优异的性能,其过电位低至164±2 mV,在100 mA cm-2下稳定运行1000小时。在实际的PEMWE系统中,Ta1/RuO2在2 A cm-2时达到1.58 V,超过了2026年美国能源部的目标,并在500 mA cm-2下保持650小时的卓越稳定性。这一突破提供了一种高活性和耐用的PEMWE系统,适用于工业规模的应用。
Atomically Dispersed High-Valent d0-Metal Breaks the Activity–Stability Trade-Off in Proton Exchange Membrane Water Electrolysis
Green hydrogen production via proton exchange membrane water electrolysis (PEMWE) faces economic feasibility challenges, primarily due to its reliance on noble metal catalysts. While cost-effective Ru-based catalysts show promise as alternatives to expensive Ir-based catalysts for an anodic oxygen evolution reaction, their long-term performance is compromised by overoxidation at high current densities. In addressing this challenge, we present a cooperative dual-site strategy for atomic-scale incorporation of high-valent d0-metal cations into RuO2. This synthesis results in uniformly distributed Ru–O–d0metal bonds, effectively reconciling the activity and stability trade-off. Leveraging these effects, our optimized Ta1/RuO2 catalyst demonstrates exceptional performance, with a low overpotential of 164 ± 2 mV and stable operation for 1000 h at 100 mA cm–2. In practical PEMWE systems, Ta1/RuO2 achieves 1.58 V at 2 A cm–2, surpassing the 2026 Department of Energy target, and maintains remarkable stability over 650 h at 500 mA cm–2. This breakthrough offers a highly active and durable PEMWE system suitable for industrial-scale applications.
期刊介绍:
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