Atomically Dispersed High-Valent d0-Metal Breaks the Activity–Stability Trade-Off in Proton Exchange Membrane Water Electrolysis

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
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
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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 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.

Abstract Image

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
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。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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