Oxophilic gallium single atoms bridged ruthenium clusters for practical anion-exchange membrane electrolyzer.

IF 14.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2024-08-08 DOI:10.1038/s41467-024-51200-4

Chenhui Zhou, Jia Shi, Zhaoqi Dong, Lingyou Zeng, Yan Chen, Ying Han, Lu Li, Wenyu Zhang, Qinghua Zhang, Lin Gu, Fan Lv, Mingchuan Luo, Shaojun Guo

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Abstract

The development of highly efficient and durable alkaline hydrogen evolution reaction (HER) catalysts is crucial for achieving high-performance practical anion exchange membrane water electrolyzer (AEMWE) at ampere-level current density. Herein, we report a design concept by employing Ga single atoms as an electronic bridge to stabilize the Ru clusters for boosting alkaline HER performance in practical AEMWE. Experimental and theoretical results collectively reveal that the bridged Ga sites trigger strong metal-support interaction for the homogeneous distribution of Ru clusters with high density, as well as optimize the Ru-H bond strength due to the electron transfer between Ru and Ga for enhanced intrinsic HER activity. Moreover, the oxophilic Ga sites near the Ru clusters tend to adsorb the hydroxyl species and accelerate the water dissociation for sufficient proton supplement in an alkaline medium. The Ru-Ga_SA/N-C catalyst exhibits a low overpotential of 4 ± 1 mV (10 mA cm^-2) and high mass activity of 9.3 ± 0.5 A mg^-1_Ru at -0.05 V vs RHE. In particular, the Ru-Ga_SA/N-C-based AEMWE in 1 M KOH delivers a voltage of only 1.74 V to reach an industrial current density of 1 A cm^-2, and can steadily operate at 1 A cm^-2 for more than 170 h.

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用于实用阴离子交换膜电解器的亲氧化镓单原子桥接钌簇。

要在安培级电流密度下实现高性能的实用阴离子交换膜水电解槽（AEMWE），开发高效耐用的碱性氢进化反应（HER）催化剂至关重要。在此，我们报告了一种设计理念，即利用 Ga 单原子作为电子桥来稳定 Ru 簇，从而提高实用 AEMWE 中碱性氢进化反应的性能。实验和理论结果共同表明，桥接的镓位点会引发强烈的金属-支撑相互作用，从而使 Ru 簇群均匀分布并具有较高的密度，同时由于 Ru 和镓之间的电子转移，Ru-H 键的强度也得到了优化，从而增强了 HER 的内在活性。此外，Ru 团簇附近的亲氧化镓位点倾向于吸附羟基物种并加速水的解离，从而在碱性介质中补充足够的质子。Ru-GaSA/N-C 催化剂的过电位很低，仅为 4 ± 1 mV（10 mA cm-2），而在 -0.05 V 与 RHE 相比时，质量活性高达 9.3 ± 0.5 A mg-1Ru。特别是在 1 M KOH 中，基于 Ru-GaSA/N-C 的 AEMWE 只需 1.74 V 的电压即可达到 1 A cm-2 的工业电流密度，并可在 1 A cm-2 的条件下稳定运行 170 小时以上。

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

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.