Electron–phonon coupling and coherent energy superposition induce spin-sensitive orbital degeneracy for enhanced acidic water oxidation

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2025-01-21 DOI:10.1038/s41467-025-56315-w

Yanfeng Shi, Lupeng Wang, Miao Liu, Zuozheng Xu, Peilin Huang, Lizhe Liu, Yuanhong Xu

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Abstract

The development of acid-stable water oxidation electrocatalysts is crucial for high-performance energy conversion devices. Different from traditional nanostructuring, here we employ an innovative microwave-mediated electron–phonon coupling technique to assemble specific Ru atomic patterns (instead of random Ru-particle depositions) on Mn_0.99Cr_0.01O₂ surfaces (Ru_MW-Mn_1-xCr_xO₂) in RuCl₃ solution because hydrated Ru-ion complexes can be uniformly activated to replace some Mn sites at nearby Cr-dopants through microwave-triggered energy coherent superposition with molecular rotations and collisions. This selective rearrangement in Ru_MW-Mn_1-xCr_xO₂ with particular spin-differentiated polarizations can induce localized spin domain inversion from reversed to parallel direction, which makes Ru_MW-Mn_1-xCr_xO₂ demonstrate a high current density of 1.0 A cm⁻² at 1.88 V and over 300 h of stability in a proton exchange membrane water electrolyzer. The cost per gallon of gasoline equivalent of the hydrogen produced is only 43% of the 2026 target set by the U.S. Department of Energy, underscoring the economic significance of this nanotechnology.

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电子-声子耦合和相干能量叠加诱导自旋敏感轨道简并增强酸性水氧化

开发耐酸型水氧化电催化剂是实现高性能能量转换装置的关键。与传统的纳米结构不同，本研究采用了一种创新的微波介导电子-声子耦合技术，在RuCl3溶液中在mn0.99 cr0.010 o2表面（RuMW-Mn1-xCrxO2）上组装特定的Ru原子模式（而不是随机的Ru粒子沉积），因为水合Ru离子配合物可以通过微波触发的能量相干叠加与分子旋转和碰撞，均匀激活以取代附近cr掺杂剂上的一些Mn位点。RuMW-Mn1-xCrxO2具有特殊的自旋分化极化，这种选择性重排可以诱导局部自旋畴从反向向平行方向反转，使RuMW-Mn1-xCrxO2在1.88 V下表现出1.0 a cm−2的高电流密度，并在质子交换膜水电解槽中稳定运行300 h以上。每加仑汽油生产氢气的成本仅为美国能源部设定的2026年目标的43%，强调了这种纳米技术的经济意义。

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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.