Updating the sub-nanometric cognition of reconstructed oxyhydroxide active phase for water oxidation

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Yu Sun, Yong Xie, Xiaoxuan Chen, Jing Wu, Pengfei Liu, Xin Wang, Zhen Tian, Wenhao Zheng, Zhouyu Jiang, Zhuo Kang, Yue Zhang
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Abstract

Unveiling structure-activity correlations at the sub-nanoscale remains an essential challenge in catalysis science. During electrocatalysis, dynamic structural evolution drives the ambiguous entanglement of crystals and electrons degrees of freedom that obscure the activity origin. Here, we track the structural evolution of Ni-based model pre-catalysts (Ni(OH)2, NiS2, NiSe2, NiTe), detailing their catalytically active state during water oxidation via operando techniques and theoretical calculations. We reveal the sub-nanometric structural difference of NiO6 unit with a regular distortion in the reconstructed active phase NiOOH, codetermined by the geometric (bond lengths) and electronic (covalency) structure of the pre-catalysts on both spatial and temporal scales. The symmetry-broken active units induce the delicate balance of the p and d orbitals in NiOOH, further steering the modulation of catalytic intermediate configurations and mechanisms, with improved performance. This work recognizes the fine structural differences of the active phases from the sub-nanometer scale, and quantitatively explains their influence on activity. Our findings provide a more intuitive design framework for high-efficiency materials through targeted symmetry engineering of active units.

Abstract Image

揭示亚纳米尺度的结构-活性相关性仍然是催化科学中的一项重要挑战。在电催化过程中,动态结构演化驱动着晶体和电子自由度的模糊纠缠,从而掩盖了活性的起源。在这里,我们跟踪了镍基模型前催化剂(Ni(OH)2、NiS2、NiSe2、NiTe)的结构演变,通过操作技术和理论计算详细说明了它们在水氧化过程中的催化活性状态。我们揭示了在重建的活性相 NiOOH 中,NiO6 单元的亚纳米结构差异和规则变形,这是由前催化剂在空间和时间尺度上的几何(键长)和电子(共价)结构共同决定的。对称性断裂的活性单元诱导 NiOOH 中 p 和 d 轨道的微妙平衡,进一步引导催化中间构型和机制的调节,从而提高性能。这项工作从亚纳米尺度认识到了活性相的细微结构差异,并定量解释了它们对活性的影响。我们的发现为通过有针对性的活性单元对称工程设计高效材料提供了一个更直观的设计框架。
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来源期刊
Nature Communications
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.
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