具有本征手性的拓扑半金属作为氧进化反应的自旋控制电催化剂

IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Nature Energy Pub Date : 2024-11-25 DOI:10.1038/s41560-024-01674-9
Xia Wang, Qun Yang, Sukriti Singh, Horst Borrmann, Vicky Hasse, Changjiang Yi, Yongkang Li, Marcus Schmidt, Xiaodong Li, Gerhard H. Fecher, Dong Zhou, Binghai Yan, Claudia Felser
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引用次数: 0

摘要

电催化水分离是一种很有前景的清洁制氢方法,但由于电子传递过程依赖于自旋,阳极氧进化反应(OER)的动力学缓慢,阻碍了这一过程的进行。通过手性和磁化控制自旋的努力已显示出提高阳极氧演化性能的潜力。在这里,我们利用拓扑手性半金属(RhSi、RhSn 和 RhBiS)及其自旋极化费米面的潜力,在 OER 中促进自旋依赖性电子转移,解决了传统火山图的局限性。我们发现,随着自旋轨道耦合(SOC)程度的增加,OER 活动也呈现出 RhSi < RhSn < RhBiS 的趋势。手性单晶在碱性电解质中的表现优于非手性单晶(RhTe2、RhTe 和 RuO2),其中 RhBiS 的比活度比 RuO2 高两个数量级。我们的研究揭示了手性和 SOC 在自旋依赖催化中的关键作用,有助于设计超高效手性催化剂。
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Topological semimetals with intrinsic chirality as spin-controlling electrocatalysts for the oxygen evolution reaction

Electrocatalytic water splitting is a promising approach for clean hydrogen production, but the process is hindered by the sluggish kinetics of the anodic oxygen evolution reaction (OER) owing to the spin-dependent electron transfer process. Efforts to control spin through chirality and magnetization have shown potential in enhancing OER performance. Here we harnessed the potential of topological chiral semimetals (RhSi, RhSn and RhBiS) and their spin-polarized Fermi surfaces to promote the spin-dependent electron transfer in the OER, addressing the traditional volcano-plot limitations. We show that OER activities follow the trend RhSi < RhSn < RhBiS, corresponding to the increasing extent of spin–orbit coupling (SOC). The chiral single crystals outperform achiral counterparts (RhTe2, RhTe and RuO2) in alkaline electrolyte, with RhBiS exhibiting a specific activity two orders of magnitude higher than RuO2. Our work reveals the pivotal roles of chirality and SOC in spin-dependent catalysis, facilitating the design of ultra-efficient chiral catalysts.

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来源期刊
Nature Energy
Nature Energy Energy-Energy Engineering and Power Technology
CiteScore
75.10
自引率
1.10%
发文量
193
期刊介绍: Nature Energy is a monthly, online-only journal committed to showcasing the most impactful research on energy, covering everything from its generation and distribution to the societal implications of energy technologies and policies. With a focus on exploring all facets of the ongoing energy discourse, Nature Energy delves into topics such as energy generation, storage, distribution, management, and the societal impacts of energy technologies and policies. Emphasizing studies that push the boundaries of knowledge and contribute to the development of next-generation solutions, the journal serves as a platform for the exchange of ideas among stakeholders at the forefront of the energy sector. Maintaining the hallmark standards of the Nature brand, Nature Energy boasts a dedicated team of professional editors, a rigorous peer-review process, meticulous copy-editing and production, rapid publication times, and editorial independence. In addition to original research articles, Nature Energy also publishes a range of content types, including Comments, Perspectives, Reviews, News & Views, Features, and Correspondence, covering a diverse array of disciplines relevant to the field of energy.
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A hybrid modelling approach to compare chemical separation technologies in terms of energy consumption and carbon dioxide emissions Topological semimetals with intrinsic chirality as spin-controlling electrocatalysts for the oxygen evolution reaction Capacity estimation of home storage systems using field data Scalable fabrication of wide-bandgap perovskites using green solvents for tandem solar cells Polyanions stabilize anion redox
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