Lattice-Matched Ru/W2C Heterointerfaces with Reversible Hydrogen Spillover for Efficient Alkaline Hydrogen Evolution

IF 24.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Advanced Energy Materials Pub Date : 2024-12-24 DOI:10.1002/aenm.202405546

Jian-Zhong Jiang, Shangguo Liu, Zijian Li, Min Gyu Kim, Haeseong Jang, Xien Liu, Liqiang Hou

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Abstract

The effect of lattice-matched heterointerfaces on the hydrogen reverse spillover process for accelerating alkaline hydrogen evolution reaction (HER) kinetics has not yet been reported. Herein, a lattice-matched Ru/W₂C heterostructure is successfully constructed for effective hydrogen production. Experimental and theoretical results reveal that the Ru nanocluster can effectively stabilize W₂C and thus promote the formation of phase-pure W₂C in the Ru/W₂C heterostructure. In addition, it is revealed that H₂O dissociation proceeded on W₂C, and the formed H intermediates are subsequently migrated to adjacent interfacial Ru sites for H─H coupling and H₂ release. This is enabled via a reversible hydrogen spillover mechanism promoted by the lattice-matched heterointerfaces that can weaken interfacial proton adsorption. As expected, the Ru/W₂C heterogeneous electrocatalyst exhibited a superior HER performance with a low overpotential of 17 mV at 10 mA cm⁻², a high mass current density (6.44 A mg_Ru⁻¹), and a low turnover frequency (TOF) value (2.8 s⁻¹) at the overpotential of 100 mV, far overwhelming the benchmark Ru/C and Pt/C. The study may offer a new perspective for the design of highly active electrocatalysts for alkaline HER.

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具有可逆氢溢出的栅格匹配Ru/W2C异质界面高效碱氢演化

晶格匹配异质界面对氢逆向溢出过程加速碱性析氢反应动力学的影响尚未见报道。本文成功构建了晶格匹配的Ru/W2C异质结构，用于有效制氢。实验和理论结果表明，Ru纳米团簇可以有效地稳定W2C，从而促进Ru/W2C异质结构中相纯W2C的形成。此外，研究还揭示了W2C上的H2O解离，形成的H中间体随后迁移到相邻的界面Ru位点进行H─H偶联和H2释放。这是通过一种可逆的氢溢出机制实现的，这种机制是由晶格匹配的异质界面促进的，它可以削弱界面质子的吸附。正如预期的那样，Ru/W2C非均相电催化剂表现出优异的HER性能，在10 mA cm−2时具有17 mV的低过电位，在100 mV过电位时具有高质量电流密度（6.44 a mgRu−1）和低周转率（TOF）值（2.8 s−1），远远超过基准Ru/C和Pt/C。该研究为高效电催化剂的设计提供了新的思路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS

CiteScore

41.90

自引率

4.00%

发文量

889

审稿时长

1.4 months

期刊介绍： Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.