Strongly Coupled Metal/Amorphous Ru/RuOx Heterostructure for Efficient Electrocatalytic Hydrogen Production

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Ramireddy Boppella, , , P. Muthu Austeria, , , Geun Ho Gu*, , and , Tae Kyu Kim*, 
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Abstract

Constructing well-defined heterostructure interfaces in catalysts is an effective strategy to break scaling relationships and accelerate reactions involving multiple intermediates. In this study, a heterostructure catalyst consisting of crystalline ruthenium (Ru) and amorphous ruthenium oxide (RuOx) nanoparticles uniformly distributed on N-doped carbon was developed by using a low-temperature (500 °C) pyrolysis method. The strong and well-defined electronic interactions at the interface between Ru and RuOx synergistically optimize hydrogen adsorption and desorption at the heterointerfaces of each particle, thereby significantly accelerating the kinetics of the hydrogen evolution reaction (HER). Consequently, the synthesized catalysts achieve pH-universal HER performance and exhibit impressively low overpotentials of 11 mV to reach a current density of 10 mA cm–2 under alkaline conditions. Additionally, the anion exchange membrane electrolyzer delivers remarkably low voltages of 2.08 V to achieve a current density of 0.82 A cm–2 and demonstrates prolonged stability over 100 h at a current density of 500 mA cm–2, outperforming Pt/C catalysts. Density functional theory calculations further reveal that amorphous RuOx effectively reduces the free energy barrier of the water dissociation step, while adjacent Ru promotes hydrogen evolution. This synthesis strategy offers a viable approach for the rational design and synthesis of superior HER electrocatalysts.

Abstract Image

Abstract Image

高效电催化制氢的强耦合金属/非晶Ru/RuOx异质结构
在催化剂中构建定义良好的异质结构界面是打破标度关系和加速涉及多个中间体的反应的有效策略。本研究采用低温(500℃)热解的方法,制备了一种由结晶钌(Ru)和非晶氧化钌(RuOx)纳米颗粒组成的异质结构催化剂,均匀分布在n掺杂碳上。Ru和RuOx之间在界面上的强而明确的电子相互作用协同优化了每个颗粒在异质界面上的氢吸附和解吸,从而显著加快了析氢反应的动力学。因此,合成的催化剂实现了pH-universal HER性能,并在碱性条件下表现出令人印象深刻的低过电位(11 mV),电流密度达到10 mA cm-2。此外,阴离子交换膜电解槽提供2.08 V的极低电压,实现0.82 a cm-2的电流密度,并在500 mA cm-2的电流密度下表现出超过100小时的长时间稳定性,优于Pt/C催化剂。密度泛函理论计算进一步表明,无定形的RuOx有效地降低了水解离步骤的自由能垒,而相邻的Ru促进了氢的析出。该合成策略为合理设计和合成优质HER电催化剂提供了可行的途径。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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