激活BaRuO3薄膜催化活性表面以促进碱性析氢反应

doi:10.1016/S1872-2067(26)64972-8

催化学报 ›› 2026, Vol. 83: 341-350.DOI: 10.1016/S1872-2067(26)64972-8

激活BaRuO₃薄膜催化活性表面以促进碱性析氢反应

Jegon Lee^a^,¹, Do-Hyun Kim^a^,¹, Seulgi Ji^b^,¹, Sangmoon Yoon^c, Seung Hyun Nam^a, Jucheol Park^d, Jin Young Oh^a, Seung Gyo Jeong^a, Jong-Seong Bae^e, Sang A. Lee^f^,^*(), Heechae Choi^b^,^g^,^*(), Woo Seok Choi^a^,^*()

^a成均馆大学物理系, 水原, 韩国
^b科隆大学无机与材料化学研究所, 科隆, 德国
^c嘉泉大学物理与半导体科学系, 城南, 韩国
^d固美电子信息技术研究所庆北科技促进中心, 固美, 韩国
^e韩国基础科学研究所永南区域中心, 釜山, 韩国
^f釜庆国立大学物理系, 釜山, 韩国
^g西交-利物浦大学理学院化学与材料科学系, 先进材料研究中心(AMRC), 江苏苏州 215123, 中国

收稿日期:2025-08-14 接受日期:2025-10-09 出版日期:2026-04-18 发布日期:2026-03-04
通讯作者: * 电子信箱: sangalee@gmail.com (S. A. Lee), heechae.choi@xjtlu.edu.cn (H. Choi), choiws@skku.edu (W. S. Choi).
作者简介:¹共同第一作者.
基金资助:
苏州科技开发计划项目(SYC2022101);苏州工业园区功能分子材料与设备优质创新平台(YZCXPT2023105);西交-利物浦大学研究发展基金(RDF-23-01-089);西交-利物浦大学先进材料研究中心(AMRC)

Awakening catalytically active surface of BaRuO₃ thin film for alkaline hydrogen evolution

^aDepartment of Physics, Sungkyunkwan University, Suwon 16419, Republic of Korea
^bInstitute of Inorganic and Materials Chemistry, University of Cologne, Greinstr. 6, Cologne 50939, Germany
^cDepartment of Physics and Semiconductor Science, Gachon University, Seongnam 13120, Republic of Korea
^dKENTECH Shared Research Facility, Korea Institute of Energy Technology, Naju 58330, Republic of Korea
^eYeongnam Regional Center, Korea Basic Science Institute, Busan 46742, Republic of Korea
^fDepartment of Physics, Pukyong National University, Busan 48513, Republic of Korea
^gAdvanced Materials Research Center (AMRC) & Department of Chemistry and Materials Science, School of Science, Xi’an Jiaotong-Liverpool University, Suzhou 215123, Jiangsu, China

Received:2025-08-14 Accepted:2025-10-09 Online:2026-04-18 Published:2026-03-04
Contact: * E-mail: sangalee@gmail.com (S. Lee), heechae.choi@xjtlu.edu.cn (H. Choi), choiws@skku.edu (W. Choi).
About author:¹Contributed equally to this work.
Supported by:
Suzhou Science and Technology Development Planning Programme(SYC2022101);Suzhou Industrial Park High Quality Innovation Platform of Functional Molecular Materials and Devices(YZCXPT2023105);Xi'an Jiaotong-Liverpool University through Research Development Fund(RDF-23-01-089);XJTLU Advanced Materials Research Center(AMRC)

摘要/Abstract

摘要：

电化学反应过程中表面的动态重构在决定电催化剂的性能方面起着至关重要的作用. 然而, 由于重建发生在原子水平, 对于晶格结构不明确的传统粉末型催化剂来说, 直接观察和阐明其潜在机制是具有挑战性的. 本文在碱性析氢反应(HER)中, 3C BaRuO₃ (BRO)外延薄膜的催化活性表面是通过动态引入表面钌(Ru)团簇实现的. 在100 mV过电位为条件下, 基于单位质量活性, 本征析氢反应性能在首次循环后立即从0.11 A mg_Ru^‒1急剧提升至7.72 A mg_Ru^‒1, 在持续运行后最后稳定在1.05 A mg_Ru^‒1. 实验证实, 在碱性HER条件下, 选择性Ba浸出驱动催化剂表面形成Ru簇. 密度泛函理论计算表明, 由于Ru₆团簇的动态形成, HER活性随着H*吸附的增强而增加. 通过验证薄膜厚度的原子尺度控制可以有效地保持高活性状态, 进一步提出了一种稳定BRO “唤醒”活性表面的策略. 本研究为碱性HER的高活性钌基电催化剂的设计和稳定性提供了基础见解.

关键词: 析氢反应, 钙钛矿氧化物, 外延薄膜, 表面重构

Abstract:

The dynamic reconstruction of surfaces during electrochemical reactions plays a crucial role in determining the performance of electrocatalysts. However, because reconstructions occur at the atomic level, direct observation and elucidation of the underlying mechanism are challenging for conventional powder-type catalysts with ill-defined lattices. In this study, the catalytically active surface of 3C BaRuO₃ (BRO) epitaxial thin films emerges upon the dynamic introduction of surface Ru clusters, for the alkaline hydrogen evolution reaction (HER). Based on the mass activity at overpotential 100 mV, the intrinsic HER performance increases dramatically from 0.11 to 7.72 A mg_Ru⁻¹ immediately after the initial HER cycle and eventually saturates at 1.05 A mg_Ru⁻¹ after continuous operation. The formation of Ru clusters on the catalyst surface, driven by selective Ba leaching under alkaline HER conditions, is observed experimentally. Density functional theory calculations demonstrate that HER activity increased with enhanced H* adsorption owing to the dynamic Ru₆ cluster formation. A strategy for stabilizing the ‘awakened’ active surface of BRO is further proposed by validating that the atomic-scale control of the film thickness can effectively maintain the highly active state. This study offers fundamental insights into the design and stabilization of the highly active Ru-based electrocatalysts for the alkaline HER.

Key words: Hydrogen evolution reaction, Perovskite oxide, Epitaxial thin film, Surface reconstruction

Jegon Lee, Do-Hyun Kim, Seulgi Ji, Sangmoon Yoon, Seung Hyun Nam, Jucheol Park, Jin Young Oh, Seung Gyo Jeong, Jong-Seong Bae, Sang A. Lee, Heechae Choi, Woo Seok Choi. 激活BaRuO₃薄膜催化活性表面以促进碱性析氢反应[J]. 催化学报, 2026, 83: 341-350.

Jegon Lee, Do-Hyun Kim, Seulgi Ji, Sangmoon Yoon, Seung Hyun Nam, Jucheol Park, Jin Young Oh, Seung Gyo Jeong, Jong-Seong Bae, Sang A. Lee, Heechae Choi, Woo Seok Choi. Awakening catalytically active surface of BaRuO₃ thin film for alkaline hydrogen evolution[J]. Chinese Journal of Catalysis, 2026, 83: 341-350.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)64972-8

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图/表 5

Fig. 1. Evolution of electrocatalytic activity with HER cycling. (a) Schematic of surface self-reconstruction. (b) CV measurement for 100 HER cycles. The 100 cycles are represented by rainbow-colored lines from violet (1st) to red (100th). The black, blue, and red squares indicate the experimental points for the 1st, 2nd, and 100th HER cycles, respectively. (c) HER overpotential at ?1 mA cm?2. (d) Comparison of mass activity for the Ru loading at an overpotential of 0.1 V for various Ru-based catalysts; experimental conditions for each catalyst are provided in Table S2.

Fig. 2. Modification of lattice structures with HER cycling. XRD θ-2θ scans near (002) Bragg peak of 3C BRO for pristine (a), activated (b), saturated (c) thin films. STEM images in low- (d-f) and high- (g-i) magnification of pristine- (d,g), activated- (e,h), and saturated- (f,i) BROs. (g-i) Fast Fourier-transforms (FFTs) of four white box regions in the STEM images are displayed on the right panels of each image.

Fig. 3. Alteration of surface chemistry with HER cycling. XPS profiles of Ba 3d (a) and Ru 3d (b) core-level for BRO thin films with HER cycling, before Ar etching. (c) The Ba/Ru ratio was determined from spectral areas of each region for Ba 3d and Ru 3d, excluding carbon-related peaks. The depth-profiling results of Ba 3d (d) and Ru 3d (e) XPS spectra of BRO thin films with increasing time of Ar+ ion etching. (f) Atomic concentrations of dissolved ions in electrolytes after HER cycles, in which zero-cycle means pristine electrolyte. Note that the black and red dashed lines represent the experimental quantification limits for the Ba and Ru atoms, respectively, in the ICP-MS measurement. XPS profiles and deconvolution of peaks in Ru 3d spectra for pristine- (g), activated- (h), and saturated- (i) BRO. The navy, magenta, and grey lines indicate Ru4+ 3d peaks with satellite peaks, Ru3+ 3d peaks, and surface carbon-related peaks, respectively.

Fig. 4. DFT calculation results of the built-in electric field and the modeled supercells of BRO(7) (a), BRO(11) (b), and BRO(25) (c) models. (d) The magnitude of the dipole moment at the Ru6/BRO surface with different Ru coverages. (e) Gibbs free energy diagram for the H* intermediate with the reaction coordinate. (f) Gibbs free energy profiles for the H2O* intermediate in Ru6/BRO surfaces.

Fig. 5. Stabilization of the active phase of the BRO catalyst through film thickness engineering. (a) A color map representing the onset overpotential as a function of the number of HER cycles and film thickness. (b) Variation of onset overpotential trends for BRO thin films with thickness of 10 (top panel) and 200 nm (bottom panel).

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激活BaRuO₃薄膜催化活性表面以促进碱性析氢反应

Awakening catalytically active surface of BaRuO₃ thin film for alkaline hydrogen evolution

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