TY - JOUR
T1 - Boosting hydrogen evolution activity
T2 - next-nearest oxygen coordination in dual-phase supra-nanostructured multiprincipal element alloy catalysts
AU - Lyu, Fucong
AU - Liu, Chang
AU - Zeng, Shanshan
AU - Bu, Xiuming
AU - Chen, Yuhan
AU - Jia, Zhe
AU - Xie, Youneng
AU - Sun, Ligang
AU - Mao, Zhengyi
AU - Shen, Junda
AU - Li, Gan
AU - Luan, Juanhua
AU - Yan, Yang
AU - Yao, Lu
AU - Li, Lanxi
AU - Wang, Xianying
AU - Wu, Ge
AU - Li, Yang Yang
AU - Lu, Jian
PY - 2024/10/21
Y1 - 2024/10/21
N2 - Achieving near-zero overpotential for a large-scale hydrogen evolution reaction (HER) using multi-principal element alloys is a formidable challenge. These alloys, characterized by their diverse compositions and complex atomic configurations, offer a broad spectrum of catalytic sites, positioning them as candidates of interest in energy and environmental applications. However, conventional methods for improving the catalytic performance of these alloys, which focus on element composition and the cocktail effect, frequently undervalue the role of structural design. In this work, we introduce an innovative approach that integrates oxygen incorporation with dual-phase supra-nanostructuring to boost the catalytic efficacy of a multi-principal element alloy via industrial magnetron sputtering at ambient temperature. Specifically, the oxygen-incorporated crystal-amorphous dual-phase supra-nanostructured palladium/multi-principal element alloy (denoted as SNDP-Pd@HEAA) presents a plethora of uniformly distributed interfaces enriched with unique next-nearest oxygen-coordinated active sites, which contribute to its exceptional HER performance. The SNDP-Pd@HEAA exhibits a near zero overpotential of 10.16 mV at a current density of 10 mA cm−2, which is much lower than that of 34.01 mV of commercial 20% Pt/C. Remarkably, it retains a reliable long-term stability of ∼1000 h at 500 mA cm−2 in an anion exchange membrane (AEM) device, which is significantly higher than that of the reported commercial Pt/C||IrO2 system. The structural and computational results reveal that the SNDP-Pd@HEAA comprising Pd-rich nanocrystalline cores and O-rich amorphous glassy shells produces plentiful active interfaces and special active Pd sites with next-nearest O coordination, thus actively promoting water adsorption capacity and accelerating hydrogen proton adsorption/desorption. This SNDP nanostructure production and oxygen-incorporated manipulation technique, as well as the next-nearest O-coordinated active sites mechanism, establishes a new paradigm for hydrogen evolution reaction catalysts. © 2024 The Royal Society of Chemistry.
AB - Achieving near-zero overpotential for a large-scale hydrogen evolution reaction (HER) using multi-principal element alloys is a formidable challenge. These alloys, characterized by their diverse compositions and complex atomic configurations, offer a broad spectrum of catalytic sites, positioning them as candidates of interest in energy and environmental applications. However, conventional methods for improving the catalytic performance of these alloys, which focus on element composition and the cocktail effect, frequently undervalue the role of structural design. In this work, we introduce an innovative approach that integrates oxygen incorporation with dual-phase supra-nanostructuring to boost the catalytic efficacy of a multi-principal element alloy via industrial magnetron sputtering at ambient temperature. Specifically, the oxygen-incorporated crystal-amorphous dual-phase supra-nanostructured palladium/multi-principal element alloy (denoted as SNDP-Pd@HEAA) presents a plethora of uniformly distributed interfaces enriched with unique next-nearest oxygen-coordinated active sites, which contribute to its exceptional HER performance. The SNDP-Pd@HEAA exhibits a near zero overpotential of 10.16 mV at a current density of 10 mA cm−2, which is much lower than that of 34.01 mV of commercial 20% Pt/C. Remarkably, it retains a reliable long-term stability of ∼1000 h at 500 mA cm−2 in an anion exchange membrane (AEM) device, which is significantly higher than that of the reported commercial Pt/C||IrO2 system. The structural and computational results reveal that the SNDP-Pd@HEAA comprising Pd-rich nanocrystalline cores and O-rich amorphous glassy shells produces plentiful active interfaces and special active Pd sites with next-nearest O coordination, thus actively promoting water adsorption capacity and accelerating hydrogen proton adsorption/desorption. This SNDP nanostructure production and oxygen-incorporated manipulation technique, as well as the next-nearest O-coordinated active sites mechanism, establishes a new paradigm for hydrogen evolution reaction catalysts. © 2024 The Royal Society of Chemistry.
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U2 - 10.1039/d4ee03150d
DO - 10.1039/d4ee03150d
M3 - RGC 21 - Publication in refereed journal
SN - 1754-5692
VL - 17
SP - 7908
EP - 7918
JO - Energy and Environmental Science
JF - Energy and Environmental Science
IS - 20
ER -
