Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes

Yinghao Li, Chun-Kuo Peng, Yuntong Sun (), L. D. Nicole Sui, Yu-Chung Chang, San-Yuan Chen, Yingtang Zhou (), Yan-Gu Lin () and Jong-Min Lee ()
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Yinghao Li: 62 Nanyang Drive
Chun-Kuo Peng: National Yang Ming Chiao Tung University
Yuntong Sun: 62 Nanyang Drive
L. D. Nicole Sui: 62 Nanyang Drive
Yu-Chung Chang: National Synchrotron Radiation Research Center
San-Yuan Chen: National Yang Ming Chiao Tung University
Yingtang Zhou: Zhejiang Ocean University
Yan-Gu Lin: National Yang Ming Chiao Tung University
Jong-Min Lee: 62 Nanyang Drive

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Precise morphological control and identification of structure-property relationships pose formidable challenges for high-entropy alloys, severely limiting their rational design and application in multistep and tandem reactions. Herein, we report the synthesis of sub-nanometric high-entropy metallenes with up to eight metallic elements via a one-pot wet-chemical approach. The PdRhMoFeMn high-entropy metallenes exhibit high electrocatalytic hydrogen evolution performances with 6, 23, and 26 mV overpotentials at −10 mA cm−2 in acidic, neutral, and alkaline media, respectively, and high stability. The electrochemical measurements, theoretical simulations, and operando X-ray absorption spectroscopy reveal the actual active sites along with their dynamics and synergistic mechanisms in various electrolytes. Specially, Mn sites have strong binding affinity to hydroxyl groups, which enhances the water dissociation process at Pd sites with low energy barrier while Rh sites with optimal hydrogen adsorption free energy accelerate hydride coupling, thereby markedly boosting its intrinsic ability for hydrogen production.

Date: 2024
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DOI: 10.1038/s41467-024-54589-0

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