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

Autor: Li Y; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore., Peng CK; Department of Material Science and Engineering, National Yang Ming Chiao Tung University, Hsinchu, 300093, Taiwan.; Scientific Research Division, National Synchrotron Radiation Research Center, Hsinchu, 300092, Taiwan., Sun Y; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore. yuntong.sun@ntu.edu.sg., Sui LDN; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore.; Environmental Chemistry and Materials Centre, Nanyang Environment & Water Research Institute (NEWRI), Interdisciplinary Graduate Programme, Nanyang Technological University, Singapore, 637141, Singapore., Chang YC; Scientific Research Division, National Synchrotron Radiation Research Center, Hsinchu, 300092, Taiwan., Chen SY; Department of Material Science and Engineering, National Yang Ming Chiao Tung University, Hsinchu, 300093, Taiwan., Zhou Y; Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control, Marine Science and Technology College, Zhejiang Ocean University, Zhoushan, 316004, China. zhouyingtang@zjou.edu.cn., Lin YG; Department of Material Science and Engineering, National Yang Ming Chiao Tung University, Hsinchu, 300093, Taiwan. lin.yg@nsrrc.org.tw.; Scientific Research Division, National Synchrotron Radiation Research Center, Hsinchu, 300092, Taiwan. lin.yg@nsrrc.org.tw., Lee JM; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore. jmlee@ntu.edu.sg.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2024 Nov 25; Vol. 15 (1), pp. 10222. Date of Electronic Publication: 2024 Nov 25.
DOI: 10.1038/s41467-024-54589-0
Abstrakt: 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.
Competing Interests: Competing interests: The authors declare no competing interests.
(© 2024. The Author(s).)
Databáze: MEDLINE
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