Designing ruthenium-complexed hydrophenezine-linked covalent organic frameworks for pH-Universal electrocatalysis in hydrogen evolution reaction.

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Bibliographic Details
Title: Designing ruthenium-complexed hydrophenezine-linked covalent organic frameworks for pH-Universal electrocatalysis in hydrogen evolution reaction.
Authors: Wang, Dongming1 (AUTHOR), Lv, Jiaqi1 (AUTHOR), Han, Jiaming1 (AUTHOR), Han, Hongxing1 (AUTHOR), Zhang, Zhibo1 (AUTHOR), Liu, Jiapei1 (AUTHOR), Zhai, Pengda1,2 (AUTHOR), Liu, Haining1 (AUTHOR) liuhn@hebust.edu.cn, Zhang, Bin1,3 (AUTHOR) zhangbin-1984@hotmail.com, Xu, Zhice1,4 (AUTHOR) xujinghan2004@126.com
Source: International Journal of Hydrogen Energy. Dec2024, Vol. 96, p300-308. 9p.
Subjects: Hydrogen evolution reactions, Sustainability, Hydrogen production, Density functional theory, Proton transfer reactions, Oxygen evolution reactions
Abstract: It is an urgent challenge to discover hydrogen evolution reaction (HER) electrocatalysts which possess low overpotential and advanced stability. Covalent organic frameworks (COFs) have emerged as promising electrocatalysts for HER due to their controllable structures and ordered porosities. In this study, we synthesized a highly efficient universal-pH HER catalyst, by complexing ladder-shaped hydrophenazine (HP)-linked aromatic COF (HP–COF) with ruthenium ions (Ru@HP-COF). The HP-COF structure, composed of fused HP and pyrazine rings, provides nucleophilic sites for protonation and enables efficient proton capture. Ru@HP-COF exhibiting overpotentials of 54 mV, 251 mV, and 67 mV under acidic, near-neutral, and alkaline conditions, respectively, at a current density of 10 mA cm−2. This performance surpasses that of commercial 20% Pt/C catalysts, highlighting its potential to revolutionize sustainable hydrogen production. Density functional theory (DFT) calculations confirm that the Ru–N 2 coordination configuration contributes significantly to the exceptional HER performance. This work present novel insights into the fabrication and synthesis of highly efficient, sustainable, and cost-effective single-atom catalysts derived from COFs. • A novel hydrophenazine (HP)-linked aromatic COF (HP–COF) was prepared by solvothermal method. • Ruthenium-complexed HP-COF is beneficial to achieve high electroactivity. • The as-prepared catalyst displays remarkable performance for HER. [ABSTRACT FROM AUTHOR]
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Database: Engineering Source
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