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1.
J Colloid Interface Sci ; 664: 389-399, 2024 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-38479275

RESUMEN

Electrochemical water electrolysis is a promising method for sustainable hydrogen production while transiting towards hydrogen economy. Among many, the Anion Exchange Membrane (AEM) based water electrolyzer is an emerging yet potentially affordable technology on maturity for producing large-scale hydrogen accommodating the usage of Non-Platinum Group Metal (non-PGM) based inexpensive electrocatalysts. Herein, we demonstrate the excellent performance of a bifunctional Nickel Copper Phosphide-Nickel sulphide (NCP-NS) electrocatalyst with a unique tensile nanostructure obtained via a facile, controlled ambient galvanic displacement route. An AEM electrolyzer with a larger active area of 10 cm2 stacked with the symmetric NCP-NS electrodes and a membrane demonstrates scalability with a requirement of a mere 1.66 V to reach a current density of 10 mA cm-2. The nickel-copper phosphide boosts the kinetics of charge transfer between the electrode and electrolyte interface, while a unique combination of a few nickel sulphide phases present in the catalyst provides sufficiently appropriate active sites for the overall water electrolysis. For the first time, we report a room temperature performance of âˆ¼ 230 mA cm-2 at 2 V for a non-PGM-based bifunctional electrocatalyst with exceptional durability for over 300 h of operation in an AEM water electrolyser with a retention rate of 95 %-97 % at a current density range of 80-800 mA cm-2.

2.
Adv Mater ; 34(26): e2110696, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35460119

RESUMEN

Nickel-iron-based layered double hydroxides (NiFe LDHs) have attracted tremendous research and industrial interests for oxygen evolution reaction (OER) electrocatalysis. However, methodologies on simultaneous regulation of performance-influencing factors remain scarce and their real synergistic effects are not clear enough. Herein, a versatile polyoxometallic acids (POMs) etching approach is reported to ingeniously reconstruct NiFe LDH, including 3D morphological nanotailoring, Fe3+ and α-Ni(OH)2 active species reconfiguration, creation of multiple Ni, Fe, and O vacancies, and intercalation of POM polyanionic clusters. The experimental and theoretical data collaboratively unveil that control of the key performance-influencing factors and their multiple synergistic mechanisms dominantly contribute to the step-like OER performance enhancement. The reinforced electrocatalyst is further produced with low cost and high performance up to Ф180 mm in diameter, showing its feasibility and advancement of the promising configuration of NiFe LDH-PMo12(+) II Ni@NiFe LDH(-) for alkaline anion-exchange-membrane electrode stack cells. Furthermore, to mathematically evaluate the evolution, a novel empirical formula is proposed for quantitative identification of structure-activity correlations, which offers an opportunity for first and fast reliability on materials screening.

3.
Small ; 17(13): e2007333, 2021 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-33590693

RESUMEN

The hydrogen evolution reaction (HER) is a significant cathode step in electrochemical devices, especially in water splitting, but developing efficient HER catalysts remains a great challenge. Herein, comprehensive density functional theory calculations are presented to explore the intrinsic HER behaviors of a series of ruthenium dichalcogenide crystals (RuX2 , X = S, Se, Te). In addition, a simple and easily scaled production strategy is proposed to synthesize RuX2 nanoparticles uniformly deposited on carbon nanotubes. Consistent with theoretical predictions, the RuX2 catalysts exhibit impressive HER catalytic behavior. In particular, marcasite-type RuTe2 (RuTe2 -M) achieves Pt-like activity (35.7 mV at 10 mA cm-2 ) in an acidic electrolyte, and pyrite-type RuSe2 presents outstanding HER performance in an alkaline media (29.5 mV at 10 mA cm-2 ), even superior to that of commercial Pt/C. More importantly, a RuTe2 -M-based proton exchange membrane (PEM) electrolyzer and a RuSe2 -based anion exchange membrane (AEM) electrolyzer are also carefully assembled, and their outstanding single-cell performance points to them being efficient cathode candidates for use in hydrogen production. This work makes a significant contribution to the exploration of a new class of transition metal dichalcogenides with remarkable activity toward water electrolysis.

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