The noble, metal-free materials capable of efficiently catalyzing water splitting reactions currently hold a great deal of promise. In this study, we reported the structure and electrochemical performance of new MoS-based material synthesized with L-cysteine. For this, a facile one-pot hydrothermal process was developed and an array of densely packed nanoplatelet-shaped hybrid species directly on a conductive substrate were obtained. The crucial role of L-cysteine was determined by numerous methods on the structure and composition of the synthesized material and its activity and stability for hydrogen evolution reaction (HER) from the acidic water. A low Tafel slope of 32.6 mV dec, close to a Pt cathode, was registered for the first time. The unique HER performance at the surface of this hybrid material in comparison with recently reported MoS-based electrocatalysts was attributed to the formation of more defective 1T, 2H-MoS/MoO, C nanostructures with the dominant 1T-MoS phase and thermally degraded cysteine residues entrapped. Numerous stacks of metallic (1T-MoS and MoO) and semiconducting (2H-MoS and MoO) fragments relayed the formation of highly active layered nanosheets possessing a low hydrogen adsorption free energy and much greater durability, whereas intercalated cysteine fragments had a low Tafel slope of the HER reaction. X-ray photoelectron spectroscopy, scanning electron microscopy, thermography with mass spectrometry, high-resolution transmission electron microscopy, Raman spectroscopy techniques, and linear sweep voltammetry were applied to verify our findings.
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http://dx.doi.org/10.3390/ma14051165 | DOI Listing |
J Am Chem Soc
January 2025
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, PR China.
A prevalent challenge in particulate photocatalytic water splitting lies in the fact that while numerous photocatalysts exhibit outstanding hydrogen evolution reaction (HER) activity in organic sacrificial reagents, their performance diminishes markedly in a Z-scheme water splitting system using electronic mediators. This underlying reason remains undefined, posing a long-standing issue in photocatalytic water splitting. Herein, we unveiled that the primary reason for the decreased HER activity in electronic mediators is due to the strong adsorption of shuttle ions on cocatalyst surfaces, which inhibits the initial proton reduction and results in a severe backward reaction of the oxidized shuttle ions.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
School of Physics, State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China.
Electrochemical nitrogen conversion for ammonia (NH) synthesis, driven by renewable electricity, offers a sustainable alternative to the traditional Haber-Bosch process. However, this conversion process remains limited by a low Faradaic efficiency (FE) and NH yield. Although transition metals have been widely studied as catalysts for NH synthesis through effective electron donation/back-donation mechanisms, there are challenges in electrochemical environments, including competitive hydrogen evolution reaction (HER) and catalyst stability issues.
View Article and Find Full Text PDFACS Nano
January 2025
School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen 518000, China.
Electrochemical nitrate reduction (NORR) to ammonia presents a promising alternative strategy to the traditional Haber-Bosch process. However, the competitive hydrogen evolution reaction (HER) reduces the Faradaic efficiency toward ammonia, while the oxygen evolution reaction (OER) increases the energy consumption. This study designs IrCu alloy nanoparticles as a bifunctional catalyst to achieve efficient NORR and OER while suppressing the unwanted HER.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
Hydrogen spillover is an important process in catalytic hydrogenation reactions, facilitating H activation and modulating surface chemistry of reducible oxide catalysts. This study focuses on the unveiling of platinum-induced hydrogen spillover on monoclinic tungsten trioxide (γ-WO), employing ambient pressure X-ray photoelectron spectroscopy, density functional theory calculations and microkinetic modeling to investigate the dynamic evolution of surface states at varied temperatures. At room temperature, hydrogen spillover results in the formation of W and hydrogen intermediates (hydroxyl species and adsorbed water), facilitated by Pt metal clusters.
View Article and Find Full Text PDFJ Appl Biomater Funct Mater
January 2025
MOE Key Lab for Liquid-Solid Structure Evolution and Materials Processing, Shandong University, Jinan, China.
In current study, microstructural, mechanical and corrosion behaviour were investigated with incorporation of dual reinforced AZ91D surface composites. This research was carried out for enhancement of the bio-degradability in biological environment. The surface composites were successfully fabricated by friction stir processing method with a rotation speed of 800 rpm, travel speed of 80 mm/min and 2.
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