In situ high-pressure Raman spectroscopy, with corroborating density functional calculations, is used to probe C-H chemical bonds formed when dissociated hydrogen diffuses from a platinum nanocatalyst to three distinct graphenic surfaces. At ambient temperature, hydrogenation and dehydrogenation are reversible in the combined presence of an active catalyst and oxygen heteroatoms. Hydrogenation apparently occurs through surface diffusion in a chemisorbed state, while dehydrogenation requires diffusion of the chemisorbed species back to an active catalyst.
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http://dx.doi.org/10.1021/nl303673z | DOI Listing |
Inorg Chem
January 2025
State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China.
The low sulfur selectivity of Fe-based HS-selective catalytic oxidation catalysts is still a problem, especially at a high O content. This is alleviated here through anchoring FeO nanoclusters on UiO-66 via the formation of Fe-O-Zr bonds. The introduced FeO species exist in the form of Fe and Fe.
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 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 PDFAngew Chem Int Ed Engl
January 2025
Chinese Academy of Sciences Dalian Institute of Chemical Physics, State Key Laboratory of Catalysis, 457 Zhongshan Road, 116023, Dalian, CHINA.
The reduction of CO2 to CO provides a promising approach to the production of valuable chemicals through CO2 utilization. However, challenges persist with the rapid deactivation and insufficient activity of catalysts. Herein, we developed a soft-hard dual-template method to synthesize layered MoS2 using inexpensive and scalable templates, enabling facile regulation of sulfur vacancies by controlling the number of layers.
View Article and Find Full Text PDFNat Commun
January 2025
WA School of Mines: Minerals, Energy and Chemical Engineering (WASM-MECE), Curtin University, Perth, WA, 6102, Australia.
Reducing green hydrogen production cost is critical for its widespread application. Proton-exchange-membrane water electrolyzers are among the most promising technologies, and significant research has been focused on developing more active, durable, and cost-effective catalysts to replace expensive iridium in the anode. Ruthenium oxide is a leading alternative while its stability is inadequate.
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