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Strategies for controlling the size of metal species using zeolites and their catalytic behavior in industrially relevant processes have attracted widespread attention, but the effect of H2O and CO2 on the catalytic performance of zeolite-based metal catalysts remains obscure. This study investigated the influence of H2O and CO2 on CO oxidation over zeolite-based metal catalysts, along with the precise control of active sites through the regulation of Lewis acidity. It was found that the presence of H2O enhanced CO oxidation and alleviated the inhibitory effect of CO2. Abundant Lewis acid sites of low SiO2/Al2O3 ratios in the Pt/SSZ-13 catalyst facilitate Pt dispersion (61.07%), a high Ptn+/Pt ratio (4.43), and small Pt particles (2.31 nm) formation. In situ DRIFTS revealed that CO2 inhibits CO adsorption and the decomposition of carbon intermediates. Water alters the CO adsorption configuration of Pt0, thereby weakening the Pt-CO bond to promote the CO oxidation reaction. Meanwhile, water dissociated into hydroxyl groups on the surface adsorbs oxygen species, participating in reactions and promoting CO2 production from carbon intermediates. H218O isotope labeling experiments validated the water involvement in the reaction and emphasized the importance of the presence of oxygen species during the water dissociation process. Regulation of Lewis acid sites promotes the Ptn+ species formation, enhancing the CO oxidation activity, while Pt0 species enhance the water-promotion effect.
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http://dx.doi.org/10.1063/5.0242302 | DOI Listing |
J Mass Spectrom
October 2025
Department of Chemistry and Biomolecular Sciences, University of Ottawa, Ottawa, Canada.
The strong C-F bond found in per- and poly-fluorinated alkyl substances (PFAS) makes them resistant to degradation and thus persistent in the environment. One of the most common methods for quantifying PFAS in environmental matrices is to use tandem mass spectrometry. However, the dissociation of ions made by deprotonating PFAS alcohols and acids has only been qualitatively explored.
View Article and Find Full Text PDFACS Omega
September 2025
Ming Hsieh Department of Electrical Engineering, University of Southern California, Los Angeles, California 90089, United States.
A nanosecond pulse transient plasma is employed to initiate and control the exothermic decomposition of ionic liquids, namely, a mixture of hydroxylammonium nitrate (HAN) and 1-ethyl-3-methylimidazolium ethyl sulfate [EMIM]/[EtSO], as well as some noncombustible ionic liquids. Here, the plasma is discharged in a cylindrical geometry with a coaxial center wire electrode. High voltage (20 kV) nanosecond pulses (20 ns) at various frequencies up to 10 kHz produce a plasma discharge in the ionic liquid that initiates its nonthermal decomposition.
View Article and Find Full Text PDFInorg Chem
September 2025
College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou, Jiangsu 215123, China.
The electrochemical reduction of CO into valuable C products presents a sustainable and efficient strategy for the utilization of CO and long-term renewable energy storage. Yet, enhancing the efficiency of the electrocatalytic CO reduction reaction (eCORR) in aqueous systems remains challenging due to the difficulty in activating both CO and HO molecules. In this study, we focus on water activation generating reactive hydrogen species (*H) to boost C product selectivity.
View Article and Find Full Text PDFACS Nano
September 2025
Key Laboratory for Power Machinery and Engineering of Ministry of Education, Shanghai Jiao Tong University, Shanghai 200240, China.
Coelectrolysis of HO and CO using high-temperature solid oxide cells offers a highly efficient solution for converting greenhouse gases into valuable fuels and chemicals. Although Pt is an effective catalyst for this reaction, its high cost has limited its usage. Herein, we present that Pt-containing alloy catalysts with increased entropy exhibit high Pt utilization efficiency, catalytic performance, and thermal stability.
View Article and Find Full Text PDFChem Sci
August 2025
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science, Zhejiang Normal University Jinhua Zhejiang 321004 P. R. China
Selective photoreduction of CO with HO to hydrocarbons is challenged by inadequate and uncontrollable electron and proton feeding. Herein, this limitation is overcome by integrating HO dissociation, CO reduction, and O evolution catalysts into a dual S-scheme heterojunction and regulating exposed facets of the heterojunction supports. In this design, H and OH species generated by HO dissociation on the NH-MIL-125 support transfer to the T-COF shell and FeO insert for CO reduction and O evolution, respectively.
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