Ru/Al O is a highly stable, but less active catalyst for methanation reactions. Herein we report an effective approach to significantly improve its performance in the methanation of CO /H mixtures. Highly active and stable Ru/γ-Al O catalysts were prepared by high-temperature treatment in the reductive reaction gas. Operando/in situ spectroscopy and STEM imaging reveals that the strongly improved activity, by factors of 5 and 14 for CO and CO methanation, is accompanied by a flattening of the Ru nanoparticles and the formation of highly basic hydroxylated alumina sites. We propose a modification of the metal-support interactions (MSIs) as the origin of the increased activity, caused by modification of the Al O surface in the reductive atmosphere and an increased thermal mobility of the Ru nanoparticles, allowing their transfer to modified surface sites.
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http://dx.doi.org/10.1002/anie.202007228 | DOI Listing |
Adv Colloid Interface Sci
December 2024
Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, School of Materials Science and Engineering, Hubei University, Wuhan 430062, China. Electronic address:
Catalytic species such as molecular catalysts and metal catalysts are commonly attached to varieties of supports to simplify their separation and recovery and accommodate various reaction conditions. The physicochemical microenvironments surrounding catalytic species play an important role in catalytic performance, and the rational design and engineering of microenvironments can achieve more efficient chemical synthesis, leading to greener and more sustainable catalysis. In this review, we highlight recent works addressing the topic of the design and engineering of microenvironments of supported catalysts, including supported molecular catalysts and supported metal catalysts.
View Article and Find Full Text PDFChemSusChem
November 2024
Institute of Inorganic Chemistry, Kiel University, Max-Eyth-Str. 2, 24118, Kiel, Germany.
This perspective focuses on the modulation of metal-support interaction (MSI) in catalysts for CO hydrogenation, highlighting their profound impact on catalytic performance. Firstly, it outlines different strategies, including the use of highly reducible oxides and moderate reduction treatments, which induce the classical strong metal-support interaction (SMSI) effect and the electronic metal-support interaction (EMSI) effect. Morphology engineering and crystalline phase manipulation of oxides presented as effective methods to control EMSI are also discussed.
View Article and Find Full Text PDFSmall Methods
November 2024
College of Chemistry and Chemical Engineering, Qingdao University, Qingdao, Shandong, 266071, China.
Small
December 2024
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, China.
The Cu active sites have gained great attention in electrochemical nitrate reduction, offering a highly promising method for nitrate removal from water bodies. However, challenges arise from the instability of the Cu state and microscopic structure over prolonged operation, limiting the selectivity and durability of Cu-based electrodes. Herein, a self-reconstructed CuO/TiO nanofibers (CuO/TiO NFs) catalyst, demonstrating exceptional stability over 50 cycles (12 h per cycle), a high NO -N removal rate of 90.
View Article and Find Full Text PDFJ Colloid Interface Sci
February 2025
State Key Laboratory Base of Eco-Chemical Engineering, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China. Electronic address:
The sluggish kinetics and inherent instability over the Ru/RuO clusters are still enormous challenges in proton exchange membrane (PEM) water electrolyzer. Herein, we innovatively report synergistic modulation of dynamic electron modification and strong metal-support interaction (SMSI) to activate and stabilize bifunctional fluorine doped Ru/RuO clusters anchored on carbon nanotube (CNT), thus achieving efficient and stable acidic overall water splitting. Theoretical and experimental studies found that surface metal-fluorine modification layer could dynamically regulate the interfacial electronic environment to stabilize and activate multiple active Ru species; and the SMSI between Ru/RuO cluster and CNT maintains stable electronic environment for dynamic electron modification and avoids migrating or shedding of active species in acidic environment.
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