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Unlocking hexafluoroisopropanol as a practical anion-binding catalyst for living cationic polymerization.
Angew Chem Int Ed Engl
January 2025
Chang Chun Institute of Applied Chemistry Chinese Academy of Sciences, Key Laboratory of Polymer Ecomaterials, 5625 Renmin Street, Changchun, , 130022, Changchun, CHINA.
Living cationic polymerization (LCP) is a classical technique for precision polymer synthesis; however, due to the high sensitivity of cationic active species towards chain-transfer/termination events, it is notoriously difficult to control polymerization under mild conditions, which inhibits its progress in advanced materials engineering. Here, we unlock a practical anion-binding catalytic strategy to address the historical dilemma in LCP. Our experimental and mechanistic studies demonstrate that commercially accessible hexafluoroisopropanol (HFIP), when used in high loading, can create higher-order HFIP aggregates to tame dormant-active species equilibrium via non-covalent anion-binding principle, in turn inducing distinctive polymerization kinetics behaviors that grant efficient chain propagation while minimizing competitive side reactions.
View Article and Find Full Text PDFGuanine-Assisted Contrived Low Pt-Integrated MoC/C for Hydrogen Evolution Reaction.
Langmuir
January 2025
Materials Chemistry Department, CSIR-Institute of Minerals and Materials Technology, Bhubaneswar, Odisha 751013, India.
Due to the high cost of the available Pt electrocatalysts, the large-scale water electrolysis production of hydrogen has been hindered. Hydrogen generation via electrochemical water splitting is a renewable energy essential to a sustainable society, creating a distinct material interface that shows Pt-like properties with long-term stability crucial to hydrogen evolution reactions (HERs). Here, we synthesized the guanine-assisted facile synthesis of 1 wt % Pt/MoC/C having a layered type morphology via solid state calcined process followed by chemical reduction.
View Article and Find Full Text PDFOperando Electro-Oxidation Reconstitution of a Newly Designed 2D Co(II)-MOF on Nickel Foam to Cobalt Oxyhydroxide Nanosheets towards Energy Sustainability: A Holy Grail in Electrocatalytic Water Splitting.
ACS Appl Mater Interfaces
January 2025
Laboratory for Structural Engineering and Sustainable Catalysis, Department of Chemistry, University of North Bengal, Darjeeling 734013, India.
The upsurging of cost-effective electrocatalysts through the operando electro-oxidation approaches holds great promise for the scalable production of green energy in the pursuit of energy sustainability. This work introduces an operando electro-oxidation reconstitution strategy in producing a smart electrocatalyst, cobalt "oxyhydroxide" derived from a newly designed 2D cobalt(II) metal-organic framework (-) directly grown on nickel foam (NF), . The electrocatalyst, , exhibits an outstanding overpotential of 76 mV for the hydrogen evolution reaction and 336 mV for the oxygen evolution reaction to achieve a current density of 10 mA/cm with remarkable Faradaic efficiencies of 97.
View Article and Find Full Text PDFMusculoskeletal model predictions sensitivity to upper body mass scaling during gait.
Comput Biol Med
January 2025
Khalifa University, Abu Dhabi, United Arab Emirates. Electronic address:
Musculoskeletal modeling based on inverse dynamics provides a cost-effective non-invasive means for calculating intersegmental joint reaction forces and moments, solely relying on kinematic data, easily obtained from smart wearables. On the other hand, the accuracy and precision of such models strongly hinge upon the selected scaling methodology tailored to subject-specific data. This study investigates the impact of upper body mass distribution on internal and external kinetics computed using a comprehensive musculoskeletal model during level walking in both normal weight and obese individuals.
View Article and Find Full Text PDFMechanistic Insights into the Aerobic Oxidation of 2,5-Bis(hydroxymethyl)furfural to 2,5-Furandicarboxylic Acid on Pd Catalysts.
ACS Appl Mater Interfaces
January 2025
Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province, Ningbo Institute of Materials Technology & Engineering, Chinese Academy of Sciences, 1219 Zhongguan West Road, Ningbo 315201, China.
2,5-Furandicarboxylic acid (FDCA) is one of the top selected value-added chemicals, which can be obtained by the aerobic oxidation of 2,5-bis(hydroxymethyl)furfural (BHMF) over a Pd-based catalyst. However, the elucidation of the reaction mechanism was hindered by its rapid kinetics. Herein, employing the density functional theory (DFT) calculations, we delve into the detailed reaction pathways of the BHMF oxidation into FDCA over Pd(111) and PdH(111) identifying the rate-determining steps.
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