Designing high-efficiency catalyst is at the heart of a transition to future renewable energy systems. Great achievements have been made to optimize thermodynamics to reduce energetic barriers of the catalytic reactions. However, little attention has been paid to design catalysts to improve kinetics to enrich the local concentration of reactant molecules surrounding electrocatalysts. Here, we find that well-designed nanocatalysts with periodic structures can optimize kinetics to accelerate mass-transport from bulk electrolyte to the catalyst surface, leading to the enhanced catalytic performance. This achievement stems from regulation of the surface reactant flux due to the gradient of the microelectric field directing uniformly to the nearest catalyst on ordered pattern, so that all of the reactant molecules are utilized sufficiently for reactions, enabling the boost of the electrocatalytic performance. This novel concept is further confirmed in various catalytic systems and nanoassemblies, such as nanoparticles, nanorods, and nanoflakes.
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http://dx.doi.org/10.1021/jacs.9b03617 | DOI Listing |
Inorg Chem
January 2025
School of Chemistry and Chemical Engineering, and Institute for Innovative Materials and Energy, Yangzhou University, 180 Si-Wang-Ting Road, Yangzhou 225002, China.
The interaction between electrocatalytic active centers and their support is essential to the electrocatalytic performance, which could regulate the electronic structure of the metal centers but requires precise design. Herein, we report on covalent grafting of graphene quantum dots (GQDs) on stepped TiO as a support to anchoring cobalt phosphide nanoparticles (CoP/GQD/S-TiO) for electrocatalytic hydrogen evolution reaction (HER). The covalent ester bonds between GQDs and TiO endow enlarged anchoring sites to achieve highly dispersed electroactive CoP nanoparticles but, more importantly, provide an efficient electron-transfer pathway from TiO to GQDs which could regulate the electronic structure of CoP.
View Article and Find Full Text PDFNanomaterials (Basel)
January 2025
Department of Materials, School of Natural Science, The University of Manchester, Oxford Road, Manchester M13 9PL, UK.
Platinum (Pt)-based heterogeneous catalysts show excellent performance for the electrocatalytic hydrogen evolution reaction (HER); however, the high cost and earth paucity of Pt means that efforts are being directed to reducing Pt usage, whilst maximizing catalytic efficiency. In this work, a two-step laser annealing process was employed to synthesize Pt single-atom catalysts (SACs) on a MOF-derived carbon substrate. The laser irradiation of a metal-organic framework (MOF) film (ZIF67@ZIF8 composite) by rapid scanning of a ns pulsed infrared (IR; 1064 nm) laser across the freeze-dried MOF resulted in a metal-loaded graphitized film.
View Article and Find Full Text PDFNanomaterials (Basel)
January 2025
Institute of Materials Science & Devices, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China.
Carbon catalysts have shown promise as an alternative to the currently available energy-intensive approaches for nitrogen fixation (NF) to urea, NH, or related nitrogenous compounds. The primary challenges for NF are the natural inertia of nitrogenous molecules and the competitive hydrogen evolution reaction (HER). Recently, carbon-based materials have made significant progress due to their tunable electronic structure and ease of defect formation.
View Article and Find Full Text PDFAdv Mater
January 2025
School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore, 639798, Singapore.
Catalysts are essential for achieving high-performance lithium-sulfur batteries. The precise design and regulation of catalytic sites to strengthen their efficiency and robustness remains challenging. In this study, spinel sulfides and catalyst design principles through element doping are investigated.
View Article and Find Full Text PDFHeliyon
January 2025
Environmental Health Research Center, Research Institute for Health Development, Kurdistan University of Medical Sciences, Sanandaj, Iran.
In this study, a Cu@Ag core-shell was synthesized using a co-precipitation method. To create a new electrochemical sensor, a Cu@Ag core-shell with conductive polymers such as polyalizarin yellow R (PA) and Nafion (Nf) was immobilized on the surface of a glassy carbon electrode (Cu@Ag-Nf/PA/GCE). X-ray diffraction analysis (XRD), energy dispersive X-ray analysis (EDX), transmission electron microscopy (TEM), and Fourier Transform Infrared Spectroscopy (FTIR) techniques were employed to characterize the Cu@Ag-Nf/PA/GCE.
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