Rationalizing efficient and economical electrocatalysts for ethanol electro-oxidation (EOR) is crucial for the development of sustainable energy sources. Herein, porous carbon-supported PtPdCu ternary alloy heterostructures (PtPdCu/C, : : = atomic ratio) were constructed using Cu-BTC as the precursor. Benefiting from the advantages of its three-dimensional spatial network structure, flexible ternary alloy composition and strong metal-support interaction, the as-designed PtPdCu/C catalyst presents impressive EOR performance. Specifically, it achieved an EOR specific activity of 37.89 mA cm in alkaline electrolyte, which is 6 and 11.4 times higher than those of Pt/C (6.3 mA cm) and Pd/C (3.32 mA cm), respectively, and more than 90% of the initial activity was retained after 1000 consecutive CV cycles. FTIR studies further reveal that the PtPdCu/C catalyst requires a potential of only 0.45 V to oxidize poisonous CO intermediates in the EOR. This work provides valuable insights for the rationalization of MOF-derived ternary alloy electrocatalysts for ethanol electro-oxidation.
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http://dx.doi.org/10.1039/d4nr05301j | DOI Listing |
Anal Chem
March 2025
Beckman Institute for Advanced Science and Technology, University of Illinois Urbana-Champaign, Urbana, Illinois 61801, United States.
Molecular electrocatalysis campaigns often require tuning multiple experimental parameters to obtain kinetically insightful electrochemical measurements, a prohibitively time-consuming task when performing comprehensive studies across multiple catalysts and substrates. In this work, we present an autonomous workflow that combines Bayesian optimization and automated electrochemistry to perform fully unsupervised cyclic voltammetry (CV) studies of molecular electrocatalysis. We developed CV descriptors that leveraged the conceptual framework of the EC' (where EC' denotes an electrochemical step followed by a catalytic chemical step) kinetic zone diagram to enable efficient Bayesian optimization.
View Article and Find Full Text PDFNanoscale
March 2025
Xi'An Flit Heat Treatment Co. Ltd, Xi'an, 710075, China.
Rationalizing efficient and economical electrocatalysts for ethanol electro-oxidation (EOR) is crucial for the development of sustainable energy sources. Herein, porous carbon-supported PtPdCu ternary alloy heterostructures (PtPdCu/C, : : = atomic ratio) were constructed using Cu-BTC as the precursor. Benefiting from the advantages of its three-dimensional spatial network structure, flexible ternary alloy composition and strong metal-support interaction, the as-designed PtPdCu/C catalyst presents impressive EOR performance.
View Article and Find Full Text PDFAdv Mater
January 2025
Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
Electrochemical oxidation of small molecules shows great promise to substitute oxygen evolution reaction (OER) or hydrogen oxidation reaction (HOR) to enhance reaction kinetics and reduce energy consumption, as well as produce high-valued chemicals or serve as fuels. For these oxidation reactions, high-valence metal sites generated at oxidative potentials are typically considered as active sites to trigger the oxidation process of small molecules. Isolated atom site catalysts (IASCs) have been developed as an ideal system to precisely regulate the oxidation state and coordination environment of single-metal centers, and thus optimize their catalytic property.
View Article and Find Full Text PDFNanomaterials (Basel)
December 2024
Unidad Multidisciplinaria de Docencia e Investigación-Juriquilla, Facultad de Ciencias, Universidad Nacional Autónoma de México (UNAM), Juriquilla, Querétaro 76230, Mexico.
This work investigates the relationship between the mean diameter of palladium (Pd) nanoparticles and their surface energy, specifically in the context of alkaline ethanol electro-oxidation for fuel cell applications. Employing a recent generalization of the classical Laviron equation, we derive crucial parameters such as surface energy (), adsorption-desorption equilibrium constant (), and electron transfer coefficient () from linear voltammograms obtained from Pd-based nanoparticles supported on Vulcan carbon. Synthesized using two distinct methods, these nanocatalysts exhibit mean diameters ranging from 10 to 41 nm.
View Article and Find Full Text PDFMolecules
October 2024
College of Chemistry & Chemical and Environmental Engineering, Weifang University, Weifang 261061, China.
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