Tuning CO binding strengthviaengineering the copper/borophene interface for highly efficient conversion of CO into ethanol

Currently, copper is the most active monometallic catalyst to generate hydrocarbon and oxygenated products. Nevertheless, the huge kinetic barrier of Cu surfaces for the formation of a C-C bond on the path toward C2+products has remained unsolved to date. In this work, inspired by the successful growth of 2D borophene on Cu (111) surfaces [Nat. Nanotechnol., 2019,14(1), 44], we introduce a high density of one-dimensional copper/borophene interface sites for the C-C coupling reaction by using a framework of density functional theory calculations. Cu alone interacts very weakly with CO, while its synergistic interfacial interactions with boron atoms could significantly boost the CO binding strength, thus facilitating C-C coupling. The Cu-boron interface delivers an ultra-low kinetic energy barrier of only 0.42 eV for the CO dimerization step and a thermodynamic potential limiting step of only 0.61 V for the hydrogenation process toward ethanol production, inhibiting the hydrogen evolution reaction. The improved intrinsic catalytic activity can be ascribed to both the synergistic electronic and structural interactions between metal Cu and non-metal B atoms at the interface. Our work predicts an unprecedented family of low-dimensional nanohybrid catalysts towards the efficient electroreduction of CO to ethanol, thus providing a new class of guiding design principles for the broad experimentalist community. © The Royal Society of Chemistry 2021.

He T.1, 2 , Tang C.1 , Puente Santiago A.R. , Luque R. 4, 5 , Pan H.2, 6 , Du A.1
Royal Society of Chemistry
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  • 1 Centre for Materials Science, School of Chemistry and Physics, Queensland University of Technology, Garden Point Campus, Brisbane, QLD 4001, Australia
  • 2 Institute of Applied Physics and Materials Engineering, University of Macau999078, Macau
  • 3 Department of Chemistry, University of Texas at El Paso, 500 West University Avenue, El Paso, TX 79968, United States
  • 4 Department of Organic Chemistry, University of Cordoba, Campus de Rabanales, Edificio Marie Curie (C-3), Ctra Nnal IV-A, Km 396, Cordoba, E14014, Spain
  • 5 Peoples Friendship University of Russia (RUDN University), 6 Miklukho-Maklaya Str.Moscow 117198, Russian Federation
  • 6 Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau999078, Macau
Ключевые слова
Binding energy; Boron; Catalyst activity; Chemical bonds; Density functional theory; Electrolytic reduction; Ethanol; Kinetic energy; Kinetics; Nanocatalysts; C-C coupling reactions; Ethanol production; Hydrogenation process; Interfacial interaction; Monometallic catalysts; Oxygenated products; Structural interactions; Thermodynamic potentials; Copper
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