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Synthesis of Metal Nanoparticles Supported on Carbon Nanotube with Doped Co and N Atoms and its Catalytic Applications in Hydrogen Production
Published on: December 6, 2021
Nature of C─N Coupling in Urea Electrosynthesis for Catalyst Design
Yanxu Chen1, Buqi Ke1, Bocheng Zhang1
1Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China Hefei, Anhui, China.
Abstract:
Electrocatalytic co-reduction of CO2 and NO3 - offers a low-carbon route to urea, yet practical deployment is constrained by unsatisfactory efficiency due to the absence of a quantitative, theory-guided catalyst design principle. In this study, we propose the generalized dipole moment (GDM) of active sites as a transferable descriptor guided by charge-locking asymmetric site polarization (CLASP) mechanism, that can quantify polarization strength correlated with selectivity prediction for catalysts. Constant-potential simulations show that increasing GDM strengthens *CO2 adsorption, promotes H2O dissociation, and progressively favors C─N coupling relative to the competing protonation pathway. The slow-growth method further tracks charge evolution along the *CO─*NO coupling coordinate, confirming that polarized active sites precharge *CO and facilitate the predominant C-to-N charge-redistribution tendency during formation of critical coupling intermediates. Guided by this descriptor, a series of Ln─Cu alloy catalysts were designed to validate the predicted scaling, with La─Cu as the best candidate.
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