Insights into the activity of nickel boride/nickel heterostructures for efficient methanol electrooxidation
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TLDR
In this paper , a heterostructure of nickel boride/nickel catalyst is developed to enable methanol electrooxidation into formate with a Faradaic efficiency of nearly 100%.Abstract:
Designing efficient catalysts and understanding the underlying mechanisms for anodic nucleophile electrooxidation are central to the advancement of electrochemically-driven technologies. Here, a heterostructure of nickel boride/nickel catalyst is developed to enable methanol electrooxidation into formate with a Faradaic efficiency of nearly 100%. Operando electrochemical impedance spectroscopy and in situ Raman spectroscopy are applied to understand the influence of methanol concentration in the methanol oxidation reaction. High concentrations of methanol inhibit the phase transition of the electrocatalyst to high-valent electro-oxidation products, and electrophilic oxygen species (O* or OH*) formed on the electrocatalyst are considered to be the catalytically active species. Additional mechanistic investigation with density functional theory calculations reveals that the potential-determining step, the formation of *CH2O, occurs most favorably on the nickel boride/nickel heterostructure rather than on nickel boride and nickel. These results are highly instructive for the study of other nucleophile-based approaches to electrooxidation reactions and organic electrosynthesis. read more
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Porous Nanoarchitectures of Nonprecious Metal Borides: From Controlled Synthesis to Heterogeneous Catalyst Applications
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References
More filters
Journal ArticleDOI
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
Georg Kresse,Jürgen Furthmüller +1 more
TL;DR: A detailed description and comparison of algorithms for performing ab-initio quantum-mechanical calculations using pseudopotentials and a plane-wave basis set is presented in this article. But this is not a comparison of our algorithm with the one presented in this paper.
Journal ArticleDOI
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals
TL;DR: In this paper, a simple formulation of a generalized gradient approximation for the exchange and correlation energy of electrons has been proposed by Perdew, Burke, and Ernzerhof (PBE), which improves the chemisorption energy of atoms and molecules on transition-metal surfaces.
Journal ArticleDOI
In Operando Identification of Geometrical-Site-Dependent Water Oxidation Activity of Spinel Co3O4
TL;DR: This work investigated the geometrical-site-dependent OER activity of Co3O4 catalyst by substituting Co(2+)(Td) and Co(3+)(Oh) with inactive Zn(2+) and Al( 3+), respectively, and revealed that Co( 2+)Td site is responsible for the formation of cobalt oxyhydroxide (CoOOH), which acted as the active site for water oxidation.
Journal ArticleDOI
CoP-Doped MOF-Based Electrocatalyst for pH-Universal Hydrogen Evolution Reaction
TL;DR: Density functional theory calculations and experimental results reveal that the electron transfer from CoP to Co-MOF through N-P/N-Co bonds could lead to the optimized adsorption energy of H2 O and hydrogen, which contributes to the remarkable HER performance.