Theoretical Exploration of Electrochemical Nitrate Reduction Reaction Activities on Transition-Metal-Doped h-BP

Abstract

Electrocatalytic conversion of nitrate (NO3 –) into ammonia can not only eliminate harmful pollutant but also provide a green method for a low-temperature ammonia synthesis. The electrochemical NO3 – reduction reactions (NO3RRs) of a series of transition-metal-doped hexagonal boron phosphide (h-BP) monolayers were comprehensively evaluated using density functional theory. The V-doped h-BP monolayer was found to stand near the top of the volcano plot with the limiting potential of −0.22 V versus a reversible hydrogen electrode, exhibiting the lowest overpotential among the investigated systems in this work. Besides, the competing hydrogen evolution reaction is significantly suppressed due to the weak adsorption of the H atom. Importantly, the structure of the V-doped h-BP monolayer can be retained very well until 900 K, illustrating the initial indication of high thermal stability and great promise for synthesis. This study not only offers an eligible NO3RR electrocatalyst but also provides an atomic understanding of the behind mechanisms of the NO3RR process.

Anchoring boron on a covalent organic framework as an efficient single atom metal-free photo-electrocatalyst for nitrogen fixation: a first-principles analysis

“…According to the previous reports, SACs are efficient for various types of electrochemical and photochemical reaction, such as the hydrogen evolution reaction (HER), 11 oxygen evolution reaction (OER), 12 oxygen reduction reaction (ORR), 13 CO 2 reduction reaction (CO 2 RR), 14,15 N 2 reduction reaction (NRR), [16][17][18] NO reduction reaction (NORR), 19,20 N 2 O reduction reaction (N 2 ORR), 21 and nitrate reduction reaction (N 3 ORR). 22,23 Various noble or non-noble atoms anchored on 2D substrates as NRR catalysts have been designed and explored both theoretically and experimentally. For example, Xue and co-workers theoretically investigated the NRR performance of Mo anchored on a C 9 N 4 monolayer.…”

The synergetic effect of an aqua ligand and metal site on the performance of single-atom catalysts in H2O2synthesis: a density functional theory study

“…14,15 So far, SACs have shown good catalytic performance for a variety of electrocatalytic systems, e.g. , water-splitting reaction, 16 N 2 O reduction, 17 NO 3 reduction, 18,19 oxygen reduction, 18,19 and N 2 20 and CO 2 reduction. 21 Substantially, H 2 O 2 is derived from the partial reduction of O 2 via the 2e − ORR process on the cathode, of which the side reactions are the 4e − ORR and the hydrogen evolution reaction (HER).…”

“…23,24 For instance, Jin et al reported that the N-doped carbon dry gel showed good ORR electrocatalytic activity and stability under acidic conditions. 18,19 Ma et al indicated that N-HCNPs carbon nanoparticles had better stability, methanol permeability resistance and CO toxicity resistance, as well as compatible catalytic activity to the Pt/C catalyst. 25 The porous C 6 N 6 material 26 synthesized by the solvothermal method, featuring a well-distributed hole and N-rich characteristic, exhibited the narrow-band semiconductor (band gap of 1.58 eV 27 ) and anchoring sites with respect to other CN systems (C 2 N, 28 α-C 2 N 2 , 29 β-C 2 N 2 , 29 g-C 3 N 4 , 30 C 4 N 31 and γ-C 4 N 29 ).…”

Highly Efficient Electrocatalytic Upgrade of n‐Valeraldehyde to Octane over Au SACs–NiMn2O4 Spinel Synergetic Composites

“…However, the one-step electrocatalytic upgrade of n-valeraldehyde to high-value-added octane has remained unexplored. In recent years, single-atom catalysts have been gradually utilized in the elimination of inorganic and organic pollutants, such as NO, [40] carbon monoxide, [41] carbon dioxide, [42] nitrate, [43,44] 1, 2-dichloroethane, [34] and upgrade of N 2 and 1, 2-dichloroethane, [34,45] and good results are obtained. Herein, we fabricate an Au SACs-NiMn 2 O 4 spinel synergetic composites via simple and feasible adsorption-deposition method and apply it in the one-step electrocatalytic upgrade of n-valeraldehyde to octane.…”