Computational Design of Single Mo Atom Anchored Defective Boron Phosphide Monolayer as a High‐performance Electrocatalyst for the Nitrogen Reduction Reaction

Abstract

Electrochemical nitrogen reduction reaction is considered as an energy‐saving technology for artificial N2 fixation at ambient conditions. Here, the single Mo atom supported by the P‐vacancy defected BP monolayer is proved to be a promising single‐atom electrocatalyst for N2 fixation with a considerably small overpotential.

Salty Ice Electrolyte with Superior Ionic Conductivity Towards Low‐Temperature Aqueous Zinc Ion Hybrid Capacitors

“…DFT‐based first‐principles calculations were performed with the generalized gradient approximation (GGA) in the form of the Perdew–Burke–Ernzerhof (PBE) exchange‐correlation functional, as implemented in the DMol 3 module of Materials Studio 2017 package. [ 50–52 ] In the present work, the ice crystal structure (Ih structure, hexagonal unit cell, P63/mc space group, the lattice constants in the calculation were consistent with experimental XRD data) was adopted as the original structural model, and 2 × 1 × 2 supercell (containing 96 H atoms and 48 O atoms) was used during geometry optimization. The double numerical basis with polarization (DNP) functions was adopted as the basis set.…”

Insights into Tuning of Mo‐Based Structures toward Enhanced Electrocatalytic Performance of Nitrogen‐to‐Ammonia Conversion

“…It is of primary importance to further investigate such a correlation of Mo‐based structures through systematic theoretical models or automated machine learning. [ 8,73 ] Especially, from both aspects of electronic and geometric structures of Mo coordination spheres, their impacts on the activation of N 2 and the competing HER process should be deeply clarified. Through the efforts, we expect that it could precisely stimulate novel catalytic structures and further achieve improved NRR activity and selectivity.…”

“…[ 7 ] This activity trend is also demonstrated even at an atomic level. [ 8 ] However, under the NRR turnover conditions, H + from water would also cover metal sites to afford serious H 2 gas formation as a competing reaction of NRR, which seriously degrades the Faradic efficiency of NH 3 production (FE −NH3 ), as well as NH 3 yields. The NRR catalytic selectivity and activity of metal sites can be primarily optimized by structural tuning of the coordination spheres of metal sites, and the Mo‐based materials have shown rich coordination states in various nanostructures and atomic structures.…”

Nanomaterials for the electrochemical nitrogen reduction reaction under ambient conditions

“…Due to the homogeneity of the catalytically active sites, low coordination environment and maximal utilization efficiency, SACs have high catalytic activity, stability and selectivity for a series of electrochemical processes. [63][64][65][66] Some reports have explored the application of SACs anchored on N-doped porous carbon for the NRR. 53,67,68 In 2018, Zeng's group prepared single Ru atoms distributed on N-doped C by pyrolyzing a Ru-containing derivative of ZIF-8.…”