Mo-based 2D MOF as a highly efficient electrocatalyst for reduction of N₂ to NH₃: a density functional theory study

Abstract

A Mo-based MOF is an efficient electrocatalyst for the N2 reduction reaction with a low overpotential of 0.18 V.

Theoretical Screening of Single Transition Metal Atoms Embedded in MXene Defects as Superior Electrocatalyst of Nitrogen Reduction Reaction

“…The Δ E N2‐adsorption ranging from −0.3 to −0.6 eV is comparable to the adsorption energies of CO 2 with commonly used industrial sorbents, indicating that N 2 can be effectively physisorbed on the surface. On the other hand, the moderate Δ G NH3‐desorption under 1 eV is lower than these most active catalysts that were predicted based on theoretical design . Numerous calculations combined with experimental works also implied that the ammonia desorption with barrier over 1 eV can proceed in the acidic solution .…”

The Chemistry of Reticular Framework Nanoparticles: MOF, ZIF, and COF Materials

“…Although the many-body problem can be greatly reduced, DFT calculations are highly time-consuming as they calculate the electron density of the full framework, to describe the nanoparticles' physical properties. DFT is hence not suited for a structural optimization of complete particles, but can rather address localized questions such as host-guest interaction, [178] charge transfer reactions on the 10-100 ps time scale, [179] catalytic reactions, [180] or the comparison of known framework structures. [181] DFT can investigate cell parameters and elastic properties [182] of the periodic structure of reticular framework.…”

Two-dimensional metal-organic frameworks for energy-related electrocatalytic applications

“…The downsizing of MOFs into 2D nanosheets has attracted increasing attention in research due to its many unique properties originating from its ultrathin thickness [2,6,[10][11][12][13]. 2D MOF-related research is one of the fast-growing directions in the fields of chemistry, materials, and renewable energy.…”

“…In other applications, 2D MOFs can also be viable candidates for the nitrogen reduction reaction (NRR) in N 2 electrolysis. Sun et al [11] have used density functional theory to propose a 2D MOF-based on molybdenum for NRR. With highly ordered structure and exposed metal active sites, the Mo-based MOF could exhibit an excellent catalytic performance for the conversion of N 2 into NH 3 at room temperature with a very low overpotential of 0.18 V. Further, Wu et al [20] have demonstrated copper porphyrin metal-organic framework nanosheets as highly selective and efficient electrocatalysts for the electroreduction of CO 2 to formate and acetate (CO 2 RR), with a maximum faradaic efficiency of 61.5% and 12.3% respectively.…”