Strain effect on the catalytic activities of B- and B/N-doped black phosphorene for electrochemical conversion of CO to valuable chemicals

Abstract

Designed metal-free electrocatalysts combined with compressive strain can efficiently convert CO to valuable chemicals and fuels.

In silico design of dual-doped nitrogenated graphene (C2N) employed in electrocatalytic reduction of carbon monoxide to ethylene

“…The hydrogen evolution reaction (HER) is often considered to be a key competing reaction to the CORR and results in low faradaic efficiency. 13 The hydrogen adsorption free energy (Δ G H ) is an effective descriptor for predicting the activity of catalysts. Hence, as the free energy, Δ G (*H), approaches zero, a higher catalytic HER activity is observed.…”

“…Besides being an abundant and low-cost feedstock, CO is also considered as the most important component in the reduction of CO 2 to valuable products such as ethanol 11 and ethane. 12,13 Experimental observations 14,15 present evidence that the CO reduction reaction (CORR) delivers similar overpotentials and product distributions to those of the CO 2 RR. 16 As an abundant and cheap carbon feedstock, CO exists in nature or can be facilely produced from various carbon-containing resources including coal, natural gas, biomass, or organic wastes.…”

“…2D materials provide numerous anchoring sites for active atoms, and have attracted great attention. 63 The introduction of atomically dispersed metal-free B atoms led to superior C 2 faradaic efficiency in recent studies, and was reported to promote the electro(photo)-catalytic hydrogenation of nitrogen 36–38 and CO. 13,39 Note that the catalyst contained multiple reactive sites which would be beneficial for carbon–carbon (C–C) coupling, which is the first step in the CORR toward the formation of multi-carbon products. Studies on atom pair-doped catalysts containing metal-free atoms have been reported, and have demonstrated their immense potential for practical applications.…”

The Influence of Single-Atom Fe2+/3+N4 Spin State on the Electroreduction of CO2 to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

“…11 However, the configurations of *HCOO and *HCOOH intermediates with Fe as the adsorbed site are more favorable in energy relative to other binding sites. This phenomenon was attributed to strong electrostatic interactions between positively charged Fe ions in 52,55 The N sites have more negative charge than the neighboring C sites, indicating the exposed N site prefers to accept a proton from the electrolyte solution rather than the neighboring C sites. Additionally, the adsorption energy between the hydrogen atom (H atom) and the N or C site is in the range of −1.03 to −2.17 eV, which strongly supports the formation of the N−H/ C-H bond on the surface of Fe II N 4 C. Therefore, the N or C site is the lower catalytic activity for HER because the site with high catalytic activity requires a low H adsorption energy (or near zero).…”

Strain Modulation of Black Phosphorene for the Hydrogen Evolution Reaction Activity

“…[ 40 ] Also, the compressive strain applying to the B doped and B—N codoped 2D black phosphorene can effectively enhanced the catalytic activity for CO reaction. [ 41 ] A proper tensile strain makes the intrinsic inertia of divacancies phosphorene catalytically active of HER. [ 30 ] In particular, Lu et al expressed that straining and metal doping can improve the HER activity of phosphorene by adjusting the electron distribution.…”