Tuning the adsorption and interaction of CO and O₂ on graphene-like BC₃-supported non-noble metal atoms

Abstract

Research into suitable substrate-supported single-atom catalysts has become a major challenge for electrochemical sensors and energy devices. Firstly, we investigate the adsorption properties of metal atoms (MA = Fe, Co, Ni, Cu and Al) on pristine and defective BC3 sheets through using first-principles calculations. It is found that the MA-doped BC3 configurations (MA-BC3) are quite stable at high temperature and the positively charged MAs as surface active sites can effectively regulate the stability of reactive gases. Secondly, the adsorption of individual O2 molecules is more stable than that of CO molecules, which can modify the electronic and magnetic properties of MA-BC3 systems. Moreover, the possible reaction processes of CO oxidation on the Fe-BC3 substrate are comparably analyzed through the Eley-Rideal (ER) and Langmuir-Hinshelwood (LH) mechanisms. In the LH mechanism, the coadsorbed O2 and CO as starting materials start to form an OOCO complex with a smaller energy barrier (0.38 eV), which is an energetically more favorable process than that of the OOCO (0.65 eV) or CO3 complex (0.42 eV) formed through ER mechanisms. This result indicates that the functionalized MA-BC3 sheets have low cost and high activity.

Computational screening of defective BC3-supported single-atom catalysts for electrochemical CO2 reduction

“…The C-C and C-B bond lengths of the BC 3 monolayer are 1.42 Å and 1.56 Å, and the calculated band gap based on the PBE level is 0.63 eV. As summarized in Table S1 (ESI †), the structural parameters and band gap calculated in our work are consistent with previously reported theoretical 86,87,100 and experimental 101 studies.…”

Inorganic molecule (O2, NO) adsorption on nitrogen- and phosphorus-doped MoS2 monolayer using first principle calculations

“…On the other hand, the adsorption energy is appreciably large compared to that in the case of O 2 molecule adsorption on N-doped graphene and BC3 graphene-like sheet doped with metal atoms. [41][42][43][44][45][46][47][48] Next, we observed the adsorption of two oxygen molecules on the 2N-MoS 2 monolayer, where two N atoms were doped afar to avoid interaction with the O 2 gas molecules. Fig.…”

Spontaneous DNA translocation through a van der Waals heterostructure nanopore for single-molecule detection

“…27,28 The significantly high stability, thermal conductivity and carrier mobility of BC 3 and C 3 N, especially their matching lattice [29][30][31] , make them qualified candidates to build the vdW heterostructures. 29,[31][32][33] A theoretical work has proposed the optoelectronic application of BC 3 /C 3 N vdW heterostructure. 34 Due to the different electronegativity of the boron, carbon and nitrogen atoms, there are intrinsic electron transfers in the BC 3 and C 3 N monolayers.…”