Theoretical prediction of graphene-based single-atom iron as a novel catalyst for catalytic oxidation of Hg0 by O2

Design of Single-Atom Catalysts for Hg0 Oxidation Using H2O2

“…To further investigate the bonding mechanism of Zn 1 –N 4 –C with oxidation products, we obtained information on the Zn–O bond by COHP (Crystal Orbital Hamilton Population) analysis. Compared to our previous study of Fe 1 –N 4 –C, there is antibonding orbital occupation in the bond of O ( p )–Zn ( d ), as shown in Figure e,f. It indicates that the O–Zn bond connecting the Hg­(OH) 2 to Zn 1 –N 4 –C is unstable, making Hg­(OH) 2 extremely easy to desorb.…”

“…Other reports 9,10 analyzed catalytic Hg 0 oxidation on graphene-based Pt SACs using O 2 ; they showed that the Pt/3N-GN catalyst had excellent catalytic activity for catalytic Hg 0 oxidation, with a rate-determining step (RDS) barrier of 2.016 eV. Yang et al 11,12 used a combined theoretical and experimental method to analyze the reaction mechanism of Fe SACs for the catalytic Hg 0 oxidation using O 2 ; they found that Fe SA /DV-N 4 has the highest catalytic activity, with an RDS energy barrier of 2.34 eV. Our previous study 13 predicted the catalytic activity of 3d, 4d, and 5d metal SACs (in the form of metal 1 −N 4 −C) for catalytic Hg 0 oxidation by the derived volcano activity plots; the results showed that Fe 1 −N 4 −C has the highest catalytic activity.…”

Understanding trends in the mercury oxidation activity of single-atom catalysts

“…Other reports 31,32 analyzed catalytic oxidation of Hg 0 on g-C 3 N 4 supported single TMs and Fe/Co/Ni-based bi-metallic catalysts using O 2 in coal-fired flue gas; they showed that Nig-C 3 N 4 and Ni 2 @g-C 3 N 4 had promising catalytic efficiencies for Hg 0 oxidation. Theoretically, 33,34 Fe-based SACs also showed high catalytic activities in Hg 0 oxidation. In a very recent study, 35 experiments for the first time unrevealed the outstanding catalytic performance of Fe SACs in Hg 0 oxidation.…”

“…(HgO) 2 can be divided into (HgO) 2 -chain and (HgO) 2 -ring according to different atomic arrangements. Previous research 34 showed that (HgO) 2 -chain has the lowest energy, which can be formed by the reaction of two mercury oxide molecules by releasing an energy of Environmental Science: Nano Paper 2.31 eV. (HgO) 2 -Chain has the highest thermodynamic stability among these three structures, which is consistent with the research of Tossell et al 51 Therefore, (HgO) 2 -chain was selected as the final product of the reaction in our analysis.…”

Excellent room temperature catalytic activity for formaldehyde oxidation on a single-atom iron catalyst in a moist atmosphere

“…27 In addition, SACs also have application potential in volatile organic compound incineration and degradation of toluene. 28,29 Similarly, SACs exhibit excellent properties in the field of catalytic oxidation: Fe SA shows high catalytic activity for the catalysis of benzene, 30 methane, 31 and mercury 32 at room temperature. Reactants have a lower energy barrier for catalytic oxidation or may create reaction-promoting free radicals on the surface of SACs, which is beyond the reach of conventional catalysts.…”