Selective Oxidation of H2S via P and Transition-Metal Dual Sites on Polymeric Carbon Nitride
Yu Huang1, Huanglan Xue1, Yi Li1,2
1State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, P.R. China.
Abstract:
The development of catalysts featuring high-density active sites and superior stability is critical for achieving efficient and selective H2S oxidation. This study systematically investigates the catalytic performance and reaction mechanisms of transition metal-embedded phosphorus-doped carbon nitride catalysts (i.e., TM-P@melon, TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn) for H2S oxidation using density functional theory calculations. Our calculations identified FeN4-P@melon and MnN4-P@melon as the most promising candidates, with Gibbs free energy changes (ΔG) of -0.24 eV and 0.07 eV for the potential-determining step in the selective oxidation of H2S to elemental sulfur, respectively. Anchored TM and P atoms act synergistically to narrow the melon-CN band gap and enhance O2 adsorption/activation, thereby boosting the catalytic reaction. This work provides fundamental theoretical insights for designing highly efficient and selective H2S oxidation catalysts while elucidating the atomic-level mechanisms governing the catalytic process.
More Related Videos
Related Concept Videos
02:24Reduction of Alkynes to cis-Alkenes: Catalytic Hydrogenation
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
02:17Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
02:50Catalysis
02:13Reduction of Alkenes: Catalytic Hydrogenation
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
02:36Regioselectivity and Stereochemistry of Hydroboration
Hydroboration proceeds in a concerted fashion with the attack of borane on the π bond, giving a cyclic four-centered transition state. The –BH2 group is bonded to the less substituted carbon and –H to the more substituted carbon. The concerted nature requires the simultaneous addition of –H and –BH2 across the same face of the alkene giving syn stereochemistry.
02:44Oxidation of Alkenes: Syn Dihydroxylation with Osmium Tetraoxide