Low Temperature Catalytic Decomposition of Hydrogen Sulfide into Hydrogen and Diatomic Gaseous Sulfur

摘要

A new catalytic reaction of hydrogen sulfide decomposition is discovered, the reaction occurs on metal catalysts in gas phase according to equation 2H2S <->2H2 + S_2~((gas)) to produce hydrogen and gaseous diatomic sulfur, conversion of hydrogen sulfide at room temperature is close to 15 %. The thermodynamic driving force of the reaction is the formation of the chemical sulfur-sulfur bond between two hydrogen sulfide molecules adsorbed on two adjacent metal atoms in the key surface intermediate and elimination of hydrogen into gas phase. "Fingerprints" of diatomic sulfur adsorbed on the solid surfaces and dissolved in different solvents are studied. In closed vessels in adsorbed or dissolved states, this molecule is stable for a long period of time (weeks). A possible electronic structure of diatomic gaseous sulfur in the singlet state is considered. According to DFT/CASSCF calculations, energy of the singlet state of S2 molecule is over the triplet ground state energy for 10.4/ 14.4 kcal/mol. Some properties of gaseous diatomic sulfur are also investigated. Catalytic solid systems, both bulk and supported on porous carriers, are developed. When hydrogen sulfide is passing through the solid catalyst immersed in liquid solvent which is capable of dissolving sulfur generated, conversion of hydrogen sulfide at room temperature achieves 100 %, producing hydrogen in gas phase. This gives grounds to consider hydrogen sulfide as inexhaustible potential source of hydrogen—a very valuable chemical reagent and environmentally friendly energy product.