Designing sulfide catalysts for H2S dissociation to H2 based on reaction descriptors and microkinetics

Molybdenum disulfide (MoS 2 ) is a promising catalyst for the challenging transformation of hydrogen sulfide (H 2 S) into sulfur and hydrogen (H 2 ). However, a detailed understanding of its structure-function correlation still needs to be provided. We used density functional theory calculations to extract relevant reaction indexes (binding energies and free energy barriers) over different MoS 2 surfaces. We used these indexes as inspiration in developing new catalysts and a microkinetic model to compare the results, extracting insights into the reaction mechanisms and surface coverages. The turnover frequencies obtained experimentally and through microkinetic modeling are analogous, validating our approach. The findings pave the way for developing more efficient H 2 S decomposition catalysts and establish a descriptor-based design for other metal sulfide catalysts. • Ab initio calculations provide H2S to H2 reaction descriptors. • These reaction descriptors are used to design and synthesize MoS2 catalysts. • Microkinetic modeling validated experimental turnover frequencies. • The 2 H phase of MoS2, particularly S-edge sites, exhibited the best performance. • VS2 and NbS2 are potential candidates for H2S dissociation based on descriptors.