Two-dimensional MOF-derived porous nanosheets dotted with in-situ MgO/ carbon heterostructure achieving striking performance in H2S catalytic oxidation at room temperature

H2S catalytic oxidation at room temperature is a promising scheme to satisfy industrial and environmental requirements. Herein, 2D magnesium-based MOF nanosheets were controllably synthesized through a facile bottom-up solvothermal method using PVP as a structure-directing agent. Further, in-situ omasum-like MOFderived porous nanosheets dotted with MgO/C heterostructures were obtained via one-step self-templating pyrolysis to avoid random blockage to porosity. The two-dimensional character endows the catalyst with fully exposed active sites and abundant interlayers to achieve ultrahigh activity and capacity with an unprecedented performance of 11.2 g H2S/g. DFT calculations reveal a lower barrier from 3O2 to 1O2 on defect carbon than that on pristine and hydrogen-saturated graphene. Ions and electrons may migrate directionally through the water film and the carbon substrate, respectively, constituting numerous circuits for rapid redox reactions. The advantages of in-situ-type catalysts are innovatively emphasized, and a potential guide to the rational design of catalysts is provided.