An Integrated Photoelectrochemical–Chemical Loop for Solar‐Driven Overall Splitting of Hydrogen Sulfide

Abundant and toxic hydrogen sulfide (H2 S) from industry and nature has been traditionally considered a liability. However, it represents a potential resource if valuable H2 and elemental sulfur can be simultaneously extracted through a H2 S splitting reaction. Herein a photochemical-chemical loop linked by redox couples such as Fe(2+) /Fe(3+) and I(-) /I3 (-) for photoelectrochemical H2 production and H2 S chemical absorption redox reactions are reported. Using functionalized Si as photoelectrodes, H2 S was successfully split into elemental sulfur and H2 with high stability and selectivity under simulated solar light. This new conceptual design will not only provide a possible route for using solar energy to convert H2 S into valuable resources, but also sheds light on some challenging photochemical reactions such as CH4 activation and CO2 reduction.