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

Abundant and toxic hydrogen sulfide (H 2 S) from industry and nature has been traditionally considered a liability. However, it represents a potential resource if valuable H 2 and elemental sulfur can be simultaneously extracted through a H 2 S splitting reaction. Herein a photochemical‐chemical loop linked by redox couples such as Fe 2+ /Fe 3+ and I − /I 3 − for photoelectrochemical H 2 production and H 2 S chemical absorption redox reactions are reported. Using functionalized Si as photoelectrodes, H 2 S was successfully split into elemental sulfur and H 2 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 H 2 S into valuable resources, but also sheds light on some challenging photochemical reactions such as CH 4 activation and CO 2 reduction.