Enhanced Charge\nTransfer Dynamics in a NiCo<sub>2</sub>S<sub>4</sub>–Zn<sub><i>x</i></sub>Cd<sub>1–<i>x</i></sub>S\nPhotothermal Catalyst for Efficient Photoreforming\nof Waste

The green circular utilization of waste plastics is crucial\nfor\nenvironmental protection. Converting waste plastics into H<sub>2</sub> fuel and valuable chemicals by utilization of the solar spectrum\nis highly attractive. Herein, a photothermal catalyst composed of\nmetallic NiCo<sub>2</sub>S<sub>4</sub> and semiconductor Zn<sub><i>x</i></sub>Cd<sub>1–<i>x</i></sub>S (NCS–ZCS)\nmaterials is rationally designed. The photogenerated electrons are\nshown to flow from Zn<sub><i>x</i></sub>Cd<sub>1–<i>x</i></sub>S to NiCo<sub>2</sub>S<sub>4</sub> and are excited\ninto hot electrons via the localized surface plasmon resonance effect,\npromoting H<sub>2</sub> evolution. The holes on Zn<sub><i>x</i></sub>Cd<sub>1–<i>x</i></sub>S serve as the oxidation\nactive species for efficiently converting waste plastic into value-added\nchemicals. Systematic studies show that the photoreforming process\ncan be enhanced with a photothermal effect from NiCo<sub>2</sub>S<sub>4</sub>. Theoretical calculations confirmed experimental results.\nUnder visible to infrared irradiation, H<sub>2</sub> evolution rates\nof 57.0 and 106.0 mmol·g<sub>cat</sub><sup>–1</sup>·h<sup>–1</sup> along with the yields of value-added chemicals of\n39.18 and 206.05 μmol mL<sup>–1</sup> in polyethylene\nterephthalate and polylactic acid substrates are achieved.