H. Miao, Chengyang Feng, Jumanah Alharbi, Shouwei Zuo, Viko Ladelta, Ghassan S. Alshehry, Khalid Ruwaili, Hassan S. Al Qahtani, Deyan Luan, Wan‐Lu Li, Nikos Hadjichristidis, Huabin Zhang
Although polylactic acid is a promising biodegradable plastic, its slow degradation under natural conditions, microplastic formation, and CO2 emissions during decomposition undermine its sustainability. Photoreforming offers a promising strategy for polylactic acid conversion; however, current methods suffer from sluggish kinetics and low selectivity. Here, we design a Ni single-atom catalyst anchored on CdS (Ni/CdS) to enable alkali-free photoreforming of real polylactic acid plastic waste under mild conditions. Ni single atom sites facilitate sequential cleavage of α-OH and Cα-H bonds, enabling efficient H2 evolution and significantly improving the yield and selectivity of polylactic acid conversion to H2 and pyruvic acid, achieving an apparent quantum efficiency of 46%. Furthermore, we successfully scaled up the synthesis of Ni/CdS and implemented a square-meter-scale reaction system, demonstrating stable outdoor photoreforming of real polylactic acid plastic waste under sunlight. This work paves a promising pathway for solar-driven upcycling of polylactic acid plastic waste. A Ni single-atom catalyst on CdS efficiently converts polylactic acid bioplastic into hydrogen and valuable chemicals using sunlight, offering a sustainable strategy for bioplastic waste recycling.