Photo-electroactive p-n heterojunction catalyst with dual Co sites for high-performance light-enhanced zinc–air batteries

作者：Tuo Lu, Nengneng Xu, Benji Zhou, Liyuan Guo, Xiaodan Wen, Shuaifeng Lou, Guicheng Liu, Woochul Yang, Nianjun Yang, Momo Safari, Haitao Huang, Jinli Qiao · 发表于：eScience · 年份：2025 · DOI：10.1016/j.esci.2025.100450 · 被引用次数：19 · 研究领域：Electrocatalysts for Energy Conversion、Advanced Photocatalysis Techniques、Advanced battery technologies research

Highly electrocatalytic and durable Co-Nx-C frameworks containing carbon nanofibers (CNFs)/carbon nitrides (CNs) are vital materials for rechargeable zinc–air batteries (RZABs). However, the existing Co-Nx-C frameworks experience severe agglomeration during synthesis and limited active site accessibility/mechanical robustness. In this work, a photo-enhanced bifunctional catalyst with a type II p-n heterojunction (g–C 3 N 4 –Co@CNT/Co–N 4 /C@CNF) is achieved through a combined “electrospinning + calcination + ball milling” approach. The composite integrates graphitic carbon nitride (g-C 3 N 4 ) nanosheets with dual active Co sites (nanoparticles and Co–N 4 single atoms) anchored on conductive carbon nanofibers. This architecture enables efficient charge separation, enhanced light absorption, and accelerated oxygen redox kinetics. DFT calculations reveal that g-C 3 N 4 modulates the electronic structure and lowers the reaction free-energy barriers, leading the d-band center closer to the Fermi level. Under light irradiation, the g–C 3 N 4 –Co@CNT/Co–N 4 /C@CNF exhibits outstanding ORR/OER catalytic performance, with a small overpotential gap of 0.684 V (E 1/2 = 0.930 V, E j:10 = 1.614 V). In practical application: 1) light-enhanced liquid ZABs with g–C 3 N 4 –Co@CNT/Co–N 4 /C@CNF photoactive catalysts manifest a peak power density of 310 mW cm −2 and a long cycle life exceeding 1100 h. 2) Light-enhanced flexible ZABs also can reach a peak power density of 96 mW cm −2 and tolera...