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Photo-rechargeable batteries based on photocathodes that have the dual function of collecting and storing solar energy offer an efficient method for solar energy utilization. Herein, NiCo-layered double hydroxides (NiCo-LDH)/ZnIn2S4/carbon nanotubes (CNTs) (recorded as CZN), a heterostructure photocathode, has been synthesized by layer-by-layer growth for photo-driven rechargeable aqueous zinc batteries (AZBs). The proposed photocathode exhibits typical photoelectric properties and offers the following advantages: good photoresponse in the visible light range, energy level/potential matching between ZnIn2S4 and NiCo-LDH, and the conductive network formed by CNTs to promote charge transfer. The photo-driven rechargeable AZBs can harvest solar energy and store charge simultaneously, showing enhanced energy storage capability under illumination. The discharge capacity reaches 274.8 mAh·g−1 with a high photo-conversion efficiency of 1.120% at 8.0 A·g−1 (100 mW·cm−2, white light). In particular, the photo-driven rechargeable AZBs can be charged by light solely, achieving a discharge capacity of 116.3 mAh·g−1. This study shows that the novel design and synthesis of the heterostructure photocathode is crucial and significant to enhancing the practicality of solar energy.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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