A Rootless Duckweed-Inspired Flexible Artificial Leaf from Plasmonic Photocatalysts.

Abstract

The naturally existing leaves are ubiquitous two-dimensional flexible solar-to-chemical conversion systems that can run continuously in a sustainable manner. However, the current artificial photocatalytic systems are unable to achieve this due to the grand challenge in integrating existing photocatalysts in a flexible layout with high conversion efficiency and the ability to function independently. Here, we report on a rootless duckweed-inspired artificial leaf based on a lightweight, flexible, Janus plasmonic nanosheet-integrated sponge. The Janus plasmonic catalytically active nanosheet was made from self-assembled gold nanocube nanoassemblies grown on the porous sponges, which were further coated with an ultrathin palladium layer on one side via a ligand symmetry-breaking method. This sponge-based photocatalytic system is lightweight yet able to float on a water surface and conducts the gas-liquid reaction without auxiliary pumping and mixing devices. In a model reaction of 4-nitrophenol reduction, this floating leaf could achieve 2.5-fold and 65-fold higher efficiency than the corresponding dispersion and precipitation systems, respectively. The film theory is used to explain the sponge-based lightweight solar-to-chemical conversion system in a detailed kinetic and thermodynamic analysis, including the reaction rate constant, activation energy, enthalpy, entropy, Gibbs energy, and equilibrium constant.