Abstract
Solar-driven water splitting using powdered catalysts is considered as the most economical means for hydrogen generation. However, four-electron-driven oxidation half-reaction showing slow kinetics, accompanying with insufficient light absorption and rapid carrier combination in photocatalysts leads to low solar-to-hydrogen energy conversion efficiency. Here, we report amorphous cobalt phosphide (Co-P)-supported black phosphorus nanosheets employed as photocatalysts can simultaneously address these issues. The nanosheets exhibit robust hydrogen evolution from pure water (pH = 6.8) without bias and hole scavengers, achieving an apparent quantum efficiency of 42.55% at 430 nm and energy conversion efficiency of over 5.4% at 353 K. This photocatalytic activity is attributed to extremely efficient utilization of solar energy (~75% of solar energy) by black phosphorus nanosheets and high-carrier separation efficiency by amorphous Co-P. The hybrid material design realizes efficient solar-to-chemical energy conversion in suspension, demonstrating the potential of black phosphorus-based materials as catalysts for solar hydrogen production.
Highlights
Solar-driven water splitting using powdered catalysts is considered as the most economical means for hydrogen generation
Amorphous cobalt phosphide (Co-P) nanoparticles are supported on the few-layer black phosphorus (BP) nanosheets via the same procedure but using Co (NO3)2·6H2O as raw material
Layered red phosphorus is formed initially via the conversion of white phosphorus at room temperature with the assistance of ethylenediamine, which is revealed by Raman and transmission electron microscopy (TEM) characterizations (Supplementary Fig. 1)
Summary
Solar-driven water splitting using powdered catalysts is considered as the most economical means for hydrogen generation. The nanosheets exhibit robust hydrogen evolution from pure water (pH = 6.8) without bias and hole scavengers, achieving an apparent quantum efficiency of 42.55% at 430 nm and energy conversion efficiency of over 5.4% at 353 K This photocatalytic activity is attributed to extremely efficient utilization of solar energy (~75% of solar energy) by black phosphorus nanosheets and high-carrier separation efficiency by amorphous Co-P. As one of phosphorus allotropes, black phosphorus (BP) is a fascinating two-dimensional material, consisting of corrugated planes of phosphorus atoms with strong intralayer bonding and weak interlayer interactions and showing thickness-tunable bandgap from 0.46 to 1.51 eV, as well as highly free-carrier mobility[19] These unique properties render few-layer BP nanosheets promising as photocatalyst for hydrogen production. Lack of wet-chemical approach toward the preparation of few-layer BP nanosheets, is restricting the further development of BP-based materials as photocatalysts for water splitting[22,23]
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