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MXene-Derived Highly Oriented TiN Enables Ta3N5 Photoanodes for Transmission-Mode Bias-Free Solar Water Splitting
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DOI：10.1002/aenm.71412.png)
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Abstract
En 中文
The incompatibility between optical transparency and photocarrier extraction in Ta3N5 photoanodes, arising from the harsh ammonolysis process, has constrained their potential for bias-free water splitting, despite intrinsically ideal band structures. Here, we report a transparent and nitridation-compatible bottom electrode based on 2D MXene-derived TiN thin films. The (111)-preferred orientation of MXene-derived TiN facilitates efficient electron extraction from Ta3N5, while maintaining high optical transmittance at an ultrathin thickness. By integrating with n-GaN, we design a heterostructured electron collector that further improves charge separation, corroborating the directional electron extraction in Ta3N5/TiN/n-GaN via photoelectron spectroscopy and carrier dynamics studies. The transparent photoanode generates a photocurrent density of 9.2 mA cm−2 at 1.23 V versus a reversible hydrogen electrode for water oxidation, also enabling transmission-mode bias-free solar water splitting. A triple-tandem photoelectrochemical device with optimized band gap matching achieves a solar-to-hydrogen conversion efficiency of 13.2%, approaching 83% of the theoretical limit of Ta3N5. This study opens up an unexplored interface engineering for carrier and light utilization in metal nitrides toward efficient solar hydrogen production.
Keywords:
bias-free water splitting
electron extraction
light harvesting
MXene
photoanode
photoelectrochemical
tantalum nitride
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