Decoupling light absorption and carrier transport via heterogeneous doping in Ta3N5 thin film photoanode

Yequan Xiao, Zeyu Fan, Mamiko Nakabayashi, Qiaoqiao Li, Liujiang Zhou, Qian Wang, Changli Li, Naoya Shibata, Kazunari Domen and Yanbo Li ()
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Yequan Xiao: University of Electronic Science and Technology of China
Zeyu Fan: University of Electronic Science and Technology of China
Mamiko Nakabayashi: The University of Tokyo
Qiaoqiao Li: University of Electronic Science and Technology of China
Liujiang Zhou: University of Electronic Science and Technology of China
Qian Wang: Nagoya University
Changli Li: Sun Yat‐sen University
Naoya Shibata: The University of Tokyo
Kazunari Domen: Office of University Professors, The University of Tokyo
Yanbo Li: University of Electronic Science and Technology of China

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract The trade-off between light absorption and carrier transport in semiconductor thin film photoelectrodes is a major limiting factor of their solar-to-hydrogen efficiency for photoelectrochemical water splitting. Herein, we develop a heterogeneous doping strategy that combines surface doping with bulk gradient doping to decouple light absorption and carrier transport in a thin film photoelectrode. Taking La and Mg doped Ta3N5 thin film photoanode as an example, enhanced light absorption is achieved by surface La doping through alleviating anisotropic optical absorption, while efficient carrier transport in the bulk is maintained by the gradient band structure induced by gradient Mg doping. Moreover, the homojunction formed between the La-doped layer and the gradient Mg-doped layer further promotes charge separation. As a result, the heterogeneously doped photoanode yields a half-cell solar-to-hydrogen conversion efficiency of 4.07%, which establishes Ta3N5 as a leading performer among visible‐light‐responsive photoanodes. The heterogeneous doping strategy could be extended to other semiconductor thin film light absorbers to break performance trade-offs by decoupling light absorption and carrier transport.

Date: 2022
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DOI: 10.1038/s41467-022-35538-1

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