Spinodal decomposition enables coherent plasmonic metal/semiconductor heterostructure for full spectrum photocatalysis

Lisha Lu, Muhua Sun, Aomiao Zhi, Hao Ling, Yingying Lan, Hongbo Han, Jianlin Wang, Xiaowei Zhang, Yu Zhao, Meiyun Li, Lejuan Cai, Xiaomin Li, Xuedong Bai and Wenlong Wang ()
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Lisha Lu: Chinese Academy of Sciences
Muhua Sun: Tsinghua University
Aomiao Zhi: Chinese Academy of Sciences
Hao Ling: Chinese Academy of Sciences
Yingying Lan: Songshan Lake Materials Laboratory
Hongbo Han: Chinese Academy of Sciences
Jianlin Wang: Chinese Academy of Sciences
Xiaowei Zhang: Chinese Academy of Sciences
Yu Zhao: Chinese Academy of Sciences
Meiyun Li: Chinese Academy of Sciences
Lejuan Cai: Songshan Lake Materials Laboratory
Xiaomin Li: Chinese Academy of Sciences
Xuedong Bai: Chinese Academy of Sciences
Wenlong Wang: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Nanoscale metal/semiconductor heterostructures are critical components for a variety of light energy conversion applications. Herein, with plasmonic hafnium nitride (HfN) as a model system, we show that spinodal decomposition can be exploited as a unique means to produce the lattice-coherent metal/semiconductor heterostructure between HfN and its native oxynitride semiconductor—Hf2ON2. Atomic-resolution electron microscopy imaging provides direct visualization of the complete lattice coherency over the interface region with precisely controlled spatial modulation. The light-harvesting HfN component exhibits a broadband plasmonic absorption covering visible and near-infrared regions, and the plasmonically excited hot electrons can be efficiently injected into neighboring Hf2ON2 across interface. When combined with a small amount of Pt co-catalyst, the coherent HfN/Hf2ON2 heterostructure achieves high-efficiency photocatalytic H2 production from methanol decomposition under visible and NIR light illumination, with apparent quantum yields of 27% at 600 nm and 13.9% at 850 nm, respectively. This performance contributes to the efficient utilization of a broad solar spectrum in photocatalysis and solar energy conversion applications.

Date: 2025
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DOI: 10.1038/s41467-025-61872-1

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