Robust Tunnel TaO <sub>x</sub> Passivating Interlayer Enables Long‐Term Solar Water Oxidation
Silicon-based photoelectrochemical (PEC) cells offer significant advantages for solar-to-clean fuel conversion but face challenges such as surface recombination and poor stability, necessitating a comprehensive understanding of device failure mechanisms and effective mitigation strategies. Using nickel-decorated n-type silicon (n-Si/Ni) as a model photoelectrode, we demonstrate that surface restructuring during operation initially passivates surface recombination but eventually blocks photogenerated hole transfer, leading to device failure. To mitigate this challenge, an ultrathin (<1 nm) tantalum oxide (TaO<sub>x</sub>) interlayer is introduced via atomic layer deposition (ALD). This TaO<sub>x</sub> layer serves as both a passivating contact and a corrosion-resistant coating. The n-Si/TaO<sub>x</sub>/Ni electrode achieves an increased photovoltage from 150 to 500 mV during the activation process, and then significantly extends the device lifespan, maintaining over 90% performance for 500 h in 1 M KOH at 1.52 V versus RHE. These results highlight the implementation of amorphous TaO<sub>x</sub> in enhancing both the efficiency and durability of silicon-based PEC systems, providing a simultaneously passivating and protective strategy for solar-to-fuel conversion technologies under harsh conditions.
Authors
- Wangxi Liu (ORCID: https://orcid.org/0000-0002-4592-5061)
- Zhigang Zou (ORCID: https://orcid.org/0000-0003-2092-8335)
- Jia-Cheng Jian (ORCID: https://orcid.org/0000-0002-6277-6088)
- Bin Gao (ORCID: https://orcid.org/0000-0003-3769-0191)
- Zhaosheng Li (ORCID: https://orcid.org/0000-0001-8114-0432)
- Zengguang Huang (ORCID: https://orcid.org/0000-0001-9903-3504)
- Jianyong Feng (ORCID: https://orcid.org/0000-0003-4275-8306)
- Yu Zhu (ORCID: https://orcid.org/0000-0002-0339-8283)
- Huiting Huang (ORCID: https://orcid.org/0000-0001-7906-6122)
- Yu Tao (ORCID: https://orcid.org/0000-0003-3768-4250)
- Huihui Yan (ORCID: https://orcid.org/0009-0002-1946-4190)
- Changhao Liu (ORCID: https://orcid.org/0009-0005-8149-1351)
- Yuanqi Wang (ORCID: https://orcid.org/0000-0003-3408-302X)
- Lijuan Zhang (ORCID: https://orcid.org/0000-0002-9076-1000)
Institutions
- Nanjing Tech University (CN)
- Hankou University (CN)
- Nanjing University of Science and Technology (CN)
- Collaborative Innovation Center of Advanced Microstructures (CN)
- Ocean University of China (CN)
- Nanjing University (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-04-17
- DOI
- https://doi.org/10.1002/anie.202506326
- Citations
- 3
- Primary Topic
- Semiconductor materials and devices
- Type
- article
- Field-Weighted Citation Impact
- 2.19
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Government of Jiangsu Province
- Natural Science Foundation of Jiangsu Province
- National Key Research and Development Program of China
- National Science Fund for Distinguished Young Scholars