Abstract
Herein, we report a three-dimensional porous TiO2/Fe2TiO5/Fe2O3 (TFF) inverse opal through in situ thermal solid reactions for photoelectrochemical water splitting. The Fe2TiO5 interfacial layer within TFF acting as a bridge to tightly connect to TiO2 and Fe2O3 reduces the interfacial charge transfer resistance, and suppresses the bulk carrier recombination. The optimized TFF displays a remarkable photocurrent density of 0.54 mA cm−2 at 1.23 V vs. reversible hydrogen electrode (RHE), which is 25 times higher than that of TiO2/Fe2O3 (TF) inverse opal (0.02 mA cm−2 at 1.23 V vs. RHE). The charge transfer rate in TFF inverse opal is 2–8 times higher than that of TF in the potential range of 0.7 −1.5 V vs. RHE. The effects of the Fe2TiO5 interfacial layer are further revealed by X-ray absorption spectroscopy and intensity-modulated photocurrent spectroscopy. This work offers an interfacial engineering protocol to improve charge separation and transfer for efficient solar water splitting.
摘要
活性材料中的载流子转移是太阳能高效利用的一大挑战. 本文 通过固相反应原位制备了三维多孔TiO2/Fe2TiO5/Fe2O3 (TFF)反蛋白石 结构, 用于光电化学分解水. Fe2TiO5作为桥接层与TiO2和Fe2O3紧密相 连, 降低了界面电荷转移电阻, 抑制了体相载流子复合. 优化后的TFF在 1.23 V(相对于可逆氢电极)的光电流密度为0.54 mA cm−2, 是TiO2/Fe2O3 (TF)反蛋白石结构(0.02 mA cm−2)的25倍. 在偏压范围为0.7−1.5 V(相 对于可逆氢电极)时, TFF光阳极的电荷转移速率是TF的2−8倍. 此外, 我们通过X射线吸收光谱和强度调制光电流光谱进一步探索了Fe2TiO5 对界面电荷传输动力学的影响. 该工作为揭示界面工程对光生电荷分 离和转移的调控作用, 设计开发高效的界面异质结构光电极提供了一 种新策略.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (21771001 and 51872002), Anhui Provincial Natural Science Foundation (1708085ME120), the Program of Anhui Scientific and Technical Leaders Reserve Candidates (2018RH168), the Scholar Program for the Outstanding Innovative Talent of College Discipline (Specialty), and the doctoral start-up fund and open fund for Discipline Construction, Institute of Physical Science and Information Technology, Anhui University.
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Zhang M, Liu P, Tan H and Li S designed the research; Zhang M, Liu P, Zhang H, Huang F, Zhang K and Li S synthesized the samples, performed the current-potential curve, XRD, UV-vis spectra, SEM and IPCE measurements; all authors discussed the results and co-wrote the paper.
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Miaomiao Zhang received her BSc degree in applied chemistry from Anhui Jianzhu University. She is currently pursuing her MSc degree at Anhui University under the supervision of Prof. Shikuo Li. Her research focuses on the interfacial catalysis.
Pianpian Liu obtained her BSc degree in chemical engineering and technology from Huainan Normal College. Then she joined Anhui University and conducted research under the supervision of Prof. Shikuo Li. Her research interest is designing porous nanostructures for investigating interfacial catalysis.
Shikuo Li received his BSc degree from Anhui University in 2004, and PhD degree from the University of Science and Technology of China in 2017. He joined the Department of Chemistry at the University of Pittsburgh as a visiting scholar in 2018. Since Dec 2020, he has been a full professor of materials science and chemistry at the School of Chemistry and Chemical Engineering, Anhui University. His current research interest is developing novel nanostructures for photoelectrochemistry.
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The authors declare that they have no conflict of interest.
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Zhang, M., Liu, P., Tan, H. et al. Engineering the heterogeneous interfaces of inverse opals to boost charge transfer for efficient solar water splitting. Sci. China Mater. 65, 124–130 (2022). https://doi.org/10.1007/s40843-021-1725-2
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DOI: https://doi.org/10.1007/s40843-021-1725-2