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External-field-driven molecular polarization manipulates reactant interface toward efficient hydrogen evolution

外场驱动分子极化调控反应物界面及其电催化析氢 性能

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Abstract

The reaction interface which governs the electrocatalytic behavior is notoriously hard to understand due to inadequate regulatory and detection methods. By using on-chip microdevices, we employ variable back-gate voltages to generate molecular polarization and thus fine-tune the concentration of hydronium ions (H3O+) in electrochemical double layers for efficient hydrogen evolution. Taking C60/ MoS2 heterojunction as a prototype, electrical tests reveal that the back-gate promotes the charge transfer from C60 to MoS2, leading to the polarization of C60. In situ photoluminescence spectra verify that the polarized C60 can attract H3O+ to accumulate in the vicinity of MoS2 in the external electric field. Profiting from the back-gated H3O+ enrichment, the hydrogen evolution current is increased by five times at −0.45 VRHE when a 1.5-V back-gate voltage is applied. The insight into the reaction interface from manipulation to detection can facilitate diverse catalytic reactions.

摘要

反应物界面对电催化反应至关重要. 然而, 由于调控和表征手段 的不足, 对反应物界面的深入研究仍难以实现. 本文中, 我们借助单片 电催化微纳器件, 通过调节背栅电压引入分子极化, 实现了对电化学双 电层中水合氢离子(H3O+)浓度的调控, 进而提高了催化剂的电催化析 氢性能. 以C60/MoS2异质结为例, 电学性能测试表明背栅电场促进了电 子从C60向MoS2的转移, 并导致了C60分子的极化. 原位光致发光光谱表 征显示, 在背栅电场的作用下, 极化的C60分子会吸引H3O+, 使其聚集在 MoS2附**. 而电催化测试表明, 在1.5 V背栅电压下, 由于发生了H3O+的 富集, C60/MoS2异质结在−0.45 VRHE电位下的析氢电流密度增加了5倍. 我们提出的调控和监测反应物界面的方法能够促进对多种电催化反应 的研究.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (22071069 and 22275060). We also acknowledge technical support from the Analytical and Testing Center at Huazhong University of Science and Technology.

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Authors and Affiliations

  1. School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China

    Yang Zhao  (赵阳), Jiazhao Huang  (黄家钊), Jianqiang Chen  (陈建**), **aojuan Gan  (干晓娟), Qunlei Wen  (温群磊), Huang**gwei Li  (**黄经纬), Junyuan Duan  (段君元), Bowen Chen  (陈搏文), Tianyou Zhai  (翟天佑) & Youwen Liu  (刘友文)

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  1. Yang Zhao  (赵阳)
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  2. Jiazhao Huang  (黄家钊)
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  3. Jianqiang Chen  (陈建**)
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  4. **aojuan Gan  (干晓娟)
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  5. Qunlei Wen  (温群磊)
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  6. Huang**gwei Li  (**黄经纬)
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  7. Junyuan Duan  (段君元)
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  9. Tianyou Zhai  (翟天佑)
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  10. Youwen Liu  (刘友文)
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Contributions

Zhai T and Liu Y supervised the project. Zhao Y conducted all the experiments, during which Huang J, Chen J, Chen B, and Gan X gave some help. Wen Q, Li H and Duan J assisted Zhao Y in analyzing the data and solving problems. Zhao Y wrote the paper with the help of all coauthors.

Corresponding author

Correspondence to Youwen Liu  (刘友文).

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The authors declare that they have no conflict of interest.

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Supplementary information

Calculation details and supporting data are available in the online version of the paper.

Yang Zhao received his BS degree from Huazhong University of Science and Technology in 2020. He is currently a postgraduate at the School of Materials Science and Engineering under the supervision of Prof. Tianyou Zhai and Dr. Youwen Liu at Huazhong University of Science and Technology. His work focuses on on-chip electrocatalysis.

Youwen Liu received his BS degree from China University of Geosciences in 2012, and his PhD degree in inorganic chemistry from the University of Science and Technology of China in 2017. Then he joined the School of Materials Science and Engineering, Huazhong University of Science and Technology as an associate professor. His current research interests include the design, synthesis, and regulation of electrocatalytic materials.

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Zhao, Y., Huang, J., Chen, J. et al. External-field-driven molecular polarization manipulates reactant interface toward efficient hydrogen evolution. Sci. China Mater. 66, 3501–3508 (2023). https://doi.org/10.1007/s40843-023-2480-x

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