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Single Ti atoms coupled with Ti–O clusters enable low temperature hydrogen cycling by sodium alanate

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Abstract

Ti-based catalysts are known to improve the hydrogen storage performance of NaAlH4 by facilitating the dissociation/recombination of H–H and Al–H bonds. The catalytic activity of metallic Ti species strongly depends on its particle size and dispersity. Ti clusters and even single atoms are therefore highly desirable, but their controllable fabrication has been highly challenging. Herein, we demonstrate a novel facile sonochemical synthesis of a Ti–O clusters featuring single Ti atom catalyst at room temperature. Through reducing TiCl4 by MgBu2 with ultrasound instead of heating as driving force, numerous single Ti atoms coupled with Ti–O clusters with Ti loading on graphene (Ti1/Ti–O@G) up to 22.6 wt% have been successfully obtained. The prepared Ti1/Ti–O@G contributes high reactivity and superior catalytic activity, therefore enabling full dehydrogenation of NaAlH4 at 80 °C in thermogravimetric mode and re-hydrogenation at 30 °C and 10 MPa with 4.9 wt% H2. This fact indicates for the first time that single Ti atom catalyst with high loading is highly effective in catalyzing hydrogen cycling of NaAlH4 at remarkably reduced temperatures.

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摘要

众所周知，Ti基催化剂能够促进NaAlH4中H-H键和Al-H键的解离/重建，从而改善NaAlH4的储氢性能。由于Ti基催化剂的活性主要取决于其粒径大小和分散性，因此，减小Ti基催化剂的粒径至纳米团簇甚至单原子级别有望激发其高催化活性。但是，如何实现该类催化剂的可控制备一直是个大挑战。本文报道了一种在室温下通过超声化学合成制备具有Ti单原子和Ti–O团簇特性的Ti基催化剂的新方法。利用超声波作为反应驱动力引发MgBu2和TiCl4之间的氧化还原反应，避免高温加热，成功制备了石墨烯负载Ti单原子/Ti–O团簇耦合的Ti基催化剂（Ti1/Ti–O@G），其中Ti元素的负载量高达22.6 wt％。所制备的Ti1/Ti–O@G催化剂表现出优异的反应活性和催化活性，能够使NaAlH4在80 °C热重测试中完全放氢，放氢产物在30 °C和10 MPa H2条件下能够完全氢化。本研究首次阐明了提高Ti单原子催化剂的负载率能够有效降低NaAlH4材料的循环储氢温度。

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Acknowledgements

This study was financially supported by the National Outstanding Youth Foundation of China (No. 52125104), the Natural Science Foundation of Zhejiang Province (No. LD21E010002), the National Natural Science Foundation of China (Nos. 52071285 and 52001277), the Fundamental Research Funds for the Central Universities (Nos. 2021FZZX001-09 and 226-2022-00246), and the National Youth Top-Notch Talent Support Program.

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  1. Zhuang-He Ren and Xin Zhang have contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Silicon and Advanced Semiconductor Materials, Zhejiang University, Hangzhou, 310027, China

    Zhuang-He Ren, Xin Zhang, Wen-Xuan Zhang, Wen-Ping Sun, Ming-Xia Gao, Hong-Ge Pan & Yong-Feng Liu

  2. School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310058, China

    Zhuang-He Ren, Xin Zhang, Wen-Xuan Zhang, Wen-Ping Sun, Ming-Xia Gao, Hong-Ge Pan & Yong-Feng Liu

  3. School of Civil & Environmental Engineering, University of Technology Sydney, Sydney, 2007 NSW, Australia

    Zhen-Guo Huang & Li-Mei Yang

  4. Institute of Science and Technology for New Energy, Xi’an Technological University, Xi’an, 710021, China

    Ya-Xiong Yang, Zheng-Long Li, Hong-Ge Pan & Yong-Feng Liu

  5. College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, 310014, China

    Juan Li

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Ren, ZH., Zhang, X., Zhang, WX. et al. Single Ti atoms coupled with Ti–O clusters enable low temperature hydrogen cycling by sodium alanate. Rare Met. 43, 2671–2681 (2024). https://doi.org/10.1007/s12598-023-02608-2

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