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Heterostructured Co3O4–SnO2 composites containing oxygen vacancy with high activity and recyclability toward NH3BH3 dehydrogenation

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Abstract

Ammonia borane (NH3BH3, AB) has been regarded as a promising chemical hydrogen storage material owing to its high hydrogen density and superior stability. Thus, the development of low-cost and high-efficient heterogeneous catalysts for the dehydrogenation of AB has attracted considerable scholarly attention. In this study, heterostructured Co3O4–SnO2 catalysts containing oxygen vacancy (Vo) with different Co/Sn atomic ratios (designated as Vo–Co–Sn5:x) were synthesized via a simple co-precipitation–calcination method under mild reaction conditions. The catalyst containing an optimized Co/Sn atomic ratio of 5:2 (Vo–Co–Sn5:2) exhibited robust catalytic performance with a turnover frequency value of 17.6 \(\text{mol}_{{\text{H}}_{2}}\)·molmetal−1·min−1. Moreover, 82.6% of the original activity of the catalyst was retained after 14 catalytic cycles, indicating the high stability of the catalyst. Diversified characterization combined with the density functional theory (DFT) calculation confirmed the transfer of electrons from Co3O4 to SnO2 and the distribution of the separated charges on SnO2–Co3O4 interface. The transfer of electrons and the distribution of charges facilitated the adsorption and activation of water on the catalyst, thus accelerating the dissociation of H2O molecule (the rate-determining step of AB hydrolysis). It was found that the Vo adjusted the electron structure of the catalysts rather than acted as active sites. These findings will provide researchers with useful information for designing cheap and highly efficient catalysts for catalytic AB hydrolysis.

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摘要

氨硼烷（NH3BH3，AB）由于具有较高的氢含量和优越的稳定性，被认为是一种很有前景的化学储氢材料。低成本、高效的多相AB产氢催化剂的开发是实现氨硼烷水解制氢的关键。在本研究中，我们通过简单的共沉淀-煅烧法，合成了不同Co/Sn比例（称为Vo–Co–Sn5:x）的异质结构Co3O4–SnO2催化剂。其中Co/Sn比为5:2（Vo–Co–Sn5:2）的催化剂具有良好的催化性能，TOF为17.6 molH 2•molmetal‒1•min−1。经过14次催化循环后，该催化剂的原有活性保持了82.6%，表明该催化剂的稳定性较高。多种表征结合密度泛函理论计算，证实了电子从Co3O4转移SnO2上，电荷集中分布在SnO2–Co3O4界面上。电子转移和电荷的集中分布促进了H2O在催化剂上的吸附和活化，进而加速了水分子中O-H键的断裂（AB水解的速率决定步骤）。我们发现，Vo调整了催化剂的电子结构，而不是作为活性位点。这些发现将为研究人员设计廉价和高效的催化AB水解催化剂提供有价值的信息。

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Acknowledgements

This work was financially supported by the Professorial and Doctoral Scientific Research Foundation of Huizhou University (Nos. 2018JB036, 2020JB046 and 2022JB009); the Major and Special Project in the Field of Intelligent Manufacturing of the Universities in Guangdong Province (No. 2020ZDZX2067); the Natural Science Foundation of Huizhou University (No. HZU202004); Open Project Program of Guangdong Provincial Key Laboratory of Electronic Functional Materials and Devices, Huizhou University (Nos. EFMDN2021001Z and EFMDN2021004M); Youth Innovative Talents Project in Colleges and Universities in Guangdong Province (No. 2019KQNCX151). Basic and Applied Basic Research Fund of Guangdong Province (No. 2020A1515110038).

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  1. Hui-Ze Wang and You-Xiang Shao have contributed equally to this work.

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  1. School of Chemistry and Materials Engineering, Huizhou University, Huizhou, 516007, China

    Hui-Ze Wang, You-Xiang Shao, Yu-Fa Feng, Yu-Jie Tan, Qing-Yu Liao, Xiao-Dong Chen, Xue-Feng Zhang & Hao Li

  2. Guangdong Provincial Key Laboratory for Electronic Functional Materials and Devices, Huizhou University, Huizhou, 516007, China

    Hui-Ze Wang, You-Xiang Shao, Yu-Fa Feng, Yu-Jie Tan, Qing-Yu Liao, Xiao-Dong Chen, Xue-Feng Zhang, Zhao-Hui Guo & Hao Li

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Wang, HZ., Shao, YX., Feng, YF. et al. Heterostructured Co3O4–SnO2 composites containing oxygen vacancy with high activity and recyclability toward NH3BH3 dehydrogenation. Rare Met. 42, 3013–3023 (2023). https://doi.org/10.1007/s12598-023-02305-0

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