Abstract
Herein, the successful preparation of a single-atom catalyst V–N–C using vanadium-doped zeolitic imidazolate framework (ZIF)-8 as a precursor is reported. The experimental results showed that the V–N–C had a good promoting effect on the hydrogen storage performance of MgH2, and the optimal addition amount of V–N–C was 10 wt%. The hydrogenation and dehydrogenation apparent activation energies of 10 wt% V–N–C-catalyzed MgH2 were reduced by 44.9 and 53.5 kJ·mol−1, respectively, compared to those of additive-free MgH2. The 10 wt% V–N–C-catalyzed MgH2 could reabsorb 5.92 wt% of hydrogen in 50 min at 150 °C, with a capacity retention rate of 99.1% after 30 cycles of hydrogen absorption and desorption. Mechanism analysis showed that V–N–C was partially transformed into VN and metallic V when it was milled with MgH2; the in-situ-formed VN and metallic V played an important role in improving the hydrogen storage performance of MgH2. This approach provides a potential solution for obtaining high-performance Mg-based hydrogen storage materials through synergistic interactions between V, N and C.
Graphical abstract
摘要
本文报道了以掺钒ZIF-8为前驱体成功制备单原子催化剂V-N-C的案例。实验结果表明,V-N-C对MgH2的储氢性能有较好的促进作用,V-N-C的最佳添加量为10 wt%。与无添加剂MgH2相比,10 wt% V-N-C催化的MgH2的加氢和脱氢表观活化能分别降低了44.9和53.5 kJ•mol−1。10 wt% V-N-C催化的MgH2在150 °C下可在50 min内重吸收5.92 wt%的氢,吸氢和解吸30次循环后的容量保持率为99.1%。机理分析表明,V-N-C在与MgH2研磨时部分转化为VN和金属V;原位形成的VN和金属V对提高MgH2的储氢性能起着重要作用。该方法为通过V、N和C之间的协同相互作用获得高性能Mg基储氢材料提供了一种潜在的解决方案。
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This work was financially supported by the National Natural Science Foundation of China (Nos. 52261038 and 51861002) and Nanning Excellent Young Talents Cultivation Project of Scientific and Technological Innovation and Entrepreneurship (No. RC20220102).
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Hong, FF., Shi, WT., Zhao, RL. et al. Improvement in hydrogen storage performance of MgH2 by vanadium doped with ZIF-8 derived a single-atom catalyst V–N–C. Rare Met. 43, 2623–2635 (2024). https://doi.org/10.1007/s12598-024-02639-3
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DOI: https://doi.org/10.1007/s12598-024-02639-3