左佑华, 李蓉, 花俊峰, 郝思雨, 谢婧, 许立信, 叶明富, 万超. Co0.5Cu0.5/CNR催化剂制备及其氨硼烷水解制氢性能研究[J]. 燃料化学学报(中英文), 2024, 52(9): 1307-1317. DOI: 10.1016/S1872-5813(24)60442-1
引用本文: 左佑华, 李蓉, 花俊峰, 郝思雨, 谢婧, 许立信, 叶明富, 万超. Co0.5Cu0.5/CNR催化剂制备及其氨硼烷水解制氢性能研究[J]. 燃料化学学报(中英文), 2024, 52(9): 1307-1317. DOI: 10.1016/S1872-5813(24)60442-1
ZUO Youhua, LI Rong, HUA Junfeng, HAO Siyu, XIE Jing, XU Lixin, YE Mingfu, WAN Chao. Preparation of Co0.5Cu0.5/CNR catalyst and its performance in hydrogen production by hydrolysis of ammonia borane[J]. Journal of Fuel Chemistry and Technology, 2024, 52(9): 1307-1317. DOI: 10.1016/S1872-5813(24)60442-1
Citation: ZUO Youhua, LI Rong, HUA Junfeng, HAO Siyu, XIE Jing, XU Lixin, YE Mingfu, WAN Chao. Preparation of Co0.5Cu0.5/CNR catalyst and its performance in hydrogen production by hydrolysis of ammonia borane[J]. Journal of Fuel Chemistry and Technology, 2024, 52(9): 1307-1317. DOI: 10.1016/S1872-5813(24)60442-1

Co0.5Cu0.5/CNR催化剂制备及其氨硼烷水解制氢性能研究

Preparation of Co0.5Cu0.5/CNR catalyst and its performance in hydrogen production by hydrolysis of ammonia borane

  • 摘要: 以硝酸钴和硝酸铜制备溶液A,苯二甲酸(PTA)和N,N-二甲基甲酰胺(DMF)制备溶液B,两种溶液通过溶剂热法制备Co/Cu拉瓦希尔骨架系列材料(Co/Cu-MIL前驱体),进一步直接碳化前驱体制备出MOFs衍生物,即双金属碳纳米棒(CoxCu1−x/CNR)催化剂。通过SEM、TEM、XRD、XPS等表征手段探究其形貌和组成。结果表明,Co/Cu-MIL经过高温焙烧后成功得到CoxCu1−x/CNR,当x=0.5、溶剂热温度为120 ℃、焙烧温度为650 ℃时得到的催化剂催化活性最优,Co0.5Cu0.5/CNR催化剂催化氨硼烷(AB)水解制氢的TOF值为2718.21 h−1,反应的活化能为51.64 kJ/mol,且催化剂的循环稳定性较好,在循环10次后催化活性虽然有所下降,但对AB仍然保持100%的转化率。

     

    Abstract: Cobalt nitrate and copper nitrate was mixed to prepare solution A. Phenyldicarboxylic acid and N,N-dimethylformamide was mixed to prepare solution B. Co/Cu Lavashield skeleton series materials (Co/Cu-MIL precursors) was then synthesized by mixing the above two solution via solvothermal method. The precursor was further carbonized to produce the MOFs derivatives, i.e. bimetallic carbon nanorods (CoxCu1−x/CNR) catalysts. The morphology and composition of the catalysts were explored by SEM, TEM, XRD, XPS and other characterization means. The results showed that CoxCu1−x/CNR was successfully obtained after calcination of Co/Cu-MIL at high temperature. The activity of the catalyst was optimal when x=0.5, the solvothermal temperature of 120 ℃ and the calcination temperature of 650 ℃. The TOF value of the Co0.5Cu0.5/CNR catalyst for the hydrolysis of ammonia borane for the production of hydrogen was 2718.21 h−1 with activation energy of 51.64 kJ/mol. The catalyst had good cyclic stability. Although the activity decreased, the conversion of AB still maintained 100% after 10 cycles.

     

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