钴装饰蛋壳型活性炭颗粒:催化硼基固体燃料释氢的应用

B. Coşkuner Filiz
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摘要

氢成为燃料电池或内燃机使用的零碳燃料,在能源领域绿色氢也成为商业应用的能源载体。为了支持基于氢的脱碳战略,硼燃料是安全储存用于移动技术的好选择。氨硼烷(NH3BH3)是硼基燃料中的一种,在其结构中化学储存了19.6 wt.%的H2。合成了钴(Co)修饰的蛋壳型活性炭颗粒,用于催化NH3BH3的氢释放。采用改进的真空浸渍法和热固还原相结合的工艺对两种不同粒径的球团型活性炭进行钴修饰。采用光学显微镜(OM)、扫描电镜(SEM)、x射线能谱(EDS)、透射电镜(TEM)、氮吸附表面分析(BET)等手段对催化剂进行了表征。活性炭具有多孔结构,可有效分散Co颗粒,而其外壳具有催化产氢活性。结构表征结果和初步活性测试证实,与Co@ACPS催化剂相比,制备的Co@ACPB具有更薄的壳厚度和更高的BET表面积/孔体积性能,具有更好的性能。动力学研究结果表明,核壳型Co基催化剂催化了该反应,反应动力学模型为41.78 kJmol-1,符合零级反应模型。活性炭颗粒具有良好的活性Co位点分散性和稳定性,反应后催化剂易于分离,可实现催化材料的实际再生。
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Cobalt decorated egg-shell-type activated carbon pellets: Catalytic application in hydrogen release from boron based solid fuel
Hydrogen became zero-carbon fuel used in fuel-cell or internal combustion engines, regard- ing energy sector green-hydrogen also has become an energy carrier in commercial appli- cations. For supporting decarbonization strategies based on hydrogen, boron-fuels are good options to safely store for mobile technologies. Ammonia borane (NH3BH3) is the one of the boron based fuels that stored 19.6 wt.% H2 in its structure chemically. Cobalt (Co) decorated egg-shell-type activated carbon pellets were synthesized for catalytic application of hydrogen release from NH3BH3. Two different sized pellet type activated carbon was decorated with co- balt by combined procedure as modified vacuum-impregnation method with heat fixation and reduction. The obtained catalysts were characterized by applying optical microscope (OM), scanning electron microscope/energy dispersive X-ray spectroscopy (SEM/EDS), transmis- sion electron microscopy (TEM), nitrogen sorption based surface analyses (BET). Activated carbon provides porous structure for effectively dispersion Co particles while the outer shell shows the catalytic activity for hydrogen generation. Structural characterization results and preliminary activity tests confirmed that fabricated Co@ACPB exhibited better performance compared with Co@ACPS catalysts thanks to thinner shell thickness and higher BET surface area/pore volume properties. The results of the kinetic study showed the core-shell type Co based catalyst catalyzed the reaction and follows the zero-order reaction kinetic model with 41.78 kJmol-1. Activated carbon pellets provide well dispersion and stability of active Co sites, easy separation of used catalysts after the reaction and enable practical regeneration of cata- lytic materials.
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