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Efficient hydrogen production by methanol aqueous phase reforming over KMnO4 modified PtMnK/AC catalyst: Regulating the hydrophilicity of carbon support
Molecular Catalysis ( IF 4.6 ) Pub Date : 2024-04-03 , DOI: 10.1016/j.mcat.2024.114105
Peng Wang , Yuankai Huang , Riyang Shu , Junyao Wang , Jianping Liu , Chao Wang , Zhipeng Tian , Ying Chen

The production of hydrogen through the aqueous phase reforming of biomass-derived oxygenates has broad application prospects in distributed hydrogen energy systems. Activated carbon is commonly employed as a catalyst support in catalytic aqueous phase reforming due to its high surface area and hydrothermal stability. Nevertheless, its hydrophobicity hinders the efficient adsorption of water molecules, which affects the activity of the aqueous phase reforming reaction. In this study, catalysts using carbon as support with varying hydrophilicity were synthesized using nitric acid and potassium permanganate as modifiers. The efficiency of these catalysts was then examined in the aqueous phase reforming reaction of methanol and the water gas shift reaction, respectively. The impact of the hydrophilicity of the support on the reaction performances was examined with diverse characterization techniques. The results demonstrated that the PtMnK/AC catalyst exhibited 1.2 times the hydrogen production yield compared to the conventional Pt/AC catalyst, indicating that enhancing the hydrophilicity of the support promoted the water gas shift reaction while limiting methanation side reactions in methanol aqueous phase reforming. The effective interaction between hydrophilic surfaces and oxygen vacancies enhances the catalyst's capability to dissociate HO and react with CO* intermediates to generate more hydrogen, which is regarded as the rate determining step of methanol aqueous phase reforming.

中文翻译:

KMnO4 改性 PtMnK/AC 催化剂上甲醇水相重整高效制氢:调节碳载体的亲水性

通过生物质含氧化合物水相重整制氢在分布式氢能系统中具有广阔的应用前景。由于其高表面积和水热稳定性,活性炭通常用作催化水相重整中的催化剂载体。然而,其疏水性阻碍了水分子的有效吸附,从而影响了水相重整反应的活性。在这项研究中,以硝酸和高锰酸钾为改性剂,合成了以碳为载体的具有不同亲水性的催化剂。然后分别在甲醇的水相重整反应和水煤气变换反应中检查这些催化剂的效率。使用不同的表征技术检查了载体的亲水性对反应性能的影响。结果表明,与传统Pt/AC催化剂相比,PtMnK/AC催化剂的氢气产率是传统Pt/AC催化剂的1.2倍,表明增强载体的亲水性促进了水煤气变换反应,同时限制了甲醇水相重整中的甲烷化副反应。亲水表面和氧空位之间的有效相互作用增强了催化剂解离H2O并与CO*中间体反应产生更多氢气的能力,这被认为是甲醇水相重整的速率决定步骤。
更新日期:2024-04-03
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