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Boosting methylcyclohexane dehydrogenation over Pt-based structured catalysts by internal electric heating
Nano Research ( IF 9.5 ) Pub Date : 2023-06-10 , DOI: 10.1007/s12274-023-5771-2
Wenhan Wang , Guoqing Cui , Cunji Yan , Xuejie Wang , Yang Yang , Chunming Xu , Guiyuan Jiang

Methylcyclohexane (MCH) serves as an ideal hydrogen carrier in hydrogen storage and transportation process. In the continuous production of hydrogen from MCH dehydrogenation, the rational design of energy-efficient catalytic way with good performance remains an enormous challenge. Herein, an internal electric heating (IEH) assisted mode was designed and proposed by the directly electrical-driven catalyst using the resistive heating effect. The Pt/Al2O3 on Fe foam (Pt/Al2O3/FF) with unique three-dimensional network structure was constructed. The catalysts were studied in a comprehensive way including X-ray diffraction (XRD), scanning electron microscopy (SEM)-mapping, in situ extended X-ray absorption fine structure (EXAFS), and in situ CO-Fourier transform infrared (FTIR) measurements. It was found that the hydrogen evolution rate in IEH mode can reach up to above 2060 mmol·g −1Pt ·min−1, which is 2–5 times higher than that of reported Pt based catalysts under similar reaction conditions in conventional heating (CH) mode. In combination with measurements from high-resolution infrared thermometer, the equations of heat transfer rate, and reaction heat analysis results, the Pt/Al2O3/FF not only has high mass and heat transfer ability to promote catalytic performance, but also behaves as the heating component with a low thermal resistance and heat capacity offering a fast temperature response in IEH mode. In addition, the chemical adsorption and activation of MCH molecules can be efficiently facilitated by IEH mode, proved by the operando MCH-FTIR results. Therefore, the as-developed IEH mode can efficiently reduce the heat and mass transfer limitations and prominently boost the dehydrogenation performance, which has a broad application potential in hydrogen storage and other catalytic reaction processes.



中文翻译:

通过内部电加热在 Pt 基结构催化剂上促进甲基环己烷脱氢

甲基环己烷(MCH)是氢储运过程中理想的氢载体。在MCH脱氢连续制氢中,合理设计高效节能、性能良好的催化方式仍然是一个巨大的挑战。在此,利用电阻加热效应,设计并提出了直接电驱动催化剂的内部电加热(IEH)辅助模式。构建了具有独特三维网络结构的Pt/Al 2 O 3 on Fe泡沫(Pt/Al 2 O 3 /FF)。对催化剂进行了全面的研究,包括 X 射线衍射 (XRD)、扫描电子显微镜 (SEM) 映射、原位扩展 X 射线吸收精细结构 (EXAFS) 和原位CO-傅里叶变换红外 (FTIR) 测量。结果发现,IEH 模式下的析氢速率可达 2060 mmol·g −1 Pt ·min −1以上,比传统加热类似反应条件下报道的 Pt 基催化剂高 2-5 倍(频道)模式。结合高分辨率红外测温仪的测量、传热速率方程和反应热分析结果,Pt/Al 2 O 3 /FF不仅具有良好的传质和传热能力以提升催化性能,而且作为加热元件具有低热阻和热容量,在IEH模式下提供快速温度响应。此外,原位MCH -FTIR 结果证明,IEH 模式可以有效促进 MCH 分子的化学吸附和活化。因此,所开发的IEH模式可以有效降低传热传质限制,显着提高脱氢性能,在储氢和其他催化反应过程中具有广泛的应用潜力。

更新日期:2023-06-11
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