Affiliation:
1. Engineering Research Center of Eco‐environment in Three Gorges Reservoir Region College of Materials and Chemical Engineering China Three Gorges University Yichang Hubei 443002 P. R. China
2. Department of chemistry and chemical engineering Liaocheng University Liaocheng 252059 P. R. China
3. Institute of Circular Economy, Faculty of Materials and Manufacturing Beijing University of Technology Beijing 100124 P. R. China
Abstract
AbstractH2 generation from methanol‐water mixtures often requires high pressure and high temperature (200–300 °C). However, CO can be easily generated and poison the catalytic system under such high temperature. Therefore, it is highly desirable to develop the efficient catalytic systems for H2 production from methanol at room temperature, even at sub‐zero temperatures. Herein, carbon nanotube‐supported Pt nanocomposites are designed and synthesized as high‐performance nano‐catalysts, via stabilization of Pt nanoparticles onto carbon nanotube (CNT), for H2 production upon methanol dehydrogenation at sub‐zero temperatures. Therein, the optimal Pt/CNT nanocomposite presents the superior catalytic performance in H2 production upon methanol dehydrogenation at the expense of B2(OH)4, with the TOF of 299.51 min‐130 oC. Compared with other common carriers, Pt/CNT exhibited the highest catalytic performance in H2 production, emphasizing the critical role of CNT in methanol dehydrogenation. The confinement of Pt nanoparticles by CNTs is conducive to inhibiting the aggregation of Pt nanoparticles, thereby significantly increasing its catalytic performance and stability. The kinetic study, detailed mechanistic insights, and density functional theory (DFT) calculation confirm that the breaking of O─H bond of CH3OH is the rate‐controlling step for methanol dehydrogenation, and both H atoms of H2 are supplied by methanol. Interestingly, H2 is also successfully produced from methanol dehydrogenation at −10 °C, which absolutely solves the freezing problem in the H2 evolution upon water‐splitting reaction.
Funder
China Three Gorges University
National Natural Science Foundation of China
Subject
General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)