TY - JOUR
T1 - Size-Tunable Synthesis of Palladium Nanoparticles Confined within Topologically Distinct Metal-Organic Frameworks for Catalytic Dehydrogenation of Methanol
AU - Wang, Yu Hsiang
AU - Chuang, Cheng Hsun
AU - Chiu, Te An
AU - Kung, Chung Wei
AU - Yu, Wen Yueh
N1 - Funding Information:
This work was financially supported by the Ministry of Science and Technology (MOST) of Taiwan, under projects MOST 107-2218-E-006-054-MY3 and MOST 107-2218-E-002-029-MY3, and by the “Advanced Research Center for Green Materials Science and Technology” from The Featured Area Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education (108L9006) and the Ministry of Science and Technology in Taiwan (108-3017-F-002-002). We also thank the support from the Yushan Young Scholar Program, under Ministry of Education (MOE), Taiwan. This work was also supported in part by Higher Education Sprout Project, MOE, Taiwan to the Headquarters of University Advancement at National Cheng Kung University. We thank the support from Formosa Plastics Group, Taiwan. We also thank Ms. C.-Y. Chien of Ministry of Science and Technology (National Taiwan University) for the assistance in TEM experiments.
PY - 2020/6/11
Y1 - 2020/6/11
N2 - In this study, three topologically distinct zirconium-based metal-organic frameworks (Zr-MOFs), i.e., UiO-66, NU-902, and PCN-222, were synthesized and employed as porous supports to immobilize Pd nanoparticles (NPs) via the solvothermal deposition in MOFs (SIM) technique. Physicochemical characterizations show that the structural, morphological, and textural features of pristine Zr-MOFs are mainly preserved upon the incorporation of Pd NPs. It is shown that the sizes of Pd NPs are controllable by the pore confinement of Zr-MOFs. Reaction testing reveals that Pd@UiO-66 displays significantly higher catalytic activity and lower activation energy as compared to Pd@NU-902 and Pd@PCN-222 for methanol dehydrogenation. The observed enhanced performance of Pd@UiO-66 is attributed to the smaller size of Pd NPs due to the smaller pore size of UiO-66. In situ infrared spectroscopy characterizations suggest that methanol is activated on the surface of UiO-66 to form methoxy adspecies, and the Pd NPs within the framework of UiO-66 aid in the further dehydrogenation of methoxy adspecies, thereby facilitating the overall dehydrogenation of methanol.
AB - In this study, three topologically distinct zirconium-based metal-organic frameworks (Zr-MOFs), i.e., UiO-66, NU-902, and PCN-222, were synthesized and employed as porous supports to immobilize Pd nanoparticles (NPs) via the solvothermal deposition in MOFs (SIM) technique. Physicochemical characterizations show that the structural, morphological, and textural features of pristine Zr-MOFs are mainly preserved upon the incorporation of Pd NPs. It is shown that the sizes of Pd NPs are controllable by the pore confinement of Zr-MOFs. Reaction testing reveals that Pd@UiO-66 displays significantly higher catalytic activity and lower activation energy as compared to Pd@NU-902 and Pd@PCN-222 for methanol dehydrogenation. The observed enhanced performance of Pd@UiO-66 is attributed to the smaller size of Pd NPs due to the smaller pore size of UiO-66. In situ infrared spectroscopy characterizations suggest that methanol is activated on the surface of UiO-66 to form methoxy adspecies, and the Pd NPs within the framework of UiO-66 aid in the further dehydrogenation of methoxy adspecies, thereby facilitating the overall dehydrogenation of methanol.
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U2 - 10.1021/acs.jpcc.0c02743
DO - 10.1021/acs.jpcc.0c02743
M3 - Article
AN - SCOPUS:85088894944
VL - 124
SP - 12521
EP - 12530
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 23
ER -