Abstract
Zr-based metal-organic framework nanocable catalysts comprising MTe(M = Pt, PtCu)@UIO-67 resembling “sugarcoated haws on a stick” were assembled. Ultrathin Te nanowires with diameters of about 8.48 nm served as a sacrificial template for the epitaxial growth of an outer M (Pt or PtCu) to obtain cable cores comprising MTe nanowires with good dispersity, which were then successfully encapsulated in the center of a monodisperse MTe@UIO-67 cable nano-structured catalyst. Transmission electron microscopy (TEM), scanning electron microscopy (SEM), powder X-ray diffraction (XRD) and energy dispersive X-ray (EDX) element mapping were used to investigate the morphology, structure and composition of the nanocable catalysts. Six types of catalysts were synthesized, and all of the catalysts demonstrated superior product selectivity to CO for reverse water-gas shift (RWGS) reaction. Especially, the morphology and dispersion of PtCuTe@UIO-67 nanocable catalyst can be maintained to some extent after catalysis at high temperature, and PtTe@UIO-67 catalyzed CO2 conversion was achieved with 99.86% CO selectivity.
摘要
本文以锆系金属有机骨架为载体合成了具有“糖葫芦”结构形貌的纳米电缆状催化剂MTe (M = Pt, PtCu)@UIO-67. 首先以直径大约为8.48 nm的超细Te纳米线作为牺牲模板, 用于外延生长外部的金属粒子(Pt或PtCu), 得到具有良好分散性的电缆芯形状的MTe纳米线, 然后成功地封装在单分散的MTe@UIO-67电缆状纳米结构催化剂的中心. 采用透射电子显微镜、 扫描电子显微镜、 粉末X射线衍射和能谱等方法对纳米电缆催化剂的形貌结构和组成进行了表征. 本文合成的六种催化剂均表现出良好的CO产物选择性, 在高温催化后, PtCuTe@UIO-67催化剂的形貌和分散性能得到一定程度的保持, 而PtTe@UIO-67催化CO2转化成CO的选择性可以达到99.86%.
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We gratefully acknowledge the financial support from the National Natural Science Foundation of China (21371058).
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Author contributions Zhang H performed the experiments, analyzed the data and wrote the draft of manuscript under the guidance of Xu H; Li Y, Pan X and Li L provided some suggestions.
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Huaqian Zhang is a master candidate at East China University of Science and Technology (ECUST). Her current research interest focuses on the synthesis of functional nanomaterials and CO2 conversion.
Haitao Xu obtained his Master and PhD degrees from the University of Science and Technology of China (USTC) in 1999 and 2002, respectively. After a postdoctoral fellowship at Tsinghua University, he became an associate professor at Tongji University in 2005. He studied in Kyushu University as a JSPS fellow in 2007. He moved to ECUST in 2009. His research focuses on multifunction materials, metal-organic frameworks, nanocatalyst, adsorption/separation, and CO2 conversion.
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Zhang, H., Xu, H., Li, Y. et al. Nanocable catalysts MTe (M = Pt, PtCu)@UIO-67 for CO2 conversion. Sci. China Mater. 63, 769–778 (2020). https://doi.org/10.1007/s40843-019-1258-8
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DOI: https://doi.org/10.1007/s40843-019-1258-8