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高孔隙率铂-二氧化铈纳米海绵作为氧化催化剂。

High-porosity Pt-CeO nanosponges as oxidation catalyst.

作者信息

Falkner Simon, Maliakkal Carina B, Liebertseder Mareike, Czechowsky Joachim, Casapu Maria, Grunwaldt Jan-Dierk, Kübel Christian, Feldmann Claus

机构信息

Institute of Inorganic Chemistry (IAC), Karlsruhe Institute of Technology (KIT) Engesserstraße 15 D-76131 Karlsruhe Germany

Institute of Nanotechnology (INT), Karlsruhe Nano Micro Facility (KNMFi), Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen Germany.

出版信息

Nanoscale Adv. 2024 Dec 30;7(4):1173-1182. doi: 10.1039/d4na00525b. eCollection 2025 Feb 11.

Abstract

Pt-CeO nanosponges (1 wt% Pt) with high surface area (113 m g), high pore volume (0.08 cm g) and small-sized Pt nanoparticles (1.8 ± 0.4 nm) are prepared by thermal decomposition of a cerium oxalate precursor and examined for catalytic oxidation of CO, volatile organic compounds (VOCs), and NH. The cerium oxalate precursor Ce(CO)·10HO is prepared by aqueous precipitation from Ce(NO)·6HO and KCO·HO and thermally converted to CeO nanosponges by heating in air. Optimal conditions for decomposition in terms of surface area and porosity are observed at 350 °C for 20 min. Finally, the CeO nanosponges are decorated with small-sized Pt nanoparticles, using a wet-chemical impregnation with Pt(ac) in methanol. Electron microscopy with tomography, electron spectroscopy and further methods (TG, XRD, FT-IR, sorption analysis) are used to characterize the catalyst composition and especially the structure and porosity of the Pt-CeO nanosponges as well as the uniform distribution of the Pt nanoparticles. The Pt-CeO nanosponges show good thermal stability (up to 400 °C) and, already as a new, non-optimized catalyst, promising activity for catalytic oxidation of CO, VOCs, NH as indicated by high activities in terms of low and stable light-out and light-off temperatures as well as a high selectivity to N (for NH oxidation) with >80% at 170-250 °C.

摘要

通过草酸铈前驱体的热分解制备了具有高比表面积(113 m²/g)、高孔容(0.08 cm³/g)和小尺寸铂纳米颗粒(1.8±0.4 nm)的Pt-CeO纳米海绵(1 wt% Pt),并对其催化氧化CO、挥发性有机化合物(VOCs)和NH₃的性能进行了研究。草酸铈前驱体Ce₂(C₂O₄)₃·10H₂O通过Ce(NO₃)₃·6H₂O和K₂C₂O₄·H₂O的水相沉淀法制备,并通过在空气中加热热转化为CeO₂纳米海绵。在350℃下加热20分钟时,观察到了在比表面积和孔隙率方面的最佳分解条件。最后,使用Pt(ac)₂在甲醇中的湿化学浸渍法,在CeO₂纳米海绵上负载小尺寸的Pt纳米颗粒。采用电子显微镜断层扫描、电子能谱和其他方法(TG、XRD、FT-IR、吸附分析)来表征催化剂的组成,特别是Pt-CeO₂纳米海绵的结构和孔隙率以及Pt纳米颗粒的均匀分布。Pt-CeO₂纳米海绵表现出良好的热稳定性(高达400℃),并且作为一种新型的、未经优化的催化剂,对CO、VOCs、NH₃的催化氧化已经显示出有前景的活性,这表现为在低且稳定的起燃和熄灭温度方面具有高活性,以及在170-250℃下对N₂具有>80%的高选择性(对于NH₃氧化)。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5771/11812633/0114c7899beb/d4na00525b-f1.jpg

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