High-porosity Pt-CeO2 nanosponges as oxidation catalyst.

IF 4.6 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Nanoscale Advances Pub Date : 2024-12-30 DOI:10.1039/d4na00525b
Simon Falkner, Carina B Maliakkal, Mareike Liebertseder, Joachim Czechowsky, Maria Casapu, Jan-Dierk Grunwaldt, Christian Kübel, Claus Feldmann
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Abstract

Pt-CeO2 nanosponges (1 wt% Pt) with high surface area (113 m2 g-1), high pore volume (0.08 cm3 g-1) 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 NH3. The cerium oxalate precursor Ce2(C2O4)3·10H2O is prepared by aqueous precipitation from Ce(NO3)3·6H2O and K2C2O4·H2O and thermally converted to CeO2 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 CeO2 nanosponges are decorated with small-sized Pt nanoparticles, using a wet-chemical impregnation with Pt(ac)2 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-CeO2 nanosponges as well as the uniform distribution of the Pt nanoparticles. The Pt-CeO2 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, NH3 as indicated by high activities in terms of low and stable light-out and light-off temperatures as well as a high selectivity to N2 (for NH3 oxidation) with >80% at 170-250 °C.

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高孔隙率Pt-CeO2纳米海绵作为氧化催化剂。
通过草酸铈前驱体的热分解制备了高表面积(113 m2 g-1)、高孔体积(0.08 cm3 g-1)和小尺寸Pt纳米颗粒(1.8±0.4 nm)的Pt- ceo2纳米海绵(1 wt% Pt),并对CO、挥发性有机化合物(VOCs)和NH3的催化氧化进行了研究。以Ce(NO3)3·6H2O和K2C2O4·H2O为原料,采用水相沉淀法制备草酸铈前驱体Ce2(C2O4)3·10H2O,在空气中加热后热转化为CeO2纳米海绵。在350°C、20 min的温度下,观察了分解的最佳条件(表面积和孔隙率)。最后,用Pt(ac)2在甲醇中湿化学浸渍的方法,用小尺寸的Pt纳米颗粒装饰CeO2纳米海绵。利用电子显微镜、断层扫描、电子能谱和其他方法(TG、XRD、FT-IR、吸附分析)表征了催化剂的组成,特别是Pt- ceo2纳米海绵的结构和孔隙度,以及Pt纳米颗粒的均匀分布。Pt-CeO2纳米海绵具有良好的热稳定性(高达400°C),并且作为一种新型的,未经优化的催化剂,具有催化氧化CO, VOCs, NH3的活性,这表明在低且稳定的熄灯和熄灯温度方面具有高活性,并且在170-250°C时对N2(用于NH3氧化)具有80%的高选择性(>)。
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来源期刊
Nanoscale Advances
Nanoscale Advances Multiple-
CiteScore
8.00
自引率
2.10%
发文量
461
审稿时长
9 weeks
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