Partially embedding Pt nanoparticles in the skeleton of 3DOM Mn2O3: An effective strategy for enhancing catalytic stability in toluene combustion
Partially embedding Pt nanoparticles in the skeleton of 3DOM Mn2O3: An effective strategy for enhancing catalytic stability in toluene combustion
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将 Pt 纳米颗粒部分嵌入 3DOM Mn2O3 骨架中：增强甲苯燃烧催化稳定性的有效策略
DOI：
10.1016/j.apcatb.2019.117814
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发表时间：
2019-11
期刊：
影响因子：
--
通讯作者：
Hongxing Dai
中科院分区：
文献类型：
--
作者：
Wenbo Pei;Yuxi Liu;Jiguang Deng;Kunfeng Zhang;Zhiquan Hou;Xingtian Zhao;Hongxing Dai
采用聚甲基丙烯酸甲酯模板法和乙二醇还原法制备了部分嵌入三维有序大孔(3DOM) 骨架的纳米铂催化剂(xwt%Pt/3DOM Mn2O3；x=3DOM 0.2-2.3)。这些材料的比表面积为33-36 m~2/g，其中铂纳米粒子(尺寸为3.6-4.4 nm)被很好地嵌入到3DOM-Mn_2O_3骨架中。2.3 质量分数铂/3DOM Mn2 O3催化剂对甲苯的燃烧活性最高，表观活化能最低(41 kJ/m ol)，这与其吸附氧物种浓度高和低温还原性能好有关.与胶体吸附法制备的2.0 质量分数铂/3DOM Mn2O-IMP催化剂相比，2.3 质量分数铂/3DOM Mn2O_3催化剂在甲苯燃烧60 h内表现出更好的稳定性。经6 5 0 °C焙烧3 h后，2.3 wt%Pt/3DOM Mn2 O3催化剂中铂纳米粒子的平均粒径从4.3 nm增大到4.9 nm，甲苯转化率略有下降，而2.0 wt%铂/3DOM Mn2 O3-IMP催化剂中的铂纳米粒子平均粒径从4.4 nm增加到13.7 nm，甲苯转化率显著下降。考察了H_2O、CO_2和SO_2对2.3wt%Pt/3DOM Mn2O_3和2.0 wt%Pt/3DOM Mn2O-IMP催化剂活性的影响。加入H2O或CO2引起的部分失活是可逆的，而引入SO2引起的部分失活是不可逆的。结果表明，铂纳米粒子与3DOM-Mn2O3之间的强相互作用是部分嵌入铂的3DOM-Mn2O3样品在甲苯燃烧中具有良好稳定性的原因。
Polymethyl methacrylate-templating and ethylene glycol reduction methods were adopted to prepare the nanosized Pt catalysts (xwt% Pt/3DOM Mn2O3;x= 0.2–2.3) that were partially embedded in the skeleton of three-dimensionally ordered macroporous (3DOM) Mn2O3. These materials possessed a surface area of 33–36 m2/g, with the Pt NPs (3.6–4.4 nm in size) being well embedded in the skeleton of 3DOM Mn2O3. The 2.3 wt% Pt/3DOM Mn2O3sample showed the best activity and the lowest apparent activation energy (41 kJ/mol) for toluene combustion, which was related to its high adsorbed oxygen species concentration and good low-temperature reducibility. Compared with 2.0 wt% Pt/3DOM Mn2O3-imp derived from the colloid adsorption method, 2.3 wt% Pt/3DOM Mn2O3exhibited a better catalytic stability within 60 h of toluene combustion. After calcination at 650 °C for 3 h, the average particle size of Pt nanoparticles (NPs) in 2.3 wt% Pt/3DOM Mn2O3grew up slightly from 4.3 to 4.9 nm and toluene conversions decreased slightly, while that of Pt NPs in 2.0 wt% Pt/3DOM Mn2O3-imp increased greatly from 4.4 to 13.7 nm and toluene conversions dropped significantly. Effects of H2O, CO2, and SO2on activity of 2.3 wt% Pt/3DOM Mn2O3and 2.0 wt% Pt/3DOM Mn2O3-imp were also examined. Partial deactivation induced by H2O or CO2addition was reversible, whereas that due to SO2introduction was irreversible. It is concluded that the strong interaction between Pt NPs and 3DOM Mn2O3was responsible for excellent stability of the partially Pt-embedded 3DOM Mn2O3sample in toluene combustion.
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