Ag supported on CeO2 with different morphologies for the catalytic oxidation of HCHO
Ag supported on CeO2 with different morphologies for the catalytic oxidation of HCHO
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不同形貌的 CeO2 负载 Ag 用于 HCHO 的催化氧化
DOI：
10.1016/j.cej.2017.11.121
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发表时间：
2018-02
影响因子：
15.1
通讯作者：
Ye Daiqi
中科院分区：
文献类型：
--
作者：
Yu Lian;Peng Ruosi;Chen Limin;Fu Mingli;Wu Junliang;Ye Daiqi
采用水热浸渍法制备了不同形状的CeO2（纳米棒、纳米颗粒和纳米立方）的Ag/CeO2催化剂，并将其用于低温催化氧化HCHO。TEM和XRD结果表明，Ag纳米颗粒在CeO2表面分散良好。XPS、H2-TPR和拉曼光谱结果表明，Ag/r-CeO2、Ag/p- ceo2和Ag/c- ceo2表现出不同的氧空位浓度，Ag/r-CeO2中存在较多的氧空位和表面化学吸附氧。Ag与CeO2之间可能存在协同作用，Ag纳米粒子的存在可以促进表面化学吸附氧的活化，有利于HCHO氧化。催化剂的催化性能与CeO2的形状密切相关，Ag/r-CeO2具有最高的表面氧空位浓度和最佳的还原性，对HCHO氧化表现出最佳的催化活性。Ag/r- ceo2在HCHO浓度为810 ppm和GHSV浓度为84,000 h−1时的比反应速率为7.43 nmol/(s·m2)， TOFAg在100 °C时的比反应速率为0.0071 s−1。Ag/r- ceo2在110 ℃左右可以达到完全的HCHO氧化，低于Ag/p- ceo2和Ag/ C - ceo2。Ag/r- ceo2具有较高的低温还原性、更多的表面氧空位、表面晶格氧种类以及Ag与ceo2相互作用产生的晶格缺陷，这些都是Ag/r- ceo2对HCHO氧化具有优异催化性能的原因。这些结果表明，HCHO催化氧化活性依赖于ceo_2载体的形状，本研究表明，金属/ ceo_2催化剂的催化活性可以通过修饰ceo_2载体的形状来调节。
Ag/CeO2catalysts with various shapes of CeO2(nanorods, nanoparticles, and nanocubes) were prepared by the hydrothermal and impregnation method and then used for the catalytic oxidation of HCHO at low temperature. TEM and XRD results showed that Ag nanoparticles were well dispersed on the surface of CeO2. According to the results from XPS, H2-TPR and Raman spectra, Ag/r-CeO2, Ag/p-CeO2and Ag/c-CeO2exhibited different oxygen vacancy concentration, more oxygen vacancy and surface chemisorbed oxygen formed in Ag/r-CeO2. There might existed synergetic interaction between Ag and CeO2, and the presence of Ag nanoparticles could promoted the activation of surface chemisorbed oxygen, which is favorable for HCHO oxidation. The catalytic properties of the catalysts were significantly dependent on the shapes of CeO2, due to the highest surface oxygen vacancy concentration and best reducibility, Ag/r-CeO2exhibited the best catalytic activity for HCHO oxidation. Ag/r-CeO2showed higher specific reaction rate (7.43 nmol/(s·m2) at 100 °C) and TOFAg(0.0071 s−1at 100 °C) under 810 ppm of HCHO and 84,000 h−1of GHSV. Ag/r-CeO2could reach complete HCHO oxidation at around 110 °C, which was lower than that of Ag/p-CeO2and Ag/c-CeO2. Higher low-temperature reducibility, more surface oxygen vacancies, surface lattice oxygen species, and lattice defects produced by the interaction of Ag and CeO2contributed to the excellent catalytic performance of Ag/r-CeO2for HCHO oxidation. These results revealed that the HCHO catalytic oxidation activity was dependent on the shapes of CeO2supports, this study suggested that the catalytic activity of the metal/CeO2catalysts can be regulated by engineering the shapes of CeO2supports.
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