Pd/MnOx+Pd/γ-Al2O3整体式催化剂降解地表臭氧

引用本文: 周丽娜, 陈耀强, 任成军, 龚茂初. Pd/MnO_x+Pd/γ-Al₂O₃整体式催化剂降解地表臭氧[J]. 无机化学学报, 2013, 29(11): 2363-2369. doi: 10.3969/j.issn.1001-4861.2013.00.357 shu

Citation: ZHOU Li-Na, CHEN Yao-Qiang, REN Cheng-Jun, GONG Mao-Chu. Pd/MnO_x+Pd/γ-Al₂O₃ Monolith Catalysts for Ground-Level Ozone Decomposition[J]. Chinese Journal of Inorganic Chemistry, 2013, 29(11): 2363-2369. doi: 10.3969/j.issn.1001-4861.2013.00.357 shu

Pd/MnO_x+Pd/γ-Al₂O₃整体式催化剂降解地表臭氧

基金项目:
四川大学化学学院基地能力提高项目基金(No.J1103315)资助项目。 (No.J1103315)

摘要: 用高锰酸钾与硝酸锰氧化还原反应制备了高活性的氧化锰(MnO_x)催化组分,用胶溶法制备了高比表面积的γ-Al₂O₃载体,分别用等体积浸渍法制备了Pd/MnO_x和Pd/γ-Al₂O₃催化剂,然后将两者机械混合涂覆于堇青石上制得Pd/MnO_x+Pd/γ-Al₂O₃整体式催化剂。采用X射线衍射(XRD)、X射线光电子能谱(XPS)、程序升温还原(H₂-TPR)和低温N₂吸附-脱附对催化剂进行了表征。考察了在300至700℃焙烧MnO_x对催化剂降解地表O₃活性的影响。结果表明,Pd和MnO_x之间存在协同作用;MnO_x焙烧温度对催化剂活性有一定的影响,其中以600℃焙烧时催化剂的活性最高,O₃的起始(12℃)转化率达到88%,完全转化温度为18℃。MnO_x的物相和催化剂表面的吸附氧物种对催化活性影响较大,适当比例的MnO₂和Mn₂O₃共存有利于O₃分解,表面吸附氧为O₃分解的活性氧物种。

关键词:

锰氧化物;钯;臭氧;催化降解;焙烧温度

English

Pd/MnO_x+Pd/γ-Al₂O₃ Monolith Catalysts for Ground-Level Ozone Decomposition

1.
Key Laboratory of Green Chemistry & Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, China
Received Date: 25 February 2013
Fund Project:
四川大学化学学院基地能力提高项目基金(No.J1103315)资助项目。

Abstract: Ahighly active MnO_x materials were prepared by an oxidation-reduction reaction between KMnO₄ and Mn(NO₃)₂. The γ-Al₂O₃ support with large surface area was synthesized by the peptizing method. Subsequently, Pd was loaded on MnO_x and γ-Al₂O₃ by incipient wetness impregnation, respectively. Then, the Pd/MnO_x and Pd/γ-Al₂O₃ were mixed and coated on the cordierite. Finally, the Pd/MnO_x+Pd/γ-Al₂O₃ monolithic catalysts were obtained. The catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Temperature-programmed reduction (H₂-TPR) and low temperature N₂ adsorption/desorption measurement, respectively. Asynergetic effect took place between Pd and MnO_x when O₃ was decomposed on the surface of the Pd/MnO_x+Pd/γ-Al₂O₃ catalysts. The effect of calcination temperature on the catalytic performance for the decomposition of ground-level ozone was investigated. It revealed that the activity of catalysts was considerably influenced by the calcination temperature of MnO_x. When the MnO_x was calcined at 600 ℃, the catalyst had the highest activity, where ozone conversion reached 88% at 12 ℃ and it was completely decomposed at 18 ℃. The results show that catalytic activity mainly depends on the MnO_x phase and oxygen species adsorbed on the surface of catalysts. The MnO₂ and Mn₂O₃ with proper proportion can efficiently promote the decomposition of ozone. And oxygen adsorbed on the surface of catalysts is active oxygen species during ozone decomposition.

Key words:

manganese oxide;palladium;ozone;catalytic decomposition;calcination temperature

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

Pd/MnO_x+Pd/γ-Al₂O₃整体式催化剂降解地表臭氧

English

Pd/MnO_x+Pd/γ-Al₂O₃ Monolith Catalysts for Ground-Level Ozone Decomposition

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