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室温下 Co3O4-Ce2 和 Au/Co3O4-CeO2 催化剂上甲醛氧化的研究:有效去除和反应机理的确定。

Investigation of formaldehyde oxidation over Co3O4-Ce2 and Au/Co3O4-CeO2 catalysts at room temperature: effective removal and determination of reaction mechanism.

机构信息

State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences , Beijing 100085, PR China.

出版信息

Environ Sci Technol. 2011 Apr 15;45(8):3628-34. doi: 10.1021/es104146v. Epub 2011 Mar 4.

DOI:10.1021/es104146v
PMID:21375237
Abstract

Formaldehyde is regarded as the major indoor pollutant emitted from widely used building and decorative materials in airtight buildings, which should be eliminated under indoor environmental conditions. We report here catalytic oxidation process of formaldehyde over mesoporous Co(3)O(4), Co(3)O(4)-CeO(2), Au/Co(3)O(4), and Au/Co(3)O(4)-CeO(2) catalysts and their excellent catalytic performances at room temperature. These catalysts were prepared by a "nanocasting" method with the mesostructure generated from SBA-15 silica with 2D structure. The adsorbed surface species in the formaldehyde oxidation process are analyzed, and some key steps in the oxidation pathway, active sites, and intermediate species are proposed. Among the detected species, some kinds of formate species formed on the catalysts were indentified as intermediates, which further transformed into bicarbonate or carbonate and which decomposed to carbon dioxide. The role of the mesoporous Co(3)O(4) and the gold nanoparticles in the mechanism are also revealed.

摘要

甲醛被认为是密闭建筑中广泛使用的建筑和装饰材料释放的主要室内污染物,应在室内环境条件下予以消除。我们在此报告介孔 Co(3)O(4)、Co(3)O(4)-CeO(2)、Au/Co(3)O(4 和 Au/Co(3)O(4)-CeO(2)催化剂上甲醛的催化氧化过程及其在室温下的优异催化性能。这些催化剂是通过具有二维结构的 SBA-15 硅的“纳米铸造”方法制备的,具有介孔结构。分析了甲醛氧化过程中吸附的表面物种,并提出了氧化途径、活性位和中间物种的一些关键步骤。在所检测的物种中,一些在催化剂上形成的甲酸盐物种被鉴定为中间体,进一步转化为碳酸氢盐或碳酸盐,并分解为二氧化碳。还揭示了介孔 Co(3)O(4 和金纳米粒子在该机制中的作用。

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