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Mn(x)Ce(1)-(x)O(2) 催化剂上甲醛的去除:热催化氧化与臭氧催化氧化。

Removal of formaldehyde over Mn(x)Ce(1)-(x)O(2) catalysts: thermal catalytic oxidation versus ozone catalytic oxidation.

机构信息

Graduate Institute of Environmental Engineering, National Central University, Chungli 32001, Taiwan, Chinese Taipei.

Industrial Technology Research Institute, Hsinchu 31040, Taiwan, Chinese Taipei.

出版信息

J Environ Sci (China). 2014 Dec 1;26(12):2546-53. doi: 10.1016/j.jes.2014.05.030. Epub 2014 Oct 22.

Abstract

Mn(x)Ce(1)-(x)O(2) (x: 0.3-0.9) prepared by Pechini method was used as a catalyst for the thermal catalytic oxidation of formaldehyde (HCHO). At x=0.3 and 0.5, most of the manganese was incorporated in the fluorite structure of CeO(2) to form a solid solution. The catalytic activity was best at x=0.5, at which the temperature of 100% removal rate is the lowest (270°C). The temperature for 100% removal of HCHO oxidation is reduced by approximately 40°C by loading 5wt.% CuO(x) into Mn(0.5)Ce(0.5)O(2). With ozone catalytic oxidation, HCHO (61 ppm) in gas stream was completely oxidized by adding 506 ppm O₃over Mn(0.5)Ce(0.5)O(2) catalyst with a GHSV (gas hourly space velocity) of 10,000 hr⁻¹ at 25°C. The effect of the molar ratio of O(3) to HCHO was also investigated. As O(3)/HCHO ratio was increased from 3 to 8, the removal efficiency of HCHO was increased from 83.3% to 100%. With O(3)/HCHO ratio of 8, the mineralization efficiency of HCHO to CO(2) was 86.1%. At 25°C, the p-type oxide semiconductor (Mn(0.5)Ce(0.5)O(2)) exhibited an excellent ozone decomposition efficiency of 99.2%, which significantly exceeded that of n-type oxide semiconductors such as TiO(2), which had a low ozone decomposition efficiency (9.81%). At a GHSV of 10,000 hr⁻¹, [O(3)]/[HCHO]=3 and temperature of 25°C, a high HCHO removal efficiency (≥ 81.2%) was maintained throughout the durability test of 80 hr, indicating the long-term stability of the catalyst for HCHO removal.

摘要

采用柠檬酸络合法制备的 Mn(x)Ce(1)-(x)O(2) (x: 0.3-0.9) 作为催化剂用于甲醛 (HCHO) 的热催化氧化。在 x=0.3 和 0.5 时,大部分锰掺入到 CeO(2) 的萤石结构中形成固溶体。在 x=0.5 时催化活性最佳,此时达到 100%去除率的温度最低(270°C)。通过在 Mn(0.5)Ce(0.5)O(2) 中负载 5wt.% CuO(x),可将 HCHO 氧化的 100%去除温度降低约 40°C。在气体流速为 10,000 hr⁻¹、臭氧浓度为 506 ppm 时,在 25°C 下,Mn(0.5)Ce(0.5)O(2) 催化剂对气相中浓度为 61 ppm 的 HCHO 进行催化氧化,可将其完全氧化。此外,还考察了 O(3)与 HCHO 的摩尔比的影响。当 O(3)/HCHO 从 3 增加到 8 时,HCHO 的去除效率从 83.3%增加到 100%。当 O(3)/HCHO 为 8 时,HCHO 向 CO(2)的矿化效率为 86.1%。在 25°C 下,p 型氧化物半导体 (Mn(0.5)Ce(0.5)O(2)) 对臭氧的分解效率高达 99.2%,显著高于 n 型氧化物半导体(TiO(2))的低臭氧分解效率(9.81%)。在 GHSV 为 10,000 hr⁻¹、[O(3)]/[HCHO]=3 和温度为 25°C 的条件下,在 80 小时的耐久性测试中,始终保持较高的 HCHO 去除效率(≥81.2%),表明该催化剂在去除 HCHO 方面具有长期稳定性。

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