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具有良好抗低温 HO 和 SO 性能的 MnNiO 尖晶石催化剂,用于高效选择性催化还原氮氧化物。

MnNiO spinel catalyst for high-efficiency selective catalytic reduction of nitrogen oxides with good resistance to HO and SO at low temperature.

机构信息

School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China; Beijing Key Laboratory of Resource-Oriented Treatment of Industrial Pollutants, University of Science and Technology Beijing, Beijing 100083, China.

School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China; Beijing Key Laboratory of Resource-Oriented Treatment of Industrial Pollutants, University of Science and Technology Beijing, Beijing 100083, China.

出版信息

J Environ Sci (China). 2020 Mar;89:145-155. doi: 10.1016/j.jes.2019.10.010. Epub 2019 Nov 9.

Abstract

Mn-Ni oxides with different compositions were prepared using standard co-precipitation (CP) and urea hydrolysis-precipitation (UH) methods and optimized for the selective catalytic reduction of nitrogen oxides (NO) by NH at low temperature. MnNiO-CP and MnNiO-UH (with Mn:Ni molar ratio of 2:1) catalysts showed almost identical selective catalytic reduction (SCR) catalytic activity, with about 96% NO conversion at 75°C and ~99% in the temperature range from 100 to 250°C. X-ray diffraction (XRD) results showed that MnNiO-CP and MnNiO-UH catalysts crystallized in the form of MnNiO and MnO-MnNiO spinel, respectively. The latter gave relatively good selectivity to N, which might be due to the presence of the MnO phase and high metal-O binding energy, resulting in low dehydrogenation ability. According to the results of various characterization methods, it was found that a high density of surface chemisorbed oxygen species and efficient electron transfer between Mn and Ni in the crystal structure of MnNiO spinel played important roles in the high-efficiency SCR activity of these catalysts. MnNiO catalysts presented good resistance to HO or/and SO with stable activity, which benefited from the MnNiO spinel structure and Eley-Rideal mechanism, with only slight effects from SO.

摘要

采用标准共沉淀(CP)和尿素水解沉淀(UH)法制备了不同组成的 Mn-Ni 氧化物,并对其进行了优化,以在低温下通过 NH 选择性催化还原(SCR)氮氧化物(NO)。MnNiO-CP 和 MnNiO-UH(Mn:Ni 摩尔比为 2:1)催化剂具有几乎相同的选择性催化还原(SCR)催化活性,在 75°C 时的 NO 转化率约为 96%,在 100 至 250°C 的温度范围内约为 99%。X 射线衍射(XRD)结果表明,MnNiO-CP 和 MnNiO-UH 催化剂分别以 MnNiO 和 MnO-MnNiO 尖晶石的形式结晶。后者对 N 的选择性相对较好,这可能是由于 MnO 相的存在和金属-O 结合能高,导致脱氢能力低。根据各种表征方法的结果,发现 MnNiO 尖晶石晶体结构中表面化学吸附氧物种的高密度和 Mn 和 Ni 之间有效的电子转移对这些催化剂的高效 SCR 活性起着重要作用。MnNiO 催化剂表现出良好的抗 HO 或/和 SO 性能,活性稳定,这得益于 MnNiO 尖晶石结构和 Eley-Rideal 机制,仅受到 SO 的轻微影响。

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