不同合成法对Ce-MnOx选择性催化氧化NH3性能的影响

盛雨佳; 陈冬; 刘海波; 陈天虎; 束道兵; 张斌

doi:10.13205/j.hjgc.202201010

不同合成法对Ce-MnO_x选择性催化氧化NH₃性能的影响

doi: 10.13205/j.hjgc.202201010

合肥工业大学资源与环境工程学院纳米矿物与污染控制安徽普通高校重点实验室, 合肥 230009

基金项目:

国家自然科学基金项目(41672040)

详细信息

作者简介:
盛雨佳(1996-),男,硕士,主要研究方向为环境工程材料。290852795@qq.com

通讯作者:
陈冬(1980-),男,博士,副教授,主要研究方向为环境工程材料。cdxman@hfut.edu.cn

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- 被引次数: 0
出版历程
- 收稿日期: 2021-01-12
- 网络出版日期: 2022-03-30
- 刊出日期: 2022-03-30

EFFECT OF SYNTHESIS METHOD ON PERFORMANCE OF Ce-MnO_x FOR SELECTIVE CATALYTIC OXIDATION OF AMMONIA

Key Laboratory of Nano-minerals and Pollution Control of Anhui Higher Education Institutes, School of Resources & Environmental Engineering, Hefei University of Technology, Hefei 230009, China

摘要

摘要: 分别采用水热法和浸渍法2种合成方法制备了Ce-MnO_x催化剂,应用于氨的选择性催化氧化。实验结果表明:水热法制备的Ce-MnO_x具有更高的催化氧化NH₃活性,其中,在反应温度为200℃时,Ce(5)-MnO_x(HY)具有98%的NH₃转化率及91%的N₂选择性。XRD、BET、Raman、XPS、SEM、H₂-TPR等方法对催化剂的表征结果表明,水热法合成的Ce-MnO_x具有更大的比表面积(94.37 m²/g),其优异的催化活性归因于表面丰富的Mn⁴⁺和Ce³⁺、大量的化学吸附氧、丰富的活性位点、Mn和Ce间的相互作用等。In-situ DRIFTS分析表明,催化剂表面吸附态的NH₃经过脱氢作用生成—NH₂、—NH中间体,其中,—NH与原子氧结合生成的—HNO能被O₂快速氧化形成NO,NO再与—NH₂继续反应生成N₂和H₂O。研究可为锰基催化剂在低温氨氧化及选择性方面的研究提供重要参考。
- 氨气 /
- 选择性催化氧化 /
- 水热法 /
- 浸渍法 /
- Ce-MnOx
Abstract: In this paper, Ce-MnO_x was prepared for selective catalytic oxidation(SCO) of ammonia by hydrothermal and impregnation method respectively. The results demonstrated that Ce-MnO_x catalysts exhibited the best NH₃ oxidation activity which composited by hydrothermal method. Among them, Ce(5)-MnO_x(HY) reached 98% of NH₃ conversion rate and 91% of N₂ selectivity, at reaction temperature of 200 ℃. The properties of the Ce-MnO_x catalysts were analyzed by XRD, BET, Raman, XPS, SEM, and H₂-TPR. Hydrothermally prepared Ce-MnO_x possessed larger surface area(94.37 m²/g). At the same time, the distinguished catalytic activity of Ce-MnO_x was attributed to abundant Mn⁴⁺ and Ce³⁺, high adsorbed oxygen concentration on the surface, a large number of active sites, and interaction between Mn and Ce. The results of in-situ DRIFTS showed that the —NH₂ and —NH intermediates could be generated by adsorbed NH₃ dehydrogenation. Consequently, —NH and atomic oxygen combined to form —HNO, which could be quickly oxidized to NO by O₂. Finally, N₂ and H₂O were formed during the following reaction of NO with —NH₂. This dissertation has significant reference value for the study of manganese-based catalysts in low-temperature ammonia oxidation and selectivity.
- ammonia /
- selective catalytic oxidation /
- hydrothermal /
- impregnation /
- Ce-MnO_x

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