| 不同合成法对Ce-MnOx选择性催化氧化NH3性能的影响 |
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| 引用本文： | 盛雨佳,陈冬,刘海波,陈天虎,束道兵,张斌.不同合成法对Ce-MnOx选择性催化氧化NH3性能的影响[J].环境工程,2022,40(1):60-68. |
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| 作者姓名： | 盛雨佳 陈冬 刘海波 陈天虎 束道兵 张斌 |
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| 作者单位： | 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 |
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| 基金项目： | 国家自然科学基金项目(41672040)； |
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| 摘 要： | 分别采用水热法和浸渍法2种合成方法制备了Ce-MnOx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-MnOx具有更高的催化氧化NH3活性,其中,在反应温度为200℃时,Ce(5)-MnOx(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-MnOx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。
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| 关 键 词： | 氨气 选择性催化氧化 水热法 浸渍法 Ce-MnOx |
| 收稿时间： | 2021-01-12 |
EFFECT OF SYNTHESIS METHOD ON PERFORMANCE OF Ce-MnO_x FOR SELECTIVE CATALYTIC OXIDATION OF AMMONIA |
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| SHENG Yujia,CHEN Dong,LIU Haibo,CHEN Tianhu,SHU Daobing,ZHANG Bin.EFFECT OF SYNTHESIS METHOD ON PERFORMANCE OF Ce-MnO_x FOR SELECTIVE CATALYTIC OXIDATION OF AMMONIA[J].Environmental Engineering,2022,40(1):60-68. |
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| Authors: | SHENG Yujia CHEN Dong LIU Haibo CHEN Tianhu SHU Daobing ZHANG Bin |
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| Affiliation: | 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 |
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| Abstract: | In this paper, Ce-MnOx was prepared for selective catalytic oxidation(SCO) of ammonia by hydrothermal and impregnation method respectively. The results demonstrated that Ce-MnOx catalysts exhibited the best NH3 oxidation activity which composited by hydrothermal method. Among them, Ce(5)-MnOx(HY) reached 98% of NH3 conversion rate and 91% of N2 selectivity, at reaction temperature of 200 ℃. The properties of the Ce-MnOx catalysts were analyzed by XRD, BET, Raman, XPS, SEM, and H2-TPR. Hydrothermally prepared Ce-MnOx possessed larger surface area(94.37 m2/g). At the same time, the distinguished catalytic activity of Ce-MnOx 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. |
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