改性镍铝催化剂氧化零价汞及抗氨干扰机理

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摘要采用尿素水解法制备NiAlO和NiAlMO(M=Zn、Ba、Mn、La、Cr)催化剂用于Hg⁰催化氧化研究.结果表明, 在NH₃存在时, NiAlZnO催化剂展现出最好的Hg⁰氧化活性, 250 ℃时Hg⁰的转化率超过80%, 并在350 ℃达到最高(90%).Raman和XPS结果显示, Zn掺杂构成Ni-O-Zn固溶体, 引起NiAlZnO催化剂的Jahn-Teller畸变, 使催化剂产生大量的氧空位, 促进O₂的活化, 提高了催化剂的表面化学吸附氧含量.H₂-TPR和Hg⁰-TPD结果表明, Zn的掺杂能提高催化剂的氧化还原性和Hg⁰的吸附量, 使催化剂在NH₃存在时依然保持高的Hg⁰吸附性能.NH₃-TPD和NH₃-DRIFT证实Zn掺杂为催化剂引入新的Hg⁰吸附位点(B酸位点).因此, NiAlZnO催化剂展现出优异的Hg⁰氧化活性和抗NH₃干扰性能.

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关键词 ： NiAlZnO催化剂, Hg⁰氧化, Hg⁰吸附, 抗NH₃干扰

Abstract：NiAlO and NiAlMO (M=Zn、Ba、Mn、La、Cr) catalysts were prepared to evaluate the efficiency of Hg⁰ oxidation of NiAlZnO catalyst using urea hydrolyzation, Raman and XPS experiments, etc. The results indicate that NiAlZnO catalyst exhibited the highest Hg⁰ oxidation activity in the presence of NH₃ and the Hg⁰ oxidation efficiency of NiAlZnO catalyst was above 80% at 250℃ and reached 90% at 350℃. Doping Zn enabled the NiAlZnO catalyst to form Ni-O-Zn solid solution and generate Jahn-Teller distortions which could increase the content of surface chemisorbed oxygen and promote the activation of O₂, and thus increase the surface chemisorption oxygen content of catalyst. The incorporation of Zn could improve the redox and Hg⁰ adsorption performance of NiAlZnO catalyst, even in the presence of NH₃. NH₃-TPD and NH₃-DRIFT experiments also proved that the addition of Zn introduced the new Hg⁰ adsorption site (B acid site) for NiAlZnO catalyst. Obviously, NiAlZnO catalyst can greatly promote Hg⁰ oxidation and possesses the resistance to NH₃ interference.

Key words： NiAlZnO catalyst Hg⁰ oxidation Hg⁰ adsorption anti-NH₃ interference

收稿日期: 2021-06-03

PACS:

X505

通讯作者: 常化振, 教授, chz@ruc.edu.cn E-mail: chz@ruc.edu.cn

作者简介: 邱磊(1996-), 男, 四川邻水人, 中国人民大学硕士研究生, 研究方向为大气污染控制

引用本文:

邱磊, 郭磊, 韩金池, 余杰, 常化振. 改性镍铝催化剂氧化零价汞及抗氨干扰机理[J]. 中国环境科学, 2022, 42(1): 11-19. QIU Lei, GUO Lei, HAN Jin-chi, YU Jie, CHANG Hua-zhen. Hg⁰ oxidation of modified Ni-Al catalysts and its anti-ammonia interference mechanism. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(1): 11-19.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2022/V42/I1/11

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