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Journal of Zhejiang University SCIENCE A
ISSN 1673-565X(Print), 1862-1775(Online), Monthly
2024 Vol.25 No.8 P.680-686
Enhancement in the Hg0 oxidation efficiency and sulfur resistance of CuCl2-modified MnOx-CeOx nanorod catalysts
Abstract: In this study, a series of CuCl2-modified MnOx-CeOx nanorods were synthesized for the oxidation of Hg0. The addition of CuCl2 resulted in an enhancement in the catalyst's Hg0 oxidation ability, and Hg0 oxidation efficiency reached >97% from 150 to 250 °C. In the MnOx-CeOx catalysts, Mn4+ played the role of the active species for Hg0 oxidization, but in the CuCl2-doped catalysts Cl- also contributed to Hg0 oxidation, conferring the superior performance of these samples. The introduction of SO2 led to a decrease in the availability of Mn4+, and the Hg0 oxidation efficiency of MnOx-CeOx decreased from about 100% to about 78%. By contrast, CuCl2-promoted samples maintained a Hg0 oxidation efficiency of about 100% during the SO2 deactivation cycle due to the high reactivity of Cl-.
Key words: Hg0 oxidation; CuCl2 modification; MnOx-CeOx nanorods; Sulfur resistance; Oxidation activity
机构：1中国计量大学，质量与安全工程学院，中国杭州，310018；2浙江大学，化工学院，工业生态与环境研究所，中国杭州，310027；3浙大宁波理工学院，机电与能源工程学院，中国宁波，315100
目的：针对燃煤电站多变的烟气条件，研究适用于高汞、含硫烟气的催化剂。
创新点：1.通过水热法合成锰铈氧化物纳米棒，可实现高汞含硫烟气条件下的高效脱汞；2.通过添加CuCl2，在保证催化剂的汞氧化性能的同时，提升其抗硫性能。
方法：利用固定床微反应器对催化剂的汞氧化性能进行研究，并结合物化表征建立催化剂的构效关系，进而揭示CuCl2改性催化剂的抗硫机理。
结论：1.添加CuCl2提升了催化剂的汞氧化性能：在150~250°C温度区间内，催化剂的汞养护效率为100%；在含硫气氛下反应320 min后，锰铈氧化物的汞氧化效率由100%下降到78%；对于CuCl2改性催化剂，共氧化性能依旧维持在100%。2.对于锰铈氧化物催化剂，Mn4+为主要的活性位点；对于CuCl2改性催化剂，除了Mn4+外，Cl?也是其中的活性位点。3.在含硫气氛下，Mn4+利用量的下降是导致锰铈氧化物催化剂活性下降的主要原因，而高反应活性Cl?的存在是CuCl2改性催化剂保持高汞脱除效率的主要原因。
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DOI:
10.1631/jzus.A2300276
CLC number:
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On-line Access:
2024-08-27
Received:
2023-10-17
Revision Accepted:
2024-05-08
Crosschecked:
2024-08-20