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On-line Access: 2024-08-27

Received: 2023-10-17

Revision Accepted: 2024-05-08

Crosschecked: 2024-08-20

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Citations:  Bibtex RefMan EndNote GB/T7714

 ORCID:

Dong YE

https://orcid.org/0000-0001-8299-224X

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Journal of Zhejiang University SCIENCE A 2024 Vol.25 No.8 P.680-686

http://doi.org/10.1631/jzus.A2300276


Enhancement in the Hg0 oxidation efficiency and sulfur resistance of CuCl2-modified MnOx-CeOx nanorod catalysts


Author(s):  Shujie GAO, Yongjin HU, Zhichang JIANG, Xiaoxiang WANG, Dong YE, Changxing HU

Affiliation(s):  College of Quality & Safety Engineering, China Jiliang University, Hangzhou 310018, China; more

Corresponding email(s):   Richard32@126.com, huchx@zju.edu.cn

Key Words:  Hg0 oxidation, CuCl2 modification, MnOx-CeOx nanorods, Sulfur resistance, Oxidation activity


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Shujie GAO, Yongjin HU, Zhichang JIANG, Xiaoxiang WANG, Dong YE, Changxing HU. Enhancement in the Hg0 oxidation efficiency and sulfur resistance of CuCl2-modified MnOx-CeOx nanorod catalysts[J]. Journal of Zhejiang University Science A, 2024, 25(8): 680-686.

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author="Shujie GAO, Yongjin HU, Zhichang JIANG, Xiaoxiang WANG, Dong YE, Changxing HU",
journal="Journal of Zhejiang University Science A",
volume="25",
number="8",
pages="680-686",
year="2024",
publisher="Zhejiang University Press & Springer",
doi="10.1631/jzus.A2300276"
}

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%T Enhancement in the Hg0 oxidation efficiency and sulfur resistance of CuCl2-modified MnOx-CeOx nanorod catalysts
%A Shujie GAO
%A Yongjin HU
%A Zhichang JIANG
%A Xiaoxiang WANG
%A Dong YE
%A Changxing HU
%J Journal of Zhejiang University SCIENCE A
%V 25
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%D 2024
%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A2300276

TY - JOUR
T1 - Enhancement in the Hg0 oxidation efficiency and sulfur resistance of CuCl2-modified MnOx-CeOx nanorod catalysts
A1 - Shujie GAO
A1 - Yongjin HU
A1 - Zhichang JIANG
A1 - Xiaoxiang WANG
A1 - Dong YE
A1 - Changxing HU
J0 - Journal of Zhejiang University Science A
VL - 25
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SP - 680
EP - 686
%@ 1673-565X
Y1 - 2024
PB - Zhejiang University Press & Springer
ER -
DOI - 10.1631/jzus.A2300276


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-.

CuCl2改性对MnOx-CeOx纳米棒催化剂汞氧化性能及抗硫性能的提升机理研究

作者:高淑洁1,胡永金1,蒋志昌1,王晓祥2,叶栋1,胡长兴3
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。

关键词:汞氧化;CuCl2改性;锰铈氧化物纳米棒;抗硫性能;氧化活性

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Reference

[1]BaltrusJP, GraniteEJ, StankoDC, et al., 2008. Surface characterization of Pd/Al2O3 sorbents for mercury capture from fuel gas. Main Group Chemistry, 7(3):217-225.

[2]ChalkidisA, JampaiahD, HartleyPG, et al., 2019. Regenerable α‍-MnO2 nanotubes for elemental mercury removal from natural gas. Fuel Processing Technology, 193:317-327.

[3]GallowayB, RoykoM, SasmazE, et al., 2018. Mercury oxidation over Cu-SSZ-13 catalysts under flue gas conditions. Chemical Engineering Journal, 336:253-262.

[4]JampaiahD, ChalkidisA, SabriYM, et al., 2019a. Low-temperature elemental mercury removal over TiO2 nanorods-supported MnOx-FeOx-CrOx. Catalysis Today, 324:174-182.

[5]JampaiahD, ChalkidisA, SabriYM, et al., 2019b. Role of ceria in the design of composite materials for elemental mercury removal. The Chemical Record, 19(7):1407-1419.

[6]JiPD, GaoX, DuXS, et al., 2016. Relationship between the molecular structure of V2O5/TiO2 catalysts and the reactivity of SO2 oxidation. Catalysis Science & Technology, 6(4):1187-1194.

[7]JiangY, LuMY, LiuSJ, et al., 2018. Deactivation by HCl of CeO2-MoO3/TiO2 catalyst for selective catalytic reduction of NO with NH3. RSC Advances, 8(32):17677-17684.

[8]LiHH, WangSK, WangX, et al., 2017. Activity of CuCl2-modified cobalt catalyst supported on Ti-Ce composite for simultaneous catalytic oxidation of Hg0 and NO in a simulated pre-sco process. Chemical Engineering Journal, 316:1103-1113.

[9]LiHH, ZhangJD, CaoYX, et al., 2020. Enhanced activity and SO2 resistance of co-modified CeO2-TiO2 catalyst prepared by facile co-precipitation for elemental mercury removal in flue gas. Applied Organometallic Chemistry, 34(4):e5463.

[10]LiHL, WuCY, LiY, et al., 2012. Superior activity of MnOx-CeO2/TiO2 catalyst for catalytic oxidation of elemental mercury at low flue gas temperatures. Applied Catalysis B: Environmental, 111-112:381-388.

[11]LiX, LiuZY, KimJ, et al., 2013. Heterogeneous catalytic reaction of elemental mercury vapor over cupric chloride for mercury emissions control. Applied Catalysis B: Environmental, 132-133:401-407.

[12]LiuH, ChangL, LiuWJ, et al., 2020. Advances in mercury removal from coal-fired flue gas by mineral adsorbents. Chemical Engineering Journal, 379:122263.

[13]LiuZY, LiX, LeeJY, et al., 2015. Oxidation of elemental mercury vapor over γ-Al2O3 supported CuCl2 catalyst for mercury emissions control. Chemical Engineering Journal, 275:1-7.

[14]MaYP, MuBL, ZhangXJ, et al., 2019. Graphene enhanced Mn-Ce binary metal oxides for catalytic oxidation and adsorption of elemental mercury from coal-fired flue gas. Chemical Engineering Journal, 358:1499-1506.

[15]SingKSW, 1985. Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity. Pure and Applied Chemistry, 57(4):603-619.

[16]WangPY, SuS, XiangJ, et al., 2014. Catalytic oxidation of Hg0 by MnOx-CeO2/γ-Al2O3 catalyst at low temperatures. Chemosphere, 101:49-54.

[17]WuJ, ZhaoZ, HuangTF, et al., 2017. Removal of elemental mercury by Ce-Mn co-modified activated carbon catalyst. Catalysis Communications, 93:62-66.

[18]YangSJ, GuoYF, YanNQ, et al., 2011. Elemental mercury capture from flue gas by magnetic Mn-Fe spinel: effect of chemical heterogeneity. Industrial & Engineering Chemistry Research, 50(16):9650-9656.

[19]YangYJ, LiuJ, ZhangBK, et al., 2017a. Density functional theory study on the heterogeneous reaction between Hg0 and HCl over spinel-type MnFe2O4. Chemical Engineering Journal, 308:897-903.

[20]YangYJ, LiuJ, ZhangBK, et al., 2017b. Experimental and theoretical studies of mercury oxidation over CeO2-WO3/TiO2 catalysts in coal-fired flue gas. Chemical Engineering Journal, 317:758-765.

[21]YeD, WangXX, LiuH, et al., 2020. Insights into the effects of sulfate species on CuO/TiO2 catalysts for NH3-SCR reactions. Molecular Catalysis, 496:111191.

[22]YeD, WangXX, WangRX, et al., 2021. Recent advances in MnO2-based adsorbents for mercury removal from coal-fired flue gas. Journal of Environmental Chemical Engineering, 9(5):105993.

[23]YeD, WangRX, WangXX, et al., 2022a. Improvement in the Hg0 removal performance of CeO2 by modifying with CuO. Applied Surface Science, 579:152200.

[24]YeD, WangXX, WangRX, et al., 2022b. Review of elemental mercury (Hg0) removal by CuO-based materials. Journal of Zhejiang University-SCIENCE A (Applied Physics & Engineering), 23(7):505-526.

[25]YeD, HuYJ, JiangZC, et al., 2023a. Mechanistic investigation on Hg0 capture over MnOx adsorbents: effects of the synthesis methods. Journal of Zhejiang University-SCIENCE A (Applied Physics & Engineering), 24(1):‍80-90.

[26]YeD, GaoSJ, WangYL, et al., 2023b. New insights into the morphological effects of MnOx-CeOx binary mixed oxides on Hg0 capture. Applied Surface Science, 613:156035.

[27]ZhangAC, ZhangZH, LuH, et al., 2015. Effect of promotion with Ru addition on the activity and SO2 resistance of MnOx-TiO2 adsorbent for Hg0 removal. Industrial & Engineering Chemistry Research, 54(11):2930-2939.

[28]ZhangD, HouLA, ChenGY, et al., 2018. Cr doping MnOx adsorbent significantly improving Hg0 removal and SO2 resistance from coal-fired flue gas and the mechanism investigation. Industrial & Engineering Chemistry Research, 57(50):17245-17258.

[29]ZhouZJ, LiuXW, HuYC, et al., 2018. An efficient sorbent based on CuCl2 loaded CeO2-ZrO2 for elemental mercury removal from chlorine-free flue gas. Fuel, 216:356-363.

[30]ZhouZJ, LiuL, LiuXW, et al., 2022. Catalytic oxidation of Hg0 over Mn-doped CeO2-ZrO2 solid solution and MnOx/CeO2-ZrO2 supported catalysts: characterization, catalytic activity and SO2 resistance. Fuel, 310:122317.

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