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On-line Access: 2023-01-20

Received: 2022-07-14

Revision Accepted: 2022-08-18

Crosschecked: 2023-02-01

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Citations:  Bibtex RefMan EndNote GB/T7714

 ORCID:

Dong YE

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

Hai-ning WANG

https://orcid.org/0000-0003-4653-0819

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Journal of Zhejiang University SCIENCE A 2023 Vol.24 No.1 P.80-90

http://doi.org/10.1631/jzus.A2200388


Mechanistic investigation on Hg0 capture over MnOx adsorbents: effects of the synthesis methods


Author(s):  Dong YE, Yongjin HU, Zhichang JIANG, Xin LIU, Haining WANG

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

Corresponding email(s):   Richard32@126.com, whnfyy@163.com

Key Words:  Synthesis methods, Hg0 capture, MnOx, Acidity, Oxidative ability


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Dong YE, Yongjin HU, Zhichang JIANG, Xin LIU, Haining WANG. Mechanistic investigation on Hg0 capture over MnOx adsorbents: effects of the synthesis methods[J]. Journal of Zhejiang University Science A, 2023, 24(1): 80-90.

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author="Dong YE, Yongjin HU, Zhichang JIANG, Xin LIU, Haining WANG",
journal="Journal of Zhejiang University Science A",
volume="24",
number="1",
pages="80-90",
year="2023",
publisher="Zhejiang University Press & Springer",
doi="10.1631/jzus.A2200388"
}

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%T Mechanistic investigation on Hg0 capture over MnOx adsorbents: effects of the synthesis methods
%A Dong YE
%A Yongjin HU
%A Zhichang JIANG
%A Xin LIU
%A Haining WANG
%J Journal of Zhejiang University SCIENCE A
%V 24
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%@ 1673-565X
%D 2023
%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A2200388

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T1 - Mechanistic investigation on Hg0 capture over MnOx adsorbents: effects of the synthesis methods
A1 - Dong YE
A1 - Yongjin HU
A1 - Zhichang JIANG
A1 - Xin LIU
A1 - Haining WANG
J0 - Journal of Zhejiang University Science A
VL - 24
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PB - Zhejiang University Press & Springer
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DOI - 10.1631/jzus.A2200388


Abstract: 
This study demonstrated the impacts of the synthesis methods on the textural structures, chemical properties, and hg0 capture capability of the mnOx system. Compared with the samples synthesized using the precipitation (PR) and hydrothermal (HT) methods, the adsorbent prepared via the sol-gel (SG) technique gave the best performance. At 150 °C, ca. 90% Hg0 removal efficiency was reached after 7.5 h for mnOx prepared by the SG method, ca. 40% higher than that of the other two methods. The specific surface area of the adsorbent synthesized via the SG technique (23 m2/g) was almost double that of the adsorbent prepared by the HT method (12 m2/g) and three times that of the one prepared by the PR method (7 m2/g). The presence of plentiful acid sites from the SG method facilitated the physisorption of Hg0, making more Hg0 available to be oxidized to HgO by the redox sites and thus giving the adsorbent prepared by the SG method the highest Hg0 removal efficiency. The strong oxidative ability accelerated the oxidation of the physically adsorbed Hg0 to HgO, which explained the higher Hg0 removal efficiency of the sample prepared using the HT method than that of the one synthesized by the PR technique. During the whole Hg0 removal cycles, chemisorption dominated, with the initial adsorption stage and the external mass-transfer process playing important roles.

锰氧化物吸附剂脱汞性能及其机理研究:制备方法的影响

作者:叶栋,胡永金,蒋志昌,刘欣,王海宁
机构:中国计量大学,质量与安全工程学院,中国杭州,310018
目的:针对当前单质汞高效脱除难题,本文旨在探讨不同制备方法对锰氧化物吸附剂单质汞捕集性能的影响,并通过对吸附剂物理化学性质的研究,揭示锰氧化物吸附剂的构效关系及脱汞机理。
创新点:1.揭示锰氧化物吸附剂脱汞性能与物化性质之间的构效关系;2.阐明锰氧化物吸附剂表面脱汞机理,并揭示其中的活性位点。
方法:1.采用常规的沉淀法、水热法及溶胶凝胶法合成锰氧化物吸附剂;2.采用微型固定床反应器研究系列锰吸附剂的脱汞性能;3.采用物化表征研究系列锰氧化物汞吸附剂的物化特性,揭示其中的构效关系;4.结合动力学计算,揭示锰氧化物汞吸附剂表面脱汞机理,并阐明影响吸附剂脱汞性能的关键因素。
结论:1.与采用沉淀法及水热法制备的汞吸附剂相比,采用溶胶凝胶法制备的汞吸附剂在150~250°C的温度区间内具有更为优异的脱汞性能;2.采用溶胶凝胶法制备的锰氧化物吸附剂具有丰富的表面酸性位点,可促进单质汞的吸附,并为接下来的单质汞氧化步骤提供充足的反应物,这也是该吸附剂具有优异脱汞性能的主要原因;3.脱汞过程中,初始吸附阶段是主要的速控阶段,而Mn4+及化学吸附氧为该反应中的主要活性位点。

关键词:合成方法;汞捕集;锰氧化物;酸性;氧化性

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