活性炭表面模拟烟气与元素汞间均/异相氧化反应特性

doi:10.3969/j.issn.0438-1157.2012.05.031

化工学报 ›› 2012, Vol. 63 ›› Issue (5): 1536-1542.DOI: 10.3969/j.issn.0438-1157.2012.05.031

活性炭表面模拟烟气与元素汞间均/异相氧化反应特性

胡长兴1，周劲松2，李建新1，王永川1，郑皎1，徐美娟1，骆仲泱2

1浙江大学宁波理工学院；2能源清洁利用国家重点实验室（浙江大学）

收稿日期:2011-09-19 修回日期:2012-01-12 出版日期:2012-05-05 发布日期:2012-05-05
通讯作者: 胡长兴

Characteristics of homogeneous/heterogeneous oxidation reaction between simulated flue gas and elemental mercury on surface of activated carbon

HU Changxing1，ZHOU Jinsong2，LI Jianxin1，WANG Yongchuan1，ZHENG Jiao1，XU Meijuan1，LUO Zhongyang2

1Ningbo Institute of Technology，Zhejiang University；2State Key Laboratory of Clean Energy Utilization，Zhejiang University

Received:2011-09-19 Revised:2012-01-12 Online:2012-05-05 Published:2012-05-05

摘要/Abstract

摘要： 通过固定床吸附实验，在130℃温度下模拟研究燃煤烟气组分在椰壳活性炭(CS-AC)表面吸附气态元素汞(Hg⁰)过程中的作用与影响，揭示模拟烟气组分、Hg⁰以及活性炭表面三者间的均相、异相氧化反应特性。实验研究了CS-AC在N₂和模拟烟气气氛下对Hg⁰的吸附，模拟烟气组分与Hg⁰间的均相氧化反应，以及吸附模拟烟气组分后CS-AC在N₂气氛下对Hg⁰的吸附。研究表明在N₂气氛下CS-AC对Hg⁰不具备物理吸附的能力，而在模拟烟气组分下CS-AC对Hg⁰具有较强的吸附能力，初始吸附效率达80%。仅在模拟烟气均相反应作用下，大约只有14%的Hg⁰被氧化为Hg²⁺。经过预先跟常规模拟烟气吸附反应，CS-AC表面具备一定氧化性化学元素基团（如NO_x）后，能够在N₂气氛下对Hg⁰进行化学吸附，初始吸附效率达67%左右。可以认为模拟烟气和Hg⁰两者间的均相作用不是促进CS-AC在模拟烟气组分下对Hg⁰具有较强的吸附能力的主因。活性炭吸附Hg⁰的过程中，活性炭表面在烟气组分氧化Hg⁰的过程中起到了积极的促进作用。无论在N₂气氛下，还是在模拟烟气下，CS-AC吸附Hg⁰是气氛中氧化性组分、Hg⁰和活性炭表面三者间的异相化学氧化吸附反应过程。

关键词: 活性炭, 元素汞, 化学吸附, 异相反应

Abstract: The role and effect of simulated flue gas on adsorption of elemental mercury (Hg⁰)on coconut shell activated carbon (CS-AC)were studied by adsorption experiment carried out at 130℃ in a bench-scale fixed bed to reveal the characteristics of homogeneous/heterogeneous oxidation reaction between components of simulated flue gas，Hg⁰ and CS-AS surface.The experiments were divided into three parts：first，adsorption of Hg⁰ on surface of CS-AC in nitrogen (N₂)gas and simulated flue gas; second，homogeneous oxidation reaction between the components of simulated flue gas and Hg⁰; and third，adsorption of Hg⁰ in N₂ gas on surface of CS-AC pre-adsorbed by simulated flue gas.The results showed that CS-AC can not adsorb Hg⁰ in N₂ gas，however，it became easy in simulated flue gas and the initial adsorption efficiency was up to 80%.According to the result of homogeneous reaction between the simulated flue gas and Hg⁰ at the temperature of 130℃，only about 14% of Hg⁰ can be oxidized to divalent mercury (Hg²⁺)which is easily adsorbed by CS-AC，which was much lower than 80% of initial Hg⁰ adsorption efficiency in the simulated flue gas.This result could indicate that homogeneous reaction between simulated flue gas and Hg⁰ was not the main reason of high Hg⁰ adsorption efficiency.It was very interesting that in N₂ gas Hg⁰ could be adsorbed by CS-AC if it was pre-treated with simulated flue gas without Hg⁰.The pre-adsorption process of simulated flue gas could fix some components in flue gas，such as NO_x，etc.，on surface of CS-AC，and these components would help adsorption of Hg⁰ in N₂ gas，and the initial adsorption efficiency was about 67%.During the oxidation adsorption process，surface of CS-AC played important role.Therefore，it could be thought that the adsorption process of Hg⁰ by CS-AC is a heterogeneous chemical oxidation reaction and adsorption process between oxidizing components in flue gas，element mercury Hg⁰ and the CS-AC’s surface，whatever in N₂ gas or in simulated flue gas.

Key words: activated carbon；elemental mercury；chemical adsorption, heterogeneous reaction

中图分类号:

TQ 534.9

胡长兴，周劲松，李建新，王永川，郑皎，徐美娟，骆仲泱. 活性炭表面模拟烟气与元素汞间均/异相氧化反应特性[J]. 化工学报, 2012, 63(5): 1536-1542.

HU Changxing，ZHOU Jinsong，LI Jianxin，WANG Yongchuan，ZHENG Jiao，XU Meijuan，LUO Zhongyang. Characteristics of homogeneous/heterogeneous oxidation reaction between simulated flue gas and elemental mercury on surface of activated carbon[J]. CIESC Journal, 2012, 63(5): 1536-1542.

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活性炭表面模拟烟气与元素汞间均/异相氧化反应特性

Characteristics of homogeneous/heterogeneous oxidation reaction between simulated flue gas and elemental mercury on surface of activated carbon

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