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V2O5/AC在含SO2气氛中对气态Hg0的吸附脱除研究
引用本文:王钧伟,杨建丽,刘振宇.V2O5/AC在含SO2气氛中对气态Hg0的吸附脱除研究[J].环境科学,2009,30(12):3455-3460.
作者姓名:王钧伟  杨建丽  刘振宇
作者单位:1. 中国科学院山西煤炭化学研究所煤转化国家重点实验室,太原,030001;中国科学院研究生院,北京,100049
2. 中国科学院山西煤炭化学研究所煤转化国家重点实验室,太原,030001
3. 北京化工大学化工资源有效利用国家重点实验室,北京,100029
基金项目:国家自然科学基金重点项目,煤转化国家重点实验室自主研究课题,国家高技术研究发展计划(863计划) 
摘    要:利用固定床反应器研究了模拟烟气(N_2、SO_2、O_2)气氛下,气态Hg~0在V_2O_5/AC催化剂上的吸附脱除行为.考察了V_2O_5担载量、SO_2浓度和吸附温度等对V_2O_5/AC吸附脱除Hg~0的影响,并对V_2O_5/AC上吸附汞的形态进行了XPS分析表征.研究发现,V_2O_5/AC对Hg~0的吸附能力远大于载体AC.汞的吸附量与V_2O_5/AC中V_2O_5的质量分数有关,随着V_2O_5质量分数从0.5%增加到1.0%,汞的吸附量从75.9 μg·g~(-1)增加到89.6 μg·g~(-1) (无氧) 和115.9 μg·g~(-1)增加到185.5 μg·g~(-1) (有氧),远高于相同吸附条件下的AC上的汞吸附量 (9.6 μg·g~(-1)和23.3 μg·g~(-1)).SO_2对Hg~0的吸附有促进作用,主要是由于SO_2和Hg~0在V_2O_5/AC上发生了化学反应.但是当SO_2体积分数从500×10~(-6)增加到2 000×10~(-6)时,V_2O_5/AC对汞的吸附量只增加了5%.不同温度下的实验结果表明,V_2O_5/AC催化剂在150℃左右的吸附脱除Hg~0的能力最高,汞的吸附量达到98.5 μg·g~(-1) (无氧) 和187.7 μg·g~(-1) (有氧).XPS 分析结果表明,在V_2O_5/AC催化剂表面有HgO和HgSO_4生成,证实了V_2O_5和SO_2的作用.

关 键 词:气态Hg~0  吸附  脱除
收稿时间:2009/1/15 0:00:00
修稿时间:2009/3/17 0:00:00

Adsorption and Removal of Gas-Phase Hg0 over a V2O5/AC Catalyst in the Presence of SO2
WANG Jun-wei,YANG Jian-li and LIU Zhen-yu.Adsorption and Removal of Gas-Phase Hg0 over a V2O5/AC Catalyst in the Presence of SO2[J].Chinese Journal of Environmental Science,2009,30(12):3455-3460.
Authors:WANG Jun-wei  YANG Jian-li and LIU Zhen-yu
Institution:WANG Jun-wei~(1,2),YANG Jian-li~1,LIU Zhen-yu~3(1.State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China,2.Graduate University of Chinese Academy of Sciences,Beijing 100049,3.State Key Laboratory of Chemical Resource Engineering,Beijing University of Chemical Technology,Beijing 100029,China)
Abstract:The adsorption and removal behaviors of gas-phase Hg~0 over V_2O_5/AC and AC were studied under a simulated flue gas (containing N_2, SO_2, O_2) in a fixed-bed reactor. The influences of the V_2O_5 loading, SO_2 concentration and adsorption temperature on Hg0 adsorption were investigated. The speciation of mercury adsorbed was determined by X-ray photoelectron spectroscopy (XPS). It was found that the V_2O_5/AC catalyst has a much higher capability than AC for Hg~0 adsorption and removal, mainly because of the catalytic oxidation activity of V_2O_5. The Hg~0 adsorption capability depends on the V_2O_5 content of the V_2O_5/AC catalyst. The amounts of mercury adsorbed increase from 75.9 μg·g~(-1) to 89.6 μg·g~(-1) (in the absence of O_2) and from 115.9 μg·g~(-1) to 185.5 μg·g~(-1) (in the presence of O_2) as the V_2O_5 loading increases from 0.5% to 1.0%,which are much higher than those over AC under the same conditions (9.6 μg·g~(-1) and 23.3 μg·g~(-1)). SO_2 in the flue gas enhances Hg~0 adsorption over the V_2O_5/AC catalyst, which is due to the reaction of SO_2 and Hg~0 on V_2O_5/AC. But as the SO_2 concentration increases from 500×10~(-6) to 2 000×10~(-6), the amount of mercury adsorbed has only a slight increase. The optimal temperature for Hg~0 adsorption over the V_2O_5/AC catalyst is around 150℃, at which the amounts of mercury adsorbed are up to 98.5 μg·g~(-1) (in the absence of O_2) and 187.7 μg·g~(-1) (in the presence of O_2). The XPS results indicate the formation of HgO and HgSO_4 on the surface of the V_2O_5/AC catalyst, which confirms the role of V_2O_5 and SO_2.
Keywords:V_2O_5/AC  SO_2  V_2O_5/AC  SO_2  gas-phase Hg~0  adsorption  removal
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