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中南大学学报(自然科学版)

Journal of Central South University

第51卷    第1期    总第305期    2020年1月

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文章编号:1672-7207(2020)01-0269-10
不同制备方法对Cu-Co/ACN同时脱除Hg0和CO性能的影响
唐晓龙1, 2,王雨禾1,易红宏1, 2,高凤雨1, 2

(1. 北京科技大学 能源与环境工程学院,北京,100083;
2. 工业典型污染物资源化处理北京市重点实验室,北京,100083
)

摘 要: 在高温烧结炉内,铁矿石和焦炭会造成汞(Hg0)和一氧化碳(CO)污染,为同时脱除烧结烟气中的Hg0和CO,选用硝酸改性后的活性焦为催化剂载体(ACN),采用过渡金属为活性组分,研究制备方法对活性焦催化剂同时脱Hg0和CO性能的影响,实现双功能活性焦催化材料的性能优化。首先,考察Co和Cu在活性焦上的负载量对同时脱除Hg0和CO的影响;然后,采用等体积浸渍法(VI)、沉淀-沉积法(DP)、水热合成法(HY)和溶胶-凝胶法(SG)制备系列Cu-Co/ACN催化剂并研究其催化活性;最后,结合BET,ICP,XRD,H2-TPR和FTIR等表征手段进行研究。实验结果表明:2% Cu-10% Co/ACN催化剂在氧体积分数为16%时同时脱Hg0和CO的效率最高;采用不同制备方法得到的活性焦催化剂脱Hg0效率由高到底依次为Cu-Co/ACN-SG,Cu-Co/ACN-HY,Cu-Co/ACN-VI和Cu-Co/ACN-DP,而脱CO效率由高到低依次为Cu-Co/ACN-VI,Cu-Co/ACN-DP,Cu-Co/ACN-SG和Cu-Co/ACN-HY;活性组分的负载导致催化剂微孔增多,有利于吸附Hg0;VI法和DP法制备的Cu-Co/ACN催化剂脱除CO性能较优,表面存在的钴氧化物主要为Co3O4;SG法和HY法制备Cu-Co/ACN催化剂脱除Hg0性能较优,表面存在更多的CuO;Co3O4和CuO可以提升活性焦催化剂同时脱Hg0和CO性能,有利于催化氧化反应,是主要的反应活性位点。

 

关键词: 催化;脱Hg0;脱CO;等体积浸渍;沉淀-沉积;水热合成;溶胶-凝胶

Effect of different preparation methods on simultaneous removal of gaseous CO and Hg0 over Cu-Co/ACN
TANG Xiaolong1, 2, WANG Yuhe1, YI Honghong1, 2, GAO Fengyu1, 2

1. School of Energy and Environmental Engineering, University of Science and Technology Beijing,Beijing 100083, China;
2. Beijing Key Laboratory of Industrial Typical Pollutants Resource Treatment, Beijing 100083, China

Abstract:Under the high temperature conditions of sintering furnace, with the presence of coke, the sintering of iron ore can cause carbon monoxide(CO) pollution and mercury(Hg) pollution. To simultaneously remove the Hg0 and CO from the sintered flue gas, the activated coke modified by nitric acid was used as the carrier of the catalyst and the transition metal was used as the active component. The effect of preparation methods on the removal of Hg0 and CO from the activated coke catalyst was studied to optimize the performance of the bifunctional active coke catalysts. First, the loadings of Co and Cu on the activated coke were investigated. Then, a series of Cu-Co/ACN catalysts were prepared by equivalent-volumetic impregnation method(VI), precipitation-deposition method (DP), hydrothermal synthesis method(HY) and sol-gel method(SG) to investigate the catalytic activity of the catalysts. Finally, the intensive research was carried out by BET, ICP, XRD, H2-TPR and FTIR. The results show that 2% Cu-10% Co/ACN exhibits the highest activity with 16% O2(volume fraction). The performance of activated coke catalysts for removal Hg0 obtained by different preparation methods is arranged as follows(from high to low): Cu-Co/ACN-SG, Cu-Co/ACN-HY, Cu-Co/ACN-VI and Cu-Co/ACN-DP. The performance of activated coke catalysts for removal CO obtained by different preparation methods is arranged as follows(from high to low): Cu-Co/ACN-VI, Cu-Co/ACN-DP, Cu-Co/ACN-SG and Cu-Co/ACN-HY. The loading of active components leads to the increase of micropores, which is conducive to the adsorption of Hg0. Co3O4 is the main cobalt oxide on the surface of Cu-Co/ACN-VI and Cu-Co/ACN-DP catalysts with excellent CO removal performance. Cu-Co/ACN-SG and Cu-Co/ACN-HY catalysts containing more CuO express better removal ability of Hg0. Co3O4 and CuO can enhance the performance of activated coke catalyst for removal Hg0 and CO, and they are beneficial to the occurrence of catalytic oxidation reaction and are the main reactive active site in the reaction.

 

Key words: catalytic; removal Hg0; removal CO; equivalent-volumetic impregnation; deposition-precipitation; hydrothermal; sol-gel

中南大学学报(自然科学版)
  ISSN 1672-7207
CN 43-1426/N
ZDXZAC
中南大学学报(英文版)
  ISSN 2095-2899
CN 43-1516/TB
JCSTFT
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