CaSO4载氧体在煤气化化学链燃烧中的脱汞

doi:10.16085/j.issn.1000-6613.2022-0901

摘要/Abstract

摘要：

为了研究载氧体在煤气化化学链燃烧中的脱汞机理，选择CaSO₄载氧体作为研究对象，900℃的反应温度下，在还原反应器中通入CO₂气体和水蒸气作为气化介质进行实验。结果表明：以CaSO₄作为载氧体的煤气化化学链燃烧中，CaSO₄载氧体本身促进Hg⁰的氧化，但CaSO₄分解产生的SO₂抑制Hg⁰的氧化。CaSO₄促进煤气化化学链燃烧产生S单质，会进一步与Hg⁰反应生成多种复杂的HgS _n，降低了烟气中Hg⁰含量，提高了脱汞效率。同时CaSO₄载氧体在还原-氧化的循环反应中具有良好的循环特性，是一种优良的化学链载氧体。

关键词: 化学链燃烧, 汞, 载氧体, 硫酸钙, 煤燃烧, 循环流化床, 气化

Abstract:

To understand the mechanism of mercury removal by oxygen carriers during in-situ gasification and chemical-looping combustion of coal, we used CaSO₄ as oxygen carrier and CO₂ and water vapor as gasification medium in a reduction reactor working at 900℃. Results showed that the CaSO₄ oxygen carrier itself promoted the oxidation of Hg⁰, but the SO₂ produced by the decomposition of CaSO₄ inhibited the oxidation of Hg⁰. CaSO₄ promoted the chemical-looping combustion of coal to produce element S, which would further react with Hg⁰ to generate a variety of complex HgS _n . This, reduced the Hg⁰ content in the flue gas and improved the mercury removal efficiency. In addition, the CaSO₄ oxygen carrier has good cycle characteristics in the reduction-oxidation cyclic reactions, indicating an excellent chemical-looping oxygen carrier.

Key words: chemical-looping combustion, mercury, oxygen carrier, CaSO₄, coal combustion, circulating fluidized bed, gasification

中图分类号:

TK16

范昀培, 金晶, 刘敦禹, 王静杰, 刘秋祺, 许开龙. CaSO₄载氧体在煤气化化学链燃烧中的脱汞[J]. 化工进展, 2023, 42(3): 1638-1648.

FAN Yunpei, JIN Jing, LIU Dunyu, WANG Jingjie, LIU Qiuqi, XU Kailong. Mercury removal by CaSO₄ oxygen carrier during in-situ gasification and chemical-looping combustion of coal[J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1638-1648.

图/表 11

表1 将军庙煤样品分析

工业分析（质量分数）/%					元素分析（质量分数）/%
M_ad	A_ad	V_ad	FC_ad		C_ad	H_ad	N_ad	S_ad	O_ad	Cl	Hg/μg·g^-1
12.34	6.85	26.37	54.44		74.62	5.83	1.43	0.46	17.66	0.063	0.4

图1 流化床反应装置示意图

图2 不同条件下煤气化化学链燃烧过程中气体浓度随时间变化

图3 还原反应器中各气体总浓度

图4 氧化反应器中各气体总浓度

图5 还原反应器中不同载氧体Hg0浓度随时间变化

图6 不同条件下CaSO4载氧体Hg0浓度随时间变化

图7 钙硫化物反应中Hg0浓度随时间变化

图8 Ca与O的XPS分析

图9 沉降炉中的S与Hg的XPS分析

图10 还原及氧化后载氧体XRD图谱

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CaSO₄载氧体在煤气化化学链燃烧中的脱汞

Mercury removal by CaSO₄ oxygen carrier during in-situ gasification and chemical-looping combustion of coal

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