碱性工业固废矿化封存二氧化碳研究进展

doi:10.16085/j.issn.1000-6613.2022-0813

摘要/Abstract

摘要：

温室效应引起的全球变暖已经影响到人类的生存和发展，CO₂减排刻不容缓。CO₂矿物碳酸化作为一种CO₂减排技术，受到越来越多的关注。相对于传统天然矿化原料，碱性工业固废具有反应速率快、碳酸化效率更高、能耗低等特点，并且利用碱性工业固废进行CO₂矿化还可以产出高附加值产物用于化工、建筑等领域。本文主要综述了碱性工业固废的矿化机理，利用碱性工业固废（粉煤灰、钢渣、电石渣）进行CO₂碳酸化的研究进展及吸收-矿化一体化（IAM）技术。对于以碱性工业固废为原料的碳酸化技术，未来应进一步加强机理和生命周期影响评价的研究并优化工艺流程；针对IAM工艺今后应开发出高效、经济的吸收剂和封存能力更好的矿化原料，并加强对IAM工艺反应机理的研究。

关键词: 二氧化碳, 碱性工业固体废物, 直接碳酸化, 间接碳酸化, 吸收-矿化一体化技术

Abstract:

The global warming caused by the greenhouse effect has affected the survival and development of human beings, and it is urgent to mitigate CO₂. CO₂ mineral carbonation is receiving more and more attention as a CO₂ reduction technology. Alkaline industrial solid waste for CO₂ carbonation has faster reaction rate, higher carbonation rate and lower energy consumption than traditional natural mineralized raw materials, and can also produce high value-added products for chemical and construction applications. This paper reviewed the carbonation mechanism of alkaline industrial solid wastes, the progress of CO₂ mineral carbonation using alkaline industrial solid wastes (fly ash, steel slag, calcium carbide slag) and the integrated absorption-mineralization (IAM) technology. Using alkaline industrial solid waste as feedstock, the carbonation technology mechanism and life cycle impact assessment should be further studied and the process should be optimized in the future. Highly efficient, economical absorbents and mineral raw materials with better mineralization capacity should be developed for the IAM process in the future and the reaction mechanism of the IAM process should be studied.

Key words: carbon dioxide, alkaline industrial solid waste, direct carbonation, indirect carbonation, integrated absorption mineralization

中图分类号:

X511

王秋华, 吴嘉帅, 张卫风. 碱性工业固废矿化封存二氧化碳研究进展[J]. 化工进展, 2023, 42(3): 1572-1582.

WANG Qiuhua, WU Jiashuai, ZHANG Weifeng. Research progress of alkaline industrial solid wastes mineralization for carbon dioxide sequestration[J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1572-1582.

图/表 8

图1 CO2矿化封存技术[9]

表1 矿化原料、主要成分及矿化主要化学反应[13-14]

矿化原料

年产量

/Mt·a^-1

主要反应

成分

CaO + CO₂ $→$ CaCO₃

CaO + H₂O $→$ Ca(OH)₂(aq)

Ca(OH)₂(aq) + CO₂ $→$ CaCO₃ + H₂O

钢渣

240

CaO、MgO

CaO + CO₂ $→$ CaCO₃

MgO + CO₂ $→$ MgCO₃

电石渣

2.8

Ca(OH)₂

Ca(OH)₂(aq) + CO₂

→

CaCO₃ + H₂O

表1 矿化原料、主要成分及矿化主要化学反应[13-14]

矿化原料

年产量

/Mt·a^-1

主要反应

成分

主要化学反应

粉煤灰

750～1000

CaO

CaO + CO₂ $→$ CaCO₃

CaO + H₂O $→$ Ca(OH)₂(aq)

Ca(OH)₂(aq) + CO₂ $→$ CaCO₃ + H₂O

钢渣

240

CaO、MgO

CaO + CO₂ $→$ CaCO₃

MgO + CO₂ $→$ MgCO₃

电石渣

2.8

Ca(OH)₂

Ca(OH)₂(aq) + CO₂

→

CaCO₃ + H₂O

图2 碱性工业固废矿化路线

表2 碱性工业固废干法直接碳酸化条件及CO2封存能力

矿化原料	Ca质量分数/%	温度/℃	压力/MPa	反应时间/h	CO₂封存能力/kg·t^-1	碳酸化效率η/%	参考文献
粉煤灰	35	300～500	0.1	0.16	250	65	Baciocchi等^[21]
粉煤灰	31.95	45	1.5	2.4	180	74	Mazzella等^[22]
电石渣	90.9	580	0.1	1.7	382.21	—	张亚朋等^[23]

图3 不同液固比与电石渣直接液相碳酸化的碳酸化效率的关系[32]

表3 碱性工业固废湿法直接碳酸化的条件及最大碳酸化效率

矿化原料	Ca质量分数 /%	添加剂	温度 /℃	压力 /MPa	液固比 /mL·g^-1	反应时间 /min	CO₂封存能力 /kg·t^-1	碳酸化效率η /%	参考文献
粉煤灰	26.6	—	70	0.01	20	120～270	230	75	Back等^[25]
粉煤灰	—	—	40	6	5	600	7.66	13.6	Ukwattage等^[26]
粉煤灰	4.1	—	25～60	1～4	6.67～20	120	26	82	Montes-Hernandez等^[27]
粉煤灰	15.72	—	35	0.015	0.67～1.67	1440	55	19	Bocheńczyk等^[28]
钢渣	52.82	—	40-160	4.83	10	720	283	68	Chang等^[29]
钢渣	42.43	—	65	0.1	20	30	290	93.5	Chang等^[30]
电石渣	—	—	25	5	4	—	470	—	Yang等^[31]
电石渣	82.1	—	常温	常压	8.26	10	—	93.58	郑鹏等^[32]
粉煤灰	24.9	NaCl	75	0.1	60	39	196	70.8	Mayoral等^[36]
粉煤灰	16.41	Na₂CO₃	275	2	10	120	102	79	Ji等^[34]
电石渣	98.5	油酸钠	80	0.167	0.67	39	—	94.65	Altiner^[37]

表4 碱性工业固废间接碳酸化的碳酸化条件及Ca2+浸出情况

矿化原料	工艺	添加剂	T/℃	液固比（L/S）	反应时间/h	Ca²⁺浸出率η或浸出浓度	CO₂封存能力或碳酸化效率	参考文献
粉煤灰	间接碳酸化	CH₃COOH	60	—	1	14g/L	264kg/t	Sun等^[38]
粉煤灰	间接碳酸化	甘氨酸	25	5mL/g	3	42%	86kg/t	Zheng等^[39]
钢渣	间接碳酸化	CH₃COOH	50	71.4mL/g	2	90%	—	Teir等^[40]
钢渣	间接碳酸化	HCl	25	60mL/g	1	93.4%	56.5%	唐海燕等^[41]
钢渣	间接碳酸化	NH₄Cl	60	20mL/g	1	15g/L	211kg/t	Sun等^[45]
粉煤灰	间接碳酸化	CH₃COONH₄	25	20mL/g	1	40%	111kg/t	He等^[42]
		NH₄Cl
		NH₄NO₃
H粉煤灰	间接碳酸化	NH₄Cl	80	60mL/g	1	32%	90%	Hosseini等^[43]
Y粉煤灰	间接碳酸化	NH₄Cl	80	60mL/g	1	37%	40%	Hosseini等^[43]
钢渣	间接碳酸化	NH₄Cl	80	—	1	60%	—	Kodama等^[44]
电石渣	间接碳酸化	NH₄Cl	40	—	0.83	—	763.33kg/t	Zhang等^[46]
电石渣	间接碳酸化	(NH₄)₂SO₄	40	9.52mL/g	0.5	—	500kg/t	Li等^[47]
钢渣	间接碳酸化（超声波）	NH₄Cl	23	50mL/g	1	96%	—	Said等^[48]
钢渣	间接碳酸化（微波照射）	NH₄Cl	60	1～10mL/g	—	55%	≈100%	Tong等^[49]

图4 IAM流程的概念图[64]

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