CO2矿化及吸收-矿化一体化（IAM）方法研究进展

doi:10.16085/j.issn.1000-6613.2020-0981

摘要/Abstract

摘要：

为避免温室效应带来的负面影响，CO₂减排已成为目前的当务之急。CO₂矿物碳酸化作为一种有潜力的CO₂减排技术，受到了学者们的广泛关注。CO₂矿物碳酸化方法主要包括直接干法碳酸化、直接湿法碳酸化以及间接碳酸化等不同工艺过程。目前，CO₂直接或间接碳酸化方法面临的关键挑战是提升CO₂碳酸化反应动力学特性；反应速率慢、碳酸化效率较低是当前该技术的主要问题。传统CO₂胺类化学吸收法具有吸收速率快、吸收容量大和吸收剂能循环再生的优点，但能耗和运行成本较高。将CO₂胺类化学吸收法与CO₂碳酸化过程结合而开发的CO₂吸收-矿化一体化技术（IAM）不仅解决了传统工艺高能耗、低转化率的问题，而且使工艺流程简化、成本降低，有利于应用于工业化。本文主要综述了近年来CO₂矿化技术的研究进展，对比了各种工艺技术路线的不同特点，并分析指出加强对IAM工艺反应机理的研究以及开发出高效、经济的吸收剂和矿化原料，将是该工艺未来研究的重点和关键。

关键词: 二氧化碳, 矿物碳酸化, 二氧化碳捕集与封存技术, 吸收-矿化一体化技术, 直接碳酸化, 间接碳酸化

Abstract:

In order to avoid the negative impact of greenhouse effect, the reduction of CO₂ emissions has become an urgent task. As a potential CO₂ emission reduction technology, CO₂ mineral carbonation has attracted extensive attention. CO₂mineral carbonation methods mainly include the direct dry carbonation route, direct aqueous carbonation route, and indirect carbonation route. At present, the key challenge in CO₂ direct or indirect carbonation methods is to improve the kinetic characteristics of CO₂ carbonation. The slow reaction rate and low carbonation efficiency are the main problems of the current technology. The traditional CO₂ amine chemical absorption method has the advantages of fast absorption rate, large absorption capacity, and absorbent recycling, but the energy consumption and operating cost are high. The integrated CO₂absorption-mineralization technology (IAM) developed by the combination of the CO₂ amine chemical absorption and CO₂ carbonation process not only solves the problems of high energy consumption and low conversion rate of the traditional process but also simplifies the process flow and reduces the cost, which is beneficial to industrialization. This paper summarizes the research progress of CO₂ mineralization technology in recent years and compares the different characteristics of various technological routes. It points out that strengthening the research on the reaction mechanism of the IAM process and the development of efficient and economical absorbent and mineralized raw materials are the key of the future research of this process.

Key words: carbon dioxide, mineral carbonation, CCS, IAM technology, direct carbonation, indirect carbonation

中图分类号:

TQ127.1⁺3

王中辉, 苏胜, 尹子骏, 安晓雪, 赵志刚, 陈逸峰, 刘涛, 汪一, 胡松, 向军. CO₂矿化及吸收-矿化一体化（IAM）方法研究进展[J]. 化工进展, 2021, 40(4): 2318-2327.

WANG Zhonghui, SU Sheng, YIN Zijun, AN Xiaoxue, ZHAO Zhigang, CHEN Yifeng, LIU Tao, WANG Yi, HU Song, XIANG Jun. Research progress of CO₂mineralization and integrated absorption-mineralization (IAM) method[J]. Chemical Industry and Engineering Progress, 2021, 40(4): 2318-2327.

图/表 7

图1 CO2矿物碳酸化封存技术示意图[12]

表1 矿化原料及其主要化学反应过程

矿化原料	主要成分	主要化学反应方程式
天然矿物
橄榄石	Mg₂SiO₄	Mg₂SiO₄+2CO₂ $→$ 2MgCO₃+SiO₂
蛇纹石	Mg₃Si₂O₅(OH)₄	Mg₃Si₂O₅(OH)₄+3CO₂ $→$ 3MgCO₃+2SiO₂+2H₂O
硅灰石	CaSiO₃	CaSiO₃+CO₂ $→$ CaCO₃+SiO₂
工业固废
粉煤灰	CaO	CaO+CO₂ $→$ CaCO₃ CaO+H₂O $→$ Ca(OH)₂(aq) Ca(OH)₂(aq)+CO₂ $→$ CaCO₃↓+H₂O
钢渣	CaO、MgO	CaO+CO₂ $→$ CaCO₃ MgO+CO₂ $→$ MgCO₃
磷石膏	CaSO₄·2H₂O	CaSO₄·2H₂O+2NH₃·H₂O+CO₂ $→$ (NH₄)₂SO₄+CaCO₃↓+3H₂O CaSO₄(s)+2KAlSi₃O₈+CO₂+2H₂O $→$ CaCO₃(s)+K₂SO₄+4SiO₂+Al₂Si₂O₅(OH)₄
电石渣	Mg(OH)₂	Ca(OH)₂(aq)+CO₂ $→$ CaCO₃↓+H₂O
盐湖苦卤	MgCl₂	MgCl₂·6H₂O(aq)+2NH₃·H₂O $→$ Mg(OH)₂↓+2NH₄Cl+6H₂O Mg(OH)₂+CO₂+2H₂O $→$ MgCO₃·3H₂O↓

表1 矿化原料及其主要化学反应过程

矿化原料	主要成分	主要化学反应方程式
天然矿物
橄榄石	Mg₂SiO₄	Mg₂SiO₄+2CO₂ $→$ 2MgCO₃+SiO₂
蛇纹石	Mg₃Si₂O₅(OH)₄	Mg₃Si₂O₅(OH)₄+3CO₂ $→$ 3MgCO₃+2SiO₂+2H₂O
硅灰石	CaSiO₃	CaSiO₃+CO₂ $→$ CaCO₃+SiO₂
工业固废
粉煤灰	CaO	CaO+CO₂ $→$ CaCO₃ CaO+H₂O $→$ Ca(OH)₂(aq) Ca(OH)₂(aq)+CO₂ $→$ CaCO₃↓+H₂O
钢渣	CaO、MgO	CaO+CO₂ $→$ CaCO₃ MgO+CO₂ $→$ MgCO₃
磷石膏	CaSO₄·2H₂O	CaSO₄·2H₂O+2NH₃·H₂O+CO₂ $→$ (NH₄)₂SO₄+CaCO₃↓+3H₂O CaSO₄(s)+2KAlSi₃O₈+CO₂+2H₂O $→$ CaCO₃(s)+K₂SO₄+4SiO₂+Al₂Si₂O₅(OH)₄
电石渣	Mg(OH)₂	Ca(OH)₂(aq)+CO₂ $→$ CaCO₃↓+H₂O
盐湖苦卤	MgCl₂	MgCl₂·6H₂O(aq)+2NH₃·H₂O $→$ Mg(OH)₂↓+2NH₄Cl+6H₂O Mg(OH)₂+CO₂+2H₂O $→$ MgCO₃·3H₂O↓

图2 直接碳酸化路线和间接碳酸化路线图

图3 CO2矿化高炉渣联产高附加值产品技术路线[38]

图4 典型CO2胺洗涤工艺及IAM工艺流程图[48]

表2 IAM工艺与传统MEA工艺实验条件及结果[48,51,59]

参数	CO₂捕获
参数	化学再生（CaO）	化学再生（粉煤灰）	传统热再生
吸收剂浓度/mol·L^-1	2	2	2
烟气CO₂压力/kPa	9	9	9
吸收温度/℃	40	40	40
再生压力/atm	1	1	2
再生温度/℃	40	40	116
换热器换热温差/℃	—	—	10
CO₂循环负荷/mol·mol^-1	0.21	0.21	0.21
再生消耗能量/MJ·kg^-1CO₂	0	0	4.7
产物	CaCO₃	富含CaCO₃的飞灰	高纯度CO₂

表3 IAM工艺与传统MEA工艺能耗和资本投入

参数	传统MEA工艺能耗	IAM工艺能耗	IAM工艺节能
汽提塔再沸器/kJ·（kg CO₂）^-1	760	—	760
压缩装置/kJ·（kg CO₂）^-1	397	—	397
泵/kJ·（kg CO₂）^-1	9.9	9.9	0
过滤装置/kJ·（kg CO₂）^-1	—	51.7	-51.7
总计/kJ·（kg CO₂）^-1	1166.9	61.6	1115.3
年能耗成本/ $×$ 10³AUD	142865	233	142632
设备投入成本/ $×$ 10³AUD	42460	5537	36923

表3 IAM工艺与传统MEA工艺能耗和资本投入

参数	传统MEA工艺能耗	IAM工艺能耗	IAM工艺节能
汽提塔再沸器/kJ·（kg CO₂）^-1	760	—	760
压缩装置/kJ·（kg CO₂）^-1	397	—	397
泵/kJ·（kg CO₂）^-1	9.9	9.9	0
过滤装置/kJ·（kg CO₂）^-1	—	51.7	-51.7
总计/kJ·（kg CO₂）^-1	1166.9	61.6	1115.3
年能耗成本/ $×$ 10³AUD	142865	233	142632
设备投入成本/ $×$ 10³AUD	42460	5537	36923

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CO₂矿化及吸收-矿化一体化（IAM）方法研究进展

Research progress of CO₂mineralization and integrated absorption-mineralization (IAM) method

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