仇东亚,赵传文,金冬玲,郭亚飞
QIU Dongya,ZHAO Chuanwen,JIN Dongling,GUO Yafei

• 1:南京师范大学能源与机械工程学院

摘要(Abstract)：

当前过量的CO_2排放已经引发了严重的气候危机，其中燃煤电厂的CO_2排放占据了较大比例，因此针对烟气碳捕集的研究成为关键。化学吸收法在碳捕集领因其成熟的技术，有望成为大规模碳减排应用的技术之一，但是较高的能耗和投资成本限制了其进一步发展。传统的碳捕集与利用（Carbon Capture and Utilization,CCU）工艺中，捕集与利用2个步骤往往是分开进行的，前人们通过研发新型吸收剂、开发节能工艺等手段对捕集过程进行优化，同时开发更加高效安全的CO_2利用和封存技术。但是单独优化每个过程带来的能源效率回报不断减少。因此研究人员开始考虑综合碳捕集和利用技术的经济和能源效益，有学者提出使用电化学转化代替传统的吸收剂在解析塔内升温再生，将CO_2捕集和电化学转化利用整合在一起。基于传统的MEA湿法捕集工艺，利用Aspen Plus对基于有机胺的电解质来实现CO_2捕集与转化利用一体化（Integrated Carbon Capture and Utilization,ICCU）的方法建模分析，对两种工艺进行了技术经济分析。结果表明：相对于常规的CCU工艺，ICCU工艺的CO_2转化率和CO产量分别提升了6%和33%;同时ICCU工艺的能源效率（38.94%）也略高于CCU工艺（37.8%）,伴随着电解能耗的相应增加，因此总体能源效益的改善并不显著。对电解温度进行灵敏度分析，发现当电解温度的升高，2种工艺的能源效率均呈下降趋势，但ICCU工艺的能效一直高于工艺；并且ICCU工艺的成本不断增加，当温度升高5℃，成本增加2%左右。在整体成本方面，ICCU工艺也具有一定的优势（6 399.17元/t），并且系统能耗的下降是进一步降低成本的关键。综合来看，ICCU工艺在经济和能源效益都实现了一定的提高。
Excessive CO_2 emissions have triggered a severe climate crisis,with emissions from coal-fired power plants accounting for a significant proportion. Hence, research into flue gas carbon capture has become critical. Chemical absorption, due to its mature technology, holds promise as one of the technologies for large-scale carbon emission reduction applications. However, its further development is constrained by high energy consumption and investment costs. In traditional Carbon Capture and Utilization(CCU)processes,the capture and utilization steps are often conducted separately. Researchers have optimized the capture process by developing new absorbents and energy-saving processes while also developing more efficient and secure CO_2 utilization and storage technologies.However,individually optimizing each process leads to diminishing returns in energy efficiency. Therefore,researchers are considering the economic and energy benefits of integrating carbon capture and utilization technologies. Some scholars propose using electrochemical conversion instead of traditional absorbents for regenerating towers, integrating CO_2 capture and electrochemical conversion for utilization. Based on traditional MEA wet capture processes,a modeling analysis of Integrated Carbon Capture and Utilization(ICCU)using organic amine electrolytes was conducted using Aspen Plus, and a technical and economic analysis of the two processes was performed. The results show that compared to conventional CCU processes,the ICCU process improves CO_2 conversion rates and CO yields by 6% and 33%,respectively. Additionally,the energy efficiency of the ICCU process(38.94%) is slightly higher than that of the CCU process(37.8%). However, with the corresponding increase in electrolysis energy consumption, the overall improvement in energy efficiency is not significant. Sensitivity analysis of the electrolysis temperature reveals a decreasing trend in energy efficiency for both processes with increasing temperature,although the efficiency of the ICCU process remains higher. Moreover,the cost of the ICCU process increases continuously,with a temperature increase of 5°C resulting in a 2% cost increase. Overall,the ICCU process has certain advantages in terms of total cost(6 399.17 yuan/t),with a reduction in system energy consumption being a key factor in further cost reduction. In conclusion,the ICCU process achieves some improvement in economic and energy benefits.

关键词(KeyWords)： 电化学;湿法捕集;碳捕集与利用;工艺分析;Aspen Plus模拟
electrochemistry;wet scrubbing;carbon capture and utilization;process analysis;Aspen Plus simulation

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金资助项目（52276120）

作者(Author): 仇东亚,赵传文,金冬玲,郭亚飞
QIU Dongya,ZHAO Chuanwen,JIN Dongling,GUO Yafei

DOI: 10.13226/j.issn.1006-6772.23122001

参考文献(References)：

• [1]IEA.Special report on carbon capture utilization and storage[R/OL].Energy Technology Perspectives 2020,2020.
• [2]LI B Y,DUAN Y H,LUEBKE D,et al.Advances in CO2 capture technology:A patent review[J].Applied Energy,2013,102:1439-1447.
• [3]LEUNG D Y C,CARAMANNA G,MAROTO-VALER M M.An overview of current status of carbon dioxide capture and storage technologies[J].Renewable and Sustainable Energy Reviews,2014,39:426-443.
• [4]BOOT-HANDFORD M E,ABANADES J C,ANTHONY E J,et al.Carbon capture and storage update[J].Energy&Environmental Science,2014,7(1):130-189.
• [5]JIANG K,ASHWORTH P,ZHANG S Y,et al.China’s carbon capture,utilization and storage (CCUS) policy:A critical review[J].Renewable and Sustainable Energy Reviews,2020,119:109601.
• [6]PALTSEV S,MORRIS J,KHESHGI H,et al.Hard-to-abate sectors:The role of industrial carbon capture and storage(CCS)in emission mitigation[J].Applied Energy,2021,300:117322.
• [7]MARTIN-ROBERTS E,SCOTT V,FLUDE S,et al.Carbon capture and storage at the end of a lost decade[J].One Earth,2021,4(11):1569-1584.
• [8]MACDOWELL N,FLORIN N,BUCHARD A,et al.An overview of CO2 capture technologies[J].Energy&Environmental Science,2010,3(11):1645-1669.
• [9]BUI M,ADJIMAN C S,BARDOW A,et al.Carbon capture and storage (CCS):The way forward[J].Energy&Environmental Science,2018,11(5):1062-1176.
• [10]GREENHALGH M D,THOMAS S P.Iron-catalyzed,highly regioselective synthesis of α-aryl carboxylic acids from styrene derivatives and CO2[J].Journal of the American Chemical Society,2012,134(29):11900-11903.
• [11]DE LUNA P,HAHN C,HIGGINS D,et al.What would it take for renewably powered electrosynthesis to displace petrochemical processes?[J].Science,2019,364(6438):eaav3506.
• [12]GARCíA DE ARQUER F P,DINH C T,OZDEN A,et al.CO2electrolysis to multicarbon products at activities greater than 1 Acm-2[J].Science,2020,367(6478):661-666.
• [13]HIGGINS D,HAHN C,XIANG C X,et al.Gas-diffusion electrodes for carbon dioxide reduction:A new paradigm[J].ACSEnergy Letters,2019,4(1):317-324.
• [14]GUTIéRREZ-SáNCHEZ O,BOHLEN B,DAEMS N,et al.A.state-of-the-art update on integrated CO2 capture and electrochemical conversion systems[J].ChemElectroChem,2022,9(5):e202101540.
• [15]LOBACCARO P,SINGH M R,CLARK E L,et al.Effects of temperature and gas-liquid mass transfer on the operation of small electrochemical cells for the quantitative evaluation of CO2reduction electrocatalysts[J].Physical Chemistry Chemical Physics,2016,18(38):26777-26785.
• [16]LEE G,LI Y C,KIM J Y,et al.Electrochemical upgrade of CO2from amine capture solution[J].Nature Energy,2020,6(1):46-53.
• [17]CHEN L,LI F W,ZHANG Y,et al.Electrochemical reduction of carbon dioxide in a monoethanolamine capture medium[J].ChemSusChem,2017,10(20):4109-4118.
• [18]GASSNER F,LEITNER W.Hydrogenation of carbon dioxide to formic acid using water-soluble rhodium catalyststs[J].Journal of the Chemical Society,Chemical Communications,1993(19):1465.
• [19]GAO N,QUIROZ-ARITA C,DIAZ L A,et al.Intensified co-electrolysis process for syngas production from captured CO2[J].Journal of CO2 Utilization,2021,43:101365.
• [20]邢晨健，王瑞林，赵传文.燃煤电站与光伏余热辅助胺法脱碳系统集成[J].洁净煤技术，2021,27(2):170-179.XING Chenjian,WANG Ruilin,ZHAO Chuanwen.Integration of coal-fired power station and photovoltaic waste heat-assisted amine decarbonization system[J].Clean Coal Technology,2021,27(2):170-179.
• [21]SINGH D,CROISET E,DOUGLAS P L,et al.Techno-economic study of CO2 capture from an existing coal-fired power plant:MEA scrubbing vs.O2/CO2 recycle combustion[J].Energy Conversion and Management,2003,44(19):3073-3091.
• [22]TOWLER G,SINNOTT R.Chemical engineering design:principles,practice and economics of plant and process design[J]2008.
• [23]武文杰.焦炉煤气燃气轮机联合循环电厂系统特性分析与优化设计[D].上海：上海交通大学，2012.