胺基CO2固体吸附剂脱碳特性及SO2的影响

doi:10.11949/j.issn.0438-1157.20170957

化工学报 ›› 2018, Vol. 69 ›› Issue (4): 1586-1594.DOI: 10.11949/j.issn.0438-1157.20170957

胺基CO₂固体吸附剂脱碳特性及SO₂的影响

张文静¹, 吴烨², 蔡天意¹, 刘道银¹, 马吉亮¹, 梁财¹, 陈晓平¹

1. 东南大学能源热转换及其过程测控教育部重点实验室, 江苏南京 210096;
2. 南京理工大学电子设备热控制工业和信息化部重点实验室, 江苏南京 210094

收稿日期:2017-07-25 修回日期:2017-09-18 出版日期:2018-04-05 发布日期:2018-04-05
通讯作者: 陈晓平
基金资助:
国家自然科学基金项目（51476030，51506095）。

Effect of SO₂ on CO₂ sorption characteristics using solid amine CO₂ sorbent

ZHANG Wenjing¹, WU Ye², CAI Tianyi¹, LIU Daoyin¹, MA Jiliang¹, LIANG Cai¹, CHEN Xiaoping¹

1. Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, Southeast University, Nanjing 210096, Jiangsu, China;
2. MIIT Key Laboratory of Thermal Control of Electronic Equipment, Nanjing University of Science and Technology, Nanjing 210094, Jiangsu, China

Received:2017-07-25 Revised:2017-09-18 Online:2018-04-05 Published:2018-04-05
Supported by:
supported by the National Natural Science Foundation of China (51476030, 51506095).

摘要/Abstract

摘要：

燃煤电厂烟气中存在的微量SO₂对胺基CO₂固体吸附剂的碳酸化反应及循环特性有不利影响。利用固定床反应器，针对采用溶胶凝胶法制备的胺基CO₂固体吸附剂的碳酸化特性及其在含SO₂气氛下的失效规律进行了实验研究，并结合红外光谱、有机元素分析、BET等测试手段，研究其失效机理。结果表明，所制备的胺基CO₂固体吸附剂在反应温度50℃时具有较好的碳酸化反应特性和循环特性。当反应气氛中存在SO₂时，由于生成了不可再生的亚硫酸/硫酸盐类物质而导致胺基活性位损失，孔隙结构发生变化，影响了吸附剂的脱碳性能，但适当提高反应温度可提高吸附剂的碳酸化反应竞争性。

关键词: CO₂捕集, 固体胺基吸附剂, 溶胶凝胶法, 失效, SO₂

Abstract:

The presence of trace SO₂ in the flue gas of the power plant will affect the CO₂ sorption performance and cyclic characteristics of the solid amine sorbent. A solid amine-based CO₂ sorbent was prepared by a one-pot sol-gel process followed by supercritical drying (SCD) and the CO₂ sorption performance. Deactivation mechanism of the sorbent were studied by using fixed-bed reactor combined with infrared spectroscopy, BET and other test methods. The results show that the solid amine-based CO₂ sorbent has excellent CO₂ sorption performance and cyclic characteristics when the reaction temperature was 50℃. However, when the reaction atmosphere contains SO₂,the non-renewable sulphite or sulfate byproducts reduces the utilization rate of active amine sites, thus significantly decreasing the CO₂ adsorption capacity, and consequently, the cyclic characteristics were seriously affected. Besides, the pore distribution of sorbent also tends to small pore volume. Increasing the sorption temperature will enhance the CO₂ sorption competivity of the amine based sorbent.

Key words: CO₂ capture, solid amine based absorbent, sol-gel method, deactivation, SO₂

中图分类号:

TK09

张文静, 吴烨, 蔡天意, 刘道银, 马吉亮, 梁财, 陈晓平. 胺基CO₂固体吸附剂脱碳特性及SO₂的影响[J]. 化工学报, 2018, 69(4): 1586-1594.

ZHANG Wenjing, WU Ye, CAI Tianyi, LIU Daoyin, MA Jiliang, LIANG Cai, CHEN Xiaoping. Effect of SO₂ on CO₂ sorption characteristics using solid amine CO₂ sorbent[J]. CIESC Journal, 2018, 69(4): 1586-1594.

参考文献 32

[1]	Climate Change 2013:the Physical Science Basis:Working Group Ⅰ Contribution to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change[M]. Cambridge:Cambridge University Press, 2014.
[2]	HALMANN M M, STEINBERG M. Greenhouse Gas Carbon Dioxide Mitigation:Science and Technology[M]. CRC Press, 1998.
[3]	ZHAO M, MINETT A I, HARRIS A T. A review of techno-economic models for the retrofitting of conventional pulverised-coal power plants for post-combustion capture (PCC) of CO2[J]. Energy & Environmental Science, 2013, 6(1):25-40.
[4]	SHARONOV V E, TYSHCHISHCHIN E A, MOROZ E M, et al. Sorption of CO2 from humid gases on potassium carbonate supported by porous matrix[J]. Russian Journal of Applied Chemistry, 2001, 74(3):409-413.
[5]	TANG Y, LANDSKRON K. CO2-sorption properties of organosilicas with bridging amine functionalities inside the framework[J]. The Journal of Physical Chemistry C, 2010, 114(6):2494-2498.
[6]	WÖRMEYER K, SMIRNOVA I. Adsorption of CO2, moisture and ethanol at low partial pressure using aminofunctionalised silica aerogels[J]. Chemical Engineering Journal, 2013, 225:350-357.
[7]	WÖRMEYER K, SMIRNOVA I. Breakthrough measurements of CO2 through aminofunctionalised aerogel adsorbent at low partial pressure:experiment and modeling[J]. Microporous and Mesoporous Materials, 2014, 184:61-69.
[8]	WÖRMEYER K, ALNAIEF M, SMIRNOVA I. Amino functionalised silica-aerogels for CO2-adsorption at low partial pressure[J]. Adsorption, 2012, 18(3/4):163-171.
[9]	BEGAG R, KRUTKA H, DONG W, et al. Superhydrophobic amine functionalized aerogels as sorbents for CO2 capture[J]. Greenhouse Gases:Science and Technology, 2013, 3(1):30-39.
[10]	齐国杰, 王淑娟, 刘今朝, 等. 燃煤烟气中SO2对氨法脱碳的影响[J]. 化工学报, 2012, 63(7):2202-2209. QI G J, WANG S J, LIU J Z, et al. Impact of SO2 on CO2 capture in coal-fired flue gas using aqueous ammonia[J]. CIESC Journal, 2012, 63(7):2202-2209.
[11]	KHATRI R A, CHUANG S S C, SOONG Y, et al. Thermal and chemical stability of regenerable solid amine sorbent for CO2 capture[J]. Energy & Fuels, 2006, 20(4):1514-1520.
[12]	REZAEI F, JONES C W. Stability of supported amine adsorbents to SO2 and NOx in postcombustion CO2 capture (1):Single-component adsorption[J]. Industrial & Engineering Chemistry Research, 2013, 52(34):12192-12201.
[13]	REZAEI F, JONES C W. Stability of supported amine adsorbents to SO2 and NOx in postcombustion CO2 capture (2):Multicomponent adsorption[J]. Industrial & Engineering Chemistry Research, 2014, 53(30):12103-12110.
[14]	HALLENBECK A P, KITCHIN J R. Effects of O2 and SO2 on the capture capacity of a primary-amine based polymeric CO2 sorbent[J]. Industrial & Engineering Chemistry Research, 2013, 52(31):10788-10794.
[15]	TAILOR R, ABBOUD M, SAYARI A. Supported polytertiary amines:highly efficient and selective SO2 adsorbents[J]. Environmental Science & Technology, 2014, 48(3):2025-2034.
[16]	GUO M, ZHANG L, YANG Z, et al. Removal of CO2 by CaO/MgO and CaO/Ca9Al6O18 in the presence of SO2[J]. Energy & Fuels, 2011, 25(11):5514-5520.
[17]	LUO C, ZHENG Y, YIN J, et al. Effect of sulfation during oxy-fuel calcination stage in calcium looping on CO2 capture performance of CaO-based sorbents[J]. Energy & Fuels, 2013, 27(2):1008-1014.
[18]	WU Y, CHEN X, FAN M, et al. Development of K and N based composite CO2 sorbents (KN) dried with a supercritical fluid[J]. Chemical Engineering Journal, 2015, 262:1192-1198.
[19]	WU Y, CHEN X, DONG W, et al. K2CO3/Al2O3 for capturing CO2 in flue gas from power plants (5):Carbonation and failure behavior of K2CO3/Al2O3 in the continuous CO2 sorption-desorption system[J]. Energy & Fuels, 2013, 27(8):4804-4809.
[20]	WU Y, CHEN X. The negative effects of SO2 on CO2 capture with K2CO3/Al2O3[J]. Journal of Thermal Analysis and Calorimetry, 2015, 122(2):1041-1049.
[21]	KIM K, YANG S, LEE J B, et al. Analysis of K2CO3/Al2O3 CO2 sorbent tested with coal-fired power plant flue gas:effect of SOx[J]. International Journal of Greenhouse Gas Control, 2012, 9:347-354.
[22]	GUO Y, LI C, LU S, et al. Understanding the deactivation of K2CO3/AC for low-concentration CO2 removal in the presence of trace SO2 and NO2[J]. Chemical Engineering Journal, 2016, 301:325-333.
[23]	MALEKI H. Recent advances in aerogels for environmental remediation applications:a review[J]. Chemical Engineering Journal, 2016, 300:98-118.
[24]	余帆, 吴烨, 董伟, 等. 氨基修饰复合型钠基吸收剂的脱碳特性[J]. 化工学报, 2015, 66(10):4218-4227. YU F, WU Y, DONG W, et al. Carbonation characteristics of sodium-based sorbents with amino modification for CO2 capture[J]. CIESC Journal, 2015, 66(10):4219-4227.
[25]	KONG Y, SHEN X, FAN M, et al. Dynamic capture of low-concentration CO2 on amine hybrid silsesquioxane aerogel[J]. Chemical Engineering Journal, 2016, 283:1059-1068.
[26]	KONG Y, JIANG G, FAN M, et al. Use of one-pot wet gel or precursor preparation and supercritical drying procedure for development of a high-performance CO2 sorbent[J]. RSC Advances, 2014, 82(4):43448-43453.
[27]	ZHENG F, TRAN D N, BUSCHE B J, et al. Ethylenediamine-modified SBA-15 as regenerable CO2 sorbent[J]. Industrial & Engineering Chemistry Research, 2005, 44(9):3099-3105.
[28]	CHANG A C C, CHUANG S S C, GRAY M M, et al. In-situ infrared study of CO2 adsorption on SBA-15 grafted with γ-(aminopropyl) triethoxysilane[J]. Energy & Fuels, 2003, 17(2):468-473.
[29]	KIM S, IDA J, GULIANTS V V, et al. Tailoring pore properties of MCM-48 silica for selective adsorption of CO2[J]. The Journal of Physical Chemistry B, 2005, 109(13):6287-6293.
[30]	SOCRATES G. Infrared and Raman Characteristic Group Frequencies:Tables and Charts[M]. John Wiley & Sons, 2004.
[31]	FERRARO J R. Infrared spectra of inorganic and coordination compounds (Nakamoto, Kazuo)[J]. Theory & Applications in Inorganic Chemistry, 1970, 5:88-97.
[32]	COLTHUP N. Introduction to Infrared and Raman Spectroscopy[M]. Elsevier, 2012.

胺基CO₂固体吸附剂脱碳特性及SO₂的影响

Effect of SO₂ on CO₂ sorption characteristics using solid amine CO₂ sorbent

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献 32

相关文章 15

编辑推荐

Metrics

本文评价

[1]	焦巡, 童成, 李存璞, 魏子栋. 锂硫电池的动力学调控策略[J]. 化工学报, 2023, 74(1): 170-191.
[2]	党迎喜, 谈朋, 刘晓勤, 孙林兵. 辐射冷却和太阳能加热驱动的CO₂变温捕获[J]. 化工学报, 2023, 74(1): 469-478.
[3]	黄顺进, 张丽, 颜井冲, 王志刚, 雷智平, 李占库, 任世彪, 王知彩, 水恒福. 高碱煤与煤矸石掺烧SO₂和NO减排及结渣抑制研究[J]. 化工学报, 2022, 73(12): 5581-5591.
[4]	季东, 王健, 王可, 李婧玮, 孟文亮, 杨勇, 李贵贤, 王东亮, 周怀荣. 不同CO₂捕集技术的CO₂耦合绿氢制甲醇工艺研究[J]. 化工学报, 2022, 73(10): 4565-4575.
[5]	李云浩, 蒋军成, 喻源, 王志荣, 张庆武. 穿孔与热辐射耦合作用下固定拱顶钢储罐的失效机理[J]. 化工学报, 2021, 72(8): 4433-4443.
[6]	尹子骏, 苏胜, 卿梦霞, 赵志刚, 王中辉, 王乐乐, 江龙, 汪一, 胡松, 向军. 一种典型钒钛系SCR催化剂SO₃生成特性研究[J]. 化工学报, 2021, 72(5): 2596-2603.
[7]	王东亮, 谢江鹏, 周怀荣, 孟文亮, 杨勇, 李德磊. 基于MDEA的烟气SO₂捕集过程工艺参数和能量集成分析[J]. 化工学报, 2021, 72(3): 1521-1528.
[8]	周毅,王永洪,张新儒,李晋平. PEBA/氮硫共掺杂多孔碳球混合基质膜的制备及CO₂分离性能研究[J]. 化工学报, 2021, 72(10): 5237-5246.
[9]	郎中敏, 吴刚强, 赫文秀, 韩晓星, 苟延梦, 李双莹. 二氧化铈/水基纳米流体核沸腾传热特性[J]. 化工学报, 2020, 71(5): 2061-2068.
[10]	刘应书,孙宁起,李子宜,杨雄,魏进超,杨本涛,吴倩倩,刘佳欣. 冷凝法回收烟气吸附脱硫解吸气中SO₂工艺参数的影响规律研究[J]. 化工学报, 2020, 71(12): 5620-5627.
[11]	肖俏欣, 林文俊, 李浩然, 王从敏. 含醚阴离子功能化离子液体高效捕集SO₂[J]. 化工学报, 2020, 71(1): 361-367.
[12]	梅道锋, 赵海波, 晏水平. 基于NiO/Ca₂Al₂SiO₇的沼气自热化学链重整制氢热分析动力学模拟[J]. 化工学报, 2019, 70(S1): 193-201.
[13]	廉玉姣, 王永洪, 张新儒, 李晋平. N₂优先渗透ZIF-8复合膜的制备及其CO₂捕集[J]. 化工学报, 2019, 70(9): 3573-3581.
[14]	李向阳, 李扬, 靳立军, 杨赫, 王德超, 胡浩权. MnO_x改性活性炭用于模拟烟气中Hg⁰的脱除[J]. 化工学报, 2019, 70(8): 3078-3085.
[15]	陈东良, 张忠林, 杨景轩, 马旭莉, 李鹏, 郝晓刚, 官国清. 基于自热再生的化学吸收法CO₂捕集工艺模拟及节能分析[J]. 化工学报, 2019, 70(8): 2938-2945.