水蒸气和H2S对白云石循环碳酸化/煅烧过程中CO2捕获性能的影响

杨新芳 赵丽凤 刘洋 肖云汉

doi:10.12034/j.issn.1009-606X.216355

过程工程学报 >

2017 , Vol. 17 >Issue 3: 594 - 599

DOI: https://doi.org/10.12034/j.issn.1009-606X.216355

过程与工艺

水蒸气和H₂S对白云石循环碳酸化/煅烧过程中CO₂捕获性能的影响

杨新芳赵丽凤刘洋肖云汉

展开

1. 中国科学院工程热物理研究所先进能源动力重点实验室，北京 100190；2. 中国科学院能源动力研究中心，江苏连云港 222069

收稿日期: 2016-11-30

修回日期: 2016-12-29

网络出版日期: 2017-06-14

基金资助

国家自然科学基金项目

收起

Effects of H₂O and H₂S on Cyclic CO₂ Capture Activity of Dolomite during Calcination/Carbonation Process

Xinfang YANG Lifeng ZHAO Yang LIU Yunhan XIAO

Expand

1. Key Lab of Advanced Energy & Power, Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing 100190, China; 2. Research Center for Clean Energy and Power, Chinese Academy of Sciences, Lianyungang, Jiangsu 222069, China

Received date: 2016-11-30

Revised date: 2016-12-29

Online published: 2017-06-14

Fold

摘要

基于水汽变换条件，利用加压热重分析仪研究了温度、压力及煤气中H₂O和H₂S对白云石煅烧/碳酸化循环捕获CO₂性能的影响. 研究表明，吸收剂在650和700℃时的吸收反应速率和循环稳定性明显优于550和600℃时；加压促进吸收剂对CO₂的吸收，且有H₂O时促进作用更明显；H₂O能有效改善吸收剂的循环稳定性，提高吸收剂在快速动力学反应控制阶段的吸收能力. 650℃时CaO硫化反应速率远小于碳酸化反应速率，煤气中H₂S对CaO吸收CO₂的反应动力学特性无明显影响，但硫化产物CaS在吸收剂表面累积会减少用于吸收CO₂的CaO量，而反应过程中H₂O的存在又会减缓CaS的累积.

关键词： 水汽变换; 白云石; 脱碳; 水蒸气; 硫化氢

本文引用格式

杨新芳赵丽凤刘洋肖云汉 . 水蒸气和H₂S对白云石循环碳酸化/煅烧过程中CO₂捕获性能的影响[J]. 过程工程学报, 2017 , 17(3) : 594 -599 . DOI: 10.12034/j.issn.1009-606X.216355

Abstract

The effects of reaction temperature, pressure, H₂O and H₂S on the cyclic CO₂capture activity of dolomite during calcination/ carbonation process were studied with a thermogravimetric analyzer, based on the water gas shift reaction condition. The results indicated that the absorption rate and the cyclic stability at 650 and 700℃ are obviously better than those at 550 and 600℃. The increase of pressure promotes the CO₂ absorption of sorbent, and the enhancement becomes more obvious with H₂O present. H₂O can effectively improve the cyclic stability of the sorbent and enhance the capture capacity at the fast kinetic reaction control stage. At 650℃, the sulfidation rate is far lower than the carbonation rate of CaO. H₂S in the syngas shows no obvious effect on the kinetics of the carbonation reaction. However, the accumulation of sulfidation product CaS over CaO sorbents will reduce the CaO amount for CO₂ absorption, and the H₂O will restrain the accumulation of CaS during the reaction process.

Key words： water - gas shift; dolomite; CO2 capture; H2O; H2S

参考文献

[1]蔡宁生，房凡，李振山.钙基吸收剂循环煅烧碳酸化法捕集CO2的研究进展[J].电机工程学报, 2010, 30(26):35-43
[2]Lin S Y, Harada M, Suzuki Y, Hatano H.Hydrogen production from coal by separating carbon dioxide during gasification[J].Fuel, 2002, 81:2079-2085.
[3]Wang Z H, Zhou J H, Wang Q H, Fan J R, Cen K F.Thermodynamic equilibrium analysis of hydrogen production by coal based on Coal/CaO/H2O gasification system[J].International Journal of Hydrogen Energy, 2006, 31:945-952
[4]乔春珍，王宝利，肖云汉.钙基CO2吸收剂循环活性衰减原因探索[J].化工学报, 2010, 61(3):720-724
[5]冯志翔，郑瑛，张璐，郑楚光.CaO碳化-煅烧循环捕获CO2高温烧结特性研究[J].工程热物理学报, 2009, 30(3):537-539
[6]Li Z S, Cai N S.Process Analysis of CO2 Capture from Flue Gas Using Carbonation Calcination Cycles[J].AIChE Journal, 2008, 54(7):1912-1925
[7]Silaban A, Narcida M, Harrison D P.Characteristics of the reversible reaction between CO2 (g) and calcined dolomite[J].Chemical Engineering Communications, 1996, 146:149-162
[8]李英杰，孙荣岳，刘红玲，赵建立，韩奎华，路春美.石灰石和白云石高温循环脱除CO2过程分析[J].化工学报, 2011, 62(6):1693-1700
[9]Patrik Yrjas, Kristiina lisa and Mikko Hupa.Limestone and dolomite as sulfur absorbents under pressurized gasification conditions[J].Fuel, 1996, 75(1):89-95
[10]宋占龙，章名耀.加压条件下石灰石同时煅烧和脱除H2S的反应特性[J].燃烧科学与技术, 2011, 17(3):215-218
[11]Yang S J, Xiao Y H.Steam catalysis in CaO carbonation under low steam partial pressure[J].Industry and Engineering Chemistry Research, 2008, 47:4043-4048
[12]Donat F, Florin N H, Anthony E J, Fennell P S.Influence of high-temperature steam on the reactivity of CaO sorbent for CO2 capture[J].Environmental Science & Technology, 2012, 46:1262-1269
[13]Harrison D.Calcium enhanced hydrogen production with CO2 capture[J].Energy Procedia, 2009, 1:675-681
[14]王峰，田文栋，肖云汉.煤直接制氢实验研究[J].电机工程学报, 2007, 27(32):40-45
[15]Ohtsuka Y, Tsubouchi N, Kikuchi T, Hashimoto H.Recent progress in Japan on hot gas cleanup of hydrogen chloride,hydrogen sulfide and ammonia in coal-derived fuel gas[J].Power Technology, 2009, 190(3):340-347
[16]Manovic V, Anthony E J.Carbonation of CaO-based sorbents enhanced by steam addition[J].Industry and Engineering Chemistry Research, 2010, 49(19):9105-9110
[17]Wu S J, Uddin M A, Nagamine S, Sasaoka E.Role of Water Vapor in Oxidative Decomposition of Calcium Sulfide[J].Fuel, 2004, 83:671-677
[18]Anthony E J, Jia L, Qiu K R.CaS oxidation by reaction with CO2 and H2O[J].Energy and Fuels, 2003, 17(2):363-368
[19]宋占龙, 董勇, 章名耀.CO2对CaS氧化反应的影响[J].燃烧科学与技术, 2009, 15(4):316-320
[20]Qiu K R, Anthony E J, Jia L.Oxidation of sulfide limestone under the conditions of pressurized fluidized bed combustion[J].Fuel, 2001, 80(4):549-558

Options

文章导航

模态框（Modal）标题

摘要

本文引用格式

Abstract

参考文献