论文总字数：31187字
摘 要
2零排放的必由之路。钙基吸收剂由于来源广泛、价格低廉，在燃煤电站碳捕捉技术中得到了广泛重视。而煅烧钙基吸收剂需要的纯氧制备代价很高，若由可自由释氧的铜基载氧体提供则可大大降低其成本。本毕业设计针对化石燃料燃烧后烟气的碳捕捉问题，首次提出了耦合钙基吸收剂循环煅烧/加压碳酸化与化学链氧解耦燃烧的新方法和技术。为了研究Ca/Cu基复合材料在煅烧反应器中释氧和在不同压力下的捕集CO2和载氧特性，首先使用机械混合法自行制备了Ca/Cu基复合材料，之后以常压管式炉和加压管式炉分别作为煅烧反应器和碳酸化反应器，在不同碳酸化压力下，进行了常压煅烧/加压碳酸化循环实验。实验结果表明，压力提高可以促进Ca/Cu基复合材料中钙基吸收剂捕集CO2和铜基载氧体吸收O2的能力。但是，Ca/Cu基复合材料释氧以及在不同压力下捕集CO2和载氧特性低于单独的钙基吸收剂或铜基载氧体。其深层次机理和制备方法优化将在进一步工作中进行。关键词：CO2捕集；钙基吸收剂；铜基载氧体；CaL-CLC；加压碳酸化
Fundamental Study on CO2 Capture from Flue Gas with Ca/Cu-based Composite Materials
Shi Tian
Supervised by Duan Lunbo
Advised by Chen Jian
Abstract： Global warming and greenhouse gas control is an emerging hot topic in the energy and environment field. Using carbon capture and storage technology is the only way leading to zero emission of CO2 in the coal-fired power plant. Since the calcium looping technology takes advantages of sorbents which can be obtained widely and cheaply, it have gained extensive attention among all the carbon capture technologies. However, pure oxygen is necessary for calcination of calcium-based sorbents, production of which will cost a lot. It will greatly reduce the cost if the copper-based oxygen carrier, which can release oxygen freely, can be introduced to the process. The thesis for the first time proposes the new method and technology of coupling of cyclic calcination/pressurized carbonation reaction for carbon capture and chemical-looping with oxygen uncoupling so as to realize the aim of carbon capture of flue gas generated from burning fossil fuel. Mechanical mixing method was employed to fabricate the Ca/Cu-based composite and its capability of CO2 capture and oxygen uptake in carbonation reactor, as well as oxygen release in calcination actor were tested. An atmospheric tube furnace and a pressurized tube furnace act as the calciner and the carbonator respectively. The experiment of cyclic calcination/pressurized carbonation was conducted under series of carbonation pressure. The results show that capability of CO2 capture and oxygen uptake for the copper-based oxygen carrier in the composite material become better with pressurized carbonation applied. But the capability of CO2 capture for the calcium-based sorbent weakens when it is composited with copper-based oxygen carriers. And the ability to release and uptake oxygen for copper-based oxygen carriers is also hindered by the calcium-based sorbent in the composite material. The exploration of its underlying mechanism and improvement of the preparation method will begin in further research.
Key words: CO2 capture；Calcium-based sorbent；Copper-based oxygen carriers；CaL-CLC; Pressurized carbonation
目录
1、绪论 1
1.1 CCS技术 1
1.2 燃烧后碳捕集 2
1.3 钙基吸收剂循环煅烧/碳酸化捕集CO2和加压碳酸化的提出 2
1.3.1 CCCR系统 2
1.3.2 钙基吸收剂 3
1.3.3 钙基吸收剂煅烧/加压碳酸化的提出 4
1.4 CaL-CLC系统 5
1.4.1 化学链氧解耦 5
1.4.2. CaL-CLC的提出 6
1.4.3 Ca/Cu基复合材料的制备 6
1.4.4 毕业设计研究目的及意义 7
1.5 本章小结 7
2、实验装置、方法及数据分析 9
2.1 实验样品 9
2.2 实验装置及仪器 9
2.2.1 加压热重分析仪 9
2.2.2 常压煅烧/加压碳酸化反应实验装置 9
2.2.3 X射线衍射仪 10
2.3 预备性实验 10
2.3.1 制备过程实验 10
2.3.2 常压煅烧/加压碳酸化实验装置实验 10
2.4 数据计算 11
2.5 本章小结 12
3、Ca/Cu基复合粉末煅烧/加压碳酸化及载氧特性 13
3.1 Ca/Cu基复合粉末煅烧释氧特性 13
3.2 Ca/Cu基复合粉末加压碳酸化特性 14
3.3 Ca/Cu复合粉末加压载氧特性 16
3.4 本章小结 17
4、结论 18
致 谢 19
参考文献 20
1、绪论
近年来，气候原因导致的极端天气对人类的生产生活造成了极大危害。政府间气候变化专门委员会（Intergovernmental Panel on Climate Change, IPCC）第五次评估报告1指出，气候变化在未来可能带来物种灭绝、粮食减产等不良影响，而其成因极大程度上归结于人为温室气体排放。针对这一点，第21届联合国气候变化大会上各方一致同意通过《巴黎协定》2。协定指出，全球将尽快实现温室气体排放达峰值，本世纪下半叶实现温室气体“净零”排放。而温室气体的主要组成部分CO2则大多来自于化石燃料，尤其是煤炭的燃烧3。表1.14展示了2014年美国、德国、中国等主要国家的能源结构。从表上可以看出，目前中国的能源消耗总量居世界第一。尽管可再生能源消费量仅次于美国，中国的一次能源结构仍以煤炭为主。从世界上其他国家来看，除德国可再生能源消耗量占总消耗量可达10%以外，其他国家的占比都很小，仍然以石油、煤炭等化石燃料为主。因此，目前可行的措施在于减少排入大气中的温室气体，特别是CO2。CCS技术在这样的背景下被提出，并在2000年首次实现商业应用5。
表1.1 2014年主要国家分燃料消费量
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