中高温钙基材料热化学储热的研究进展与展望

doi:10.11949/0438-1157.20230338

化工学报 ›› 2023, Vol. 74 ›› Issue (8): 3171-3192.DOI: 10.11949/0438-1157.20230338

中高温钙基材料热化学储热的研究进展与展望

郑玉圆¹^,²(), 葛志伟¹^,²^,³(), 韩翔宇¹^,², 王亮¹^,²^,³, 陈海生¹^,²()

^1.中国科学院工程热物理研究所，北京 100190
^2.中国科学院大学，北京 100049
^3.中国科学院洁净能源创新研究院，辽宁大连 116023

收稿日期:2023-04-06 修回日期:2023-08-15 出版日期:2023-08-25 发布日期:2023-10-18
通讯作者: 葛志伟,陈海生
作者简介:郑玉圆（1999—），女，硕士研究生，zhengyuyuan@iet.cn
基金资助:
国家自然科学基金项目(52176210);中国科学院洁净能源创新研究院合作基金项目(DNL202017);内蒙古自治区科技计划项目(2021ZD0030)

Progress and prospect of medium and high temperature thermochemical energy storage of calcium-based materials

Yuyuan ZHENG¹^,²(), Zhiwei GE¹^,²^,³(), Xiangyu HAN¹^,², Liang WANG¹^,²^,³, Haisheng CHEN¹^,²()

^1.Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing 100190, China
^2.University of Chinese Academy of Sciences, Beijing 100049, China
^3.Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2023-04-06 Revised:2023-08-15 Online:2023-08-25 Published:2023-10-18
Contact: Zhiwei GE, Haisheng CHEN

摘要/Abstract

摘要：

热化学储热由于能量密度高，材料适宜于长时储存和远距离运输，成为高效储热新兴的研究热点。钙基材料热化学储热成本低且无毒无污染，具有广阔应用前景。总结了目前热化学储热的主要体系及分类，针对中高温钙基热化学储热技术从材料改性、反应器设计及系统集成应用三个层面的研究进展进行综述。探讨钙基热化学储热技术研究中面临的挑战与机遇，并对今后的研究与发展方向提出了建议。

关键词: 热化学储热, 钙基颗粒物料, 稳定性, 反应器设计, 过程系统

Abstract:

Thermochemical energy storage has become an emerging research hotspot for efficient heat storage due to its high energy density and materials suitable for long-term storage and long-distance transportation. Calcium-based materials, which are low-cost, non-toxic, and non-polluting, have shown promising applications in this regard. This paper summarizes the current systems and categorization of the thermochemical thermal storage. It encompasses material modification, reactor design, and system integration applications for medium and high temperature calcium-based thermochemical storage. Then, the recent challenges and opportunities in calcium-based thermochemical energy storage technology are presented. Finally, this paper offers an outlook and provides suggestions for future research and development directions.

Key words: thermochemical energy storage, calcium-based granular material, stability, reactor design, process systems

中图分类号:

TK 02

郑玉圆, 葛志伟, 韩翔宇, 王亮, 陈海生. 中高温钙基材料热化学储热的研究进展与展望[J]. 化工学报, 2023, 74(8): 3171-3192.

Yuyuan ZHENG, Zhiwei GE, Xiangyu HAN, Liang WANG, Haisheng CHEN. Progress and prospect of medium and high temperature thermochemical energy storage of calcium-based materials[J]. CIESC Journal, 2023, 74(8): 3171-3192.

图/表 31

图1 部分热化学储热材料的反应温度和储热密度[9-10]

Fig.1 Reaction temperature and storage density of some thermochemical energy storage materials[9-10]

表1 热化学储热的反应类型及反应条件

Table 1 The classification and reaction conditions for thermochemical energy storage

反应类型	反应式	ΔH/(kJ/mol)	T/℃
金属氢化物反应^[12-13]	$M g H 2 (s) M g (s) + H 2 (g)$	75	450
金属氢化物反应^[12-13]	$L i H (s) L i (s) + 1 / 2 H 2 (g)$	88	947
氨类反应^[14]	$2 N H 3 (g) N 2 (g) + 3 H 2 (g)$	66	200
氨类反应^[14]	$N H 4 H S O 4 (l) H 2 O (g) + N H 3 (g) + S O 3 (g)$	335	467
氢氧化物反应^[15-16]	$M g O H 2 (s) M g O (s) + H 2 O (g)$	84	330
氢氧化物反应^[15-16]	$C a (O H) 2 (s) C a O (s) + H 2 O (g)$	104	515
碳酸盐反应^[9,17]	$C a C O 3 (s) C a O (s) + C O 2 (g)$	178	900
碳酸盐反应^[9,17]	$M g C O 3 (s) M g O (s) + C O 2 (g)$	125	400
氧化还原反应^[10,18]	$2 C o 3 O 4 (s) 6 C o O (s) + O 2 (g)$	205	914
氧化还原反应^[10,18]	$6 M n 2 O 3 (s) 4 M n 3 O 4 (s) + O 2 (g)$	910	948

表1 热化学储热的反应类型及反应条件

Table 1 The classification and reaction conditions for thermochemical energy storage

反应类型	反应式	ΔH/(kJ/mol)	T/℃
金属氢化物反应^[12-13]	$M g H 2 (s) M g (s) + H 2 (g)$	75	450
金属氢化物反应^[12-13]	$L i H (s) L i (s) + 1 / 2 H 2 (g)$	88	947
氨类反应^[14]	$2 N H 3 (g) N 2 (g) + 3 H 2 (g)$	66	200
氨类反应^[14]	$N H 4 H S O 4 (l) H 2 O (g) + N H 3 (g) + S O 3 (g)$	335	467
氢氧化物反应^[15-16]	$M g O H 2 (s) M g O (s) + H 2 O (g)$	84	330
氢氧化物反应^[15-16]	$C a (O H) 2 (s) C a O (s) + H 2 O (g)$	104	515
碳酸盐反应^[9,17]	$C a C O 3 (s) C a O (s) + C O 2 (g)$	178	900
碳酸盐反应^[9,17]	$M g C O 3 (s) M g O (s) + C O 2 (g)$	125	400
氧化还原反应^[10,18]	$2 C o 3 O 4 (s) 6 C o O (s) + O 2 (g)$	205	914
氧化还原反应^[10,18]	$6 M n 2 O 3 (s) 4 M n 3 O 4 (s) + O 2 (g)$	910	948

图2 (a)天然钙基材料在950℃下100个循环内的CaO转化率；(b)1000个循环内的CO2吸附量[37]

Fig.2 (a) CaO conversion of natural calcium-based materials within 100 cycles at 950℃; (b) CO2 adsorption within 1000 cycles[37]

表2 氧化物掺杂改性的分类及特点

Table 2 Classification and characteristics of oxide doping modification

分类	掺杂材料	特点	文献
活性掺杂	Al₂O₃, ZrO₂	在50次煅烧/碳酸化循环中保持80%以上吸附性；允许离子在整个晶体结构中迁移，对碳酸化反应起到催化作用；有效增强循环稳定性和反应活性	[42]
	CeO₂, Mn₃O₄	分散CaO颗粒，缓解烧结；Ce和Mn之间的电子转移促进了CO₂扩散和O^2-迁移；在40次循环中保持0.61 g/g的CO₂吸附量	[43]
	Fe₂O₃, Mn₃O₄	薄片状多孔结构；促进氧空位产生并降低反应活化能；在20次循环中保持95%的转化率	[44]
	Al₂O₃, CeO₂	掺杂量为5%时表现出最高的储热能力；30次循环有效转化率和能量密度仅下降7%；具有更大的比表面积和孔隙率，促进CO₂吸附	[45]
惰性掺杂	Al₂O₃	提高反应速率，缩短反应时间（减少42%）；提高循环稳定性	[46]
	SiO₂	提高材料机械强度，在100次循环内保持28 N以上	[23]
	SiO₂	提高材料导热性能，比热容提高20%；掺杂量为5%时材料反应动力学表现最佳；循环稳定性增强28%	[47]
	TiO₂	掺杂量为2.5% 储热密度达1256.68 kJ/kg，30次循环后仍为纯CaCO₃的2.26倍；反应活化能从1117.39 kJ/mol降低到997.6 kJ/mol，脱碳温度从903.56℃降低到876.13℃；总转化率降低	[48]

图3 50次循环前后CaCO3-Al2O3-ZrO2 (质量分数13.3%)样品的SEM图和EDS图（Al：蓝色；Zr：绿色；Ca：红色）[42]

Fig.3 SEM and EDS images of CaCO3-Al2O3-ZrO2 (mass fraction 13.3%) samples before and after 50 cycles (Al: blue; Zr: green; Ca: red) [42]

图4 掺杂惰性成分的抗烧结原理图[35]

Fig.4 Schematic diagram of anti-sintering with doped inert components[35]

图5 Na2CO3-CaO吸附剂对CO2的吸附机理[54]

Fig.5 Mechanism of CO2 adsorption by Na2CO3-CaO adsorbent[54]

图6 钾盐、钠盐掺杂对钙基材料循环稳定性的影响[57]

Fig.6 Effect of potassium and sodium salt doping on the cyclic stability of calcium-based materials[57]

图7 封装在半透性陶瓷材料（外壳：棕色部分）中的CaO/Ca(OH)2（核芯：白色和灰色部分）体系的水合/脱水反应原理[58]

Fig.7 Principle of hydration/ dehydration reaction of CaO/Ca(OH)2 system encapsulated in semi-permeable ceramic material (shell: brown part； core: white and gray parts)[58]

图8 采用重复浸渍-蒸发涂层工艺的核壳结构CaO基球团的形成过程[65]

Fig.8 Formation process of the core-shell-structured CaO-based pellets using the general repeated impregnation-evaporation coating process[65]

图9 固定床实验台和主要设备[69]

Fig.9 Fixed bed bench and main equipment[69]

图10 间接式固定床反应器[70]

Fig.10 Indirect fixed bed reactor[70]

图11 嵌入多孔通道的反应器示意图[72]

Fig.11 Schematic diagram of the reactor with embedded porous channels[72]

图12 多层反应器结构及监测点示意图[73]

Fig.12 The schematic of multi-layer reactor structure and monitoring points[73]

图13 用于多循环储能实验的加压反应器示意图[77]

Fig.13 The schematic diagram of pressurized reactor for multi-cycle energy storage[77]

图14 间歇式流化床实验装置示意图[79]

Fig.14 The schematic diagram of intermittent fluidized bed experimental setup[79]

图15 流化床反应器实验装置示意图[80]

Fig.15 The schematic diagram of the fluidized bed reactor experimental setup [80]

图16 基于犁铧混合器的新型流化床反应器[81]

Fig.16 A novel fluidized bed reactor based on ploughshare mixer[81]

图17 钙循环捕集CO2的双流化床装置示意图[83]

Fig.17 The schematic diagram of a double fluidized bed device for calcium cycle CO2 capture[83]

图18 有蒸汽添加的流化床反应器实验装置示意图[86]

Fig.18 The experimental setup of fluidized bed reactor with steam addition[86]

图19 间歇式流化床反应器[90]

Fig.19 Intermittent fluidized bed reactor[90]

图20 传热流体在壳内（红色箭头）和储热材料在反应器管中（绿色箭头）的流动示意图（a）及反应器的3D图像（b）[60]

Fig.20 The flow routes of the heat transfer fluid in the shell (red arrows) and the heat storage material in the reactor tube (green arrows) (a) and 3D image of the reactor (b)[60]

图21 换热板和材料通道及盖板和反应气体入口[92]

Fig.21 Heat exchanger plate and material channel and cover plate and reaction gas inlet[92]

图22 螺旋管反应器[94]

Fig.22 Spiral tube reactor[94]

图23 钙循环高温吸附捕集系统原理图

Fig.23 Schematic of the carbonate looping process for CO2 capture

图24 1 MWh规模双流化床钙基碳捕集系统[99]

Fig.24 1 MWh scale double fluidized bed calcium-based carbon capture system[99]

图25 化学热泵运行示意图[104]

Fig.25 Chemical heat pump operation diagram[104]

图26 CSP-Cal热化学储热系统概念图[113]

Fig.26 Conceptual diagram of CSP-Cal thermochemical thermal storage system[113]

图27 CSP-Cal闭式布雷顿循环系统示意图[116]

Fig.27 Diagram of CSP-Cal closed Brayton cycle system[116]

图28 双流化床系统示意图[117]

Fig.28 The schematic diagram of double fluidized bed system[117]

图29 SOCRATCES项目工厂流程图（10 kW规模）[123]

Fig.29 SOCRATCES project plant flow chart (10 kW scale) [123]

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中高温钙基材料热化学储热的研究进展与展望

Progress and prospect of medium and high temperature thermochemical energy storage of calcium-based materials

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