基于反应器设计的有机液态储氢载体脱氢反应强化研究进展

doi:10.16085/j.issn.1000-6613.2024-1077

化工进展 ›› 2024, Vol. 43 ›› Issue (S1): 189-208.DOI: 10.16085/j.issn.1000-6613.2024-1077

基于反应器设计的有机液态储氢载体脱氢反应强化研究进展

王波¹(), 王斌¹^,², 龚翔¹^,²(), 杨福胜¹^,², 方涛¹^,²()

^1.西安交通大学化学工程与技术学院，陕西西安 710049
^2.陕西氢易能源科技有限公司，陕西西安 712000

收稿日期:2024-07-05 修回日期:2024-08-24 出版日期:2024-11-20 发布日期:2024-12-06
通讯作者: 龚翔,方涛
作者简介:王波（1999—），男，博士研究生，研究方向为有机液态储氢技术。E-mail：wb15281123670@stu.edu.cn。
基金资助:
陕西省重点研发计划(2024GX-ZDCYL-04-05);陕西省青年科技新星项目(2024ZC-KJXX-073);西安市英才计划(XAYC240010);陕西省自然科学基础研究计划(2022JZ-07);西安市科技计划(23ZCKCGZH0005);中国博士后科学基金会项目(2024M752588);咸阳市重大科技成果转化落地专项项目(L2023-ZDKJ-QCY-CGLD-GY-007)

Enhancing dehydrogenation performance of liquid organic hydrogen carriers based on reactor design: Research progress

WANG Bo¹(), WANG Bin¹^,², GONG Xiang¹^,²(), YANG Fusheng¹^,², FANG Tao¹^,²()

^1.College of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, Shaanxi, China
^2.Shaanxi HydroTransformer Energy Technologies Co. , Ltd. , Xi'an 712000, Shaanxi, China

Received:2024-07-05 Revised:2024-08-24 Online:2024-11-20 Published:2024-12-06
Contact: GONG Xiang, FANG Tao

摘要/Abstract

摘要：

有机液态储氢载体（liquid organic hydrogen carriers, LOHC）技术是一种应用前景广阔的液态储氢技术，但LOHC脱氢过程中动力学缓慢等问题制约了该技术发展，基于动力学和传热传质强化的反应器设计是必然选择。本文分析了有机液态储氢载体脱氢反应动力学性能强化机制，指出催化剂表面高反应物浓度和高温是高反应速率的关键，且需减少副产物和催化剂失活。提出了传热强化、传质强化策略，以固定床反应器为例介绍了强化传热的目标和措施，指出了强化传质应提高外扩散速率并避免内扩散的影响。简述了多种类型LOHC“气液固”三相反应器的研究进展及其强化策略，最后总结了这些反应器的特点并提出了可能的新型反应器设计方向。可为针对有机液态储氢材料脱氢过程的新型反应器开发提供理论思路和参考依据。

关键词: 氢能, 有机液态储氢载体, 反应器, 脱氢, 强化

Abstract:

Liquid organic hydrogen carrier (LOHC) technology is a promising liquid hydrogen storage technology, but slow kinetics during LOHC dehydrogenation process has restricted the development of LOHC. The reactor design based on heat transfer, mass transfer and kinetics enhancement is an inevitable choice. This paper analyzed the mechanism of LOHC dehydrogenation kinetics enhancement, and pointed out that high concentration of reactants and high temperature on the catalyst surface were the key to high reaction rate, and the byproducts and catalyst deactivation should be reduced. It proposed heat transfer and mass transfer enhancement strategies and introduced the objectives and measures of heat transfer enhancement of fixed bed reactor as an example. It pointed out that mass transfer enhancement should increase the external diffusion rate and avoid the influence of internal diffusion. The research summarized progress and intensification strategies of various types of LOHC“gas-liquid-solid”three-phase reactors. Finally, it summarized the characteristics of these reactors and put forward the possible new reactor design direction. It could provide theoretical ideas and reference for developing new reactors for LOHC dehydrogenation process.

Key words: hydrogen energy, liquid organic hydrogen carriers, reactor, dehydrogenation, enhancement

中图分类号:

TQ116.2

王波, 王斌, 龚翔, 杨福胜, 方涛. 基于反应器设计的有机液态储氢载体脱氢反应强化研究进展[J]. 化工进展, 2024, 43(S1): 189-208.

WANG Bo, WANG Bin, GONG Xiang, YANG Fusheng, FANG Tao. Enhancing dehydrogenation performance of liquid organic hydrogen carriers based on reactor design: Research progress[J]. Chemical Industry and Engineering Progress, 2024, 43(S1): 189-208.

图/表 16

图1 有机液态储氢材料循环加脱氢示意图

表1 LOHC理化性质

序号	LOHC^-/LOHC⁺	储氢密度（质量分数）/%	脱氢焓/kJ·mol^-1	LOHC^-熔点/℃	LOHC⁺沸点/℃
1	TOL/MCH	6.2	68.3	-95	101
2	NEC/12H-NEC	5.8	47.5	68	280
3	NAP/十氢萘	7.3	63.9	-37	189
4	DBT/18H-DBT	6.2	65.4	-34	370
5	BT/12H-BT	6.2	63.5	-30	270
6	1-MID/8H-1-MID	5.8	51.9	95	180

图2 传统对流加热与微波加热[16]

图3 带有多孔介质燃烧器的固定床反应器[17]

图4 反应温度与扩散距离的关系[21]

图5 DehyMax中反应物向上流过热管时的温度分布[45]

图6 ARR概念图[46]及热管式脱氢反应器[47]A—填充床反应器、氢气燃烧器、PCM室耦合系统概念图；B—反应器三维模型；C—带保温夹套的反应器实物图

图7 亚单位立方金刚石晶体结构，通过SEBM工艺制造的不同尺寸孔道及三个不同阶段粉末去除[52]

图8 不同加热温度下的反应速率常数与阻滞常数及液膜态图解[22]

图9 喷雾脉冲式反应器实验装置及红外热像仪记录的催化剂表面热分布图[23]

图10 Pd/Ta复合膜反应器[55]、沸石-Al2O3-Pd膜三层膜示意图[56]及SiO2-双载体催化剂层三层膜示意图[57]

图11 多级微结构模型示意图[68]及径向流动反应器[69]

图12 有分离区与无分离区的产氢速率对比及催化精馏与液相脱氢对比[29]

图13 加脱氢一体化反应器[71-72]

图14 旋流鼓泡反应器、稳定状态涡旋鼓泡层及不稳定状态涡旋鼓泡层[74]

表2 不同类型反应器的对比

序号	反应器	LOHC体系	强化策略	温度，压力	脱氢性能	参考文献
1	批式反应釜	DBT	加氢/脱氢循环	加氢：140~200℃，3~4MPa 脱氢270℃，320℃	加氢率100%；脱氢率50%~80%	[35]
2	批式烧瓶	DBT	降低副产物	脱氢310℃，0.1MPa	最大产氢能力4g/(g_cat·min) 最低副产物2%	[38]
3	微分反应器	DBT	更准确的反应速率	脱氢250~340℃，0.1MPa， WHSV 0.5~67h^-1	转化率范围30%~54%	[43]
4	列管式固定床	BT	均匀温度分布	脱氢348~364℃，0.1MPa， LHSV 0.6~1.2h^-1	2.3m³/h(标准状况)，脱氢程度大于90%	[44]
5	热管式固定床	MCH	传热强化	脱氢260~370℃，0.1MPa， LHSV 2~8h^-1	脱氢程度100%，重整效率80%	[47]
6	交叉反向固定床	BT	传热强化	脱氢280~320℃，0.4MPa，原料流率50mL/min	脱氢程度小于70%，能量密度是传统反应器的2.3倍	[45]
7	整体涂层式反应器	NEC	传热强化、传质强化	脱氢220~260℃，0.1MPa，原料流率0.5~4mL/min	最大氢气产率65%，最大生产能力为 1.27 $g H 2 / (g P t · m i n)$	[52]
8	“湿干”多相反应器	环己烷、MCH、萘	催化剂表面高温	脱氢250~400℃，0.1MPa，环己烷1mL，萘0.75mL	环己烷/MCH/萘最大反应速率常数分别为8mmol/min、6.5mmol/min和5.7mmol/min	[22]
9	微通道反应器	DBT	传热强化、传质强化	脱氢260~320℃，0.1MPa， 0.01mL/min	最大氢气产率82%，氢气纯度99.99%	[67]
10	径向流动反应器	DBT	传热强化、反应动力学强化	脱氢340℃， 0.2MPa/0.3MPa/0.4MPa 0.38mL/min	脱氢程度18%~24%。氢气纯度99.999%，1.15 $g H 2 / (g P t · m i n)$	[68]
11	膜反应器	MCH	传质强化、反应动力学强化	脱氢350℃，0.9MPa 标准停留时间250kg·s/m³	转化率95%，H₂/N₂选择性大于85000	[59]
12	反应精馏	BT	传热强化、反应动力学强化	脱氢300℃，0.1MPa 0.2~0.8g/min	氢气流量280mL/min，脱氢程度80%，0.35 $g H 2 / (g P t · m i n)$	[70]
13	加氢脱氢一体化反应器	DBT	加氢脱氢循环	加氢：300℃，3MPa 脱氢：290℃，0.2MPa	脱氢率70% 1.2 $g H 2 / (g P t · m i n)$	[71]

表2 不同类型反应器的对比

序号	反应器	LOHC体系	强化策略	温度，压力	脱氢性能	参考文献
1	批式反应釜	DBT	加氢/脱氢循环	加氢：140~200℃，3~4MPa 脱氢270℃，320℃	加氢率100%；脱氢率50%~80%	[35]
2	批式烧瓶	DBT	降低副产物	脱氢310℃，0.1MPa	最大产氢能力4g/(g_cat·min) 最低副产物2%	[38]
3	微分反应器	DBT	更准确的反应速率	脱氢250~340℃，0.1MPa， WHSV 0.5~67h^-1	转化率范围30%~54%	[43]
4	列管式固定床	BT	均匀温度分布	脱氢348~364℃，0.1MPa， LHSV 0.6~1.2h^-1	2.3m³/h(标准状况)，脱氢程度大于90%	[44]
5	热管式固定床	MCH	传热强化	脱氢260~370℃，0.1MPa， LHSV 2~8h^-1	脱氢程度100%，重整效率80%	[47]
6	交叉反向固定床	BT	传热强化	脱氢280~320℃，0.4MPa，原料流率50mL/min	脱氢程度小于70%，能量密度是传统反应器的2.3倍	[45]
7	整体涂层式反应器	NEC	传热强化、传质强化	脱氢220~260℃，0.1MPa，原料流率0.5~4mL/min	最大氢气产率65%，最大生产能力为 1.27 $g H 2 / (g P t · m i n)$	[52]
8	“湿干”多相反应器	环己烷、MCH、萘	催化剂表面高温	脱氢250~400℃，0.1MPa，环己烷1mL，萘0.75mL	环己烷/MCH/萘最大反应速率常数分别为8mmol/min、6.5mmol/min和5.7mmol/min	[22]
9	微通道反应器	DBT	传热强化、传质强化	脱氢260~320℃，0.1MPa， 0.01mL/min	最大氢气产率82%，氢气纯度99.99%	[67]
10	径向流动反应器	DBT	传热强化、反应动力学强化	脱氢340℃， 0.2MPa/0.3MPa/0.4MPa 0.38mL/min	脱氢程度18%~24%。氢气纯度99.999%，1.15 $g H 2 / (g P t · m i n)$	[68]
11	膜反应器	MCH	传质强化、反应动力学强化	脱氢350℃，0.9MPa 标准停留时间250kg·s/m³	转化率95%，H₂/N₂选择性大于85000	[59]
12	反应精馏	BT	传热强化、反应动力学强化	脱氢300℃，0.1MPa 0.2~0.8g/min	氢气流量280mL/min，脱氢程度80%，0.35 $g H 2 / (g P t · m i n)$	[70]
13	加氢脱氢一体化反应器	DBT	加氢脱氢循环	加氢：300℃，3MPa 脱氢：290℃，0.2MPa	脱氢率70% 1.2 $g H 2 / (g P t · m i n)$	[71]

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基于反应器设计的有机液态储氢载体脱氢反应强化研究进展

Enhancing dehydrogenation performance of liquid organic hydrogen carriers based on reactor design: Research progress

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