质子导体固体氧化物电化学装置中氨的利用与合成

doi:10.19799/j.cnki.2095-4239.2021.0326

储能科学与技术 ›› 2021, Vol. 10 ›› Issue (6): 1998-2007.doi: 10.19799/j.cnki.2095-4239.2021.0326

质子导体固体氧化物电化学装置中氨的利用与合成

练文超¹(), 雷励斌¹(), 梁波¹, 王超¹, 魏磊¹, 田志鹏¹, 刘建平¹, 杨华政², 梁家健², 施涛³

^1.广东工业大学材料与能源学院，广东广州 510006
^2.佛山索弗克氢能源有限公司，广东佛山 528000
^3.佛山市攀业氢能源科技有限公司，广东佛山 528216

收稿日期:2021-07-08 修回日期:2021-07-22 出版日期:2021-11-05 发布日期:2021-11-03
通讯作者: 雷励斌 E-mail:931830289@qq.com;libinlei23@gdut.edu.cn
作者简介:练文超（1996—），男，硕士研究生，研究方向为固体氧化物燃料电池/电解池， E-mail：931830289@qq.com；
基金资助:
国家自然科学基金项目(52002082)

Utilization and synthesis of ammonia in proton-conducting solid oxide electrochemical devices

Wenchao LIAN¹(), Libin LEI¹(), Bo LIANG¹, Chao WANG¹, Lei WEI¹, Zhipeng TIAN¹, Jianping LIU¹, Huazheng YANG², Jiajian LIANG², Tao SHI³

^1.School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, Guangdong, China
^2.Foshan ISOFC Dynamic Co. Ltd. , Foshan 528000, Guangdong, China
^3.Foshan Panye Hydrogen Energy Technology Co. Ltd. , Foshan 528216, Guangdong, China

Received:2021-07-08 Revised:2021-07-22 Online:2021-11-05 Published:2021-11-03
Contact: Libin LEI E-mail:931830289@qq.com;libinlei23@gdut.edu.cn

摘要/Abstract

摘要：

氨作为一种理想的储能材料和氢能源载体，其在质子导体固体氧化物电化学装置中的利用与合成可实现高效清洁的发电和储能。本文综述了质子导体固体氧化物电化学装置中氨的利用与合成的实验和理论研究进展，在实验研究方面全面分析了电解质和氨电极材料的开发，在理论研究方面重点讨论了热力学-电化学模型和密度泛函理论(DFT)的研究概况。电解质的质子电导率和氨电极的催化活性是影响电化学装置性能的关键因素，因此开发高质子电导率的电解质和高催化活性的氨电极仍是主要的研究方向。热力学-电化学模型和基于DFT的理论研究可分别为电化学装置的结构设计/运行条件的优化和氨电极材料的开发提供有效指导和思路，但是对于更高层次(三维)的热力学-电化学模型理论研究和氨电极材料上氮气的电化学活化机理的研究仍需加强。最后总结指出了质子导体固体氧化物电化学装置中氨的利用与合成的未来研究方向。

关键词: 固体氧化物燃料电池, 质子导体反应器, 氨, 合成氨, 氨电极材料

Abstract:

Ammonia is an ideal energy storage material and hydrogen energy carrier. Its utilization and synthesis in proton-conducting solid oxide electrochemical devices can realize efficient and clean power generation and energy storage. In this paper, we review the advances in experimental and theoretical studies on the utilization and synthesis of ammonia in proton-conducting solid oxide electrochemical devices. In the aspect of experimental study, the development of electrolytes and ammonia electrode materials are comprehensively analyzed. While in the aspect of theoretical study, the research progress of thermodynamic-electrochemical models and density functional theory (DFT) are discussed emphatically. Since the proton conductivity of electrolyte materials and the catalytic activity of ammonia electrodes are the critical factors affecting the performance of electrochemical devices, the development of electrolyte materials with high proton conductivity and ammonia electrodes with high catalytic activity are still the main research topics. Thermodynamic-electrochemical models and DFT-based theoretical researches can provide guidance and ideas for the structural design of electrochemical device/optimization of operating conditions and development of ammonia electrode materials, respectively. However, theoretical studies of higher-level (three-dimensional) thermal-electrochemical models and the electrochemical activation mechanism of nitrogen on ammonia electrode materials still deserve further study. Finally, the future research directions of ammonia utilization and synthesis in electrochemical devices are also summarized.

Key words: solid oxide fuel cell, proton-conducting electrochemical reactor, ammonia, ammonia synthesis, ammonia electrode materials

中图分类号:

TQ 152

练文超, 雷励斌, 梁波, 王超, 魏磊, 田志鹏, 刘建平, 杨华政, 梁家健, 施涛. 质子导体固体氧化物电化学装置中氨的利用与合成[J]. 储能科学与技术, 2021, 10(6): 1998-2007.

Wenchao LIAN, Libin LEI, Bo LIANG, Chao WANG, Lei WEI, Zhipeng TIAN, Jianping LIU, Huazheng YANG, Jiajian LIANG, Tao SHI. Utilization and synthesis of ammonia in proton-conducting solid oxide electrochemical devices[J]. Energy Storage Science and Technology, 2021, 10(6): 1998-2007.

图/表 5

图1

图2

表1

图3

表2

质子导体反应器电化学合成氨的代表性实验研究"

质子导体反应器(氢电极 \| 电解质 \| 氨电极)	工作温度/℃	$r N H 3$ / $[m o l / (s ? c m 2)]$	FE/%	年份，文献
Pd \| SCY \| Pd	570	$4.50 × 10 - 9$	78	1998，[34]
Ag-Pd \| LCZ \| Ag-Pd	520	$2.00 × 10 - 9$	—	2004，[37]
Ag-Pd \| CLC \| Ag-Pd	650	$7.5 × 10 - 9$	—	2005，[38]
Ag-Pd \| LSGM \| Ag-Pd	550	$2.37 × 10 - 9$	70	2007，[39]
Ag-Pd \| BCC \| Ag-Pd	500	$2.69 × 10 - 9$	50	2010，[40]
Ni-BCY15 \| BCY15 \| BSCF	530	$4.10 × 10 - 9$	60	2010，[41]
LSCF \| BZY20 \| LSCF	550	$8.50 × 10 - 11$	0.33	2015，[42]
Pt \| BCY \| LSTR-BCY	500	$3.80 × 10 - 12$	—	2016，[43]
Pt \| BCY \| LST-BCYR	500	$1.10 × 10 - 11$	2.1	2017，[44]
Ni-BCZYZ \| BCZYZ \| Fe-BCZYZ	450	$4.00 × 10 - 9$	2.5	2017，[45]
Ni-BZCY44 \| BZCY44 \| BSTR	500	$1.10 × 10 - 9$	5.9	2019，[46]
Ni-BZCY72 \| BZCY81 \| VN-Fe	600	$1.89 × 10 - 9$	14	2020，[36]

表2

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燃料电池(氨电极 \| 电解质 \| 空气电极)	电解质厚度/μm	工作温度/℃	最大功率密度/(mW/cm²)	年份，文献
Pt \| BCGO \| Pt	1300	700	25	2004，[7]
Pt \| BCGP \| Pt	1300	700	35	2005，[8]
Pt \| BCE \| Pt	1000	700	32	2006，[9]
Ni-BCGO \| BCGO \| LSCO	50	650	184	2006，[10]
Ni-BCGO \| BCGO \| LSCO	50	700	355	2006，[10]
Ni-BCNO \| BCNO \| LSCO	20	700	315	2007，[11]
Ni-BCE \| BCGP \| Pt	1000	500	15	2008，[12]
Ni-BCE \| BCGP \| Pt	1000	600	28	2008，[12]
Ni-CGO \| BCGO \| BSCFO-CGO	30	600	147	2008，[13]
Ni-CGO \| BCGO \| BSCFO-CGO	30	650	200	2008，[13]
Ni-BZCY17 \| BZCY17 \| BSCF	35	450	25	2010，[14]
Ni-BZCY17 \| BZCY17 \| BSCF	35	700	325	2010，[14]
Ni-BCY25 \| BCY10 \| SSC	1000	600	165	2015，[15]
Ni-BCY25 \| BCY10 \| SSC	1000	650	210	2015，[15]
Ni-BZY20 \| BZY20 \| Pt	60～90	600	70	2017，[16]
Ni-BZY20 \| BZY20 \| Pt	60～90	700	130	2017，[16]
Ni-BZCY44 \| BCY20 \| BCY20-LSCF	50～60	600	130	2020，[17]
Ni-BZCY44 \| BCY20 \| BCY20-LSCF	50～60	700	180	2020，[17]
Ni-BZCYYbPd \| BZCYYbPd \| BCFZY	17	600	500	2021，[18]
Ni-BZCYYbPd \| BZCYYbPd \| BCFZY	17	650	724	2021，[18]

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质子导体固体氧化物电化学装置中氨的利用与合成

Utilization and synthesis of ammonia in proton-conducting solid oxide electrochemical devices

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