化学链合成氨中载氮体的设计与应用研究进展

巩宙婷; 张谭; 李娜; 杨言言; 刘守军; 郑劼; 余钟亮; 杨颂

doi:10.1016/S1872-5813(23)60397-4

化学链合成氨中载氮体的设计与应用研究进展

doi: 10.1016/S1872-5813(23)60397-4

巩宙婷^{1, 2, 3, 4, #,},
张谭^{1, 3, 4, #,},
李娜^{1, 2, 3, 4,},
杨言言^{2, 4,},
刘守军^{1, 3, 4,},
郑劼^2,,
余钟亮^{2, 4},
杨颂^{1, 3, 4, ,}

1.
太原理工大学化学工程与技术学院, 山西太原 030024
2.
上饶师范学院化学与环境科学学院, 江西上饶 334000
3.
太原理工大学省部共建煤基能源清洁高效利用国家重点实验室, 山西太原 030024
4.
山西省民用洁净燃料工程研究中心, 山西太原 030024

基金项目: 国家自然科学基金（22169017）资助

详细信息

通讯作者:
Tel: 13233620827, E-mail: yangsong@tyut.edu.cn

^# These authors contributed to the work equally
中图分类号: O6-1
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- 被引次数: 0
出版历程
- 收稿日期: 2023-09-02
- 修回日期: 2023-10-09
- 录用日期: 2023-10-09
- 网络出版日期: 2023-11-10
- 刊出日期: 2024-04-03

Progress in design and application research of nitrogen carrier in chemical looping ammonia synthesis technology

GONG Zhouting^{1, 2, 3, 4, #
,},
ZHANG Tan^{1, 3, 4, #
,},
LI Na^{1, 2, 3, 4
,},
YANG Yanyan^{2, 4
,},
LIU Shoujun^{1, 3, 4
,},
ZHENG Jie^2
,,
YU Zhongliang^{2, 4},
YANG Song^{1, 3, 4
, ,}

1.
College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China
2.
College of Chemistry and Environmental Sciences, Shangrao Normal University, Shangrao 334000, China
3.
State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan University of Technology, Taiyuan 030024, China
4.
Shanxi Engineering Center of Civil Clean Fuel, Taiyuan 030024, China

Funds: The project was supported by National Natural Science Foundation of China (22169017).

摘要

摘要: 氨不仅是氮肥生产的主要原料，也是可再生能源储存与转化过程中的能源载体之一。因此，开发温和条件下的合成氨技术是近年来重要的研究课题。化学链合成氨技术通过载氮体的传递作用，将合成氨反应解耦为固氮与释氨等多步反应，具有操作简便、反应温和、能耗低等优点。载氮体作为化学链合成氨的关键，起到传递能量及氮物种的作用，目前，载氮体固氮效率低，极大地限制了化学链合成氨技术的发展。基于此，本工作对化学链合成氨中载氮体的设计与应用研究进行综述。首先，对载氮体的设计理论进行了归纳与总结；其次，介绍了载氮体的研究现状，重点对如何提高载氮体的产氨速率以及如何提升晶格氮利用率等问题进行了综述；最后，对化学链合成氨技术所面临的机遇与挑战进行了研究，为今后载氮体的设计与开发提供了参考依据。
- 合成氨 /
- 化学链 /
- 催化剂 /
- 反应动力学 /
- 过渡金属 /
- 金属氮化物
Abstract: Ammonia is not only the main raw material of nitrogen fertilizer production, but also one of the energy carriers for the storage and conversion process of renewable energy. Therefore, the development of a mild ammonia synthesis technology has become an important research topic in recent years. The chemical looping ammonia synthesis technology decouples the ammonia synthesis reaction into several steps, including the nitrogen fixation and the ammonia release, which has the advantages of easy operation, mild reaction, and low energy consumption. As the key to the chemical looping ammonia synthesis, nitrogen carriers play the role of transferring energy and nitrogen species. However, the current low nitrogen fixation efficiency of nitrogen carriers severely limits the development of the chemical looping ammonia synthesis technology. Therefore, this article reviews the research on the design, preparation and application of nitrogen carriers for the chemical looping ammonia synthesis. Firstly, the design theory of nitrogen carrier is summarized; secondly, the current research status of nitrogen carrier is introduced, with a focus on how to improve the ammonia production rate of nitrogen carrier and the utilization rate of lattice nitrogen; finally, the opportunities and challenges of chemical looping ammonia synthesis technology are discussed, which provide a reference for the design and development of nitrogen carrier in the future.
- ammonia synthesis /
- chemical looping /
- catalyst /
- reaction kinetics /
- transition metals /
- metal nitride
注释:

1) ^# These authors contributed to the work equally

HTML全文

FIG. 3075. FIG. 3075.

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图 1 化学链合成氨原理示意图

Figure 1 Schematic diagram of chemical looping ammonia synthesis

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图 2 理想载氮体特性

Figure 2 Ideal nitrogen carrier characteristics

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图 3 铬基载氮体涉及的化学链合成氨循环示意图

Figure 3 Schematic diagram of chromium-based nitrogen carriers mediated CLAS cycle

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图 4 热催化合成氨与化学链合成氨产氨速率对比

Figure 4 Comparison of ammonia production rates between thermal catalytic synthesis of ammonia and CLAS

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图 5 Ru/ZrH₂化学链合成氨过程示意图

Figure 5 Ru/ZrH₂-Mediated CLAS process

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表 1 Ni催化剂对BaH₂固氮加氢的影响

Table 1 Effect of Ni catalyst on nitrogen fixation and hydrogenation of BaH₂

	N₂ fixation rate/ (μmol·g⁻¹·h⁻¹)	NH₃ production rate/ (μmol·g⁻¹·h⁻¹)
BaH₂	≈3000	−
50%Ni-BaH₂	≈5800	−
BaNH	−	≈9000
Nitridized 50%Ni-BaH₂	−	≈29000
−: Data not found in the literature.

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表 2 常见载氮体涉及的化学链合成氨过程

Table 2 Common nitride-mediated CLAS

No.	Nitrogen carrier pairs	Nitrogen carrier type	Hydrogen source	Reaction conditions	Reaction rate	Ref.
1	Li-Li₃N-LiOH	ionic nitride	H₂O	electrolysis: 450 ℃ nitrogen fixation: 22−100 ℃ hydrolysis: 22−100 ℃, 0.5 h/12 h	−	[56]
2	Mg-Mg₃N₂-MgO	ionic nitride	H₂O	light source heating reduction & hydrolysis: pressure<100 mtorr nitrogen fixation: 0.1 MPa	1.67 μmol/(g·h)	[60]
3	Cr₂N-Cr₂O₃	transition metal nitride	H₂O	nitrogen fixation: 983±40 ℃, 360 min hydrolysis: 500−1600 ℃, 60 min reduction: 800−1600 ℃, 30 min	108 μmol/(g·h)	[64]
4	M_aN_b-M_aN_b-_d (Mn)	transition metal nitride	H₂	nitrogen fixation: 700 ℃, 120 min 750 ℃, 240 min hydrogenation: 300−1000 ℃, 60 min	55.3 μmol/(g·h)	[51]
5	Mo-Mo₂N	transition metal nitride	H₂	nitrogen fixation: 600 ℃, 60 min hydrogenation: 400−600 ℃, 60 min	4576 μmol/(g·h)	[102]
6	MH₂-M_aN_b (Ca, Sr)	ionic nitride	H₂	nitrogen fixation: 200−1000 ℃, 240 min/420 min hydrogenation: 300−1000 ℃, 60 min	Ca₃N₂: 98 μmol/(g·h) Sr₂N: 81 μmol/(g·h)	[51]
7	BaH₂-BaNH Ni	metal Hydride	H₂	nitrogen fixation: 100−500 ℃, 300 min hydrogenation: 100−500 ℃	28800 μmol/(g·h)	[94]
−: Data not found in the literature.

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