混合导体透氧膜反应器中水分解反应研究进展

doi:10.6023/A20120561

化学学报 ›› 2021, Vol. 79 ›› Issue (5): 588-599.DOI: 10.6023/A20120561 上一篇下一篇

综述

混合导体透氧膜反应器中水分解反应研究进展

蔡莉莉^a^,^b, 王静忆^a^,^b, 朱雪峰^a^,^b^,^c^,^*(), 杨维慎^a^,^b

a 中国科学院大连化学物理研究所催化基础国家重点实验室大连 116023
b 中国科学院大学北京 100049
c 中国科学院洁净能源创新研究院大连 116023

投稿日期:2020-12-09 发布日期:2021-01-25
通讯作者: 朱雪峰

作者简介:

蔡莉莉, 博士, 2019年6月于中国科学院大连化学物理研究所获理学博士学位, 目前在中国科学院大连化学物理研究所从事博士后工作, 主要研究方向为催化膜反应器.

朱雪峰, 研究员, 博士生导师. 2006年12月于中国科学院大连化学物理研究所获理学博士学位. 主要从事用于气体分离的致密陶瓷膜、膜催化及相关电催化方面的研究.

基金资助:
项目受国家自然科学基金(22008231); 项目受国家自然科学基金(21776267); 中国科学院洁净能源创新研究院(DNL180203); 辽宁省“兴辽英才”计划(XLYC1801004)

Recent Progress on Mixed Conducting Oxygen Transport Membrane Reactors for Water Splitting Reaction

Lili Cai^a^,^b, Jingyi Wang^a^,^b, Xuefeng Zhu^a^,^b^,^c^,^*(), Weishen Yang^a^,^b

a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
b University of Chinese Academy of Sciences, Beijing 100049, China
c Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Dalian 116023, China

Received:2020-12-09 Published:2021-01-25
Contact: Xuefeng Zhu
About author:
*E-mail: zhuxf@dicp.ac.cn
Supported by:
National Natural Science Foundation of China(22008231); National Natural Science Foundation of China(21776267); Dalian National Laboratory for Clean Energy (DNL)(DNL180203); LiaoNing Revitalization Talents Program(XLYC1801004)

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摘要/Abstract

混合导体透氧膜反应器可以将供氧反应、氧分离和耗氧反应耦合在一个单元, 实现反应和分离一体化, 简化化工过程. 水分解反应参与的混合导体透氧膜反应器能够实现氢气的制备和分离, 近年来受到越来越多的关注. 这篇文章综述了混合导体透氧膜反应器中水分解反应领域的研究进展, 总结了包括膜材料、催化剂、操作条件等对透氧膜反应器中水分解反应的影响, 分析了目前存在的问题, 同时展望了该领域在膜材料、膜结构和催化剂开发等方面的未来发展方向, 希望有助于促进膜反应器中水分解反应的研究.

关键词: 氢气, 透氧膜, 水分解, 膜材料, 催化剂

Catalytic membrane reactors based on mixed conducting oxygen transport membranes (OTMs) have the ability to integrate reaction and separation, and thus simplify the chemical process by coupling oxygen supplying reaction, oxygen separation and oxygen consumption reaction into a single unit. In recent years, more and more attentions have been paid to the mixed conducting OTM reactors for water splitting reaction owing to their applications for preparation and separation of hydrogen. In this article, we summarize the recent progress on mixed conducting OTM reactors for water splitting reaction, including the effects of membrane materials, catalysts and operation conditions on the water splitting involved membrane reactors. Meanwhile, the current existing problems in the above aspects are analyzed, and the future development of membrane materials, membrane structures and catalysts in this field is prospected. We wish this paper will be helpful for the development of the water splitting in membrane reactors.

Key words: hydrogen, oxygen transport membrane, water splitting, membrane material, catalyst

引用此文

蔡莉莉, 王静忆, 朱雪峰, 杨维慎. 混合导体透氧膜反应器中水分解反应研究进展[J]. 化学学报, 2021, 79(5): 588-599.

Lili Cai, Jingyi Wang, Xuefeng Zhu, Weishen Yang. Recent Progress on Mixed Conducting Oxygen Transport Membrane Reactors for Water Splitting Reaction[J]. Acta Chimica Sinica, 2021, 79(5): 588-599.

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图/表 11

图1. 不同氧移除反应的水分解催化膜反应器

Figure 1. The catalytic membrane reactors for water splitting with different oxygen removal reactions

图2. 双相膜示意图[75]. (a)氧离子导体-纯电子导体, (b)氧离子导体-混合导体, (c)混合导体1-混合导体2双相膜

Figure 2. Schematic diagrams of dual-phase membranes[75]. (a) IC-EC (ionic conductor-electronic conductor), (b) IC-MIEC1 (mixed ionic and electronic conductor), (c) MIEC1-MIEC2. Reprinted with permission from ref. [75], ? 2015 John Wiley and Sons

Membrane materials	Thickness/mm	T/℃	Atmospheres at both sides	Catalysts at water side	F_H2/ (mL∙cm^-2∙min^-1)	Ref.
La_0.3Sr_0.7FeO_3-_δ	3.00^a	860	17%H₂O(g);He		0.005	[76]
La_0.3Sr_0.7FeO_3-_δ	3.00^a	860	17%H₂O(g);CO		0.015	[76]
La_0.7Sr_0.3Cu_0.2Fe_0.8O_3-_δ (LSCF7328)	0.53	900	49%H₂O(g);80%H₂	Pt/SDC	1.9	[82]
LSCF7328	0.02	900	49%H₂O(g);80%H₂	—	≈9	[83]
LSCF7328	0.05	900	49%H₂O(g);80%H₂	Pt/SDC	11.4	[82]
BaFe_0.9Zr_0.1O_3-_δ	1.05	900	49%H₂O(g);99.5%CO	—	3.2	[84]
Ba_0.98Ce_0.05Fe_0.95O_3-_δ (BCF)	0.50	900	90%H₂O(g);80%H₂	Ru/SDC (m_Ru/m_catalyst=1%)	10.2	[49]
BaZr_xCo_yFe_zO_3-_δ (BZCF)	0.17^a	900	75%H₂O(g);4%CH₄	—	2.2	[28]
La_0.9Ca_0.1FeO_3-_δ (LCF-91)	0.90	990	50%H₂O(g);5%CH₄	—	0.5	[31]
SrFeCo_0.5O_x(SFC2)	1.04	900	49%H₂O(g);80%H₂	—	4.0	[78]
SrFeCo_0.5O_x (SFC2)	0.02	900	69%H₂O(g);80%H₂	—	17.4	[78]
SrCo_0.4Fe_0.5Zr_0.1O_3-_δ(SCFZ)	—	900	69%H₂O(g);6%EtOH	—	3.4	[108]

表1. 单相透氧膜材料的水分解性能

Table 1. The water splitting performance of single-phase oxygen transport membranes

图3. BCF膜材料在900 ℃的水分解稳定性[49]. 膜两侧条件分别是90% H2O和50% H2

Figure 3. Water splitting stability of BCF membrane at 900 ℃ [49]. 90% H2O and 50% H2 fed to the two sides of BCF membrane, respectively. Reprinted with permission from ref.[49], ? 2016 John Wiley and Sons

Membrane materials	Ratios of two phases	Thickness/ mm	Atmospheres at both sides	Catalysts at water side	F_H2/ (mL∙cm^-2∙min^-1)	Ref.
(ZrO₂)_0.8(TiO₂)_0.1(Y₂O₃)_0.1 (TiO₂-YSZ)	—	2^a	17%H₂O(g);H₂/CO₂ (P_O2 10^-7Pa)	—	≈0.5^b	[47]
Cu-GDC	2/3 (volume ratio)	0.46	49%H₂O(g);80%H₂	—	2.3	[48]
Ni-GDC	2/3 (volume ratio)	0.13	49%H₂O(g);80%H₂	—	3.9	[85]
Ni-GDC	2/3 (volume ratio)	0.13	49%H₂O(g);80%H₂	Ni-GDC (V_Ni/V_GDC=40%)	6	[85]
Ni-GDC	2/3 (volume ratio)	0.46	49%H₂O(g);80%H₂	—	2.4	[85]
Ni-GDC	2/3 (volume ratio)	0.46	49%H₂ (g);80%H₂	Ni-GDC (V_Ni/V_GDC=40%)	3.0	[85]
Gd_0.2Ce_0.8O_1.9-_δ- Gd_0.08Sr_0.88Ti_0.95Al_0.05O_3±_δ (GDC-GSTA)	3/2 (volume ratio)	1.1	25%H₂O(g);50%H₂	—	2.0	[86]
GDC-GSTA	3/2 (volume ratio)	1.1	25%H₂O(g);50%H₂	NiO-GDC (V_NiO/V_GDC=50%)	2.6	[86]
GDC-GSTA	3/2 (volume ratio)	1.1	25%H₂O(g);100%H₂	NiO-GDC (V_NiO/V_GDC=50%)	3.1	[86]
GDC-GSTA	3/2 (volume ratio)	0.025	25%H₂O(g);-	—	≈10	[87]
Ce_0.85Sm_0.15O_1.925- Sm_0.6Sr_0.4Al_0.3Fe_0.7O_3-_δ (SDC-SSAF)	3/1 (mass ratio)	0.04	90%H₂O(g);80%H₂	Ru/SDC (m_Ru/m_catalyst=1%)	15.5	[27]
SDC-SSAF	3/1 (mass ratio)	0.40	90%H₂O(g);80%H₂	Ru/SDC (m_Ru/m_catalyst=1%)	5.0	[98]
Ce_0.85Sm_0.15O_1.925- Sm_0.6Sr_0.4Cr_0.3Fe_0.7O_3-_δ (SDC-SSCF)	3/1 (mass ratio)	0.70	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	5.3	[51]
SDC-SSCF	3/1 (mass ratio)	0.50	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.5	[51]
SDC-SSCF	3/1 (mass ratio)	0.36	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.9	[51]
SDC-SSCF	3/1 (mass ratio)	0.36	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	4.6	[51]
SDC-SSCF	3/1 (mass ratio)	0.36	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.2	[51]
Ce_0.85Sm_0.15O_1.925- Sr₂Fe_1.5Mo_0.5O_6-_δ (SDC-SFM)	7/3 (mass ratio)	0.5	90% H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.3	[50]
SDC-SSCF	3/1 (mass ratio)	0.04	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=2%)	15.8	[52]
SDC-SSCF	3/1 (mass ratio)	0.04	90%H₂O(g);80%H₂	(Ni+Ru)/SDC (m_Ni/m_SDC=1%, m_Ru/m_SDC=1%)	19.3	[52]
Ce_0.9Pr_0.1O_2-_δ- Pr_0.1Sr_0.9Mg_0.1Ti_0.9O_3-_δ (CPO-PSMTi)	3/2 (molar ratio)	0.70	88%H₂O(g);40%H₂	—	0.41	[32]

Membrane materials	Ratios of two phases	Thickness/ mm	Atmospheres at both sides	Catalysts at water side	F_H2/ (mL∙cm^-2∙min^-1)	Ref.
(ZrO₂)_0.8(TiO₂)_0.1(Y₂O₃)_0.1 (TiO₂-YSZ)	—	2^a	17%H₂O(g);H₂/CO₂ (P_O2 10^-7Pa)	—	≈0.5^b	[47]
Cu-GDC	2/3 (volume ratio)	0.46	49%H₂O(g);80%H₂	—	2.3	[48]
Ni-GDC	2/3 (volume ratio)	0.13	49%H₂O(g);80%H₂	—	3.9	[85]
Ni-GDC	2/3 (volume ratio)	0.13	49%H₂O(g);80%H₂	Ni-GDC (V_Ni/V_GDC=40%)	6	[85]
Ni-GDC	2/3 (volume ratio)	0.46	49%H₂O(g);80%H₂	—	2.4	[85]
Ni-GDC	2/3 (volume ratio)	0.46	49%H₂ (g);80%H₂	Ni-GDC (V_Ni/V_GDC=40%)	3.0	[85]
Gd_0.2Ce_0.8O_1.9-_δ- Gd_0.08Sr_0.88Ti_0.95Al_0.05O_3±_δ (GDC-GSTA)	3/2 (volume ratio)	1.1	25%H₂O(g);50%H₂	—	2.0	[86]
GDC-GSTA	3/2 (volume ratio)	1.1	25%H₂O(g);50%H₂	NiO-GDC (V_NiO/V_GDC=50%)	2.6	[86]
GDC-GSTA	3/2 (volume ratio)	1.1	25%H₂O(g);100%H₂	NiO-GDC (V_NiO/V_GDC=50%)	3.1	[86]
GDC-GSTA	3/2 (volume ratio)	0.025	25%H₂O(g);-	—	≈10	[87]
Ce_0.85Sm_0.15O_1.925- Sm_0.6Sr_0.4Al_0.3Fe_0.7O_3-_δ (SDC-SSAF)	3/1 (mass ratio)	0.04	90%H₂O(g);80%H₂	Ru/SDC (m_Ru/m_catalyst=1%)	15.5	[27]
SDC-SSAF	3/1 (mass ratio)	0.40	90%H₂O(g);80%H₂	Ru/SDC (m_Ru/m_catalyst=1%)	5.0	[98]
Ce_0.85Sm_0.15O_1.925- Sm_0.6Sr_0.4Cr_0.3Fe_0.7O_3-_δ (SDC-SSCF)	3/1 (mass ratio)	0.70	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	5.3	[51]
SDC-SSCF	3/1 (mass ratio)	0.50	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.5	[51]
SDC-SSCF	3/1 (mass ratio)	0.36	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.9	[51]
SDC-SSCF	3/1 (mass ratio)	0.36	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	4.6	[51]
SDC-SSCF	3/1 (mass ratio)	0.36	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.2	[51]
Ce_0.85Sm_0.15O_1.925- Sr₂Fe_1.5Mo_0.5O_6-_δ (SDC-SFM)	7/3 (mass ratio)	0.5	90% H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=10%)	6.3	[50]
SDC-SSCF	3/1 (mass ratio)	0.04	90%H₂O(g);80%H₂	Ni/SDC (m_Ni/m_SDC=2%)	15.8	[52]
SDC-SSCF	3/1 (mass ratio)	0.04	90%H₂O(g);80%H₂	(Ni+Ru)/SDC (m_Ni/m_SDC=1%, m_Ru/m_SDC=1%)	19.3	[52]
Ce_0.9Pr_0.1O_2-_δ- Pr_0.1Sr_0.9Mg_0.1Ti_0.9O_3-_δ (CPO-PSMTi)	3/2 (molar ratio)	0.70	88%H₂O(g);40%H₂	—	0.41	[32]

表2. 双相透氧膜材料在900 ℃的水分解性能

Table 2. The water splitting performance of dual-phase oxygen transport membranes at 900 ℃

表2. 双相透氧膜材料在900 ℃的水分解性能

Table 2. The water splitting performance of dual-phase oxygen transport membranes at 900 ℃

图4. POM膜反应器中膜两侧的氧化学势和电导率变化示意图[97]. 其中L代表膜的厚度, σ e代表电子电导率

Figure 4. Schematic illustration of oxygen chemical potential drop and conductivity change across an OTM membrane in the POM reactor, where L represents the thickness of membrane, and σ e is the electronic conductivity[97]. Reprinted with permission from ref. [97], ? 2016 Elsevier

图5. SDC-SSCF双相膜在900 ℃不同气氛下的水分解稳定性[48]. 水侧条件为90% H2O, 使用的不同还原性气体标注在图中

Figure 5. The stability of SDC-SSCF dual-phase membrane under different atomospheres at 900 ℃[48]. The condition at water side is 90% H2O, and the different reducing gases used are marked in the figure. Reprinted with permission from ref. [48], ? 2020 John Wiley and Sons

图6. 总阻力(rtot)和体相阻力(rb)对温度和膜厚度的关系图[51]

Figure 6. Dependence of the total resistance (rtot) and bulk resistance (rb) on temperature and membrane thickness (L)[51]. Reprinted with permission from ref. [51], ? 2019 Elsevier

图7. 激光刻槽技术制备多孔层具有直通槽的非对称膜[107]

Figure 7. Asymmetric membranes with straight grooves in the porous support layer were prepared by laser grooving technique[107]

图8. Ru/SDC 样品的电子显微图像[52]. (a, d)空气气氛下制备的 Ru/SDC, (b, c和e)还原后的Ru/SDC, (a和c)扫描透射电镜(STEM)图, (b)高分辨扫描电镜(HRSEM)图, (d和e)能量色散X射线(EDX)元素成像图

Figure 8. Electron microscopy images of the Ru/SDC samples[52]. (a, d) Ru/SDC prepared in air, (b, c, e) reduced Ru/SDC, (a, c) scanning transmission electron microscopy (STEM) images, (b) high-resolution scanning electron microscopy (HRSEM) image, and (d, e) energy dispersive X-ray (EDX) element mapping images. Reprinted with permission from ref. [52], ? 2019 Elsevier

图9. 两种水参与的透氧膜反应器. (a)通过分解水和空气同时得到氨合成气(VH2/VN2=3)[36], (b)通过分解水和二氧化碳得到合成气[40]

Figure 9. Two types of water-involved oxygen transport membrane reactors. (a) Synthesis gases production for ammonia (VH2/VN2=3)[36], (b) syngas production by splitting of H2O and CO2 [40]. (a) Reprinted with permission from ref. [36], ? 2016 John Wiley and Sons, (b) Reprinted with permission from ref. [ 40], ? 2017 American Chemical Society

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混合导体透氧膜反应器中水分解反应研究进展

Recent Progress on Mixed Conducting Oxygen Transport Membrane Reactors for Water Splitting Reaction

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