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Development and characterization of functional composite materials for advanced energy conversion technologies
KTH, School of Industrial Engineering and Management (ITM), Energy Technology, Heat and Power Technology. (Fuel cell)
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The solid oxide fuel cell (SOFC) is a potential high efficient electrochemical device for vehicles, auxiliary power units and large-scale stationary power plants combined heat and power application. The main challenges of this technology for market acceptance are associated with cost and lifetime due to the high temperature (700-1000 oC) operation and complex cell structure, i.e. the conventional membrane electrode assemblies. Therefore, it has become a top R&D goal to develop SOFCs for lower temperatures, preferably below 600 oC. To address those above problems, within the framework of this thesis, two kinds of innovative approaches are adopted. One is developing functional composite materials with desirable electrical properties at the reduced temperature, which results of the research on ceria-based composite based low temperature ceramic fuel cell (LTCFC). The other one is discovering novel energy conversion technology - Single-component/ electrolyte-free fuel cell (EFFC), in which the electrolyte layer of conventional SOFC is physically removed while this device still exhibits the fuel cell function. Thus, the focus of this thesis is then put on the characterization of materials physical and electrochemical properties for those advanced energy conversion applications. The major scientific content and contribution to this challenging field are divided into four aspects except the Introduction, Experiments and Conclusions parts. They are:

  1. Continuous developments and optimizations of advanced electrolyte materials, ceria-carbonate composite, for LTCFC. An electrolysis study has been carried out on ceria-carbonate composite based LTCFC with cheap Ni-based electrodes. Both oxygen ion and proton conductance in electrolysis mode are observed. High current outputs have been achieved at the given electrolysis voltage below 600 oC. This study also provides alternative manner for high efficient hydrogen production.
  2.  Compatible and high active electrode development for ceria-carbonate composite electrolyte based LTCFC. A symmetrical fuel cell configuration is intentionally employed. The electro-catalytic activities of novel symmetrical transition metal oxide composite electrode toward hydrogen oxidation reaction and oxygen reduction reaction have been experimentally investigated. In addition, the origin of high activity of transition metal oxide composite electrode is studied, which is believed to relate to the hydration effect of the composite oxide.
  3. A novel all-nanocomposite fuel cell (ANFC) concept proposal and feasibility demonstration. The ANFC is successfully constructed by Ni/Fe-SDC anode, SDC-carbonate electrolyte and lithiated NiO/ZnO cathode at an extremely low in-situ sintering temperature, 600 oC. The ANFC manifests excellent fuel cell performance (over 550 mWcm-2 at 600 oC) and a good short-term operation as well as thermo-cycling stability. All results demonstrated its feasibility and potential for energy conversion.
  4. Fundamental study results on breakthrough research Single-Component/Electrolyte-Free Fuel Cell (EFFC) based on above nanocomposite materials (ion and semi-conductive composite) research activities. This is also the key innovation point of this thesis. Compared with classic three-layer fuel cells, EFFC with an electrolyte layer shows a much simpler but more efficient way for energy conversion. The physical-electrical properties of composite, the effects of cell configuration and parameters on cell performance, materials composition and cell fabrication process optimization, micro electrochemical reaction process and possible working principle were systematically investigated and discussed. Besides, the EFFC, joining solar cell and fuel cell working principle, is suggested to provide a research platform for integrating multi-energy-related device and technology application, such as fuel cell, electrolysis, solar cell and micro-reactor etc.

This thesis provides a new methodology for materials and system innovation for the fuel cell community, which is expected to accelerate the wide implementation of this high efficient and green fuel cell technology and open new horizons for other related research fields.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2013. , xv, 60 p.
Series
Trita-KRV, ISSN 1100-7990 ; 13:10
Keyword [en]
Low temperature ceramic fuel cell, Ceria-carbonate composite, Electrolysis, Transition metal oxide, Symmetrical fuel cells, All-nanocomposite fuel cell, Electrolyte-free fuel cell, Solar cell, ion conductor and semiconductor
National Category
Energy Engineering Nano Technology Composite Science and Engineering Ceramics
Research subject
SRA - Energy
Identifiers
URN: urn:nbn:se:kth:diva-134111ISBN: 978-91-7501-827-0 (print)OAI: oai:DiVA.org:kth-134111DiVA: diva2:664934
Public defence
2013-12-13, M3, Brinellvägen 64 Entreplan, KTH, Stockholm, Stockholm, 13:00 (English)
Opponent
Supervisors
Funder
Swedish Research Council, 621-2011-4983EU, FP7, Seventh Framework Programme, TriSOFC project (Contract No.303454)Vinnova
Note

QC 20131122

Available from: 2013-11-22 Created: 2013-11-16 Last updated: 2013-11-22Bibliographically approved
List of papers
1. Low temperature ceramic fuel cells using all nano composite materials
Open this publication in new window or tab >>Low temperature ceramic fuel cells using all nano composite materials
2012 (English)In: Nano Energy, ISSN 2211-2855, Vol. 1, no 4, 631-639 p.Article in journal (Refereed) Published
Abstract [en]

The shift to low operational temperature of solid oxide or ceramic fuel cells has induced many new concepts and novel technologies. In the present study, fuel cell assembled by all nano composite materials - NiO/Fe 2O 3-SDC anode, SDC-carbonate electrolyte and lithiated NiO/ZnO cathode - is investigated. A range of techniques, i.e., X-ray diffraction (XRD), Scanning electron microscopy (SEM) and electrochemical impedance spectroscopy as well as polarization measurements are employed to characterize the crystalline structures, morphologies and electrochemical properties of the synthesized nanocomposite materials and cells. Performance comparison is made between single cells with and without a pre-sintering process. Finally, single cell short term stability and thermo cycle behaviors are also examined. Combined the facile fabrication process, relative high performance and reasonable stability, the current all nanocomposite system may be a promising functional system for low temperature ceramic fuel cells.

Keyword
All nano composite, Ceramic fuel cells, In-situ sintering, Solid oxide fuel cells, Thermal cycle stability
National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-100456 (URN)10.1016/j.nanoen.2012.04.004 (DOI)000318050300015 ()2-s2.0-84863782340 (Scopus ID)
Funder
Swedish Research Council, 621-2011-4983Vinnova
Note

QC 20120808

Available from: 2012-08-08 Created: 2012-08-08 Last updated: 2013-11-22Bibliographically approved
2. Mixed ion and electron conductive composites for single component fuel cells: I. Effects of composition and pellet thickness
Open this publication in new window or tab >>Mixed ion and electron conductive composites for single component fuel cells: I. Effects of composition and pellet thickness
Show others...
2012 (English)In: Journal of Power Sources, ISSN 0378-7753, E-ISSN 1873-2755, Vol. 217, 164-169 p.Article in journal (Refereed) Published
Abstract [en]

Electrochemical performances of single component fuel cells (SCFCs) based on mixed ion and electron conductors have been studied as a function of composition and pellet thickness by polarization curves and electrochemical impedance spectroscopy. The electronic conductor of LNCZO shows conductivities of 21.7 and 5.3 S cm(-1) in H-2 and in air, respectively. SCFC using 40 wt. % of LNCZO and 60 wt. % of ion conductive SDC-Na2CO3 with a thickness of 1.10 mm shows the highest power density of 0.35 W cm(-2) at 550 degrees C. The performance is correlated to the mixed conduction properties (ionic and electronic, p and n-type) and the microstructure of the functional SCFC layer.

Keyword
Single component fuel cells, Composite electrolyte, p and n-type semiconductors, Composition, Thickness, Electrolyte free
National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-106123 (URN)10.1016/j.jpowsour.2012.05.045 (DOI)000308782200026 ()2-s2.0-84862744309 (Scopus ID)
Funder
Swedish Research Council, 621-2011-4983VINNOVA
Note

QC 20121203

Available from: 2012-12-03 Created: 2012-11-29 Last updated: 2017-12-07Bibliographically approved
3. Electrochemical study of lithiated transition metal oxide composite as symmetrical electrode for low temperature ceramic fuel cells
Open this publication in new window or tab >>Electrochemical study of lithiated transition metal oxide composite as symmetrical electrode for low temperature ceramic fuel cells
Show others...
2013 (English)In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 38, no 26, 11398-11405 p.Article in journal (Refereed) Published
Abstract [en]

In this work, Lithiated NiCuZnOx (LNCZO) composite is synthesized and evaluated as a potential symmetrical electrode for ceria-carbonate composite electrolyte based low temperature ceramic fuel cells. Its crystal structures, the hydrogen oxidation/oxygen reduction electrochemical activities and fuel cell performances are systematically examined on the symmetrical cell configuration. Nano crystallite particles in the form of composite are observed for these oxides. The LNCZO shows relatively high catalytic activities for hydrogen oxidation and oxygen reduction reaction according to the electrochemical impedance spectroscopy measurements. A remarkable low oxygen reduction activation energy of 42 kJ mol(-1) is obtained on the LNCZO/ceria-carbonate composite, demonstrating excellent electro-catalytic activity. Especially, the catalytic activity can be further improved in the presence of water in the cathode chamber. The results show that the lithiated transition metal oxide composite is a promising symmetrical electrode for ceria-carbonate electrolyte and composite approach might a probable solution to develop super-performance electrodes for reduced temperature ceramic fuel cells.

Keyword
Low temperature ceramic fuel cell, Ceria-carbonate, Symmetrical electrode, Transition metal oxide, Hydration effect, Electro-catalytic activity
National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-129624 (URN)10.1016/j.ijhydene.2013.06.050 (DOI)000324014600022 ()2-s2.0-84882449820 (Scopus ID)
Funder
EU, FP7, Seventh Framework Programme, 303454Swedish Research Council, 621-2011-4983Vinnova
Note

QC 20131003

Available from: 2013-10-03 Created: 2013-10-03 Last updated: 2017-12-06Bibliographically approved
4. Effective hydrogen production by high temperature electrolysis with ceria-carbonate composite
Open this publication in new window or tab >>Effective hydrogen production by high temperature electrolysis with ceria-carbonate composite
(English)Manuscript (preprint) (Other academic)
Abstract [en]

The high temperature electrolysis potentially offers an effective approach for large-scale and high purity hydrogen production. Besides, the research on the hybrid oxygen ion/proton conductive behavior is a hot field in the ceria-based composite field. In this present study, single cell assembled by SDC-carbonate electrolyte and Ni-based electrode was fabricated and operated in ceramic electrolysis cells (CECs) model. The effect of the relative humidity and temperature on the electrochemical performance was investigated by electrochemical impedance spectra (EIS) and polarization curves. Under an applied electrolysis voltage of 1.6 V, the maximum consumed current density is 1.2 Acm-2 in oxygen ionic conduction mode. The electrochemical performance in proton conduction mode is comparable to the oxygen ion conduction mode. The results here again demonstrate the hybrid ionic conduction of ceria-carbonate composite, and provide a promising materials system for high efficient hydrogen production.

Keyword
ceramic electrolysis cells, ceria-carbonate composite electrolyte, hybrid oxygen ion and proton conduction, hydrogen production
National Category
Materials Engineering Nano Technology Earth and Related Environmental Sciences
Research subject
SRA - Energy
Identifiers
urn:nbn:se:kth:diva-134110 (URN)
Projects
The China Scholarship Council (CSC), the Swedish Research Council (VR, Contract No. 621-2011-4983), the Swedish Agency for Innovation Systems (VINNOVA, Contract No. P36545–1), and the EC FP7 TriSOFC project (Contract No.303454)
Funder
EU, FP7, Seventh Framework Programme, 303454Swedish Research Council, 621-2011-4983
Note

QS 2013

Available from: 2013-11-16 Created: 2013-11-16 Last updated: 2013-11-22Bibliographically approved
5. Breakthrough fuel cell technology using ceria-based multi-functional nanocomposites
Open this publication in new window or tab >>Breakthrough fuel cell technology using ceria-based multi-functional nanocomposites
2013 (English)In: Applied Energy, ISSN 0306-2619, E-ISSN 1872-9118, Vol. 106, 163-175 p.Article in journal (Refereed) Published
Abstract [en]

Recent scientific and technological advancements have provided a wealth of new information about solid oxide-molten salt composite materials and multifunctional ceria-based nano-composites for advanced fuel cells (NANOCOFC). NANOCOFC is a new approach for designing and developing of multi-functionalities for nanocomposite materials, especially at 300-600 degrees C. NANOCOFC and low temperature advanced ceramic fuel cells (LTACFCs) are growing as a new promising area of research which can be explored in various ways. The ceria-based composite materials have been developed as competitive electrolyte candidates for low temperature ceramic fuel cells (LTCFCs). In the latest developments, multifunctional materials have been developed by integrating semi- and ion conductors, which have resulted in an emerging insight knowledge concerned with their R&D on single-component electrolyte-free fuel cells (EFFCs) - a breakthrough fuel cell technology. A homogenous component/layer of the semi- and ion conducting materials can realize fuel cell all functions to avoid using three components: anode, electrolyte and cathode, i.e. "three in one" highlighted by Nature Nanotechnology (2011). This report gives a short review and advance knowledge on worldwide activities on the ceria-based composites, emphasizing on the latest semi-ion conductive nanocomposites and applications for new applied energy technologies. It gives an overview to help the audience to get a comprehensive understanding on this new field.

Keyword
Ceramic fuel cells, NANOCOFC, Ceria-based composite, Electrolyte-free fuel cell, Single component, Nanocomposite
National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-122497 (URN)10.1016/j.apenergy.2013.01.014 (DOI)000317544400016 ()2-s2.0-84874400829 (Scopus ID)
Funder
Swedish Research Council, 621-2011-4983Vinnova
Note

QC 20130523

Available from: 2013-05-23 Created: 2013-05-23 Last updated: 2017-12-06Bibliographically approved
6. A new energy conversion technology joining electrochemical and physical principles
Open this publication in new window or tab >>A new energy conversion technology joining electrochemical and physical principles
Show others...
2012 (English)In: RSC Advances, ISSN 2046-2069, Vol. 2, no 12, 5066-5070 p.Article in journal (Refereed) Published
Abstract [en]

We report a new energy conversion technology joining electrochemical and physical principles. This technology can realize the fuel cell function but built on a different scientific principle. The device consists of a single component which is a homogenous mixture of ceria composite with semiconducting materials, e.g. LiNiCuZn-based oxides. The test devices with hydrogen and air operation delivered a power density of 760mWcm(-2) at 550 degrees C. The device has demonstrated a multi-fuel flexibility and direct alcohol and biogas operations have delivered 300-500 mW cm(-2) at the same temperature. Device physics reveal a key principle similar to solar cells realizing the function based on an effective separation of electronic and ionic conductions and phases within the single-component. The component material multi-functionalities: ion and semi-conductions and bi-catalysis to H-2 or alcohol (methanol and ethanol) and air (O-2) enable this device realized as a fuel cell.

Keyword
nanocomposite, single component, fuel cell
National Category
Energy Engineering
Research subject
SRA - Energy
Identifiers
urn:nbn:se:kth:diva-94862 (URN)10.1039/C2RA01234K (DOI)000304487000012 ()2-s2.0-84865266380 (Scopus ID)
Funder
StandUp
Note

QC 20120625

Available from: 2012-05-11 Created: 2012-05-11 Last updated: 2016-12-22Bibliographically approved
7. A single-component fuel cell reactor
Open this publication in new window or tab >>A single-component fuel cell reactor
Show others...
2011 (English)In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 36, no 14, 8536-8541 p.Article in journal (Refereed) Published
Abstract [en]

We report here a single-component reactor consisting of a mixed ionic and semi-conducting material exhibiting hydrogen-air (oxygen) fuel cell reactions. The new single-component device was compared to a conventional three-component (anode/electrolyte/cathode) fuel cell showing at least as good performance. A maximum power density of 300-600 mW cm(-2) was obtained with a LiNiZn-oxide and ceria-carbonate nanocomposite material mixture at 450-550 degrees C. Adding a redox catalyst element (Fe) resulted in an improvement reaching 700 mW cm(-2) at 550 degrees C.

Keyword
Single-component, Fuel cell, Nanocomposites, Ionic conductor, Low-temperature
National Category
Mechanical Engineering
Identifiers
urn:nbn:se:kth:diva-36881 (URN)10.1016/j.ijhydene.2011.04.082 (DOI)000292223100045 ()2-s2.0-79958136313 (Scopus ID)
Note
QC 20110720Available from: 2011-07-20 Created: 2011-07-18 Last updated: 2017-12-08Bibliographically approved

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