基于BaO-CaO-Al_2O_3-B_2O_3-SiO_2体系探究BaCO_3的残余量及其对玻璃热性能的影响
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摘要
采用中温固体氧化物燃料电池(IT-SOFC,Intermediate Temperature-Solid Oxide of Fuel Cell)封接玻璃BaO-CaO-Al_2O_3-B_2O_3-SiO_2体系探究三种熔制工艺(1300℃保温1 h;1400℃保温1 h;1400℃保温3 h)对玻璃原料BaCO_3的残余量及玻璃热性能的影响。利用差热-热重分析(DTA-TG)对配方粉体和不同熔制工艺获得玻璃的热性能进行表征,根据DTA-TG数据进行了计算并验证BaCO_3的残余量。通过傅里叶红外光谱、XRD和热膨胀系数测定仪对样品进行了表征。结果表明:采取1300℃保温1 h制备的玻璃中仍有59wt%BaCO_3未分解,并且析出的单斜Ba Al2Si2O8晶体降低了玻璃的膨胀系数;1400℃保温3 h制备的玻璃由于Al_2O_3含量增加,玻璃软化点(Ts)明显升高(>800℃),1400℃保温1 h制备的玻璃在室温到玻璃温度转变点范围内的膨胀系数为10.3×10–6 K–1。因此对于本实验玻璃配方,1400℃保温1 h是最为合适的熔制工艺,可以用于SOFC电堆的封接。
A BaO-CaO-Al_2O_3-B_2O_3-SiO_2 system for the sealing glass in intermediate temperature solid oxide fuel cell(IT-SOFC) was prepared. The effects of three fusion processes(heating at 1300℃ for 1 h, heating at 1400℃for 1 h, and heating at 1400℃ for 3 h) were explored with focus on the residual amount of BaCO_3 and the thermal properties of the glasses by thermal-thermogravimetric analysis(DTA-TG). Samples were characterized by Fourier transform infrared spectroscopy(FT-IR), X-ray diffractometer(XRD) and thermal expansion coefficient meter. The results showed that 59 wt% BaCO_3 retained undecomposed in the glass prepared via heat treatment at 1300℃ for 1 h and its expansion coefficient decreased due to devitrification of monoclinic Ba Al2 Si2 O8. Softening temperature(>800℃) of the glass produced via heating at 1400℃ for 3 h increased obviously owing to the increment of Al_2O_3 amount. The expansion coefficient of the glass produced via heat treatment at 1400℃ for 1 h was 10.3×10–6 K–1 from room temperature to the glass transition temperature, indiating the process of heat treatment at 1400℃ for 1 h the optimal condition in three candidates for the specific formula, which was found to be eligible for SOFC sealing.
A BaO-CaO-Al_2O_3-B_2O_3-SiO_2 system for the sealing glass in intermediate temperature solid oxide fuel cell(IT-SOFC) was prepared. The effects of three fusion processes(heating at 1300℃ for 1 h, heating at 1400℃for 1 h, and heating at 1400℃ for 3 h) were explored with focus on the residual amount of BaCO_3 and the thermal properties of the glasses by thermal-thermogravimetric analysis(DTA-TG). Samples were characterized by Fourier transform infrared spectroscopy(FT-IR), X-ray diffractometer(XRD) and thermal expansion coefficient meter. The results showed that 59 wt% BaCO_3 retained undecomposed in the glass prepared via heat treatment at 1300℃ for 1 h and its expansion coefficient decreased due to devitrification of monoclinic Ba Al2 Si2 O8. Softening temperature(>800℃) of the glass produced via heating at 1400℃ for 3 h increased obviously owing to the increment of Al_2O_3 amount. The expansion coefficient of the glass produced via heat treatment at 1400℃ for 1 h was 10.3×10–6 K–1 from room temperature to the glass transition temperature, indiating the process of heat treatment at 1400℃ for 1 h the optimal condition in three candidates for the specific formula, which was found to be eligible for SOFC sealing.
引文
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[15]QIAN DA XING,ZHOU NAI,SUN DAO BING,et al.Some technological factors affect the volatilization of boron in glass melting.Journal of Building Materials,1998,1(2):197–200.
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[18]VISHAL KUMAR,RUPALI,PANDEY O P.Thermal and crystallization kinetics of yttrium and lanthanum calcium silicate glass sealants for solid oxide fuel cells.International Journal of Hydrogen Energy,2011,36(22):14971–14976.
[19]曹春娥,顾幸勇,王艳香,等.无机材料测试技术.南昌:江西高校出版社,2011:311–323.
[20]FU YEN PEI,CHANG CHIN CHUNG,LIN CHENG HSIUNG.Solid-state synthesis of ceramics in the Ba O–Sr O–Al2O3–Si O2system.Ceramics International,2004,30(1):41–45.
[2]MAHAPATRA M K,LU K.Glass-based seals for solid oxide fuel and electrolyzer cells–a review.Materials Science and Engineering R,2010,67(5):65–85.
[3]WANG XIU LING,OU DING RONG,ZHAO ZHE.et al.Stability of Sr O–La2O3–Al2O3–Si O2 glass sealants in high-temperature air and steam.Ceramics International,2016,42(6):7514–7523.
[4]ZHANG WEI HAO,YAN DONG,PU JIAN,et al.Development of Al2O3/glass-based multi-layer composite seals for planar intermediate-temperature solid oxide fuel cells.International Journal of Hydrogen Energy,2013,38(35):15371–15378.
[5]MAVIAEL J SILVA DA,JOSE F BARTOLOME,ANTONIO H DE AZA,et al.Glass ceramic sealants belonging to BAS(Ba O–Al2O3–Si O2)ternary system modified with B2O3 addition:a different approach to access.Journal of the European Ceramic Society,2016,36(3):631–644.
[6]LIN S E,CHENG Y R,WEI W C J.Ba O–B2O3–Si O2–Al2O3 sealing glass for intermediate temperature solid oxide fuel cell.Journal of Non-Crystalline Solids,2012,358(2):174–181.
[7]SMEACETTO F,SALVO M,FERRARIS M,et al.Characterization and performance of glass–ceramic sealant to join metallic interconnects to YSZ and anode-supported-electrolyte in planar SOFCs.Journal of European Ceramic Society,2008,28(13):2521–2527.
[8]MAHAPATRA M K,LU K,REYNONDS W T JR.Thermophysical properties and devitrification of Sr O-La2O3-Al2O3-B2O3-Si O2based glass sealant for solid oxide fuel/electrolyzer cells.Journal of Power Sources,2008,179(1):106–112.
[9]XIAO ZHUO HAO,LU AN XIAN.Relationship between thermal expansion coefficient and composition of R2O-MO-Al2O3-Si O2system glass.Journal of Central South University(Natural Science Edition),2005,36(4):566–570.
[10]LUO LING HONG,YU HUI,HUANG ZU ZHI.Research progress of the sealing glass for intermediate temperature solid oxide fuel cell.Journal of Inorganic Materials,2015,30(2):113–121.
[11]ARVANITIDIS I,SICHE D,SEETHARAMAN S.A study of the thermal decomposition of Ba CO3.Metallurgical&Materials Transactions B,1996,27(3):409–416.
[12]HANCOCK J D,SHARP J H.Method of comparing solid-state kinetic data and its application to the decomposition of kaolinite,brucite,and Ba CO3.Journal of the American Ceramic Society,2010,55(2):74–77.
[13]MAITR S,BANDYOPADHYAY N,PAL J.Application of non-Arrhenius method for analyzing the decomposition kinetics of Sr CO3 and Ba CO3.Journal of the American Ceramic Society,2008,91(1):337–341.
[14]LUO LINGHONG,LIN YOU CHEN,HUANG ZU ZHI.Application of Ba O–Ca O–Al2O3–B2O3–Si O2 glass–ceramic seals in large size planar IT-SOFC.Ceramics International,2015,41(8):9239–9243.
[15]QIAN DA XING,ZHOU NAI,SUN DAO BING,et al.Some technological factors affect the volatilization of boron in glass melting.Journal of Building Materials,1998,1(2):197–200.
[16]HANS VAN LIMPT,RUUD BEERKENS.Modelling the evaporation of boron species.Part 1.Alkali-free borosilicate glass melts.Glass Technology:European.Journal of Glass Science Technology Part A,2011,52(3):77–87.
[17]PENG LIN,ZHAO GAO LING,YING HAO,et al.Infrared spectra of alkali-free aluminoborosilicate glass structure.Journal of the Chinese Ceramic Society,2007,35(7):856–860.
[18]VISHAL KUMAR,RUPALI,PANDEY O P.Thermal and crystallization kinetics of yttrium and lanthanum calcium silicate glass sealants for solid oxide fuel cells.International Journal of Hydrogen Energy,2011,36(22):14971–14976.
[19]曹春娥,顾幸勇,王艳香,等.无机材料测试技术.南昌:江西高校出版社,2011:311–323.
[20]FU YEN PEI,CHANG CHIN CHUNG,LIN CHENG HSIUNG.Solid-state synthesis of ceramics in the Ba O–Sr O–Al2O3–Si O2system.Ceramics International,2004,30(1):41–45.