固相真空转晶法制备α-AlH_3及其稳定化
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摘要
AlH_3由于其极高氢含量和潜在的应用价值而得到了国内外广泛的关注,然而,现有的α-AlH_3制备工艺复杂、成本高及长期稳定性能差等问题,而限制了其广泛研究与应用。采用固态真空转晶法制备晶型单一、高品质的α-AlH_3。而后采用小分子化合物对α-AlH_3进行包覆实验,并通过X射线衍射、电子顺磁共振仪、热失重差热分析、扫描电子显微镜和透射电子显微镜证实包覆成功。对包覆前后的α-AlH_3在室温和90%湿度条件下进行稳定性对比实验,结果表明,未包覆的α-AlH_3在10 d后即分解,而包覆后的α-AlH_3在16 d后仍保持很好的稳定性。该技术摒弃高毒甲苯溶液转晶行为,兼具成本低和连续化工业生产的优点,为α-AlH_3的规模化生产和长期贮存提供了新的思路。
Aluminum hydride is particularly attractive as a hydrogen storage material due to its high hydrogen volumetric capacities.However,issues of complicated preparation process,poor stability and high cost of α-AlH_3 restrict its further development and applications.Herein,high-quality α-AlH_3 has been prepared based on a solid-state crystal transformation method under vacuum condition.It has been successfully coated,which was confirmed by a combined analysis of XRD,EPR,TGA-DSC,SEM and TEM.In the condition of room temperature and 90% humidity,the pristine α-AlH_3 decomposed 10 days later,whereas the coated α-AlH_3 shows good stability even after 16 days storage.This technique excludes the traditional crystallization transformation behavior of AlH_3 in toxic toluene,providing a new idea way of large-scale production of the α-AlH_3 with long-term storage capability.
Aluminum hydride is particularly attractive as a hydrogen storage material due to its high hydrogen volumetric capacities.However,issues of complicated preparation process,poor stability and high cost of α-AlH_3 restrict its further development and applications.Herein,high-quality α-AlH_3 has been prepared based on a solid-state crystal transformation method under vacuum condition.It has been successfully coated,which was confirmed by a combined analysis of XRD,EPR,TGA-DSC,SEM and TEM.In the condition of room temperature and 90% humidity,the pristine α-AlH_3 decomposed 10 days later,whereas the coated α-AlH_3 shows good stability even after 16 days storage.This technique excludes the traditional crystallization transformation behavior of AlH_3 in toxic toluene,providing a new idea way of large-scale production of the α-AlH_3 with long-term storage capability.
引文
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[18]Jan Petter Maehlen,Volodymyr Yartys,Roman Denys,et al.Thermal decomposition of Al H3studied by in situ synchrotron X-ray diffraction and thermal desorption spectroscopy[J].Journal of Alloys and Compounds,2007,446-447:280-289.
[19]Kato T,Yuko Nakamori,Shinichi Orimo,et al.Thermal properties of Al H3-etherate and its desolvation reaction into Al H3[J].Journal of Alloys and Compounds,2007,446-447:276-279.
[20]邢校辉,夏宇,张晓勤,等.提高三氢化铝热稳定性的研究进展[J].化学推进剂与高分子材料,2018,16(2):21-25.XING Xiaohui,XIA Yu.,ZHANG Xiaoqin,et al.Research progress in improving thermal stability of aluminum trihydride[J].Chemical Propellants&Polymeric Materials,2018,16(2):21-25.
[21]Ismail M K Ismail,Tom W Hawkins.Kinetics of thermal decomposition of aluminium hydride:I-non-isothermal decomposition under vacuum and in inert atmosphere(argon)[J].Thermochimica,2005,439(1-2):32-43
[22]Mark A R,Jeffrey C B,Paul E P,et al.Preparation of Aluminum Hydride polymorphs particlularly stabilizedα-Al H3[P].US 6228338,2001.
[2]AnikóBorbás,Zoltán BSzabó,LászlóSzilágyi,et al.Dioxanetype(2-naphthyl)methylene acetals of glycosides and their hydrogenolytic transformation into 6-O-and 4-O-(2-naphthyl)methyl(NAP)ethers[J].Tetrahedron,2002,58(28):5723-5732.
[3]Andrew Bootle-Wilbraham,Steve Head,James Longstaff,et al.Alane-A chemoselective way to reduce phosphine oxides[J].Tetrahedron Letters,1999,40(28):5267-5270.
[4]Sara Griffin.,Lucy Heath,Paul Wyatt.Alane-A novel way to reduce phosphine oxides[J].Tetrahedron Letters,1998,39(24):4405-4406.
[5]LIU Haizhen,WANG Xinhu,LIU Yongan,et al.Hydrogen desorption properties of the MgH2-Al H3composites[J].The Journal of Physical Chemistry C,2013,118(1):37-45.
[6]LIU Haizhen,WANG Xinhua,DONG Zhaohui,et al.Dehydriding properties ofγ-Al H3[J].International Journal of Hydrogen Energy,2013,38(25):10851-10856.
[7]王建伟,夏宇,池俊杰,等.三氢化铝在推进剂中的应用研究进展[J].化学推进剂与高分子材料,2016,14(5):23-28.WANG Jianwei,XIA Yu,CHI Junjie,et al.Research progress in application of aluminum trihydride in propellants[J].Chemical Propellants&Polymeric Materials,2016,14(5):23-28
[8]陈晓丽,唐安江,韦德举,等.三氢化铝的合成工艺研究[J].广东化工,2014,41(16):92-93CHEN Xiaoli,TANG Anjiang,WEI Deju,et al.Research of synthesis process in AIH3[J].Guangdong Chemical Industry,2014,41(16):92-93.
[9]Young G,Piekiel N,Chowdhury S,et al.Ignition behavior of alpha-AIH(3)[J].Combustion Science and Technology,2010,182(9):1341-1359.
[10]Jason Graetz,James J Reilly,Volodymyr Yartys,et al.Aluminum hydride as a hydrogen and energy storage material:Past,present and future[J].Journal of Alloys and Compounds,2011,509(2):517-528.
[11]刘明星,何金选,曹一林.三氢化铝的合成及性能研究[J].固体火箭技术,2008,31(1):75-78.LIU Mingxing,HE Jinxuan,CAO Yilin.Study on synthesis and properties of almuminum hydride[J].Journal of Solid Rocket Technology,2008,31(1):75-78.
[12]罗永春,松科,阎汝煦,等.机械球磨固相化学反应制备Al H3及放氢性能[J].物理化学学报,2009,25(2):237-241.LUO Yongchun,SONG Ke,YAN Ruxu,et al.Synthesis of Al H3 by a ball-milling solid-phase chemical reaction and its hydrogen desorption properties[J].Acta Physico-Chimica Sinica,2009,25(2):237-241.
[13]Saitoh H,Machida A,Katayama Y,et al.Formation and decomposition of Al H(3)in the aluminum-hydrogen system[J].Applied Physics Letters,2008,93(15):151918-15918/3.
[14]McGrady G S.Hydrogenation of aluminum using a supercritical fluid medium[P].CA 2671963 2009.
[15]瓦约J J,刘P.合成铝烷的装置和方法[P].CN101410555A,2009.Wayue J J,Liu P.Apparatus and method for synthesis of alane[P].CN 101410555A,2009.
[16]张斌,毛根旺,王赫,等.AlH3的最新研究进展[J].金属功能材料,2009,16(6):71-75.ZHANG Bin,MAO Genwang,WANG He,et al.Recent progress in Al H3[J].Metallic Functional Materials,2009,16(6):71-75.
[17]Luigi De Luca,Luciano Galfetti,Febo Severini,et al.Physical and ballistic characterization of Al H3-based space propellants[J].Aerospace Science and Technology,2007,11(1):18-25.
[18]Jan Petter Maehlen,Volodymyr Yartys,Roman Denys,et al.Thermal decomposition of Al H3studied by in situ synchrotron X-ray diffraction and thermal desorption spectroscopy[J].Journal of Alloys and Compounds,2007,446-447:280-289.
[19]Kato T,Yuko Nakamori,Shinichi Orimo,et al.Thermal properties of Al H3-etherate and its desolvation reaction into Al H3[J].Journal of Alloys and Compounds,2007,446-447:276-279.
[20]邢校辉,夏宇,张晓勤,等.提高三氢化铝热稳定性的研究进展[J].化学推进剂与高分子材料,2018,16(2):21-25.XING Xiaohui,XIA Yu.,ZHANG Xiaoqin,et al.Research progress in improving thermal stability of aluminum trihydride[J].Chemical Propellants&Polymeric Materials,2018,16(2):21-25.
[21]Ismail M K Ismail,Tom W Hawkins.Kinetics of thermal decomposition of aluminium hydride:I-non-isothermal decomposition under vacuum and in inert atmosphere(argon)[J].Thermochimica,2005,439(1-2):32-43
[22]Mark A R,Jeffrey C B,Paul E P,et al.Preparation of Aluminum Hydride polymorphs particlularly stabilizedα-Al H3[P].US 6228338,2001.