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Effect of Li3N additive on the hydrogen storage properties of Li-Mg-N-H system

Published online by Cambridge University Press:  31 January 2011

Ping Wang*
Affiliation:
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, People’s Republic of China
Hui-Ming Cheng
Affiliation:
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, People’s Republic of China
*
a) Address all correspondence to this author. e-mail: pingwang@imr.ac.cn
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Abstract

The effect of Li3N additive on the Li-Mg-N-H system was examined with respect to the reversible dehydrogenation performance. Screening study with varying Li3N additions (5, 10, 20, and 30 mol%) demonstrates that all are effective for improving the hydrogen desorption capacity. Optimally, incorporation of 10 mol% Li3N improves the practical capacity from 3.9 wt% to approximately 4.7 wt% hydrogen at 200 °C, which drives the dehydrogenation reaction toward completion. Moreover, the capacity enhancement persists well over 10 de-/rehydrogenation cycles. Systematic x-ray diffraction examinations indicate that Li3N additive transforms into LiNH2 and LiH phases and remains during hydrogen cycling. Combined structure/property investigations suggest that the LiNH2 “seeding” should be responsible for the capacity enhancement, which reduces the kinetic barrier associated with the nucleation of intermediate LiNH2. In addition, the concurrent incorporation of LiH is effective for mitigating the ammonia release.

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Articles
Copyright
Copyright © Materials Research Society 2009

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References

1Schlapbach, L. and Züttel, A.: Hydrogen-storage materials for mobile applications. Nature 414, 353 (2001).Google Scholar
2Buschow, K.H.J.: Handbook on the Physics and Chemistry of Rare Earths, Vol. 6 (North-Holland, New York, 1984), Ch. 47.Google Scholar
3Schwarz, R.B.: Hydrogen storage in magnesium-based alloys. MRS Bull. 24, 40 (1999).Google Scholar
4Grochala, W. and Edwards, P.P.: Thermal decomposition of the non-interstitial hydrides for the storage and production of hydrogen. Chem. Rev. 104, 1283 (2004).Google Scholar
5Schüth, F., Bogdanović, B., and Felderhoff, M.: Light metal hydrides and complex hydrides for hydrogen storage. Chem. Commun. 2249 (2004).Google Scholar
6Orimo, S., Nakamori, Y., Eliseo, J.R., Züttel, A., and Jensen, C.M.: Complex hydrides for hydrogen storage. Chem. Rev. 107, 4111 (2007).Google Scholar
7Chen, P., Xiong, Z.T., Luo, J.Z., Lin, J.Y., and Tan, K.L.: Interaction of hydrogen with metal nitrides and imides. Nature 420, 302 (2002).Google Scholar
8Xiong, Z.T., Wu, G.T., Hu, J.J., and Chen, P.: Ternary imides for hydrogen storage. Adv. Mater. 16, 1522 (2004).Google Scholar
9Luo, W.F.: (LiNH2-MgH2): A viable hydrogen storage system. J. Alloys Compd. 381, 284 (2004).Google Scholar
10Leng, H.Y., Ichikawa, T., Hino, S., Hanada, N., Isobe, S., and Fujii, H.: New metal-N-H system composed of Mg(NH2)2 and LiH for hydrogen storage. J. Phys. Chem. B 108, 8763 (2004).Google Scholar
11Nakamori, Y., Kitahara, G., Miwa, K., Towata, S., and Orimo, S.: Reversible hydrogen-storage functions for mixtures of Li3N and Mg3N2. Appl. Phys. A 80, 1 (2005).Google Scholar
12Rijssenbeek, J., Gao, Y., Hanson, J., Huang, Q., Jones, C., and Toby, B.: Crystal structure determination and reaction pathway of amide-hydride mixtures. J. Alloys Compd. 454, 233 (2008).Google Scholar
13Chen, Y., Wu, C.Z., Wang, P., and Cheng, H.M.: Structure and hydrogen storage property of ball-milled LiNH2/MgH2 mixture. Int. J. Hydrogen Energy 31, 1236 (2006).Google Scholar
14Chen, P., Xiong, Z.T., Yang, L., Wu, G., and Luo, W.: Mechanistic investigations on the heterogeneous solid-state reaction of magnesium amides and lithium hydrides. J. Phys. Chem. B 110, 14221 (2006).Google Scholar
15Wang, J.: DOE Program Annual Review. Available at: http://www.hydrogen.energy.gov/annualreview05storage.html#metal (2005).Google Scholar
16Kojima, Y. and Kawai, Y.: IR characterizations of lithium imide and amide. J. Alloys Compd. 395, 236 (2005).Google Scholar
17Xiong, Z.T., Hu, J.J., Wu, G.T., Chen, P., Luo, W.F., Gross, K., and Wang, J.: Thermodynamic and kinetic investigations of the hydrogen storage in the Li-Mg-N-H system. J. Alloys Compd. 398, 235 (2005).Google Scholar
18Yang, J., Sudik, A., and Wolverton, C.: Activation of hydrogen-storage materials in the Li-Mg-N-H system: Effect on storage properties. J. Alloys Compd. 430, 334 (2007)CrossRefGoogle Scholar
19Chen, P., Xiong, Z., Wu, G., Liu, Y., Hu, J., and Luo, W.: Metal-N-H systems for the hydrogen storage. Scr. Mater. 56, 817 (2007).Google Scholar
20Luo, S., Flanagan, T.B., and Luo, W.: The effect of exposure of the H-storage system (LiNH2+MgH2) to water-saturated air. J. Alloys Compd. 440, L13 (2007).CrossRefGoogle Scholar
21Sudik, A., Yang, J., Halliday, D., and Wolverton, C.: Kinetic improvement in the Mg(NH2)2-LiH storage system by product seeding. J. Phys. Chem. C 111, 6568 (2007).Google Scholar
22Liu, Y., Hu, J., Xiong, Z., and Wu, G.: Improvement of the hydrogen-storage performances of Li-Mg-N-H system. J. Mater. Res. 22, 1339 (2007).Google Scholar
23Yang, J., Sudik, A., Siegel, D.J., Halliday, D., Drews, A., Carter, R.O., Wolverton, C., Lewis, G.J., Sachtler, J.W.A., Low, J.J., Faheem, S.A., Lesch, D.A., and Ozolins, V.: A self-catalyzing hydrogen-storage material. Angew. Chem. Int. Ed. 47, 882 (2008).Google Scholar
24Hu, J., Liu, Y., Wu, G., Xiong, Z., Chua, Y.S., and Chen, P.: Improvement of hydrogen storage properties of the Li-Mg-N-H system by addition of LiBH4. Chem. Mater. 20, 4398 (2008).Google Scholar
25Nakamura, Y., Hino, S., Ichikawa, T., Fujii, H., Brinks, H.W., and Hauback, B.C.: Dehydrogenation reaction of Li-Mg-N-H systems studied by in situ synchrotron powder x-ray diffraction and powder neutron diffraction. J. Alloys Compd. 457, 362 (2008).CrossRefGoogle Scholar
26Hu, J., Liu, Y., Wu, G., Xiong, Z., and Chen, P.: Structural and compositional changes during hydrogenation/dehydrogenation of the Li-Mg-N-H system. J. Phys. Chem. C 111, 18439 (2007).Google Scholar
27Hu, Y. and Ruckenstein, E.: Ultrafast reaction between LiH and NH3during H2 storage in Li3N. J. Phys. Chem. A 107, 9737 (2003).Google Scholar
28Ichikawa, T., Hanada, N., Isobe, S., Leng, H., and Fujii, H.: Mechanism of novel reaction from LiNH2 and LiH to Li2NH and H2 as a promising hydrogen storage system. J. Phys. Chem. B 108, 7887 (2004).Google Scholar