Impurity Gas Analysis of the Decomposition of Complex Hydrides

被引：36

作者：

Borgschulte, A. ^{[1
]}

Callini, E. ^{[1
]}

Probst, B. ^{[1
]}

Jain, A. ^{[1
,2
]}

Kato, S. ^{[1
]}

Friedrichs, O. ^{[1
]}

Remhof, A. ^{[1
]}

Bielmann, M. ^{[1
]}

Ramirez-Cuesta, A. J. ^{[3
]}

Zuttel, A. ^{[1
]}

机构：

[1] Empa, Swiss Fed Labs Mat Testing & Res Hydrogen & Energ, CH-8600 Dubendorf, Switzerland

[2] Univ Rajasthan, Ctr Nonconvent Energy Resources, Jaipur 302004, Rajasthan, India

[3] Rutherford Appleton Lab, ISIS Facil, Didcot OX11 0QX, Oxon, England

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2011年 / 115卷 / 34期

基金：

瑞士国家科学基金会;

关键词：

DIBORANE; TETRAHYDROBORATE; CHEMISORPTION; REVERSIBILITY; DESORPTION; CHEMISTRY; RELEASE; SPECTRA;

D O I：

10.1021/jp205566q

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

This study aims at an investigation of the impurity gases emitted during the decomposition of borohydrides. For this we have set up a quantitative gas analysis based on a combination of FTIR spectroscopy and gravimetry. We show that the emission of various intermediates, in particular diborane, depends sensitively on the reaction conditions, including gas mean free path lengths, hydrogen backpressure, and sample pretreatment. Adduct-free Mg(BH4)(2) and LiBH4 emit diborane only at the impurity level, while for LiZn2(BH4)(5) diborane is the main decomposition product. The decomposition reaction of LiZn2(BH4)(5) proceeds via a collision-induced dissociation of Zn(BH4)(2) in Ar at ambient pressures. Various additives were tested aiming at catalyzing the decomposition of the desorbed diborane.

引用

页码：17220 / 17226

页数：7

共 41 条

[1] First-principles prediction of phase stability and crystal structures in Li-Zn and Na-Zn mixed-metal borohydrides [J].

Aidhy, Dilpuneet S. ;

Wolverton, C. .

PHYSICAL REVIEW B, 2011, 83 (14)

[2]

[Anonymous], 2008, Hydrogen as a Future Energy Carrier

[3]

[Anonymous], 2005, NIST CHEM WEBBOOK MA

[4] COLLISION-INDUCED DISSOCIATIVE CHEMISORPTION OF CH4 ON NI(111) BY INERT-GAS ATOMS - THE MECHANISM FOR CHEMISTRY WITH A HAMMER [J].

BECKERLE, JD ;

JOHNSON, AD ;

YANG, QY ;

CEYER, ST .

JOURNAL OF CHEMICAL PHYSICS, 1989, 91 (09) :5756-5777

[5] AZn2(BH4)5 (A = Li, Na) and NaZn(BH4)3: Structural Studies [J].

Cerny, Radovan ;

Kim, Ki Chul ;

Penin, Nicolas ;

D'Anna, Vincenza ;

Hagemann, Hans ;

Sholl, David S. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (44) :19127-19133

[6] The unique chemistry of hydrogen beneath the surface: Catalytic hydrogenation of hydrocarbons [J].

Ceyer, ST .

ACCOUNTS OF CHEMICAL RESEARCH, 2001, 34 (09) :737-744

[7] Formation and bonding of alane clusters on Al(111) surfaces studied by infrared absorption spectroscopy and theoretical modeling [J].

Chaudhuri, Santanu ;

Rangan, Sylvie ;

Veyan, Jean-Francois ;

Muckerman, James T. ;

Chabal, Yves J. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (32) :10576-10587

[8] Synthesis and properties of magnesium tetrahydroborate, Mg(BH4)2 [J].

Chlopek, Krzysztof ;

Frommen, Christoph ;

Leon, Aline ;

Zabara, Oleg ;

Fichtner, Maximilian .

JOURNAL OF MATERIALS CHEMISTRY, 2007, 17 (33) :3496-3503

[9] Reversible dehydrogenation of magnesium borohydride to magnesium triborane in the solid state under moderate conditions [J].

Chong, Marina ;

Karkamkar, Abhi ;

Autrey, Tom ;

Orimo, Shin-ichi ;

Jalisatgi, Satish ;

Jensen, Craig M. .

CHEMICAL COMMUNICATIONS, 2011, 47 (04) :1330-1332

[10] First principles methods using CASTEP [J].

Clark, SJ ;

Segall, MD ;

Pickard, CJ ;

Hasnip, PJ ;

Probert, MJ ;

Refson, K ;

Payne, MC .

ZEITSCHRIFT FUR KRISTALLOGRAPHIE, 2005, 220 (5-6) :567-570

← 1 2 3 4 5 →