Gaining insight into the catalytic dehydrogenation of hydrazine borane in water

被引:16
作者
Cakanyildirim, Cetin [1 ]
Petit, Eddy [1 ]
Demirci, Umit B. [1 ]
Moury, Romain [1 ]
Petit, Jean-Fabien [1 ]
Xu, Qiang [2 ]
Miele, Philippe [1 ]
机构
[1] Univ Montpellier 2, IEM, UMR 5635, CNRS ENSCM UM2, F-34095 Montpellier, France
[2] Natl Inst Adv Ind Sci & Technol, Ikeda, Osaka 5638577, Japan
关键词
Chemical hydrogen storage; Decomposition of N2H4; Hydrazine borane; Hydrolysis of BH3; NiPt nanocatalyst; HIGH-EXTENT DEHYDROGENATION; HYDROGEN GENERATION; AMMONIA-BORANE; SODIUM-BOROHYDRIDE; HYDROLYSIS; DECOMPOSITION; NANOCATALYSTS; N2H4BH3; ISSUES; FUEL;
D O I
10.1016/j.ijhydene.2012.08.032
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
Dehydrogenation of hydrazine borane H2NNH2BH3 (HB, 15.3 wt% H), an attractive chemical hydrogen storage material, can be performed in water, mild conditions (ambient pressure and 50 degrees C) and the presence of a NiPt nanocatalyst. In the present work, the main objective was to gain insight into the reaction mechanisms as well as the evolution of the catalyst. From operando and in situ characterization and measurements, it was shown that the dehydrogenation of HB in water consists of hydrolysis of the BH3 group and decomposition/dehydrogenation of the H2NNH2 moiety. Both reactions take place concomitantly but at different kinetics, the former being at least 40 times faster in our optimized experimental conditions. From ex situ characterization, it was found that the NiPt nanocatalyst surface is stable during the overall reaction but it is sensitive to its recovery upon the reaction completion. XPS measurements showed that the washing-drying process is a critical process during which Ni segregates and the catalytic surface changes. Both findings and other ones herein reported are of importance for better understanding the HB dehydrogenation reaction and the role of the nanocatalyst as well as for future works. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:15983 / 15991
页数:9
相关论文
共 30 条
[1]   A safe, portable, hydrogen gas generator using aqueous borohydride solution and Ru catalyst [J].
Amendola, SC ;
Sharp-Goldman, SL ;
Janjua, MS ;
Spencer, NC ;
Kelly, MT ;
Petillo, PJ ;
Binder, M .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2000, 25 (10) :969-975
[2]  
Broom DP, 2011, GREEN ENERGY TECHNOL, P1
[3]   Nickel-based bimetallic nanocatalysts in high-extent dehydrogenation of hydrazine borane [J].
Cakanyildirim, Cetin ;
Demirci, Umit B. ;
Sener, Tansel ;
Xu, Qiang ;
Miele, Philippe .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2012, 37 (12) :9722-9729
[4]   Hydrogen generation from the hydrolysis of hydrazine-borane catalyzed by rhodium(0) nanoparticles supported on hydroxyapatite [J].
Celik, Derya ;
Karahan, Senem ;
Zahmakiran, Mehmet ;
Ozkar, Saim .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2012, 37 (06) :5143-5151
[5]   Dissociation and hydrolysis of ammonia-borane with solid acids and carbon dioxide: An efficient hydrogen generation system [J].
Chandra, Manish ;
Xu, Qiang .
JOURNAL OF POWER SOURCES, 2006, 159 (02) :855-860
[6]   Cobalt in NaBH4 hydrolysis [J].
Demirci, U. B. ;
Miele, P. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2010, 12 (44) :14651-14665
[7]   Sodium Borohydride Hydrolysis as Hydrogen Generator: Issues, State of the Art and Applicability Upstream from a Fuel Cell [J].
Demirci, U. B. ;
Akdim, O. ;
Andrieux, J. ;
Hannauer, J. ;
Chamoun, R. ;
Miele, P. .
FUEL CELLS, 2010, 10 (03) :335-350
[8]  
Demirci UB, 2010, BORON HYDRIDES HIGH
[9]   Hydrolysis of solid ammonia borane [J].
Demirci, Umit B. ;
Miele, Philippe .
JOURNAL OF POWER SOURCES, 2010, 195 (13) :4030-4035
[10]   Sodium tetrahydroborate as energy/hydrogen carrier, its history [J].
Demirci, Umit B. ;
Miele, Philippe .
COMPTES RENDUS CHIMIE, 2009, 12 (09) :943-950