Electronic structure and decomposition pathways of monoammoniate of lithium borohydride Li(NH3)BH4: A first-principles investigation

被引：2

作者：

Zhong, B. ^{[1
]}

Huang, X. X. ^{[1
]}

Wen, G. ^{[1
]}

Zhang, X. D. ^{[1
]}

Bai, H. W. ^{[1
]}

Zhang, T. ^{[1
]}

Yu, H. M. ^{[1
]}

机构：

[1] Harbin Inst Technol, Sch Mat Sci & Engn, Harbin 150001, Peoples R China

来源：

SOLID STATE COMMUNICATIONS | 2010年 / 150卷 / 33-34期

基金：

美国国家科学基金会;

关键词：

Borohydride; First-principles calculation; Electronic structure; Hydrogen storage; HYDROGEN STORAGE; AMMONIA; HYDRIDES;

D O I：

10.1016/j.ssc.2010.06.002

中图分类号：

O469 [凝聚态物理学];

学科分类号：

070205 ;

摘要：

The monoammoniate of lithium borohydride (Li(NH3)BH4) is a potential candidate for hydrogen storage owing to its high hydrogen capacity (18 wt%). In this work, electronic structure, bonding characters, and decomposition pathways of Li(NH3)BH4 are investigated from first-principles calculations. We find that NH3 molecules are covalently attached to Li atoms through N atoms and the ionization of Li atoms plays an essential role in stabilizing the compound. A general correlation between the stability of X(NH3)BH4 (X = H, Li, Na, K) and the electronegativities of X atoms is established. The thermal stability of X(NH3)BH4 could be modulated by manipulating the cation electronegativities. Free energy computations indicate that Li(NH3)BH4 -> LiBH4 + NH3 is the most likely thermal decomposition route. (C) 2010 Elsevier Ltd. All rights reserved.

引用

页码：1552 / 1555

页数：4

共 21 条

[11] Correlation between thermodynamical stabilities of metal borohydrides and cation electronegativites:: First-principles calculations and experiments [J].

Nakamori, Yuko ;

Miwa, Kazutoshi ;

Ninomiya, Akihito ;

Li, Haiwen ;

Ohba, Nobuko ;

Towata, Shin-ichi ;

Zuettel, Andreas ;

Orimo, Shin-ichi .

PHYSICAL REVIEW B, 2006, 74 (04)

[12] Complex hydrides for hydrogen storage [J].

Orimo, Shin-ichi ;

Nakamori, Yuko ;

Eliseo, Jennifer R. ;

Zuettel, Andreas ;

Jensen, Craig M. .

CHEMICAL REVIEWS, 2007, 107 (10) :4111-4132

[13] Diarylstannylene activation of hydrogen or ammonia with arene elimination [J].

Peng, Yang ;

Ellis, Bobby D. ;

Wang, Xinping ;

Power, Philip P. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (37) :12268-+

[14]

Perdew JP, 1997, PHYS REV LETT, V78, P1396, DOI 10.1103/PhysRevLett.77.3865

[15] Electronic structure, stability and bonding of the Li-N-H hydrogen storage system [J].

Song, Y. ;

Guo, Z. X. .

PHYSICAL REVIEW B, 2006, 74 (19)

[16] Ammonia-borane: The hydrogen source par excellence? [J].

Chemistry Division, Los Alamos National Laboratory, Los Alamos, NM, United States .

Dalton Trans., 2007, 25 (2613-2626) :2613-2626

[17] THE LITHIUM BOROHYDRIDE-AMMONIA SYSTEM - PRESSURE-COMPOSITION-TEMPERATURE RELATIONSHIPS AND DENSITIES [J].

SULLIVAN, EA ;

JOHNSON, S .

JOURNAL OF PHYSICAL CHEMISTRY, 1959, 63 (02) :233-238

[18] SOFT SELF-CONSISTENT PSEUDOPOTENTIALS IN A GENERALIZED EIGENVALUE FORMALISM [J].

VANDERBILT, D .

PHYSICAL REVIEW B, 1990, 41 (11) :7892-7895

[19] Hydrogen in aluminum: First-principles calculations of structure and thermodynamics [J].

Wolverton, C ;

Ozolins, V ;

Asta, M .

PHYSICAL REVIEW B, 2004, 69 (14) :144109-1

[20]

Wolverton C, 2001, PHYS REV B, V63

← 1 2 3 →