A high-density ammonia storage/delivery system based on Mg(NH3)6Cl2 for SCR-DeNOx in vehicles

被引:86
作者
Elmoe, TD
Sorensen, RZ
Quaade, U
Christensen, CH
Norskov, JK
Johannessen, T
机构
[1] Tech Univ Denmark, Dept Chem Engn, DK-2800 Lyngby, Denmark
[2] Tech Univ Denmark, ICAT, Interdisciplinary Res Ctr Catalysis, DK-2800 Lyngby, Denmark
[3] Tech Univ Denmark, Dept Chem, Ctr Sustainable & Green Chem, DK-2800 Lyngby, Denmark
[4] Tech Univ Denmark, Dept Phys, CAMP, DK-2800 Lyngby, Denmark
关键词
reaction engineering; energy; materials; environment; automotive SCR-DeNO(x); compact ammonia delivery system;
D O I
10.1016/j.ces.2005.11.038
中图分类号
TQ [化学工业];
学科分类号
0817 [化学工程与技术];
摘要
In this paper, we present a new benchmark for the automobile selective catalytic reduction of NOx: Mg(NH3)(6)Cl-2. This solid complex releases ammonia upon heating and can be compacted into a dense shape which is both easy to handle and safe. Furthermore, the material has a high volumetric ammonia density of up to 93% of that of liquid ammonia. This provides a long lasting ammonia storage (approximate to 20000 km of driving per 6.2 L Mg(NH3)(6)Cl-2 for an average medium-sized vehicle). The controlled thermal decomposition of Mg(NH3)(6)Cl-2 was demonstrated. A small reactor with a volume of 785 mL was filled with approximate to 260 g of Mg(NH3)(6)Cl-2 yielding a bed density of 331 kg/m(3). The reactor was coupled to a buffer with a free volume of roughly 200 mL. A heating wire wrapped around the outside of the reactor supplied the heat-energy. A mass-flow controller was used to simulate a varying NO, signal. It was demonstrated that it was possible to control the desorption using a simple ON-OFF controller with the buffer pressure as the control variable. Approximately 99% of the ammonia contained in the salt could be desorped and dosed, while maintaining the 5 bars used as the set-point pressure. The low density was improved by compressing the Mg(NH3)(6)Cl-2 powder to a density of 1219 kg/m(3), which is very close to the theoretical crystal density of 1252 kg/m(3). Temperature programmed desorption showed that the ammonia could easily be desorped by heating the densified material. Stoichiometric calculations have shown, that compared to the current choice of ammonia delivery for mobile DeNO(x) (thermal decomposition of a 32.5% wt/wt aqueous urea solution), the high-density Mg(NH3)(6)Cl-2 compound weighs 2.8 times less and takes up 3.1 times less space. This makes Mg(NE3)(6)Cl-2 ideal for use as an ammonia storage compound in both diesel and lean-burn gasoline-driven automobiles. (c) 2005 Elsevier Ltd. All rights reserved.
引用
收藏
页码:2618 / 2625
页数:8
相关论文
共 15 条
[1]
[Anonymous], 1997, Catalysis Surveys from Japan
[2]
Choi S, 2001, SAE TECHNICAL PAPER
[3]
CRC, 2004, HDB CHEM PHYS
[4]
Urea thermolsis and NOx reduction with and without SCR catalysts [J].
Fang, HL ;
DaCosta, HFM .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 46 (01) :17-34
[5]
*GMEL, 1939, GMEL HDB
[6]
A MODEL FOR REVERSIBLE SOLID GAS REACTIONS SUBMITTED TO TEMPERATURE AND PRESSURE CONSTRAINTS - SIMULATION OF THE RATE OF REACTION IN SOLID GAS REACTOR USED AS CHEMICAL HEAT-PUMP [J].
GOETZ, V ;
MARTY, A .
CHEMICAL ENGINEERING SCIENCE, 1992, 47 (17-18) :4445-4454
[7]
HUMMELSHOJ J, 2005, IN PRESS J AM CHEM S
[8]
Kipouros G.J., 2001, J. Light Met., V1, P111, DOI DOI 10.1016/S1471-5317(01)00004-9
[9]
Urea-SCR:: a promising technique to reduce NOx emissions from automotive diesel engines [J].
Koebel, M ;
Elsener, M ;
Kleemann, M .
CATALYSIS TODAY, 2000, 59 (3-4) :335-345
[10]
Ammonia absorption on alkaline earth halides as ammonia separation and storage procedure [J].
Liu, CY ;
Aika, K .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 2004, 77 (01) :123-131