Efficient synthesis of ammonia from N2 and H2 alone in a ferroelectric packed-bed DBD reactor

被引:123
作者
Gomez-Ramirez, A. [1 ,2 ]
Cotrino, J. [2 ,3 ]
Lambert, R. M. [2 ,4 ]
Gonzalez-Elipe, A. R. [2 ]
机构
[1] Univ Seville, Inst Ciencia Mat Sevilla, Lab Nanotechnol Surfaces, CSIC, Avda Amer Vespucio 49, Seville 41092, Spain
[2] Univ Seville, Inst Ciencia Mat Sevilla, Lab Nanotechnol Surfaces, CSIC, Seville 41092, Spain
[3] Univ Seville, Dept Fis Atom Mol & Nucl, Seville 42022, Spain
[4] Univ Cambridge, Dept Chem, Cambridge CB2 1EW, England
关键词
ammonia production; plasma assisted catalysis; ferroelectric moderator; dielectric barrier discharge; DIELECTRIC-BARRIER-DISCHARGE; HIGH-FREQUENCY DISCHARGES; ATMOSPHERIC-PRESSURE; MICROWAVE-DISCHARGE; CARBON-DIOXIDE; PLASMA; CATALYST; NITROGEN; ENERGY;
D O I
10.1088/0963-0252/24/6/065011
中图分类号
O35 [流体力学]; O53 [等离子体物理学];
学科分类号
070204 ; 080103 ; 080704 ;
摘要
A detailed study of ammonia synthesis from hydrogen and nitrogen in a planar dielectric barrier discharge (DBD) reactor was carried out. Electrical parameters were systematically varied, including applied voltage and frequency, electrode gap, and type of ferroelectric material (BaTiO3 versus PZT). For selected operating conditions, power consumption and plasma electron density were estimated from Lissajous diagrams and by application of the Bolsig + model, respectively. Optical emission spectroscopy was used to follow the evolution of plasma species (NH*, N*, N-2(+) and N-2*) as a function of applied voltage with both types of ferroelectric material. PZT gave both greater energy efficiency and higher ammonia yield than BaTiO3: 0.9 g NH3 kWh(-1) and 2.7% single pass N-2 conversion, respectively. This performance is substantially superior to previously published findings on DBD synthesis of NH3 from N-2 and H-2 alone. The influence of electrical working parameters, the beneficial effect of PZT and the importance of controlling reactant residence time are rationalized in a reaction model that takes account of the principal process variables
引用
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页数:7
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