Sustainable NOx production from air in pulsed plasma: elucidating the chemistry behind the low energy consumption

被引:60
作者
Vervloessem, Elise [1 ,2 ]
Gorbanev, Yury [1 ]
Nikiforov, Anton [2 ]
De Geyter, Nathalie [2 ]
Bogaerts, Annemie [1 ]
机构
[1] Univ Antwerp, Univ Pl 1, B-2610 Antwerp, Belgium
[2] Univ Ghent, Sint Pietersnieuwstr 25, B-9000 Ghent, Belgium
基金
欧洲研究理事会;
关键词
BARRIER DISCHARGES; NITROGEN-FIXATION; GREEN AMMONIA; GENERATION; SPARK; COST;
D O I
10.1039/d1gc02762j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
N-Based fertilisers are paramount to support our still-growing world population. Current industrial N-2 fixation is heavily fossil fuel-dependent, therefore, a lot of work is put into the development of fossil-free pathways. Plasma technology offers a fossil-free and flexible method for N-2 fixation that is compatible with renewable energy sources. We present here a pulsed plasma jet for direct NOx production from air. The pulsed power allows for a record-low energy consumption (EC) of 0.42 MJ (mol N)(-1). This is the lowest reported EC in plasma-based N-2 fixation at atmospheric pressure thus far. We compare our experimental data with plasma chemistry modelling, and obtain very good agreement. Hence, we can use our model to explain the underlying mechanisms responsible for this low EC. The pulsed power and the corresponding pulsed gas temperature are the reason for the very low EC: they provide a strong vibrational-translational non-equilibrium and promote the non-thermal Zeldovich mechanism. This insight is important for the development of the next generation of plasma sources for energy-efficient NOx production.
引用
收藏
页码:916 / 929
页数:14
相关论文
共 67 条
[1]   Temperature-dependent behavior of nitrogen fixation in nanopulsed dielectric barrier discharge operated at different humidity levels and oxygen contents [J].
Abdelaziz, Ayman A. ;
Kim, Hyun-Ha .
JOURNAL OF PHYSICS D-APPLIED PHYSICS, 2020, 53 (11)
[2]   Vibrational energy transfer rates using a forced harmonic oscillator model [J].
Adamovich, IV ;
Macheret, SO ;
Rich, JW ;
Treanor, CE .
JOURNAL OF THERMOPHYSICS AND HEAT TRANSFER, 1998, 12 (01) :57-65
[3]   Life Cycle Assessment of the Nitrogen Fixation Process Assisted by Plasma Technology and Incorporating Renewable Energy [J].
Anastasopoulou, Aikaterini ;
Butala, Sughosh ;
Lang, Juergen ;
Hessel, Volker ;
Wang, Qi .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2016, 55 (29) :8141-8153
[4]  
[Anonymous], 2000, Ullmann's Encyclopedia of Industrial Chemistry, V3, Wiley-VHC, DOI [10.1002/14356007.a17_293, DOI 10.1002/14356007.A17_293]
[5]  
Asisov R.I., 1980, SOV PHYS, V14, P366
[6]   Structural modification of NADPH oxidase activator (Noxa 1) by oxidative stress: An experimental and computational study [J].
Attri, Pankaj ;
Park, Jae-Hyun ;
De Backer, Joey ;
Kim, Myeongkyu ;
Yun, Ji-Hye ;
Heo, Yunseok ;
Dewilde, Sylvia ;
Shiratani, Masaharu ;
Choi, Eun Ha ;
Lee, Weontae ;
Bogaerts, Annemie .
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES, 2020, 163 (163) :2405-2414
[7]   Nitrogen fixed into HNO3 by pulsed high voltage discharge [J].
Bian, Wenjuan ;
Song, Xuehong ;
Shi, Junwen ;
Yin, Xiangli .
JOURNAL OF ELECTROSTATICS, 2012, 70 (03) :317-326
[8]   On the oxidation of atmospheric nitrogen in electric arcs. [J].
Birkeland, K .
TRANSACTIONS OF THE FARADAY SOCIETY, 1906, 2 (02) :0098-0119
[9]   Reactive nitrogen requirements to feed the world in 2050 and potential to mitigate nitrogen pollution [J].
Bodirsky, Benjamin Leon ;
Popp, Alexander ;
Lotze-Campen, Hermann ;
Dietrich, Jan Philipp ;
Rolinski, Susanne ;
Weindl, Isabelle ;
Schmitz, Christoph ;
Mueller, Christoph ;
Bonsch, Markus ;
Humpenoeder, Florian ;
Biewald, Anne ;
Stevanovic, Miodrag .
NATURE COMMUNICATIONS, 2014, 5
[10]   Plasma Technology: An Emerging Technology for Energy Storage [J].
Bogaerts, Annemie ;
Neyts, Erik C. .
ACS ENERGY LETTERS, 2018, 3 (04) :1013-1027