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Frontiers in Energy

ISSN 2095-1701

ISSN 2095-1698(Online)

CN 11-6017/TK

Postal Subscription Code 80-972

2018 Impact Factor: 1.701

Front. Energy    2022, Vol. 16 Issue (5) : 840-851    https://doi.org/10.1007/s11708-021-0797-1
RESEARCH ARTICLE
Multi-stage ammonia production for sorption selective catalytic reduction of NOx
Chen ZHANG, Guoliang AN, Liwei WANG(), Shaofei WU
Institute of Refrigeration and Cryogenics, Key Laboratory of Power Machinery and Engineering of the Ministry of Education, Shanghai Jiao Tong University, Shanghai 200240, China
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Abstract

Sorption selective catalytic reduction of nitrogen oxides (NOx) (sorption-SCR) has ever been proposed for replacing commercial urea selective catalytic reduction of NOx (urea-SCR), while only the single-stage sorption cycle is hitherto adopted for sorption-SCR. Herein, various multi-stage ammonia production cycles is built to solve the problem of relative high starting temperature with ammonia transfer (AT) unit and help detect the remaining ammonia in ammonia storage and delivery system (ASDS) with ammonia warning (AW) unit. Except for the single-stage ammonia production cycle with MnCl2, other sorption-SCR strategies all present overwhelming advantages over urea-SCR considering the much higher NOx conversion driven by the heat source lower than 100°C and better matching characteristics with low-temperature catalysts. Furthermore, the required mass of sorbent for each type of sorption-SCR is less than half of the mass of AdBlue for urea-SCR. Therefore, the multifunctional multi-stage sorption-SCR can realize compact and renewable ammonia storage and delivery with low thermal energy consumption and high NOx conversion, which brings a bright potential for efficient commercial de-NOx technology.

Keywords selective catalytic reduction (SCR)      nitrogen oxides (NOx)      ammonia      composite sorbent      chemisorption     
Corresponding Author(s): Liwei WANG   
Online First Date: 04 January 2022    Issue Date: 28 November 2022
 Cite this article:   
Chen ZHANG,Guoliang AN,Liwei WANG, et al. Multi-stage ammonia production for sorption selective catalytic reduction of NOx[J]. Front. Energy, 2022, 16(5): 840-851.
 URL:  
https://academic.hep.com.cn/fie/EN/10.1007/s11708-021-0797-1
https://academic.hep.com.cn/fie/EN/Y2022/V16/I5/840
Fig.1  Working principle of sorption-SCR.
Fig.2  Single-stage ammonia production process.
Fig.3  Double-stage ammonia production process.
Fig.4  Triple-stage ammonia production process.
Fig.5  Double-stage triple-effect ammonia production process.
Fig.6  Experimental test unit and test procedure.
Fig.7  Thermodynamic sorption results of NH4Cl/ENG-TSA, CaCl2/ENG-TSA, and MnCl2/ENG-TSA at 0.87 MPa.
Fig.8  Ts versus ps of NH4Cl/ENG-TSA, CaCl2/ENG-TSA, and MnCl2/ENG-TSA, with experimental value shown in solid lines and theoretical value shown in dash lines.
Fig.9  Comparison of sorption-SCR and urea-SCR on NOx conversion at various driven temperatures.
Fig.10  Ammonia storage density and thermal efficiency of various ammonia production processes (s1: NH4Cl; s2: NaBr; s3: CaCl2; s4: SrCl2; s5: MnCl2; d1: CaCl2-NH4Cl; d2: SrCl2-NH4Cl; d3: MnCl2-NH4Cl; d4: CaCl2-NaBr; d5: SrCl2-NaBr; d6: MnCl2-NaBr; t1: CaCl2-NH4Cl-MnCl2; t2: SrCl2-NH4Cl-MnCl2; t3: CaCl2-NaBr-MnCl2; t4: SrCl2-NaBr-MnCl2; dt1: CaCl2/MnCl2-NH4Cl; dt2: SrCl2/MnCl2-NH4Cl; dt3: CaCl2/MnCl2-NaBr; dt4: SrCl2/MnCl2-NaBr).
Fig.11  Comparison of bulk weights of different types of sorption-SCR with urea-SCR as the benchmark.
Fig.12  Comparison of bulk volumes of different types of sorption-SCR with urea-SCR as the benchmark (The solid lines are the best candidates and the dash lines are the worst candidate of different type of sorption-SCR).
De-NOx agent Tsta/°C c NOx/% ηNH3/(g·kJ−1) ρNH3/(g·cm−3) ms/mAdBlue Vs/VAdBlue
s1 29 95.5 0.65 0.76 0.26 0.26–0.66
s5 125.6 0 0.21 0.43 0.46 0.46–1.16
d1 29 95.5 0.31 0.71 0.28 0.28–0.71
d6 32.8 95.5 0.21 0.42 0.48 0.48–1.21
t1 29 95.5 0.31 0.66 0.30 0.30–0.76
t4 32.8 95.5 0.31 0.54 0.37 0.37–0.93
dt1 29 95.5 0.30 0.69 0.29 0.29–0.73
dt4 32.8 95.5 0.30 0.57 0.35 0.35–0.88
AdBlue 160 0 0.07 0.20 1 1
Tab.1  Parameters of types of sorption-SCRs with urea-SCR as the benchmark
SCR type Pressure stability NOx conversion efficiency Thermal efficiency Ammonia storage capacity Quick launch AW
Single-stage sorption-SCR ☆-☆☆ ☆☆-☆☆☆ ☆☆-☆☆☆ ☆☆-☆☆☆ x x
Double-stage sorption-SCR ☆☆ ☆☆☆ ☆☆ ☆☆-☆☆☆ x
Triple-stage sorption-SCR ☆☆ ☆☆☆ ☆☆ ☆☆☆
Double-stage triple-effect sorption-SCR ☆☆ ☆☆☆ ☆☆ ☆☆☆
Urea-SCR ☆☆☆ x x
Tab.2  Overall evaluation of types of sorption-SCR with urea-SCR as the benchmark
c Specific heat capacity/(J?(kg?K)−1)
D Driving distance with per kilogram ammonia/km
m Mass/kg
N Cycle index
p Pressure/Pa
Q Heat/J
R Gas constant/(J?(kg?K)−1)
t Time/h
T Temperature/K
v Average driving speed/(km?h−1)
V Volume/m3
x Sorption capacity/(g?g−1)
Greek symbols
β Mass proportion of ammonia inside sorbent
ΔH Enthalpy change/(J?mol−1)
ΔS Entropy change/(J?(mol?K) −1)
ΔT Temperature difference/K
η Thermal efficiency/(g?kJ−1)
ρ Density/(kg?m−3)
Subscripts
c Cycle
de De-NOx
des Desorption
h High
m Middle
out Output
s Sorbent
sen Sensible
sta Starting
t Theoretical
tr Transfer
Abbreviations
ASDS Ammonia storage and delivery system
AT Ammonia transfer
AW Ammonia warning
DEF Diesel exhaust fluid
ENG-TSA Expanded nature graphite treated by the sulfuric acid
HC Hydrocarbon
NSR NOx storage and reduction
SCR Selective catalytic reduction of NOx
SCR-CC SCR catalytic converter
SCR-ECU SCR electronic control unit
  
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