Effect of selective catalytic reduction on exhaust nonvolatile particle emissions of Euro VI heavy-duty compression ignition vehicles

Abstract The nonvolatile particle number (PN) emissions of late technology diesel heavy-duty vehicles (HDV) are very low due to the introduction of Diesel Particulate Filters (DPF). Nevertheless, a large fraction (50%) of particles below the current lower regulated size (23 nm) was recently reported. Moreover, large differences between laboratory and PN Portable Emission Measurement Systems (PN-PEMS) have been observed. In order to better understand such differences, the physical properties of the exhaust aerosol from two Euro VI technology diesel heavy-duty engines were studied. It was found that urea injection leads to formation of nonvolatile particles. The produced particles covered a wide size range spanning from below 10 nm to above 100 nm. As such, they contribute to the regulated PN emissions, with measured concentrations corresponding to as high as 2 × 1011 #/kWh over a World Harmonized Transient Cycle (WHTC). However, a large fraction of them was undetected owing to their small particle size. Low-cutoff size (10 nm) Condensation Particle Counters (CPCs) (which are under discussion to be included in the regulations) measured up to twice as high concentrations. Considering the large particle losses in the sampling systems at this size range, the true concentrations can be two times higher from what the low-cutoff CPCs reported. When the temperature of the SCR system exceeded a threshold of 300 °C, the produced particles were found to be positively charged, increasing the average exhaust aerosol charge up to +3 elementary charges per particle. Scanning Mobility Particle Sizer (SMPS) measurements of non-neutralized samples revealed that even the smallest of them can carry more than one positive charge. The findings of this study can explain the differences reported between PEMS and laboratory systems and especially those based on diffusion charging. They also provide insight for a refinement of technical requirements prescribed in the European PEMS regulation to more accurately quantify the PN emissions from such technologies.

[1]  O. Deutschmann,et al.  Formation of Urea-Based Deposits in an Exhaust System: Numerical Predictions and Experimental Observations on a Hot Gas Test Bench , 2016, Emission Control Science and Technology.

[2]  J. Keskinen,et al.  Spray Charging of Droplets in a Wet Scrubber , 2002, Journal of the Air & Waste Management Association.

[3]  M. Maricq,et al.  On the electrical charge of motor vehicle exhaust particles , 2006 .

[4]  J. Colson,et al.  Thermal decomposition (pyrolysis) of urea in an open reaction vessel , 2004 .

[5]  D. Kittelson,et al.  Evaluation of thermal denuder and catalytic stripper methods for solid particle measurements , 2010 .

[6]  David Y. H. Pui,et al.  The Effect of Particle Pre-Existing Charge on Unipolar Charging and Its Implication on Electrical Aerosol Measurements , 2009 .

[7]  Doo-Sung Baik,et al.  Experimental study on the characteristics of nano-particle emissions from a heavy-duty diesel engine using a urea-SCR system , 2012 .

[8]  P. Koponen,et al.  Selective catalytic reduction operation with heavy fuel oil: NOx, NH3, and particle emissions. , 2015, Environmental science & technology.

[9]  Barouch Giechaskiel,et al.  Solid Particle Number Emission Factors of Euro VI Heavy-Duty Vehicles on the Road and in the Laboratory , 2018, International journal of environmental research and public health.

[10]  G. Martini,et al.  Investigation of vehicle exhaust sub-23 nm particle emissions , 2017 .

[11]  A. Faustini,et al.  Nitrogen dioxide and mortality: review and meta-analysis of long-term studies , 2013, European Respiratory Journal.

[12]  Barouch Giechaskiel,et al.  Experimental assessment of solid particle number Portable Emissions Measurement Systems (PEMS) for heavy-duty vehicles applications , 2018, Journal of Aerosol Science.

[13]  Barouch Giechaskiel,et al.  Evaluation of Portable Number Emission Systems for Heavy-Duty Applications under Steady State and Transient Vehicle Operation Conditions on a Chassis Dynamometer , 2018 .

[14]  Linjun Yang,et al.  Effect of Selective Catalytic Reduction System on Fine Particle Emission Characteristics , 2016 .

[15]  Z. Gerald Liu,et al.  The Effect of Diesel Exhaust Fluid Dosing on Tailpipe Particle Number Emissions , 2016 .

[16]  M. Gamero-Castaño,et al.  Ion-induced nucleation: Measurement of the effect of embryo’s size and charge state on the critical supersaturation , 2002 .

[17]  B. Festy Review of evidence on health aspects of air pollution – REVIHAAP Project. Technical Report. World Health Organization Regional Office for Europe 2013 , 2013 .

[18]  Bonnel Pierre,et al.  Feasibility study on the extension of the Real Driving Emissions (RDE) procedure to Particle Number (PN): Chassis dynamometer evaluation of portable emission measurement systems (PEMS) to measure particle number (PN) concentration: Phase II , 2015 .

[19]  Alberto Ayala,et al.  Effect of advanced aftertreatment for PM and NOx reduction on heavy-duty diesel engine ultrafine particle emissions. , 2011, Environmental science & technology.

[20]  B. Giechaskiel,et al.  Regulating particle number measurements from the tailpipe of light-duty vehicles: The next step? , 2019, Environmental research.

[21]  J. Andersson,et al.  Measurement of Automotive Nonvolatile Particle Number Emissions within the European Legislative Framework: A Review , 2012 .

[22]  M. Maricq,et al.  Monitoring Motor Vehicle PM Emissions: An Evaluation of Three Portable Low-Cost Aerosol Instruments , 2013 .

[23]  Suresh Dhaniyala,et al.  Instruments Based on Electrical Detection of Aerosols , 2011 .

[24]  Leonidas Ntziachristos,et al.  Impact of selective catalytic reduction on exhaust particle formation over excess ammonia events. , 2014, Environmental science & technology.

[25]  J. Czerwinski,et al.  Emission Reduction with Diesel Particle Filter with SCR Coating (SDPF) , 2015, Emission Control Science and Technology.

[26]  K. Oh,et al.  A Characteristics of Particle Number Distribution for the Urea Solution Injection to Urea SCR System of Commercial Diesel Engine for an Emission Regulation , 2007 .

[27]  Barouch Giechaskiel,et al.  Experimental Assessment of an Electrofilter and a Tandem Positive-Negative Corona Charger for the Measurement of Charged Nanoparticles formed in Selective Catalytic Reduction Systems , 2019, Applied Sciences.

[28]  Zhen Huang,et al.  Review of state of the art technologies of selective catalytic reduction of NOx from diesel engine exhaust , 2014 .

[29]  R. Flagan,et al.  Scanning Electrical Mobility Spectrometer , 1990 .