SUPPLEMENTAL INFORMATION “Assessment of a Cylindrical and a Rectangular Plate Differential Mobility Analyzer for Size Fractionation of Nanoparticles at High Aerosol Flow Rates” by Esther Hontañón, Marcel Rouenhoff, Alfredo Azabal, Emilio Ramiro, Frank Einar Kruis Esther Hontañón (), Marcel Rouenhoff, Frank Einar Kruis Institute of Technology for Nanostructures (NST) and Centre for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, Bismarckstr. 81, Duisburg, 47057 Germany Esther Hontañón E-mail: esther.hontanon@uni-due.de Telephone: +49 (0) 203 379 1047 Fax: +49 (0) 203 379 3268 Alfredo Azabal, Emilio Ramiro RAMEM S.A., Sambara 33, 28027 Madrid, Spain 1 High Flow DMAs Table S1. Parameters of the high flow DMAs relevant to particle size fractionation. High Flow DMAs Outer radius (mm) 120 a) b) c) Column length (mm) Aerosol / sheath nominal flow rates (slm) Minimum particle mobility a) (cm2V-1s-1) Flow Reynolds number b) Particle Peclet number c) 42 100 100 1000 3.27x10-3 (26 nm) 2027 5.1x104 25 230 200 2000 1.88x10-3 (35 nm) 4444 1.1x105 Inner radius (nm) (mm) Cylindrical Rectangular plate Electrode separation distance (mm) 78 Classification zone width (mm) 550 Minimum particle mobility based on the sheath nominal flow rate and a maximum attainable voltage of 35 kV; the mobility equivalent diameter for singly charged spheres is given between parentheses. Reynolds number based on the total (aerosol+sheath) nominal flow rate, the electrode distance and the kinematic viscosity of air 1.5x10-5 m2s-1 at 20°C and 1 atm. Peclet number based on the flow Reynolds number and the Schmidt number for spheres of a diameter of 3 nm with a diffusion coefficient of 6x10-7 m2s-1 in air at 20°C and 1 atm. Table S2. Laminarization screens used in the high flow DMAs. High Flow DMA Manufacturer Material Model Wire diameter (µm) Mesh Opening (µm) Open Area (%) Cylindrical HF-DMA SEFAR® PET 1000 54-70W PW 70 109 34.8 Rectangular plate DMA SEFAR® PET 1000 27-120W PW 120 249 45.3 NYTAL PA-12 XXX-112 70 112 38 2 Experimental Facility A facility called Big Monodisperse Aerosol Generator (BigMAG) has been designed and built to enhance the yield of monodisperse nanoparticles in gas phase by means of Differential Mobility Analyzer (DMA). Fig. S1 shows a layout of the facility. The aerosol carrier gas and the sheath gas which is required for operating the DMA circulate in two closed loops driven by roots pumps (Ruvac WS, Oerlikon Leybold Vacuum GmbH, Germany) with maximum pumping speeds of 251 m3h-1 and 2100 m3h-1, respectively. In each loop the gas flow rate is determined by measuring the pressure drop of the flow through a laminar flow element (FCO96-2000L and 10000L, Furness Controls Ltd., UK) with the help of a differential pressure transmitter (FCO318, Furness Controls Ltd., UK). The flow rate is then maintained by a PID controller (T16/P16, Red Lion Controls Inc., USA) acting on a frequency converter (Ruvatronic RT5, KEB GmbH, Germany) that regulates the pump rotational speed. Two homemade bypass valves are installed nearby the pumps in parallel to the flow recirculation lines for coarse adjustment of the flow rates. Also, the valves allow determining the optimal working point of the roots pumps for fine adjustment of the flow rates by the PID controller, as well as keeping a pressure balance condition between the inlet and the outlet of the pumps. The pressure in the facility is monitored by a pressure transmitter (Baratron 626B with display unit PR400B, MKS Instruments GmbH, Germany). A muffler and a water cooling unit are installed downstream of the roots pump in the sheath gas loop to reduce vibrations and noise and to cool down the sheath gas to room temperature. The particle laden gas flows are cleaned upstream and downstream of the pumps by using HEPA filters (MFCA H13, TROX Technik GmbH, Germany). The BigMAG facility is vacuum tight. All connections between the pipes and with the equipment and the instrumentation are sealed by means of standard vacuum flanges (ISO K 63, 100 and 160, Trinos Vacuum Systems Inc., USA). 3 N2 sheath gas loop aerosol loop MFC SMPS HF VV RP LFE aerosol f low control DMA BPV BV FC BV VV HF DPT PID RP BPV FC PID muf f ler HV sheath gas f low control CV water f low control cooling unit DPT aerosol generator HF capacitor charger PID HV PT TC VV LFE HF SMPS BV BPV CV VV TC PT Ball valve Bypass valve Control valve Vacuum valve Thermocouple Pressure transducer DPT Dif f erential pressure transmitter LFE Laminar f low element MFC Mass f low controller RP Roots pump FC Frequency converter PID Proportional-integral-derivative controller HV High voltage supply DMA Dif f erential mobility analyzer SMPS Scanning mobility particle sizer HF HEPA f ilter FIG. S1 Layout of the BigMAG facility with the aerosol and sheath gas recirculation loops. 4 Analytical Work The particle number mobility distribution dN/dZ of an aerosol is derived from the particle number size distribution dN/d(log dp) measured by the SMPS as follows d(log d ) 1 p dN dN dZ ln 10 Z d(log Z) d(log d ) p . [S1] To evaluate the term d(log dp)/d(log Z), the relationship between the mobility Z and the diameter dp for singly charged spheres is recalled d p C(d ) p Z ; [S2] with K = e/(3πµ) = 9.28x10-3, Z (cm2.V-1.s-1) and dp (nm); e is the elementary charge (1.6021x10-19 C); µ is the gas viscosity (1.83x10-5 Pas for air at 23 ºC and 1 bar). The Cunningham slip factor C(dp) is given by C (d ) (1 Kn) 1.142 0.558 exp 0.999 Kn ; where Kn is the particle Knudsen number p Kn 2 λ d p , and λ is the gas mean free path (67.3 nm for air at 23 ºC and 1 bar). Then, log dp is expressed as log d p log Κ log Z log C(d p ) and, for nanoparticles, this expression is fairly well matched by a linear function y=a+bx with coefficients a = 0.13739 and b = -0.5183. Hereinafter, the following relationship between the particle diameter dp and the particle mobility Z is used d 10 a Z b p . [S3] The exact expression Eq. [S2] and the approximate expression Eq. [S3] are compared to each other in Fig. S2. Therefore, d(logdp)/d(logZ)=b and by substituting this and the particle number size distribution dN/d(log dp) given by the SMPS in Eq. [S1], the particle number mobility distribution dN/dZ of the polydisperse aerosol is finally obtained, which is well fitted by a log-normal function. 5 FIG. S2 Relationship between diameter dp and electrical mobility Z for spheres (solid line) and approximate expression (dashed line). The transfer function of the ideal DMA operating with balanced flow has a triangular form and is given by the expression (Knutson and Whitby, 1975) Z Z* 1 1 Z Z* Ω(Z, Z* ) max 0, min 1, , ; [S4] where Z* is the central mobility of the particles classified by the DMA and is the aerosol to sheath flow ratio (q/Q). The log-normal particle number mobility distribution dN/dZ of a polydisperse aerosol calculated by using Eq. [S1] and the transfer function of an ideal DMA given by Eq. [S4] are plotted in Fig. S3a. It is assumed that the voltage applied to the DMA matches the voltage required to classify particles of a mobility Z* equal to the point of maximum (mode) of the log-normal function, Z* = 1.223x10-2 cm2.V-1.s-1, and that the DMA operates with = 0.5. The particle number mobility distribution dN/dZ of the particles selected by the DMA is calculated as the product of the two functions in Fig. S3a, with the result shown in Fig. S3b. A Gaussian function with a central mobility Zc of 1.24x10-2 cm2.V-1.s-1 and a relative full width at half height FWHH/Zc of 0.5 fits closely the calculated particle number mobility distribution, consistently with the values of Z* and of the transfer function of the DMA. 6 a) b) FIG. S3 a) Log-normal particle number mobility distribution (solid line) of a polydisperse aerosol and transfer function of an ideal DMA operating with balanced flow and a sheath to aerosol flow ratio of 2 (dashed line). b) Calculated number mobility distribution (solid line) of the particles classified by the DMA and Gaussian fit (dashed line). Then, the particle number size distribution dN/ddp of the particles selected by the DMA can be derived from dN/dZ and Eq. [S3], as follows dN 1 Z dN dd b d dZ p p 7 . [S5] By replacing dN/dZ by the Gaussian fit in Fig. S3b, dN/ddp is obtained, as displayed in Fig. S4. A log-normal function with a geometric mean diameter dg of 13.32 nm and a geometric standard deviation g of 1.10 matches well the calculated particle number size distribution of the aerosol leaving the DMA. FIG. S4 Calculated particle number distribution of the aerosol selected by an ideal DMA operating with balanced flow and a sheath to aerosol flow ratio of 2 (solid line) and log-normal fit (dashed line). 8