COUNTER TECHNOLOGY

37 C.F.R. § 1.71(e) AUTHORIZATION A portion of the disclosure of this patent document contains material which is subject to copyright protection. The copyright owner has no objection to the facsimile reproduction by anyone of the patent document or the patent disclosure, as it appears in the US Patent and Trademark Office patent file or records, but otherwise reserves all copyright rights whatsoever.

CROSS-REFERENCE TO RELATED APPLICATIONS, IF ANY

This application claims the benefit under 35 U.S.C. §119(e) of co-pending US Provisional Patent Application Serial No. 62/311,997, filed March 23, 2016, which is hereby incorporated by reference.

STATEMENT REGARDING FEDERALLY SPONSORED

RESEARCH OR DEVELOPMENT

Not applicable. REFERENCE TO A MICROFICHE APPENDIX, IF ANY

Not applicable.

BACKGROUND OF THE INVENTION

1. Field of the Invention.

The present invention relates, generally, to analysis methods and apparatus for analyzing material. Particularly, the invention relates to methods and apparatus for modifying properties of particles suspended in a gas. Most particularly, the invention relates to methods and apparatus for modifying particle properties within a gas by exposing the particles to a vapor of known composition and concentration. The technology is useful, for example, for aerosol

characterization, aerosol collection, and particle detection.

2. Background Information.

Existing technology in this field is believed to have significant limitations and shortcomings. For example, systems used to modify particle properties by vapor exposure require long sample paths (for cylindrical conduits) or

cumbersome flow geometry (for rectangular conduits). The additional length and flow geometries increase the response time of these devices as well as increase particle deposition to the walls of the flow conduit.

A summary of the state of the art is provided by Peter H. McMurry (2000) The History of Condensation Nucleus Counters, Aerosol Science and Technology, 33:4, 297-322, DOI: 10.1080/02786820050121512, which is incorporated by reference.

All US patents and patent applications, and all other published documents mentioned anywhere in this application are incorporated by reference in their entirety.

BRIEF SUMMARY OF THE INVENTION

The present invention provides particle- vapor reactor (PVR) apparatus which is practical, reliable, accurate and efficient, and which are believed to constitute an improvement over the background technology.

The invention relates to an apparatus where the aerosol is introduced to the device using a cylindrical conduit that transitions to a rectangular conduit in a manner that limits flow separation. In one embodiment, the properties of the conduit walls differ than that of the aerosol for the purpose of modifying the gas properties within the aerosol. The sample aerosol occupies the entire cross section of the conduit or is sheathed by a gas having different properties than the aerosol. The aerosol sample exits the device from a rectangular conduit or the sample is transitioned to a cylindrical conduit. In one embodiment, the conduit is fabricated from porous material, a sintered polymer or metal, or using composite porous aluminum (such as METAPOR™). The invention also relates to a device where the number concentration (partial pressure) of a vapor is modified within an aerosol.

In one aspect, the invention relates to a PVR where the partial pressure of a vapor is greater than the partial pressure of that vapor over a flat surface composed the vapor's condensed phase (Supersaturation). For particles larger than a critical diameter, the vapor molecules condense onto the particles resulting in an increase of the particle diameter by orders of magnitude. The enlarged droplet/particle entities are easily detected using common light scattering methods and with knowledge of the counting rate and aerosol flow, a particle concentration can be calculated. At sufficiently high supersaturation levels, the condensation process will initiate for particles which are too small to be detected using optical methods typically employed for single aerosol particle counting. In this aspect, supersaturation is achieved via diabatic heat and mass transfer which is known within literature, for example by Susanne V. Hering & Mark R. Stolzenburg (2005), A Method for Particle Size Amplification by Water Condensation in a Laminar, Thermally Diffusive Flow, Aerosol Science and Technology, 39:5, 428- 436, DOI: 10.1080/027868290953416, which is incorporated by reference. In another aspect, the invention relates to a PVR where the partial pressure of a vapor is less than the partial pressure of that vapor over a flat surface composed the vapor's condensed phase (Subsaturation). This device can be used to raise or lower the vapor pressure within an aerosol to study sorption related phenomena and or chemical reactions between particles and vapor molecules.

Further aspects of the invention include:

A. A particle vapor reactor including a reactor body with a fluid flow conduit having an inlet end and an outlet end, the crossection of the conduit having a circular geometry at the inlet end, a rectangular geometry at its midsection, and a

circular geometry at its outlet end.

B. The reactor of aspect A, wherein the geometry transition at the inlet end from circular to rectangular

minimizes flow separation.

C. The reactor of aspect B, wherein the geometry at the inlet end transitions from circular to obround, and wherein the geometry at the outlet end transitions from obround to circular. D. The reactor of aspect C, wherein the dimensions of the obround section of the fluid flow conduit reduce residence time of fluid flowing within the fluid flow conduit for a given vapor concentration.

E. The reactor of claim C, wherein the transition from obround to circular at the outlet end minimizes loss of vapor droplets due to inertia.

F. The reactor of aspect A, wherein an aerosol sample stream is input at the inlet end of the reactor body.

G. The reactor of aspect F, wherein the reactor changes the temperature and vapor concentration of a material within the aerosol sample flowing in the fluid flow conduit.

H. The reactor of aspect F, wherein the fluid flow in the conduit is laminar.

I. The reactor of aspect F, wherein the vapor concentration is changed towards the vapor concentration at the body wall of the conduit. J. The reactor of aspect F, wherein the vapor concentration is increased via diffusion of vapor supplied from a liquid surface at the body wall of the conduit.

K. The reactor of aspect F, wherein the vapor concentration is decreased via diffusion of vapor to a liquid surface at the body wall of the conduit.

L. The reactor of aspect F, wherein the vapor concentration at the conduit body wall is defined by the temperature of the conduit body wall.

M. The reactor of aspect F, wherein the temperature of the aerosol sample flow is modified towards the temperature at the conduit body wall.

N. The reactor of aspect M, wherein the temperature of the aerosol sample flow is increased via diffusion of thermal energy from the conduit body wall.

O. The reactor of aspect M, wherein the temperature of the aerosol sample flow is decreased via diffusion of thermal energy to the conduit body wall. P. The reactor of aspect F, wherein the vapor concentration within the aerosol sample is controlled to reach a predetermined, set value.

Q. The reactor of aspect P, wherein the predetermined vapor concentration of the aerosol sample flow is equivalent to the saturation vapor pressure defined by the conduit body wall temperature.

R. The reactor of aspect P, wherein the predetermined vapor concentration is not equivalent to the saturation vapor pressure defined by the conduit body wall temperature.

S. The reactor of aspect F, wherein the vapor concentration within the aerosol sample stream reaches a level above the saturation vapor pressure calculated using the aerosol sample stream temperature.

T. The reactor of aspect F, wherein a gas is coaxially input to the perimeter of the aerosol sample stream as a sheathing flow at the inlet end of the reactor body. U. The reactor of aspect T wherein the vapor concentration in the sheathing flow gas is a predetermined, fixed value.

V. The reactor of aspect T, wherein the temperature of the sheathing flow gas is a predetermined, fixed value.

W. The reactor of aspect A, wherein the fluid flow conduit has a saturator section disposed towards the inlet end and a condenser section disposed towards the outlet end.

X. The reactor of aspect W, wherein the conduit is elongated and constructed of two lateral half portions, the lateral half portions being joined along the longitudinal axis of the reactor.

Y. The reactor of claim W, wherein the conduit is elongated and constructed of four quarter portions, the quarter portions being connected into two lateral half portions, which lateral half portions are then joined along the longitudinal axis of the reactor, the quarter portions of each longitudinal half portion further being separated from each other by a thermally and electrically insulative separator member. Z. The reactor of aspect A, being communicatively coupled to a condensation particle counter comprising an aerosol sample inlet communicatively connected to the reactor inlet end, a fluid supply section communicatively connected to the reactor inlet end, a heating section communicatively connected to the exterior of the reactor body, and a detection section communicatively connected to the reactor conduit outlet end.

The present invention is believed to involve novel elements, combined in novel ways to yield more than predictable results. The problems solved by the invention were not fully recognized in the prior art.

The aspects, features, advantages, benefits and objects of the invention will become clear to those skilled in the art by reference to the following description, claims and drawings.

BRIEF DESCRIPTION OF THE SEVERAL VIEWS OF THE DRAWING

Figure 1 shows a Condensation Particle Counter (CPC). Figure 2 is a crossectional view of a first embodiment of the Condensation Particle Counter (CPC) of the present invention, including an embodiment of a Particle Vapor Reactor (PVR) used therein in a wide aspect. Figure 3 is a further crossectional view of the CPC, taken at plane which is perpendicular to the plane shown in Figure 1, showing a narrow aspect of the PVR.

Figure 4 is a perspective view of a portion of one embodiment of Particle Vapor Reactor body (PVR).

Figure 5 is an elevation view of the PVR body element of Figure 4.

Figure 6 is a crossectional view of the PVR body element taken along line 6-6 of Figure 5.

Figure 7 is an partial sectional view (the lower end portion) of an alternative embodiment of the PVR wherein the vapor is unsheathed. Figure 8 is perspective view of a second embodiment of the CPC of the invention, partially in section to show a PVR thereof. Figure 9 is sectional view of the CPC of Figure 8 showing a wide- wide aspect of the CPC, but a narrow aspect of the PVR.

Figure 10 is another sectional view of the CPC, at a plane perpendicular to that of Figure 8, showing a narrow-narrow aspect of the CPC and a wide aspect of the PVR.

Figurel 1 is an partial sectional view (the lower end portion) of an alternative embodiment of the PVR of Figures 8-10, wherein the vapor is unsheathed.

Figure 12 is a top end view of the PVR of Figures 8-11.

Figure 13 is a perspective view of one half (longitudinal half) of the PVR body.

Figure 14 is an elevation view of the PVR body portion of Figure 13.

Figure 15 is a crossectional view of the PVR portion taken along line 15- 15 of Figure 14.

Figure 16 is a perspective view of the bottom body portion of the longitudinal half body portion of Figure 13. Figure 17 is bottom end view of the quarter portion of Figure 16.

Figure 18 is an elevation view of the quarter portion.

Figure 19 is a crossectional view of the quarter portion taken along line 19-19 of Figure 18.

Figure 20 is a perspective view of the top portion of the longitudinal half portion of Figure 13.

Figure 21 is top end view of the quarter portion of Figure 20.

Figure 22 is an elevation view of the quarter portion.

Figure 23 is a crossectional view of the quarter portion taken along line 23-23 of Figure 22.

Figure 24 shows the saturation ratio within a sheathed PVR fluid section.

Figures 25 and 26 illustrate the flow within a sheathed device. Figure 27 is a graph showing a plot of temperature and vapor pressure as a function of axial position for an obround (PP) versus circular (Circ) saturator crossection.

Figure 28 is a graph showing a plot of temperature and vapor pressure as a function of axial position for the condenser section.

Figures 29 and 30 illustrate the computational fluid mechanics results for the saturation ratio within a sheathed PVR fluid section.

Figure 31 and 32 illustrate computational fluid mechanics results for vapor pressure within a sheathed device.

Figure 33 shows path lines of aerosol flow within a sheathed device.

Figure 34 is a photograph of a longitudinal half portion of another embodiment of the Particle Vapor Reactor (PVR) body of the invention constructed of one piece, instead of quarter portions, and including a continuous wick section. DETAILED DESCRIPTION

Figure 1 shows a Condensation Particle Counter (CPC) 10 including a saturator 12 with a sample input end 14, a condenser 16, and an optical detector 18. A fill pump 20 is connected to the saturator 12. A fluid supply 22 (containing for example Butanol) is connected to the fill pump 20 and also communicatively to a drain pump 24. The drain pump 24 is also connected to the saturator 12. A sheath pump 26 is connected to the input end 14 and to a filter 28. A transport pump 30 is connected to the optical detector 18. A high/low flow valve 32 is communicatively connected to the optical detector 18, transport pump 30, input end 14 and sheath pump 26.

Figures 2 and 3 show a first embodiment of the Condensation Particle Counter (CPC) 40 of the invention. The CPC 40 includes a Particle- Vapor Reactor (PVR) 42, an aerosol inlet 44, a fluid supply section 46, a heating section 48, and an optical detection section 50. In this embodiment, the CPC 40 includes sample sheathing functionality. The fluid supply section 46 includes a liquid supply 60, a sheath inlet 62, a transport outlet 64, and a vent 66. The PVR 42 amplifies the size of Nano-particles for optical detection in section 50. Referring also to Figures 4-6, in this embodiment of the invention, the PVR 42 has an elongated body of a predetermined length. The body wall defines an inner, longitudinally oriented fluid flow conduit or lumen which extends from an input end (shown disposed at the lower or bottom end in the drawings) and an outlet end (shown disposed at the upper or top end in the drawings). The PVR 42 conduit has a conditioner or saturator section 70 and a growth or condenser section 72. The sections 70 and 72 are separated in this embodiment of the PVR 42 by a separator 74. The separator 74 thermally and electrically insulates the conditioner and growth sections 70 and 72 from each other. Further, each section 70 and 72 are preferably constructed of separate but connected lateral members 70 A/B and 72 A/B.

In the CPC 40, aerosol is introduced into the conditioner section 70 of the PVR 42 using a cylindrical conduit geometry 74 that transitions to a rectangular conduit geometry 76 (as best shown in Figures 4 and 5) in a manner that limits flow separation. The properties of the conduit walls differ than that of the aerosol for the purpose of modifying the gas properties within the aerosol. The conduit members 70A/B and 72A/B is preferably fabricated from porous material such as sintered polymer or metal, or using composite porous aluminum (Metapor™). The sample aerosol is preferably sheathed by a gas having different properties than the aerosol. The aerosol sample exits the growth section 72 of the device 42 by transitioning from a rectangular conduit to a cylindrical conduit. In this embodiment, the number concentration (partial pressure) of a vapor is modified within an aerosol.

Although the aerosol is disclosed as being sheathed in this embodiment, it is within the purview of the invention may be unsheathed, and occupy the entire crossection of the conduit. An example of a CPC operating unsheathed is shown in Figure 7. Further, although the aerosol transitions from a rectangular geometry to a circular geometry upon exit, it is within the purview of the invention that it may exit at a rectangular geometry.

In one mode of use, the partial pressure of a vapor is greater than the partial pressure of that vapor over a flat surface composed the vapor's condensed phase (Supersaturation). For particles larger than a critical diameter, the vapor molecules condense onto the particles resulting in an increase of the particle diameter by orders of magnitude. The enlarged droplet/particle entities are easily detected using common light scattering methods via the detector section 50. And, with for a given counting rate and aerosol flow rate, a particle concentration is calculated. At sufficiently high supersaturation levels, the condensation process will initiate for particles which are too small to be detected using optical methods typically employed for single aerosol particle counting. In this embodiment, supersaturation is achieved via known diabatic heat and mass transfer processes. In another mode of use, the partial pressure of a vapor is less than the partial pressure of that vapor over a flat surface composed the vapor's condensed phase (Subsaturation). This embodiment of the particle-vapor reactor can be used to raise or lower the vapor pressure within an aerosol to study sorption related phenomena and or chemical reactions between particles and vapor molecules.

Figure 7 shows a modification to the bottom end of the CPC 40, forming an alternative embodiment , CPC 80, whereby the CPC 80 operates in an unsheathed mode.

Figure 34 is a photograph of an alternative embodiment of the PVR 90 including one half of a continuous wick section, wherein the conditioning and growth sections are unitary. This longitudinally unitary embodiment of the PVR 90 is preferably machined from porous aluminum, for example METAPOR™ porous aluminum.

Figures 24—26 show computational fluid mechanics results for the CPC and PVR of Figures 1-6. Figure 24 shows the saturation ratio within a sheathed PVR fluid section. In this model, the sheath and aerosol flows are each 300 cmVmin. Figures 25-26 show path lines of the aerosol flow within the sheathed device. A second embodiment of the CPC 100 is shown in Figures 8-10. The CPC 100 includes a PVR 102, an aerosol inlet 104, a fluid supply section 106, a heating section 108, and an optical detection section 110. In this embodiment, the CPC 100 includes sample sheathing functionality. The fluid supply section 106 preferably includes liquid supply, a sheath inlet, a transport outlet and a vent ingress/egress means. Such means may be associated with pumps. The PVR 102 functions include amplifying the size of Nano-particles for optical detection in section 110. Referring also to Figures 12-15, in this embodiment of the invention, the

PVR 102 also has an elongated body of a predetermined length. The body wall defines an inner, longitudinally oriented fluid flow conduit which extends from an input end (shown disposed at the lower or bottom end in the drawings) and an outlet end (shown disposed at the upper or top end in the drawings). The PVR 102 conduit has a saturator or saturation section 120 and a 1 lOcondensor section 122. The sections 120 and 122 are separated laterally in this embodiment of the PVR by a separator 124. The separator 124 thermally and electrically insulates the conditioner and growth sections 120 and 122 from each other. Further, each section 120 and 122 is preferably constructed of separate but connected lateral members 120 A/B and 122 A/B divided along their longitudinal axis.

The CPC 100 and PVR 102 function as follows. An analyte is continuously aspirated into a cylindrical conduit AI where a portion of the analyte near the conduit walls acting as a transport flow is axisymmetrically aspirated from the conduit at ST. The remaining analyte passes through a sample conduit at SC. The transport flow is filtered to remove particles and a prescribed volumetric rate is axisymmetrically reintroduced around the sample conduit as a sheath flow at SM. The sheath flowrate is nominally equivalent to the transport flowrate. Optionally, a flow valve (for example, a flow rate valve 32 as shown in Figure 1) may used to optionally operate the system 100 at a transport flowrate above the sheath flowrate. The sheathed sample exits a cylindrical conduit at SS and enters the saturator section 120 a region at TR where the cross section of the conduit transitions from circular to obround. Starting at this transition, the conduit is fabricated from a material that supplies a liquid film at the wall surface such as a porous metal, felt, membrane, or porous plastic WI and Wll. The liquid is preferably provided by a push/pull pumping system where a communicatively connected liquid supply pump (not shown) injects liquid from a supply bottle or the like (not shown) to the base of the porous section at BI and a

communicatively connected drain pump (not shown) removes the liquid at BE and returns it to the supply bottle. The drain rate is greater than the supply rate which ensures that a minimal volume of liquid is present in the system. Liquid is also confirmed by monitoring the increased conductivity between Fl and the outer metal surface of the porous conduit when liquid is present. The liquid at the surface maintains a saturated vapor pressure that diffuses into the sheathed sample flow while simultaneously the temperature of the flow is modulated to the wall temperature. The wall temperature is controlled using heaters 108 installed at HI and H2. The saturator section 120 is sufficiently long so that the vapor pressure and temperature of sheathed sample flow reach design conditions. For the device described herein the design conditions are a Log Mean Temperature Difference (LMTD) <1 % and a Saturation Ratio (S = Vapor pressure / Saturated Vapor Pressure) > 0.9.

Following the saturator section, the sheathed sample enters the condenser section 122 where the conduit walls are maintained at a prescribed temperature.

The saturator and condenser conduits are separated by a short conduit fabricated from a thermally insulating and static dissipative material at SP. As the sheathed sample traverses the condenser section 122 the temperature and vapor pressure of the flow modulates to the match the wall conditions. The wall temperature in the condenser section 122 is controlled using thermoelectrics devices installed at Tl and T2. Supersaturation is achieved by exploiting the Lewis number (Le) for the system (Le = ratio of thermal diffusivity to vapor diffusivity). For systems where Le > 1 the condenser walls are held at a lower temperature than the bulk temperature of the flow. This results in the temperature of the flow decreasing at a faster rate than the vapor pressure. The resulting ratio of the actual vapor pressure to the saturated vapor pressure calculated from the gas temperature is referred to as the Saturation ratio (S). The supersaturated vapor will then condense onto sufficiently large particles within the sheathed sample flow. The system is designed such that following supersaturation, the total condensed vapor onto the particles is controlled by reducing the residence time of the particles in this region. Controlling the amount of condensed vapor will reduce modulation of the temperature and vapor pressure caused by high particle concentrations.

Near the exit of the condenser section 122 the conduit transitions from an obround to circular shape at TE. The transition back to cylindrical flow at SE is done to facilitate focusing the sample stream at nozzle Nl. The flow then enters an optical detection device OP where the sample passes through a region with incident electromagnetic radiation that is scattered by the presence of a sufficiently large object (in this case, a particle with condensed vapor). The scattered radiation is detected by a sensor and is registered as a detected particle by the device.

Figures 16-23 shows detailed drawings of the porous sections 120 A and B, and 122 A and B. For the device described herein the condenser 122 conduit is fabricated using a porous metal (Metapor™). In the saturator section 120 a porous plastic sheet (Fritware from SP Scienceware) Wll is inserted into the porous metal housing to provide a higher pore density for supplying liquid at the surface. The angles of the transition regions are designed so that flow separation does not occur. Figure 27 is a graph shows a plot of the temperature and vapor pressure as a function of axial position for an obround (PP) versus circular (Circ) saturator cross section. For the comparisons in Figure 27, the conduit velocity was fixed at 1 m/s, sheathed sample flowrate was set a 10 cnrVsec and the aspect ratio

(obround width to height) was set to 10. The plots clearly show the advantage gained in the shorter overall length in the obround device for equivalent plug flow velocities. For the device described herein, the saturator section is designed so that the flow reaches a bulk mean saturation ratio of 0.9 with the center of the flow being below the mean and the flow near the walls being above it. The purpose of this is to provide a uniform peak supersaturation across the flow conduit which facilitates a sharper detection cutoff as a function of size. This practice also applies for the circular conduit.

Figure 28 is a graph showing a plot of the temperature and vapor pressure as a function of axial position for the condenser section

Figures 29 and 30 show computational fluid mechanics results (contours of saturation ratio S) for the saturation ratio within a sheathed PVR fluid section. In this model, the sheath and aerosol flows are each 300 cmVmin.

Figures 31-32 shows computational fluid mechanics results (contours of vapor pressure in Pa) for the vapor pressure. Figure 33 shows path lines of the aerosol flow within the sheathed device.

Figure 11 shows a modification to the bottom end of the CPC 100, fonning an alternative embodiment of the CPC 200, whereby the CPC 200 operates in an unsheathed mode.

The embodiments above are chosen, described and illustrated so that persons skilled in the art will be able to understand the invention and the manner and process of making and using it. The descriptions and the accompanying drawings should be interpreted in the illustrative and not the exhaustive or limited sense. The invention is not intended to be limited to the exact forms disclosed. While the application attempts to disclose all of the embodiments of the invention that are reasonably foreseeable, there may be unforeseeable insubstantial modifications that remain as equivalents. It should be understood by persons skilled in the art that there may be other embodiments than those disclosed which fall within the scope of the invention as defined by the claims. Where a claim, if any, is expressed as a means or step for performing a specified function it is intended that such claim be construed to cover the corresponding structure, material, or acts described in the specification and equivalents thereof, including both structural equivalents and equivalent structures, material-based equivalents and equivalent materials, and act-based equivalents and equivalent acts.