Chemical processing microsystems comprising high-temperature parallel flow microreactors

Abstract

A chemical processing microsystem useful for identifying and optimizing materials (e.g., catalysts) that enhance chemical processes or for characterizing and/or optimizing chemical processes is disclosed. The chemical processing microsystem comprises a plurality of microreactors 600 and, in a preferred embodiment, a plurality of microseparators 900 integral with the chemical processing microsystem 10. The microreactors 600 are preferably diffusion-mixed microreactors formed in a plurality of laminae that include a modular, interchangeable candidate-material array 100. The material array 100 comprises a plurality of different candidate materials (e.g., catalysts), preferably arranged at separate, individually addressable portions of a substrate (e.g., wafer). The microseparators 900 are similarly formed in a plurality of laminae that include a modular, interchangeable adsorbent array 700. The adsorbent array 700 comprises one or more adsorbents, preferably arranged at separate, individually addressable portions of a substrate to spatially correspond to the plurality of different candidate materials. Modular microfluidic distribution systems are also disclosed. The chemical processing microsystem can be integrated into a material evaluation system that enables a comprehensive combinatorial material science research program.

1 - 185 . (canceled)  
     
     
         186 . A chemical processing microsystem comprising a parallel flow microreactor for evaluating catalyzed reactions, the parallel microreactor comprising 
 a microreactor structure comprising four or more microreactors formed in a plurality of adjacent laminae, each of the four or more microreactors comprising a surface defining a reaction cavity for carrying out a chemical reaction of interest, an inlet port in fluid communication with the reaction cavity, and an outlet port in fluid communication with the reaction cavity,    a fluid distribution system for simultaneously supplying one or more reactants from one or more reactant sources to the inlet port of each of the four or more microreactors through a microfluidic fluid-supply manifold, and for simultaneously discharging a reactor effluent from the outlet port of each of the four or more microreactors to one or more effluent sinks, and    a temperature control device effective for controlling the temperature of the reaction cavity to be above 100° C. during the chemical reaction of interest,    at least one of the plurality of laminae being adaptable for use as a material-containing laminate that forms a portion of the cavity-defining surface of the four or more microreactors, the material-containing laminate comprising a substrate for containing at least four catalyst materials arranged on the substrate such that they are individually resident in the reaction cavities of the four or more microreactors, the four or more microreactors being accessible for loading the material-containing laminate prior to carrying out the chemical reaction of interest, and for unloading the material-containing laminate after the chemical reaction of interest.    
     
     
         187 . The microsystem of  claim 186  further comprising a releasable seal between the material-containing laminate and one or more adjacent laminae in which the microreactors are formed.  
     
     
         188 . The microsystem of  claim 187  wherein the releasable seal is a gasket.  
     
     
         189 . The microsystem of  claim 187  wherein the releasable seal is a graphite gasket.  
     
     
         190 . The microsystem of claims  186  wherein the microfluidic fluid-supply manifold is formed in a plurality of adjacent laminae.  
     
     
         191 . The microsystem of  claim 186  wherein the microfluidic fluid-supply manifold is formed in a plurality of adjacent laminae comprising at least one laminate separate from the plurality of adjacent laminae in which the microreactors are formed.  
     
     
         192 . The microsystem of  claim 186  wherein the microfluidic fluid-supply manifold comprises a common port adaptable for fluid communication with one or more reactant sources, four or more terminal ports adapted for fluid delivery to the four or more microreactors, and a distribution channel providing fluid communication between the common port and each of the four or more terminal ports, the flow paths defined between the common port and each microreactors having equal conductance.  
     
     
         193 . The microsystem of  claim 186  wherein the microfluidic fluid-supply manifold comprises a common port adaptable for fluid communication with one or more reactant sources, four or more terminal ports adapted for fluid delivery to the four or more microreactors, and a distribution channel providing fluid communication between the common port and each of the four or more terminal ports, the distribution channels being adapted such that the pressure drop in each of the fluid distribution channels is larger than the pressure drop in its associated microreactor.  
     
     
         194 . The microsystem of  claim 186  wherein the fluid distribution system discharges the reactor effluent from the outlet port of each of the four or more microreactors to one or more effluent sinks through a microfluidic effluent-distribution manifold.  
     
     
         195 . The microsystem of  claim 186  wherein the fluid distribution system discharges the reactor effluent from the outlet port of each of the four or more microreactors to one or more effluent sinks through a microfluidic effluent-distribution manifold formed in a plurality of adjacent laminae.  
     
     
         196 . The microsystem of  claim 186  wherein the microfluidic fluid-supply manifold is releasably sealed with a component of the microreactor structure, such that the manifold can be modularly interchanged with another microfluidic fluid distribution manifold.  
     
     
         197 . The microsystem of  claim 186  wherein the microsystem has an essential absence of active mixing elements.  
     
     
         198 . The microsystem of  claim 186  wherein the reactor geometry is adapted so that the microreactors are diffusion-mixed microreactors.  
     
     
         199 . The microsystem of  claim 186  wherein the reactor geometry and the inlet port geometry is adapted so that the microreactors are diffusion-mixed without substantial back-diffusion of reactants into a reactant supply manifold of the fluid distribution system.  
     
     
         200 . The microsystem of  claim 186  wherein the temperature control device is effective for controlling the temperature of the reaction cavity to be above about 200° C. during the chemical reaction of interest.  
     
     
         201 . The microsystem of  claim 186  wherein the temperature control device is effective for controlling the temperature of the reaction cavity during the chemical reaction of interest to range from about 100° C. to about 500° C.  
     
     
         202 . The microsystem of  claim 186  wherein the temperature control device is effective for controlling the temperature of the reaction cavity during the chemical reaction of interest to range from about 100° C. to about 800° C.  
     
     
         203 . The microsystem of  claim 186  wherein the fluid distribution system is effective for supplying one or more gaseous reactants through the microfluidic fluid-supply manifold.  
     
     
         204 . The microsystem of  claim 186  wherein the fluid distribution system is effective for supplying one or more gaseous reactants through the microfluidic fluid-supply manifold, and the temperature control device is effective for controlling the temperature of the reaction cavity to be above about 200° C. during the chemical reaction of interest.  
     
     
         205 . The microsystem of  claim 186  wherein the chemical processing microsystem further comprises four or more inorganic candidate catalyst materials individually resident in each of the four or more microreactors.  
     
     
         206 . The microsystem of  claim 186  wherein the reaction cavities of the four or more microreactors are isolated from each other.  
     
     
         207 . The microsystem of  claim 186  wherein the outlet port from a first reaction cavity is in fluid communication with an inlet port of a second reaction cavity.  
     
     
         208 . The microsystem of  claim 186  wherein the fluid distribution system discharges the reactor effluent from the outlet port of each of the four or more microreactors to one or more effluent sinks through a microfluidic effluent-distribution manifold, the microfluidic fluid-supply manifold and the microfluidic effluent-distribution manifold being formed in the same common plurality of laminae.  
     
     
         209 . The microsystem of  claim 186  wherein the fluid distribution system discharges the reactor effluent from the outlet port of each of the four or more microreactors through a microfluidic effluent-distribution manifold, the reactor effluent streams being discharged from the four or more reactor outlet ports as four or more independent streams.  
     
     
         210 . The microsystem of  claim 186  wherein the fluid distribution system discharges the reactor effluent from the outlet port of each of the four or more microreactors to one or more effluent sinks through a microfluidic effluent-distribution manifold, the microfluidic fluid-supply manifold and the microfluidic effluent-distribution manifold being formed in the same common plurality of laminae, the reactor effluent streams being discharged from the four or more reactor outlet ports as four or more independent analytical sample streams.  
     
     
         211 . The microsystem of  claim 186  further comprising four or more parallel detectors to simultaneously analyze reaction products or unreacted reactants of each of the four or more effluent streams.  
     
     
         212 . The microsystem of  claim 186  further comprising four or more parallel detectors to simultaneously analyze reaction products or unreacted reactants of each of the four or more effluent streams, wherein the fluid distribution system discharges the reactor effluent from the outlet port of each of the four or more microreactors to one or more effluent sinks through a microfluidic effluent-distribution manifold, the microfluidic fluid-supply manifold and the microfluidic effluent-distribution manifold being formed in the same common plurality of laminae, the reactor effluent streams being discharged from the four or more reactor outlet ports as four or more independent analytical sample streams to the four or more parallel detectors.  
     
     
         213 . A chemical processing microsystem comprising a parallel flow microreactor for evaluating catalyzed reactions, the parallel microreactor comprising 
 a microreactor structure comprising four or more microreactors, each of the four or more microreactors comprising a surface defining a reaction cavity for carrying out a chemical reaction of interest, an inlet port in fluid communication with the reaction cavity, and an outlet port in fluid communication with the reaction cavity,    a microfluidic fluid distribution system for simultaneously supplying one or more reactants from one or more reactant sources to the inlet port of each of the four or more microreactors through a microfluidic fluid-supply manifold, and for simultaneously discharging a reactor effluent from the outlet port of each of the four or more microreactors through a microfluidic effluent-distribution manifold, the microfluidic fluid-supply manifold and the microfluidic effluent-distribution manifold being formed in the same common plurality of laminae, the reactor effluent streams being discharged from the four or more reactor outlet ports as four or more independent effluent streams,    four or more parallel detectors in respective fluid communication with the four or more independent effluent streams, for simultaneously analyzing reaction products or unreacted reactants in each of the four or more independent effluent streams, and    a temperature control device effective for controlling the temperature of the reaction cavity to be above 100° C. during the chemical reaction of interest.    
     
     
         214 . The microsystem of  claim 213  wherein the four or more microreactors are formed in a plurality of adjacent laminae, at least one of the plurality of laminae being adaptable for use as a material-containing laminate that forms a portion of the cavity-defining surface of the four or more microreactors, the material-containing laminate comprising a substrate for containing at least four catalyst materials arranged on the substrate such that they are individually resident in the reaction cavities of the four or more microreactors, the four or more microreactors being accessible for loading the material-containing laminate prior to carrying out the chemical reaction of interest, and for unloading the material-containing laminate after the chemical reaction of interest.  
     
     
         215 . The microsystem of  claim 213  wherein the temperature control device is effective for controlling the temperature of the reaction cavity to be above about 200° C. during the chemical reaction of interest.  
     
     
         216 . The microsystem of  claim 213  wherein the temperature control device is effective for controlling the temperature of the reaction cavity during the chemical reaction of interest to range from about 100° C. to about 500° C.  
     
     
         217 . The microsystem of  claim 213  wherein the temperature control device is effective for controlling the temperature of the reaction cavity during the chemical reaction of interest to range from about 100° C. to about 800° C.  
     
     
         218 . The microsystem of  claim 213  wherein the fluid distribution system is effective for supplying one or more gaseous reactants through the microfluidic fluid-supply manifold.  
     
     
         219 . The microsystem of  claim 213  wherein the fluid distribution system is effective for supplying one or more gaseous reactants through the microfluidic fluid-supply manifold, and the temperature control device is effective for controlling the temperature of the reaction cavity to be above about 200° C. during the chemical reaction of interest.  
     
     
         220 . The microsystem of  claim 213  wherein the reaction cavities of the four or more microreactors are isolated from each other.