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1. (WO2019060989) MICROFLUIDIC ASSISTED FABRICATION OF POLYMER MICROPARTICLE-METAL NANOPARTICLE COMPOSITES
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Claims:

1 . A method for preparing a polymer microparticle-metal nanoparticle composite, the method comprising:

introducing into a microfluidic device, a composition comprising:

a cationic metal nanoparticle precursor;

a polymer microparticle precursor that comprises a plurality of photopolymerizable groups; and

a photoreducer-photoinitiator; and

irradiating the composition under conditions to simultaneously reduce the cationic metal and polymerize the photopolymerizable groups to obtain the polymer microparticle-metal nanoparticle composite.

2. The method of claim 1 , wherein the composition further comprises an agent that caps and/or stabilizes the nanoparticles.

3. The method of claim 1 , wherein the polymer microparticle precursor further comprises a plurality of metal-anchoring groups.

4. The method of any one of claims 1 to 3, wherein the conditions comprise flowing the composition through a microchannel in the microfluidic device and irradiating the flowing composition through a mask defining a microparticle shape.

5. The method of any one of claims 1 to 3, wherein the conditions comprise forming droplets of the composition then irradiating the droplets.

6. The method of claim 5, wherein the microfluidics device comprises a flow-focusing junction and droplets are formed by flowing the composition as a dispersed phase and an oil solution as a continuous phase to obtain an emulsion comprising droplets of the composition in the oil solution.

7. The method of claim 6, wherein the droplets have an average diameter of from about 1 μιη to about 1 ,000 μιη.

8. The method of any one of claims 1 to 7, wherein the cationic metal nanoparticle precursor is a cationic gold nanoparticle precursor, a cationic silver nanoparticle precursor, a cationic copper nanoparticle precursor or combinations thereof.

9. The method of claim 8, wherein the cationic metal nanoparticle precursor is a cationic gold nanoparticle precursor.

10. The method of claim 9, wherein the cationic gold nanoparticle precursor is HAuCU.

1 1 . The method of any one of claims 1 to 10, wherein the cationic metal nanoparticle precursor is present in an amount of from about 0.1 % wt to about 30% wt, based on the total weight of the composition.

12. The method of any one of claims 1 to 1 1 , wherein the photopolymerizable groups are acrylate groups.

13. The method of any one of claims 3 to 12, wherein the polymer microparticle precursor is obtained from a method comprising:

reacting a monomer comprising two or more photopolymerizable groups with an anchor precursor comprising at least one metal- anchoring group and at least one group that will react with the photopolymerizable group.

14. The method of claim 13, wherein an aqueous solution of the monomer is reacted with an aqueous solution of the anchor precursor.

15. The method of claim 13 or 14, wherein the at least one metal- anchoring group and the at least one group that will react with the photopolymerizable group are the same and the anchor precursor is a bi-functional thiol, bi-functional primary amine or bi-functional silane.

16. The method of claim 15, wherein the anchor precursor is dithiothreitol.

17. The method of any one of claims 13 to 16, wherein the monomer further comprises an oligomeric poly(ethylene glycol).

18. The method of claim 17, wherein the monomer is poly(ethylene glycol)- diacrylate (PEGDA) or ethoxylated trimethylolpropane triacrylate (ETPTA).

19. The method of claim 18, wherein the monomer is PEGDA.

20. The method of any one of claims 13 to 19, wherein the molar ratio of the monomer to the anchor precursor is from about 10: 1 to about 1 :1 .

21 . The method of claim 20, wherein the molar ratio is about 10: 1 .

22. The method of any one of claims 1 to 21 , wherein the photoreducer- photoinitiator is 2-hydroxy-2-methyl-1 -phenyl-propan-1 -one or 2- hydroxy-4'-(2-hydroxyethoxy)-2-methylpropiophenone.

23. The method of any one of claims 1 to 22, wherein the composition is irradiated for a time of from about 1 second to about 15 seconds.

24. The method of any one of claims 1 to 23, further comprising functionalizing the surface of the polymer microparticle-metal nanoparticle with an analyte-binding biomolecule.

25. The method of claim 24, wherein the analyte-binding biomolecule is a DNA probe, an antibody or an aptamer.

26. The method of any one of claims 1 to 23, wherein the composition further comprises a plurality of polymerase chain reaction (PCR) primers.

27. A polymer microparticle-metal nanoparticle composite prepared by a method as defined in any one of claims 1 to 23.

28. A surface-functionalized polymer microparticle-metal nanoparticle composite prepared by a method as defined in claim 24 or claim 25.

29. A polymer microparticle-metal nanoparticle composite prepared by a method as defined in claim 26.

30. A polymer microparticle-metal nanoparticle composite comprising a uniform distribution of metal nanoparticles embedded in a polymeric resin microparticle, the polymeric resin comprising a plurality of metal- anchoring groups, the metal anchoring groups anchored to the nanoparticles.

31 . The composite of claim 30, wherein the composite has an average diameter of from about 1 μιη to about 100 μιη.

32. The composite of claim 30 or 31 , wherein the metal nanoparticles are gold nanoparticles, silver nanoparticles, copper nanoparticles or nanoparticles comprising a combination of two or more of gold, silver and copper.

33. The composite of claim 32, wherein the metal nanoparticles are gold nanoparticles.

34. The composite of any one of claims 30 to 33, wherein the metal nanoparticles are present in an amount of from about 0.1 % wt to about 30% wt, based on the total weight of the composite.

35. The composite of any one of claims 30 to 34, wherein the polymeric resin is an acrylate resin.

36. The composite of any one of claims 30 to 35, wherein the metal- anchoring groups are derived from bi-functional thiols, bi-functional primary amines or bi-functional silanes.

37. The composite of claim 36, wherein the metal anchoring groups are derived from dithiothreitol.

38. The composite of any one of claims 30 to 37, wherein the polymeric resin further comprises an oligomeric poly(ethylene glycol).

39. The composite of claim 38, wherein the polymeric resin is a poly(ethylene glycol)-diacrylate (PEGDA) resin or an ethoxylated trimethylolpropane triacrylate (ETPTA) resin.

40. The composite of claim 39, wherein the polymeric resin is a PEGDA resin.

41 . The composite of any one of claims 30 to 40, wherein the molar ratio of the monomers comprised in the polymeric resin to the metal anchoring groups is from about 10: 1 to about 1 : 1 .

42. The composite of claim 41 , wherein the molar ratio is about 10: 1 .

43. The composite of any one of claims 30 to 42, further comprising a plurality of analyte-binding biomolecules linked to the surface of the composite.

44. The composite of claim 43, wherein the analyte-binding molecules are DNA probes, antibodies or aptamers.

45. The composite of any one of claims 30 to 44, further comprising a plurality of PCR primers embedded in the polymer resin.

46. A drug delivery system comprising the polymer microparticle-metal nanoparticle composite as defined in any one of claims 27, 28 and 30- 44.

47. The drug delivery system of claim 46, further comprising an anti-cancer drug.

48. A use of the drug delivery system as defined in claim 46 or claim 47 for treating cancer in a subject in need thereof.

49. A colorimetric method for detecting the presence of an analyte in a liquid sample, the method comprising:

exposing a composite as defined in any one of claims 28, 43 and 44 comprising an analyte binding biomolecule that binds the analyte, to the sample under conditions for the analyte-binding molecule to bind the analyte; and

colorimetrically analyzing the sample after exposure to the composite to determine if the analyte was present in the sample.

50. The method of claim 49, wherein the composite is contacted with the sample in the form of a dipstick.

51 . A use of a microparticle-metal nanoparticle composite as defined in any one of claims 27, 29-42 and 45 as a plasmonic bead heater in a chamber for carrying out a polymerase chain reaction (PCR).

A use of a microparticle-metal nanoparticle composite as defined claim 29 or claim 45 as a site for a polymerase chain reaction (PCR).