Preparation of core–shell structured Au@SiO2 nanocomposite catalyst with Au core size below 2 nm without high-temperature calcination procedure
Source abstract
Abstract
Preparing dispersed cores–shell structured Au@SiO2 nanocomposites with an active Au core size below 2 nm that exhibit excellent catalytic performance still remains a major challenge in catalytic synthesis. In this work, we report a novel preparation method for a one-pot system fabrication of an ultrafine core–shell structured Au@SiO2 intestine-shaped nanocomposite. The preparation is used to fabricate catalysts with an Au core size of about 1.4 nm and requires neither prefabricated Au cores nor special reducing agents. Upon extraction of cetyltrimethylammonium bromide, abundant pores with a size of around 1.9 nm are formed in the silica shell. During the catalytic reduction of 4-nitrophenol to 4-aminophenolate, the catalyst unambiguously exhibits superior catalytic activity. Despite having a low 1.7% Au content in catalyst, the nanocomposites achieve an activity of ʊ = 19.1 × 10−3 s−1 mg−1. This is due to the fact that the polyvinylpyrrolidone coating is transformed into discrete particles in an alkaline solution, which exposes large active areas on the Au.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Nanomaterials for catalytic reactions · Nanocluster Synthesis and Applications · Catalytic Processes in Materials Science
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References (39)
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1. Liz-Marzán LM, Giersig M, Mulvaney P (1996) Synthesis of nanosized gold-silica core–shell particles. Langmuir 12:4329–433510.1021/la9601871 ↗
2. Bumb A, Sarkar SK, Billington N, Brechbiel MW, Neuman KC (2013) Silica encapsulation of fluorescent nanodiamonds for colloidal stability and facile surface functionalization. J Am Chem Soc 135:7815–781810.1021/ja4016815 ↗
3. Liu N, Prall BS, Klimov VI (2006) Hybrid gold/silica/nanocrystal-quantum-dot superstructures: synthesis and analysis of semiconductor–metal interactions. J Am Chem Soc 128:15362–1536310.1021/ja0660296 ↗
4. Aioub MS, EI-Sayed MA (2016) A real-time surface enhanced raman spectroscopy study of plasmonic photothermal cell death using targeted gold nanoparticles. J Am Chem Soc 138:1258–126410.1021/jacs.5b10997 ↗
5. Shin Y, Song J, Kim D, Kang T (2015) Facile preparation of ultrasmall void metallic nanogap from self-assembled gold-silica core–shell nanoparticles monolayer via kinetic control. Adv Mater 27:4344–435010.1002/adma.201501163 ↗
6. Lee J, Park JC, Bang JU, Song H (2008) Precise tuning of porosity and surface functionality in Au@Sio2nanoreactors for high catalytic efficiency. Chem Mater 20:5839–584410.1021/cm801149w ↗
7. Guzman J, Gates BC (2004) Catalysis by supported gold: correlation between catalytic activity for CO oxidation and oxidation states of gold. J Am Chem Soc 126:2672–267310.1021/ja039426e ↗
8. Bedford NM, Hughes ZE, Tang Z, Li Y, Briggs BD, Ren Y, Swihart MT, Petkov VG, Naik RR, Knecht MR, Walsh TR (2016) Sequence-dependent structure/function relationships of catalytic peptide-enabled gold nanoparticles generated under ambient synthetic conditions. J Am Chem Soc 138:540–54810.1021/jacs.5b09529 ↗
9. Cassano D, Martir DR, Signore G, Piazza V, Voliani V (2015) Biodegradable hollow silica nanospheres containing gold nanoparticle arrays. Chem Commun 51:9939–994110.1039/C5CC02771C ↗
10. Lee CH, Lin TS, Mou CY (2009) Mesoporous materials for encapsulating enzymes. Nano Today 4:165–17910.1016/j.nantod.2009.02.001 ↗
11. Lin YS, Haynes CL (2010) Impacts of mesoporous silica nanoparticle size, pore ordering, and pore integrity on hemolytic activity. J Am Chem Soc 132:4834–484210.1021/ja910846q ↗
12. Slowing II, Trewyn BG, Lin VSY (2007) Mesoporous silica nanoparticles for intracellular delivery of membrane-impermeable proteins. J Am Chem Soc 129:8845–884910.1021/ja0719780 ↗
13. Olteanu NL, Lazar CA, Petcu AR, Meghea A, Rogozea EA, Mihaly M (2016) “One-pot” synthesis of fluorescent Au@SiO2 and SiO2@Au nanoparticles. ARAB J CHEM 9:854–86410.1016/j.arabjc.2015.12.014 ↗
14. Wu SH, Tseng CT, Lin YS, Lin CH, Hung Y, Mou CY (2011) Catalytic nano-rattle of Au@hollow silica: towards a poison-resistant nanocatalyst. J Mater Chem 21:789–79410.1039/C0JM02012E ↗
15. Botella P, Corma A, Navarro MT (2007) Single gold nanoparticles encapsulated in monodispersed regular spheres of mesostructured silica produced by pseudomorphic transformation. Chem Mater 19:1979–198310.1021/cm0629457 ↗
16. Pak J, Yoo H (2013) Facile synthesis of spherical nanoparticles with a silica shell and multiple Au nanodots as the core. J Mater Chem A 1:5408–541310.1039/c3ta10613f ↗
17. Yan X, Wang X, Tang Y, Ma G, Zou S, Li R, Peng X, Dai S, Fan J (2013) Unusual loading-dependent sintering-resistant properties of gold nanoparticles supported within extra-large mesopores. Chem Mater 25:1556–156310.1021/cm303816g ↗
18. Deng Y, Cai Y, Sun Z, Liu J, Liu C, Wei J, Li W, Liu C, Wang Y, Zhao D (2010) Multifunctional mesoporous composite microspheres with well-designed nanostructure: a highly integrated catalyst system. J Am Chem Soc 132:8466–847310.1021/ja1025744 ↗
19. Lu Y, Yin Y, Li ZY, Xia Y (2002) Synthesis and self-assembly of Au@SiO2 core−shell colloids. Nano Lett 2:785–78810.1021/nl025598i ↗
20. Tan L, Chen D, Liu H, Tang F (2010) A silica nanorattle with a mesoporous shell: an ideal nanoreactor for the preparation of tunable gold cores. Adv Mater 22:4885–488910.1002/adma.201002277 ↗
21. Jimenez VL, Georganopoulou DG, White RJ, Harper AS, Mills AJ, Lee D, Murray RW (2004) Hexanethiolate monolayer protected 38 gold atom cluster. Langmuir 20:6864–687010.1021/la049274g ↗
22. Mondal K, Agrawal S, Manna D, Banerjee A, Ghanty TK (2016) Effect of hydrogen atom doping on the structure and electronic properties of 20-atom gold cluster. J Phys Chem C 120:18588–1859410.1021/acs.jpcc.6b04584 ↗
23. Bore MT, Pham HN, Switzer EE, Ward TL, Fukuoka A, Datye AK (2005) The role of pore size and structure on the thermal stability of gold nanoparticles within mesoporous silica. J Phys Chem B 109:2873–288010.1021/jp045917p ↗
24. Li H, Li L, Pedersen A, Gao Y, Khetrapal N, Jónsson H, Zeng XC (2015) Magic-number gold nanoclusters with diameters from 1 to 3.5 nm: relative stability and catalytic activity for CO oxidation. Nano Lett 15:682–68810.1021/nl504192u ↗
25. Guo Y, Gu D, Jin Z, Du PP, Si R, Tao J, Xu WQ, Huang YY, Senanayake S, Song QS, Jia CJ, Schüth F (2015) Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: structure–activity relationship. Nanoscale 7:4920–492810.1039/C4NR06967F ↗
26. Jin R (2010) Quantum sized, thiolate-protected gold nanoclusters. Nanoscale 2:343–36210.1039/B9NR00160C ↗
27. Zhong RY, Sun KQ, Hong YC, Xu BQ (2014) Impacts of organic stabilizers on catalysis of Au nanoparticles from colloidal preparation. ACS Catal 4:3982–399310.1021/cs501161c ↗
28. Samanta A, Dhar BB, Devi RN (2012) Ultrasmall gold cluster arrays encapsulated in silica nanospheres: applications in fluorescence imaging and catalysis. J Phys Chem C 116:1748–175410.1021/jp2093737 ↗
29. Smith BL, Hutchison JE (2013) Transformations during sintering of small (Dcore < 2 nm) ligand-stabilized gold nanoparticles: influence of ligand functionality and core size. J Phys Chem C 117:25127–2513710.1021/jp408111v ↗
30. Yang J, Zhang F, Chen Y, Qian S, Hu P, Li W, Deng Y, Fang Y, Han L, Luqman M, Zhao D (2011) Core–shell Ag@SiO2@mSiO2 mesoporous nanocarriers for metal-enhanced fluorescence. Chem Commun 47:11618–1162010.1039/c1cc15304h ↗
31. Zhang F, Ping Yang, Matras-Postolek K (2016) Au catalyst decorated silica spheres: synthesis and high-performance in 4-Nitrophenol reduction. J Nanosci Nanotechnol 16:5966–597410.1166/jnn.2016.10858 ↗
32. JCPDS Card File No. 00-004-0784 (Au)
33. DuChene JS, Almeida RP, Wei WD (2012) Facile synthesis of anisotropic Au@SiO2 core–shell nanostructures. Dalton Trans 41:7879–788210.1039/c2dt30409k ↗
34. Li Y, Jin C, Yuan G, Han J, Wang M, Guo R (2017) Implantation of Fe3O4 nanoparticles in shells of Au@m-SiO2 Yolk@Shell nanocatalysts with both improved recyclability and catalytic activity. Langmuir 33:7486–749310.1021/acs.langmuir.7b01742 ↗
35. Hao X, Hu X, Zhang C, Chen S, Li Z, Yang X, Liu H, Jia G, Liu D, Ge K, Liang XJ, Zhang J (2015) Hybrid mesoporous silica-based drug carrier nanostructures with improved degradability by hydroxyapatite. ACS Nano 10:9614–962510.1021/nn507485j ↗
36. Zhao P, Feng X, Huang D, Yang G, Astruc D (2015) Basic concepts and recent advances in nitrophenol reduction by gold- and other transition metal nanoparticles. Coord Chem Rev 287:114–13610.1016/j.ccr.2015.01.002 ↗
37. Harish S, Mathiyarasu J, Phani KLN, Yegnaraman V (2009) Synthesis of conducting polymer supported Pd nanoparticles in aqueous medium and catalytic activity towards 4-Nitrophenol reduction. Catal Lett 128:197–20210.1007/s10562-008-9732-x ↗
38. Lee J, Park JC, Song H (2008) A nanoreactor framework of a Au@SiO2 yolk/shell structure for catalytic reduction of p-Nitrophenol. Adv Mater 20:1523–152810.1002/adma.200702338 ↗
39. Lin F, Doong R (2011) Bifunctional Au−Fe3O4 Heterostructures for magnetically recyclable catalysis of nitrophenol reduction. J Phys Chem C 115:6591–659810.1021/jp110956k ↗