Adapting the concepts of nonaqueous sol–gel chemistry to metals: synthesis and formation mechanism of palladium and palladium–copper nanoparticles in benzyl alcohol
Source abstract
Abstract
Benzyl alcohol is a versatile reaction medium for the synthesis of different types of nanoparticles. Its ability to act as an oxygen source gave access to metal oxide nanoparticles, while its reducing properties can be harnessed for the preparation of metals. Here we report the synthesis of Pd and PdCu nanoparticles in benzyl alcohol supplemented by a detailed mechanistic study for both systems. To elucidate the chemical formation mechanism of the Pd nanoparticles, we performed in situ attenuated total reflection ultraviolet–visible (ATR-UV–vis) and Fourier transform infrared spectroscopy (ATR-FTIR), providing information on the organic as well as on the inorganic side of the reaction. Potential gaseous products were analyzed by in situ gas chromatography (GC) and mass spectrometry (MS). We observed the formation of benzaldehyde, toluene, and dibenzyl ether as the three main organic products. The formation of the PdCu alloy nanoparticles was studied by ex situ powder X-ray diffraction (PXRD). A time-resolved study of the synthesis at 100 °C indicated that initially three types of particles formed, composed of an alloy with high Pd content, an alloy with high content of copper, and palladium particles, and only later in the reaction course they transformed into an alloy with a Pd-to-Cu ratio close to 1.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Catalytic Processes in Materials Science · Catalysis and Oxidation Reactions · nanoparticles nucleation surface interactions
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (58)
Show source-provided references
1. Toshima N, Yonezawa T (1998) Bimetallic nanoparticles—novel materials for chemical and physical applications. N J Chem 22:1179–120110.1039/a805753b ↗
2. Goia DV, Matijevic E (1998) Preparation of monodispersed metal particles. N J Chem 22:1203–121510.1039/a709236i ↗
3. Blin B, Fievet F, Beaupere D, Figlarz M (1989) Duplicative oxidation of ethylene-glycol in a new procedure for preparation of metallic powders. N J Chem 13:67–7210.1002/chin.198928091 ↗
4. Xiong Y, McLellan JM, Chen J, Yin Y, Li Z-Y, Xia Y (2005) Kinetically controlled synthesis of triangular and hexagonal nanoplates of palladium and their SPR/SERS properties. J Am Chem Soc 127:17118–1712710.1021/ja056498s ↗
5. Xiong Y, Washio I, Chen J, Cai H, Li Z-Y, Xia Y (2006) Poly(vinyl pyrrolidone): a dual functional reductant and stabilizer for the facile synthesis of noble metal nanoplates in aqueous solutions. Langmuir 22:8563–857010.1021/la061323x ↗
6. Viau G, Fiévet-Vincent F, Fiévet F (1996) Nucleation and growth of bimetallic CoNi and FeNi monodisperse particles prepared in polyols. Solid State Ion 84:259–27010.1016/0167-2738(96)00005-7 ↗
7. Kurihara LK, Chow GM, Schoen PE (1995) Nanocrystalline metallic powders and films produced by the polyol method. Nanostruct Mater 5:607–61310.1016/0965-9773(95)00275-J ↗
8. Yue H, Zhao Y, Ma X, Gong J (2012) Ethylene glycol: properties, synthesis, and applications. Chem Soc Rev 41:4218–424410.1039/c2cs15359a ↗
9. Kou J, Bennett-Stamper C, Varma RS (2013) Green synthesis of noble nanometals (Au, Pt, Pd) using glycerol under microwave irradiation conditions. ACS Sustain Chem Eng 1:810–81610.1021/sc400007p ↗
10. Hirai H, Nakao Y, Toshima N (1978) Colloidal rhodium in poly(vinylpyrrolidone) as hydrogenation catalyst for internal olefins. Chem Lett 545–54810.1246/cl.1978.545 ↗
11. Kim J, Kim D, Veriansyah B, Won Kang J, Kim J-D (2009) Metal nanoparticle synthesis using supercritical alcohol. Mater Lett 63:1880–188210.1016/j.matlet.2009.05.066 ↗
12. Hirai H, Chawanya H, Toshima N (1985) Colloidal palladium protected with poly(N-vinyl-2-pyrrolidone) for selective hydrogenation of cyclopentadiene. React Polym Ion Exch Sorbents 3:127–14110.1016/0167-6989(85)90055-8 ↗
13. Jia FL, Zhang LZ, Shang XY, Yang Y (2008) Non-aqueous sol–gel approach towards the controllable synthesis of nickel nanospheres, nanowires, and nanoflowers. Adv Mater 20:1050–105410.1002/adma.200702159 ↗
14. Dar MI, Sampath S, Shivashankar SA (2012) Microwave-assisted, surfactant-free synthesis of air-stable copper nanostructures and their SERS study. J Mater Chem 22:22418–2242310.1039/c2jm35629e ↗
15. Jia F, Wang F, Lin Y, Zhang L (2011) Microwave-induced formation of platinum nanostructured networks with superior electrochemical activity and stability. Chem Eur J 17:14603–1461010.1002/chem.201101179 ↗
16. Kränzlin N, Ellenbroek S, Durán-Martín D, Niederberger M (2012) Liquid-phase deposition of freestanding copper foils and supported copper thin films and their structuring into conducting line patterns. Angew Chem Int Ed 51:4743–474610.1002/anie.201200428 ↗
17. Staniuk M, Hirsch O, Kränzlin N, Böhlen R, van Beek W, Abdala PM, Koziej D (2014) Puzzling mechanism behind a simple synthesis of cobalt and cobalt oxide nanoparticles: in situ synchrotron X-ray absorption and diffraction studies. Chem Mater 26:2086–209410.1021/cm500090r ↗
18. Staniuk M, Zindel D, van Beek W, Hirsch O, Kranzlin N, Niederberger M, Koziej D (2015) Matching the organic and inorganic counterparts during nucleation and growth of copper-based nanoparticles—in situspectroscopic studies. CrystEngComm 17:6962–697110.1039/C5CE00454C ↗
19. Tukhtaev RK, Yukhin YM, Udalova TA, Bokhonov BB, NZ Lyakhov NZ (2008) In: Ifost 2008: Proceeding of the Third International Forum on Strategic Technologies, IEEE New York, pp 239–242
20. Niederberger M, Garnweitner G (2006) Organic reaction pathways in the nonaqueous synthesis of metal oxide nanoparticles. Chem Eur J 12:7282–730210.1002/chem.200600313 ↗
21. Niederberger M (2007) Nonaqueous sol–gel routes to metal oxide nanoparticles. Acc Chem Res 40:793–80010.1021/ar600035e ↗
22. Niederberger M, Pinna N (2009) In: Metal oxide nanoparticles in organic solvents, Springer-Verlag, London, pp 97–12710.1007/978-1-84882-671-7 ↗
23. Olliges-Stadler I, Rossell MD, Suess MJ, Ludi B, Bunk O, Pedersen JS, Birkedal H, Niederberger M (2013) A comprehensive study of the crystallization mechanism involved in the nonaqueous formation of tungstite. Nanoscale 5:8517–852510.1039/c3nr02020g ↗
24. Koziej D, Rossell MD, Ludi B, Hintennach A, Novak P, Grunwaldt JD, Niederberger M (2011) Interplay between size and crystal structure of molybdenum dioxide nanoparticles-synthesis, growth mechanism, and electrochemical performance. Small 7:377–38710.1002/smll.201001606 ↗
25. Ludi B, Suess MJ, Werner IA, Niederberger M (2012) Mechanistic aspects of molecular formation and crystallization of zinc oxide nanoparticles in benzyl alcohol. Nanoscale 4:1982–199510.1039/C1NR11557J ↗
26. LaMer VK, Dinegar RH (1950) Theory, production and mechanism of formation of monodispersed hydrosols. J Am Chem Soc 72:4847–485410.1021/ja01167a001 ↗
27. Watzky MA, Finke RG (1997) Transition metal nanocluster formation kinetic and mechanistic studies. a new mechanism when hydrogen is the reductant: slow, continuous nucleation and fast autocatalytic surface growth. J Am Chem Soc 119:10382–1040010.1021/ja9705102 ↗
28. Finney EE, Finke RG (2008) The four-step, double-autocatalytic mechanism for transition-metal nanocluster nucleation, growth, and then agglomeration: metal, ligand, concentration, temperature, and solvent dependency studies. Chem Mater 20:1956–197010.1021/cm071088j ↗
29. Besson C, Finney EE, Finke RG (2005) Nanocluster nucleation, growth, and then agglomeration kinetic and mechanistic studies: a more general, four-step mechanism involving double autocatalysis. Chem Mater 17:4925–493810.1021/cm050207x ↗
30. Perala SRK, Kumar S (2014) On the two-step mechanism for synthesis of transition-metal nanoparticles. Langmuir 30:12703–1271110.1021/la503199m ↗
31. Nishimura S, Takagaki A, Maenosono S, Ebitani K (2010) In situ time-resolved XAFS study on the formation mechanism of Cu nanoparticles using poly(N-vinyl-2-pyrrolidone) as a capping agent. Langmuir 26:4473–447910.1021/la904248z ↗
32. Lin C-S, Khan MR, Lin SD (2006) The preparation of Pt nanoparticles by methanol and citrate. J Colloid Interface Sci 299:678–68510.1016/j.jcis.2006.03.003 ↗
33. Yao T, Liu S, Sun Z, Li Y, He S, Cheng H, Xie Y, Liu Q, Jiang Y, Wu Z, Pan Z, Yan W, Wei S (2012) Probing nucleation pathways for morphological manipulation of platinum nanocrystals. J Am Chem Soc 134:9410–941610.1021/ja302642x ↗
34. Thanh NTK, Maclean N, Mahiddine S (2014) Mechanisms of nucleation and growth of nanoparticles in solution. Chem Rev 114:7610–763010.1021/cr400544s ↗
35. Wilkinson KE, Palmberg L, Witasp E, Kupczyk M, Feliu N, Gerde P, Seisenbaeva GA, Fadeel B, Dahlen S-E, Kessler VG (2011) Solution-engineered palladium nanoparticles: model for health effect studies of automotive particulate pollution. ACS Nano 5:5312–532410.1021/nn1032664 ↗
36. Dutilleul MCollart, Seisenbaeva GA, Kessler VG (2014) Novel solvothermal approach to hydrophilic nanoparticles of late transition elements and its evaluation by nanoparticle tracking analysis. Adv Nano Res 2:77–8810.12989/anr.2014.2.2.077 ↗
37. Wojdyr M (2010) Fityk: a general-purpose peak fitting program. J Appl Cryst 43:1126–112810.1107/S0021889810030499 ↗
38. Nemamcha A, Rehspringer J-L, Khatmi D (2006) Synthesis of palladium nanoparticles by sonochemical reduction of palladium(II) nitrate in aqueous solution. J Phys Chem B 110:383–38710.1021/jp0535801 ↗
39. Guohua J, Li W, Tao C, Haojie Y, Jianjun W (2004) Studies of preparation of palladium nanoparticles protected by dendrons. Nanotechnology 15:1716–171910.1088/0957-4484/15/12/003 ↗
40. Luo C, Zhang Y, Wang Y (2005) Palladium nanoparticles in poly(ethyleneglycol): the efficient and recyclable catalyst for Heck reaction. J Mol Catal A Chem 229:7–1210.1016/j.molcata.2004.10.039 ↗
41. Okitsu K, Bandow H, Maeda Y, Nagata Y (1996) Sonochemical preparation of ultrafine palladium particles. Chem Mater 8:315–31710.1021/cm950285s ↗
42. Chen W, Cai W, Lei Y, Zhang L (2001) A sonochemical approach to the confined synthesis of palladium nanoparticles in mesoporous silica. Mater Lett 50:53–5610.1016/S0167-577X(00)00411-0 ↗
43. Yonezawa T, Imamura K, Kimizuka N (2001) Direct preparation and size control of palladium nanoparticle hydrosols by water-soluble isocyanide ligands. Langmuir 17:4701–470310.1021/la0101954 ↗
44. Šoptrajanova L, Šoptrajanova B (1992) Vibrational studies of palladium(II) acetate compounds Ii. Infrared spectra of the diethylamine adduct of palladium(II) acetate. Spectrosc Lett 25:1141–115110.1080/00387019208018222 ↗
45. Dani A, Crocellà V, Maddalena L, Barolo C, Bordiga S, Groppo E (2016) Spectroscopic study on the surface properties and catalytic performances of palladium nanoparticles in poly(ionic liquid)s. J Phys Chem C 120:1683–169210.1021/acs.jpcc.5b11137 ↗
46. Stoyanov ES (2000) Ir study of the structure of palladium(ii) acetate in chloroform, acetic acid, and their mixtures in solution and in liquid-solid subsurface layers. J Struct Chem 4:440–44510.1007/BF02742003 ↗
47. Bowker M, Morgan C, Couves J (2004) Acetic acid adsorption and decomposition on Pd(110). Surf Sci 555:145–15610.1016/j.susc.2003.12.040 ↗
48. Aas N, Bowker M (1993) Adsorption and autocatalytic decomposition of acetic acid on Pd(110). J Chem Soc Faraday Trans 89:1249–125510.1039/ft9938901249 ↗
49. Davis JL, Barteau MA (1991) Reactions of carboxylic acids on the Pd(111)-(2 × 2)O surface: multiple roles of surface oxygen atoms. Surf Sci 256:50–6610.1016/0039-6028(91)91199-8 ↗
50. Haley RD, Tikhov MS, Lambert RM (2001) The surface chemistry of acetic acid on Pd{111}. Catal Lett 76:125–13010.1023/A:1012330230543 ↗
51. Abend AM, Chung L, Bibart RT, Brooks M, McCollum DG (2004) Concerning the stability of benzyl alcohol: formation of benzaldehyde dibenzyl acetal under aerobic conditions. J Pharm Biomed Anal 34:957–96210.1016/j.jpba.2003.11.007 ↗
52. Trautmann S, Baerns M, Auroux A (1992) In situ infrared spectroscopic and catalytic studies on the oxidation of ethane over supported palladium catalysts. J Catal 136:613–61610.1016/0021-9517(92)90092-V ↗
53. Agasti N, Kaushik NK (2014) Am J Nanomater 2:4–7
54. Pretsch E, Seibl J, Clerc T, Simon W (1986) In: Tabellen zur Strukturaufklärung organischer Verbindungen mit spektroskopischen Methoden, Springer-Verlag Berlin Heidelberg, pp M5–M2010.1007/978-3-662-10203-9_3 ↗
55. Davis JL, Barteau MA (1989) Hydrogen bonding in carboxylic acid adlayers on Pd(111): evidence for catemer formation. Langmuir 5:1299–130910.1021/la00090a004 ↗
56. Yudanov IV, Genest A, Schauermann S, Freund H-J, Rösch N (2012) Size dependence of the adsorption energy of CO on metal nanoparticles: a DFT search for the minimum value. Nano Lett 12:2134–213910.1021/nl300515z ↗
57. Denton AR, Ashcroft NW (1991) Vegard’s law. Phys Rev A 43:3161–316410.1103/PhysRevA.43.3161 ↗
58. Axon HJ, Humerothery W (1948) The lattice spacings of solid solutions of different elements in aluminium. Proc R Soc A 193:1–2410.1098/rspa.1948.0030 ↗