TY - JOUR
T1 - Fabrication and characterisation of gold nano-particle modified polymer monoliths for flow-through catalytic reactions and their application in the reduction of hexacyanoferrate
AU - Floris, Patrick
AU - Twamley, Brendan
AU - Nesterenko, Pavel N.
AU - Paull, Brett
AU - Connolly, Damian
N1 - Funding Information:
The authors would like to thank Science Foundation Ireland (Grant number 08/SRC/B1412) for research funding under the Strategic Research Cluster programme and also for equipment funding (Grant. Number 03/IN.3/1361/EC07).
PY - 2014/1
Y1 - 2014/1
N2 - Polymer monoliths in capillary (100 μm i.d.) and polypropylene pipette tip formats (vol: 20 μL) were modified with gold nano-particles (AuNP) and subsequently used for flow-through catalytic reactions. Specifically, methacrylate monoliths were modified with amine-reactive monomers using a two-step photografting method and then reacted with ethylenediamine to provide amine attachment sites for the subsequent immobilisation of 4 nm, 7 nm or 16 nm AuNP. This was achieved by flushing colloidal suspensions of gold nano-particles through each aminated polymer monolith which resulted in a multi-point covalent attachment of gold via the lone pair of electrons on the nitrogen of the free amine groups. Field emission scanning electron microscopy and scanning capacitively coupled conductivity detection was used to characterise the surface coverage of AuNP on the monoliths. The catalytic activity of AuNP immobilised on the polymer monoliths in both formats was then demonstrated using the reduction of Fe(III) to Fe(II) by sodium borohydride as a model reaction by monitoring the reduction in absorbance of the hexacyanoferrate (I{cyrillic, ukrainian}I{cyrillic, ukrainian}I{cyrillic, ukrainian}) complex at 420 nm. Catalytic activity was significantly enhanced on monoliths modified with smaller AuNP with almost complete reduction (95 %) observed when using monoliths agglomerated with 7 nm AuNPs. [Figure not available: see fulltext.]
AB - Polymer monoliths in capillary (100 μm i.d.) and polypropylene pipette tip formats (vol: 20 μL) were modified with gold nano-particles (AuNP) and subsequently used for flow-through catalytic reactions. Specifically, methacrylate monoliths were modified with amine-reactive monomers using a two-step photografting method and then reacted with ethylenediamine to provide amine attachment sites for the subsequent immobilisation of 4 nm, 7 nm or 16 nm AuNP. This was achieved by flushing colloidal suspensions of gold nano-particles through each aminated polymer monolith which resulted in a multi-point covalent attachment of gold via the lone pair of electrons on the nitrogen of the free amine groups. Field emission scanning electron microscopy and scanning capacitively coupled conductivity detection was used to characterise the surface coverage of AuNP on the monoliths. The catalytic activity of AuNP immobilised on the polymer monoliths in both formats was then demonstrated using the reduction of Fe(III) to Fe(II) by sodium borohydride as a model reaction by monitoring the reduction in absorbance of the hexacyanoferrate (I{cyrillic, ukrainian}I{cyrillic, ukrainian}I{cyrillic, ukrainian}) complex at 420 nm. Catalytic activity was significantly enhanced on monoliths modified with smaller AuNP with almost complete reduction (95 %) observed when using monoliths agglomerated with 7 nm AuNPs. [Figure not available: see fulltext.]
KW - Agglomerated monolith
KW - Flow-through catalysis
KW - Micro-reactor
KW - Nano-particles
UR - http://www.scopus.com/inward/record.url?scp=84891560647&partnerID=8YFLogxK
U2 - 10.1007/s00604-013-1108-2
DO - 10.1007/s00604-013-1108-2
M3 - Article
AN - SCOPUS:84891560647
VL - 181
SP - 249
EP - 256
JO - Microchimica Acta
JF - Microchimica Acta
SN - 0026-3672
IS - 1-2
ER -