Controllable Catalytic Activity of Temperature-Responsive Polymer Hybrid Microgels Designed Using a Gold Nanoparticle Monomer with Polymerizable Groups
“…Therefore, the higher catalytic activity of the hybrid microgels with smaller AuNP sizes is a ributed to the fact that the increased surface area allows for a more efficient adsorption of 4-NP onto the AuNP surface and that AuNPs with a smaller size have more active sites because their reduced dimensions correspond to lower coordination numbers [59,62,63]. The catalytic activity of the hybrid microgels with a small AuNP size at temperatures lower than 35 °C was relatively high compared to the AuNP hybrid assemblies reported previously [55]. This might be a ributed to the fact that the hybrid microgels have highly swollen networks and that 4-NP can easily approach the AuNP surface owing to their high permeability (Figure 6).…”
Section: Catalytic Activity Of Pnipaam-aunp Hybrid Microgels With Var...mentioning
confidence: 74%
“…According to the method reported in our previous paper [ 55 ], AuNP monomers were prepared by attaching hydrophobic polymerizable acryloyl and hydrophilic carboxyl groups to the AuNP surface ( Scheme S2 ). First, DUDP with two acryloyl groups was synthesized as a thiol to introduce polymerizable groups onto the surface of AuNPs ( Scheme S3 ).…”
Section: Resultsmentioning
confidence: 99%
“…In a previous paper, we proposed a new method to prepare temperature-responsive polymer–AuNP hybrids using an AuNP monomer with polymerizable groups [ 55 ]. The resulting PNIPAAm–AuNP hybrid microgels switched their catalytic activity upon changing their temperature.…”
Section: Resultsmentioning
confidence: 99%
“…The preparation of citrate-AuNPs of various sizes exhibited good reproducibility through the careful control of a few crucial factors, but more careful control of the preparation conditions is required for practical applications and scalability. According to the method reported in our previous paper [55], AuNP monomers were prepared by a aching hydrophobic polymerizable acryloyl and hydrophilic carboxyl groups to the AuNP surface (Scheme S2). First, DUDP with two acryloyl groups was synthesized as a thiol to introduce polymerizable groups onto the surface of AuNPs (Scheme S3).…”
Section: Preparation Of Aunp Monomers With Various Sizesmentioning
confidence: 99%
“…In general, while PNIPAAm covalently binds to the AuNP surfaces in the PNIPAAm–AuNP hybrids prepared using the first and second methods, AuNPs are physically entrapped within the PNIPAAm networks in the hybrids prepared using the third method. Unlike their standard method, our previous study proposed a simple method to prepare PNIPAAm–AuNP hybrids in which AuNPs are covalently linked with microsized PNIPAAm networks [ 55 ]. This method uses an AuNP monomer with polymerizable groups.…”
Gold nanoparticles (AuNPs) possess attractive electronic, optical, and catalytic properties, enabling many potential applications. Poly(N-isopropyl acrylamide) (PNIPAAm) is a temperature-responsive polymer that changes its hydrophilicity upon a slight temperature change, and combining PNIPAAm with AuNPs allows us to modulate the properties of AuNPs by temperature. In a previous study, we proposed a simpler method for designing PNIPAAm–AuNP hybrid microgels, which used an AuNP monomer with polymerizable groups. The size of AuNPs is the most important factor influencing their catalytic performance, and numerous studies have emphasized the importance of controlling the size of AuNPs by adjusting their stabilizer concentration. This paper focuses on the effect of AuNP size on the catalytic activity of PNIPAAm–AuNP hybrid microgels prepared via the copolymerization of N-isopropyl acrylamide and AuNP monomers with different AuNP sizes. To quantitatively evaluate the catalytic activity of the hybrid microgels, we monitored the reduction of 4-nitrophenol to 4-aminophenol using the hybrid microgels with various AuNP sizes. While the hybrid microgels with an AuNP size of 13.0 nm exhibited the highest reaction rate and the apparent reaction rate constant (kapp) of 24.2 × 10−3 s−1, those of 35.9 nm exhibited a small kapp of 1.3 × 10−3 s−1. Thus, the catalytic activity of the PNIPAAm–AuNP hybrid microgel was strongly influenced by the AuNP size. The hybrid microgels with various AuNP sizes enabled the reversibly temperature-responsive on–off regulation of the reduction reaction.
“…Therefore, the higher catalytic activity of the hybrid microgels with smaller AuNP sizes is a ributed to the fact that the increased surface area allows for a more efficient adsorption of 4-NP onto the AuNP surface and that AuNPs with a smaller size have more active sites because their reduced dimensions correspond to lower coordination numbers [59,62,63]. The catalytic activity of the hybrid microgels with a small AuNP size at temperatures lower than 35 °C was relatively high compared to the AuNP hybrid assemblies reported previously [55]. This might be a ributed to the fact that the hybrid microgels have highly swollen networks and that 4-NP can easily approach the AuNP surface owing to their high permeability (Figure 6).…”
Section: Catalytic Activity Of Pnipaam-aunp Hybrid Microgels With Var...mentioning
confidence: 74%
“…According to the method reported in our previous paper [ 55 ], AuNP monomers were prepared by attaching hydrophobic polymerizable acryloyl and hydrophilic carboxyl groups to the AuNP surface ( Scheme S2 ). First, DUDP with two acryloyl groups was synthesized as a thiol to introduce polymerizable groups onto the surface of AuNPs ( Scheme S3 ).…”
Section: Resultsmentioning
confidence: 99%
“…In a previous paper, we proposed a new method to prepare temperature-responsive polymer–AuNP hybrids using an AuNP monomer with polymerizable groups [ 55 ]. The resulting PNIPAAm–AuNP hybrid microgels switched their catalytic activity upon changing their temperature.…”
Section: Resultsmentioning
confidence: 99%
“…The preparation of citrate-AuNPs of various sizes exhibited good reproducibility through the careful control of a few crucial factors, but more careful control of the preparation conditions is required for practical applications and scalability. According to the method reported in our previous paper [55], AuNP monomers were prepared by a aching hydrophobic polymerizable acryloyl and hydrophilic carboxyl groups to the AuNP surface (Scheme S2). First, DUDP with two acryloyl groups was synthesized as a thiol to introduce polymerizable groups onto the surface of AuNPs (Scheme S3).…”
Section: Preparation Of Aunp Monomers With Various Sizesmentioning
confidence: 99%
“…In general, while PNIPAAm covalently binds to the AuNP surfaces in the PNIPAAm–AuNP hybrids prepared using the first and second methods, AuNPs are physically entrapped within the PNIPAAm networks in the hybrids prepared using the third method. Unlike their standard method, our previous study proposed a simple method to prepare PNIPAAm–AuNP hybrids in which AuNPs are covalently linked with microsized PNIPAAm networks [ 55 ]. This method uses an AuNP monomer with polymerizable groups.…”
Gold nanoparticles (AuNPs) possess attractive electronic, optical, and catalytic properties, enabling many potential applications. Poly(N-isopropyl acrylamide) (PNIPAAm) is a temperature-responsive polymer that changes its hydrophilicity upon a slight temperature change, and combining PNIPAAm with AuNPs allows us to modulate the properties of AuNPs by temperature. In a previous study, we proposed a simpler method for designing PNIPAAm–AuNP hybrid microgels, which used an AuNP monomer with polymerizable groups. The size of AuNPs is the most important factor influencing their catalytic performance, and numerous studies have emphasized the importance of controlling the size of AuNPs by adjusting their stabilizer concentration. This paper focuses on the effect of AuNP size on the catalytic activity of PNIPAAm–AuNP hybrid microgels prepared via the copolymerization of N-isopropyl acrylamide and AuNP monomers with different AuNP sizes. To quantitatively evaluate the catalytic activity of the hybrid microgels, we monitored the reduction of 4-nitrophenol to 4-aminophenol using the hybrid microgels with various AuNP sizes. While the hybrid microgels with an AuNP size of 13.0 nm exhibited the highest reaction rate and the apparent reaction rate constant (kapp) of 24.2 × 10−3 s−1, those of 35.9 nm exhibited a small kapp of 1.3 × 10−3 s−1. Thus, the catalytic activity of the PNIPAAm–AuNP hybrid microgel was strongly influenced by the AuNP size. The hybrid microgels with various AuNP sizes enabled the reversibly temperature-responsive on–off regulation of the reduction reaction.
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