Annhelen Lu
University of Warwick
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Publication
Featured researches published by Annhelen Lu.
Chemical Communications | 2012
Annhelen Lu; Pepa Cotanda; Joseph P. Patterson; Deborah A. Longbottom; Rachel K. O'Reilly
The use of functional core-shell micelles as asymmetric catalytic nanoreactors for organic reactions in water is presented. An unprecedented increase in rate of reaction was achieved, which is proposed to be associated with the ability of the nanostructures to effectively concentrate the reagents in the catalytically active micelle core.
Polymer Chemistry | 2014
Helen Willcock; Annhelen Lu; Claire F. Hansell; Emma Chapman; Ian R. Collins; Rachel K. O'Reilly
We describe the one-pot synthesis of temperature-responsive branched polymer nanoparticles. Reversible addition–fragmentation chain transfer (RAFT) polymerisation has been utilised to synthesise ultra-high molecular weight sulfobetaine polymers (up to ca. 500 kDa) with good control over molecular weight (Mn) and dispersity (Mw/Mn). The UCST cloud points of these linear polymers were found to increase with both Mn and concentration, and represent one of the few recent descriptions of polymers exhibiting UCST behaviour in aqueous solution. The incorporation of difunctional monomers results in branched polymers which display vastly reduced transition temperatures compared to their linear counterparts. Furthermore, the incorporation of a permanently hydrophilic monomer results in the formation of stable core–shell particles which no longer exhibit a cloud point in water, even at very high concentrations (ca. 50 mg mL−1). The branched polymers are shown to form discrete well-defined nanoparticles in aqueous solution, and these have been characterised by DLS, SLS, TEM and DOSY. Their reversible swelling behaviour in response to temperature is also demonstrated.
Chemical Science | 2013
Annhelen Lu; Dafni Moatsou; Deborah A. Longbottom; Rachel K. O'Reilly
L-Proline functionalized PMMA nanogels with a range of catalyst functionalization (0.5–15 wt%) and cross-linking densities (0–50 wt%) were prepared via emulsion polymerization. The catalyst efficiency in water was investigated using a model asymmetric aldol reaction and an unprecedented reduction in catalyst loading, whilst maintaining high catalytic activity, is reported. In these reactions, a marked effect on selectivity was observed and determined to be dependent on the hydrophobicity of the nanogel particles. Furthermore, the effect of increasing cross-linking density on the catalytic efficiency of these particles (and their core–shell analogues) was explored and a significant reduction in activity was observed.
Polymer Chemistry | 2013
Joseph P. Patterson; Pepa Cotanda; Elizabeth G. Kelley; Adam O. Moughton; Annhelen Lu; Thomas H. Epps; Rachel K. O'Reilly
A new amphiphilic homopolymer bearing an SCS pincer palladium complex has been synthesized by reversible addition fragmentation chain transfer polymerization. The amphiphile has been shown to form spherical and worm-like micelles in water by cryogenic transmission electron microscopy and small angle neutron scattering. Segregation of reactive components within the palladium containing core results in increased catalytic activity of the pincer compound compared to small molecule analogues. This allows carbon-carbon bond forming reactions to be performed in water with reduced catalyst loadings and enhanced activity.
Polymer Chemistry | 2013
Beth L. Moore; Annhelen Lu; Deborah A. Longbottom; Rachel K. O'Reilly
The MacMillan catalyst is an established organocatalyst capable of catalyzing a variety of organic reactions. Through the synthesis of a novel monomer containing the MacMillan catalytic functionality, a variety of copolymers have been synthesized with the comonomer, diethylene glycol methyl ether methacrylate (DEGMA). Reversible addition–fragmentation chain transfer (RAFT) polymerization was used for the synthesis of these functional polymers with good control over molecular weight, catalyst incorporation and polydispersity. These polymers showed lower critical solution temperature (LCST) behaviour where the cloud point was found to be dependent upon the degree of catalyst incorporation and catalyst loading was also found to have an effect on the Tg of the copolymers. The catalytic activity of the functional copolymers is demonstrated by the Diels–Alder reaction between cyclopentadiene and trans-hexen-1-al and shows enantioselectivity close to those previously reported by MacMillan. The polymers can be reused in multiple Diels–Alder reactions via a pseudo continuous process, maintaining high conversion and enantioselectivity throughout the cycles.
Polymer Chemistry | 2014
Beth L. Moore; Dafni Moatsou; Annhelen Lu; Rachel K. O'Reilly
The immobilization of the MacMillan catalyst within a unique hydrophobic environment created by a lightly cross-linked nanogel structure and its resulting catalytic activity is reported. The catalytic activity and selectivity of the catalyst were evaluated using the Diels–Alder (DA) reaction between cyclopentadiene and cinnamaldehyde. The relatively easy synthetic route applied allowed for the synthesis of a collection of nanogels with catalyst incorporations ranging from 0.5 to 25 wt%. In addition, core–shell type nanogels were synthesized to evaluate potential recovery and reuse of the catalytic system. The influence of the concentrator effect and possible partition coefficient on the catalyst activity was investigated. The results indicate catalyst loading/concentration can be more significantly reduced when the catalyst is embedded within the polymeric nanostructures compared to the small molecule equivalent.
Macromolecules | 2011
Annhelen Lu; Thomas P. Smart; Thomas H. Epps; Deborah A. Longbottom; Rachel K. O’Reilly
ACS Macro Letters | 2013
Hazit A. Zayas; Annhelen Lu; David Valade; Faheem Amir; Zhongfan Jia; Rachel K. O’Reilly; Michael J. Monteiro
Macromolecules | 2012
Pepa Cotanda; Annhelen Lu; Joseph P. Patterson; Nikos Petzetakis; Rachel K. O’Reilly
Current Opinion in Biotechnology | 2013
Annhelen Lu; Rachel K. O’Reilly