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Advanced Drug Delivery Reviews (v.64, #11)

Editorial Board (pp. ii).

Stimuli-responsive drug delivery systems by Jerry Yang (Theme Editor) (pp. 965-966).

Enzyme-responsive nanoparticles for drug release and diagnostics by Roberto de la Rica; Daniel Aili; Molly M. Stevens (pp. 967-978).

Enzymes are key components of the bionanotechnology toolbox that possess exceptional biorecognition capabilities and outstanding catalytic properties. When combined with the unique physical properties of nanomaterials, the resulting enzyme-responsive nanoparticles can be designed to perform functions efficiently and with high specificity for the triggering stimulus. This powerful concept has been successfully applied to the fabrication of drug delivery schemes where the tissue of interest is targeted via release of cargo triggered by the biocatalytic action of an enzyme. Moreover, the chemical transformation of the carrier by the enzyme can also generate therapeutic molecules, therefore paving the way to design multimodal nanomedicines with synergistic effects. Dysregulation of enzymatic activity has been observed in a number of severe pathological conditions, and this observation is useful not only to program drug delivery in vivo but also to fabricate ultrasensitive sensors for diagnosing these diseases. In this review, several enzyme-responsive nanomaterials such as polymer-based nanoparticles, liposomes, gold nanoparticles and quantum dots are introduced, and the modulation of their physicochemical properties by enzymatic activity emphasized. When known, toxicological issues related to the utilization nanomaterials are highlighted. Key examples of enzyme-responsive nanomaterials for drug delivery and diagnostics are presented, classified by the type of effector biomolecule, including hydrolases such as proteases, lipases and glycosidases, and oxidoreductases.Display Omitted

Keywords: Enzyme; Drug delivery; Biosensor; Sensor; Nanobiotechnology; Theragnostics; Cancer; Stimuli-responsive; Smart materials; Nanomedicine

pH-sensitive vesicles, polymeric micelles, and nanospheres prepared with polycarboxylates by Arnaud E. Felber; Marie-Hélène Dufresne; Jean-Christophe Leroux (pp. 979-992).

Titratable polyanions, and more particularly polymers bearing carboxylate groups, have been used in recent years to produce a variety of pH-sensitive colloids. These polymers undergo a coil-to-globule conformational change upon a variation in pH of the surrounding environment. This conformational change can be exploited to trigger the release of a drug from a drug delivery system in a pH-dependent fashion. This review describes the current status of pH-sensitive vesicles, polymeric micelles, and nanospheres prepared with polycarboxylates and their performance as nano-scale drug delivery systems, with emphasis on our recent contribution to this field.Protonation- (A) and ionization-induced (B) drug release from different nanocarriers containing titratable polyanions.Display Omitted

Keywords: Abbreviations; AA; acrylic acid; Al(M)A; alkyl(meth)acrylate; AlClPc; aluminum chloride phthalocyanine; AON; antisense oligonucleotide; AUC; area under the blood (plasma) concentration; vs.; time curve; BMA; butyl methacrylate; CMC; critical micelle concentration; DMAA; dimethylacrylamide; DOPE; dioleoylphosphatidylethanolamine; EA; ethyl acrylate; EMA; ethyl methacrylate; GI; gastrointestinal; HEMA; 2-hydroxyethyl methacrylate; HIV; human immunodeficiency virus; i; BA; iso; -butyl acrylate; LCST; lower critical solution temperature; MAA; methacrylic acid; MMA; methyl methacrylate; n; BA; n; -butyl acrylate; NIPAM; N; -isopropylacrylamide; ODA; octadecyl acrylate; PAA; poly(acrylic acid); PAMAM; poly(amido amine); PAsp; poly(; l; -aspartic acid); PCL; poly(ε-caprolactone); PDMAEMA; poly(; N; ,; N; -dimethylaminoethyl methacrylate); PEG; poly(ethylene glycol); PEGMA; PEG methacrylate; PG; poly(glycidol); PGA; poly(; l; -glutamic acid); PICM; polyion complex micelle; PLA; poly(; d,l; -lactide); PMAA; poly(methacrylic acid); PM; polymeric micelle; PrMA; propyl methacrylate; PUA; poly(10-undecenoic acid); siRNA; small interfering RNA; UA; 10-undecenoic acid; VBODENA; 4-(2-vinylbenzyloxy)-; N,N; -(diethylnicotinamide); VP; N; -vinyl-2-pyrrolidoneVesicle; Polymeric micelle; Nanoparticle; Nanosphere; pH-sensitive; pH-responsive; Polyanion; Carboxylic acid

Redox activation of metal-based prodrugs as a strategy for drug delivery by Nora Graf; Stephen J. Lippard (pp. 993-1004).

This review provides an overview of metal-based anticancer drugs and drug candidates. In particular, we focus on metal complexes that can be activated in the reducing environment of cancer cells, thus serving as prodrugs. There are many reports of Pt and Ru complexes as redox-activatable drug candidates, but other d-block elements with variable oxidation states have a similar potential to serve as prodrugs in this manner. In this context are compounds based on Fe, Co, or Cu chemistry, which are also covered. A trend in the field of medicinal inorganic chemistry has been toward molecularly targeted, metal-based drugs obtained by functionalizing complexes with biologically active ligands. Another recent activity is the use of nanomaterials for drug delivery, exploiting passive targeting of tumors with nano-sized constructs made from Au, Fe, carbon, or organic polymers. Although complexes of all of the above mentioned metals will be described, this review focuses primarily on Pt compounds, including constructs containing nanomaterials.Display Omitted

Keywords: Prodrugs; Pt anticancer drugs; Ru anticancer drugs; Activation by reduction; Medicinal inorganic chemistry; Nanocarriers

Photochemical mechanisms of light-triggered release from nanocarriers by Nadezda Fomina; Jagadis Sankaranarayanan; Adah Almutairi (pp. 1005-1020).

Over the last three decades, a handful of photochemical mechanisms have been applied to a large number of nanoscale assemblies that encapsulate a payload to afford spatio-temporal and remote control over activity of the encapsulated payload. Many of these systems are designed with an eye towards biomedical applications, as spatio-temporal and remote control of bioactivity would advance research and clinical practice. This review covers five underlying photochemical mechanisms that govern the activity of the majority of photoresponsive nanocarriers: 1. photo driven isomerization and oxidation, 2. surface plasmon absorption and photothermal effects, 3. photo driven hydrophobicity changes, 4. photo driven polymer backbone fragmentation and 5. photo driven de-crosslinking. The ways in which these mechanisms have been incorporated into nanocarriers and how they affect release are detailed, as well as the advantages and disadvantages of each system.Display Omitted

Keywords: Photochemical; Triggered release; Light; Near infrared; Nanocarriers; Nanoparticles

Engineering nanomedicines using stimuli-responsive biomaterials by Yapei Wang; James D. Byrne; Mary E. Napier; Joseph M. DeSimone (pp. 1021-1030).

The ability to engineer particles has the potential to shift the paradigm in the creation of new medicines and diagnostics. Complete control over particle characteristics, such as size, shape, mechanical property, and surface chemistry, can enable rapid translation and facilitate the US Food and Drug Administration (FDA) approval of particle technologies for the treatment of cancer, infectious diseases, diabetes, and a host of other major illnesses. The incorporation of natural and artificial external stimuli to trigger the release of drugs enables exquisite control over the release profiles of drugs in a given environment. In this article, we examine several readily scalable top–down methods for the fabrication of shape-specific particles that utilize stimuli-responsive biomaterials for controlled drug delivery. Special attention is given to Particle Replication In Nonwetting Templates (PRINT®) technology and the application of novel triggered-release synthetic and natural polymers.Display Omitted

Keywords: Top–down; Trigger-release; Microfluidic; Photolithography; PRINT

Amplified release through the stimulus triggered degradation of self-immolative oligomers, dendrimers, and linear polymers by Andrew D. Wong; Matthew A. DeWit; Elizabeth R. Gillies (pp. 1031-1045).

In recent years, numerous delivery systems based on polymers, dendrimers, and nano-scale assemblies have been developed to improve the properties of drug molecules. In general, for the drug molecules to be active, they must be released from these delivery systems, ideally in a selective manner at the therapeutic target. As the changes in physiological conditions are relatively subtle from one tissue to another and the concentrations of specific enzymes are often quite low, a release strategy involving the amplification of a biological signal is particularly attractive. This article describes the development of oligomers, dendrimers, and linear polymers based on self-immolative spacers. This new class of molecules is designed to undergo a cascade of intramolecular reactions in response to the cleavage of a trigger moiety, resulting in molecular fragmentation and the release of multiple reporter or drug molecules. Progress in the development of these materials as drug delivery vehicles and sensors will be highlighted.Display Omitted

Keywords: Abbreviations; Dox; doxorubicin; HPMA; poly(; N; -(2-hydroxypropyl)methacrylamide); PEO; poly(ethylene oxide); Boc; t; -butyloxycarbonyl; PGA; penicillin-G-amidase; BSA; bovine serum albumin; DMF; N; ,; N; -dimethylformamide; PBS; phosphate buffered saline; TBDMS; t; -butyldimethylsilyl; Fmoc; fluorenylmethyloxycarbonylCascade reactions; Biodegradable polymers; Depolymerization; Prodrugs; Nanoparticles; Drug delivery; Sensors

Stimuli-responsive polymers and nanomaterials for gene delivery and imaging applications by Min Suk Shim; Young Jik Kwon (pp. 1046-1059).

Multiple extra- and intracellular obstacles, including low stability in blood, poor cellular uptake, and inefficient endosomal escape and disassembly in the cytoplasm, have to be overcome in order to deliver nucleic acids for gene therapy. This review introduces the recent advances in tackling the key challenges in achieving efficient, targeted, and safe nonviral gene delivery using various nucleic acid-containing nanomaterials that are designed to respond to various extra- and intracellular biological stimuli (e.g., pH, redox potential, and enzyme) as well as external artificial triggers (e.g., light and ultrasound). Gene delivery in combination with molecular imaging and targeting enables diagnostic assessment, treatment monitoring and quantification of efficiency, and confirmation of cure, thus fulfilling the great promise of efficient and personalized medicine. Nanomaterials platform for combined imaging and gene therapy, nanotheragnostics, using stimuli-responsive materials is also highlighted in this review. It is clear that developing novel multifunctional nonviral vectors, which transform their physico-chemical properties in response to various stimuli in a timely and spatially controlled manner, is highly desired to translate the promise of gene therapy for the clinical success.Display Omitted

Keywords: Abbreviations; Au NPs; gold nanoparticles; azoTAB; azobenzene trimethylammonium bromide surfactant; CAT; chloramphenicol acetyltransferase; CDs; cyclodextrins; Chk- α; choline kinase-α; COX-2; cyclooxygenase-2; CPP; cell penetrating peptide; DODAC; dioleoyldimethylammonium chloride; DOPE; dioleoylphosphatidyl ethanolamine; DSPC; 1,2-distearoyl-; sn; -glycero-phosphatidylcholine; DSPE; 1,2-distearoyl-; sn; -glycero-3-phosphatidyl-ethanolamine; DTT; dithiothreitol; EAA; ethyl acrylic acid; EPPT; uMUC-1-specific peptide; GAGs; glycosaminoglycans; HBV; hepatitis B virus; HMA; hexyl methacrylate; i.a.; intra-arterial; i.v.; intravenous; LCST; lower critical solution temperature; MEND; multifunctional envelope-type nano device; MMP; matrix metalloproteinase; MPAP; Myr-Ala-(Arg); ₇; -Cys-CONH; ₂; MR; magnetic resonance; NIPAM; N; -isopropylacryamide; NIR; near-infrared; NLS; nuclear localization signals; OCT; optical coherence tomography; ODNs; oliogodeoxynucleotides; PAMAM; polyamidoamine; P(Asp); poly(aspartic acid); PBAA; poly(butylacrylic acid); PDMAEMA; poly(2-(dimethyl amino)ethyl methacrylate); PDPA; poly(2-(diisopropylamino)ethyl methacrylate); PEAA; poly(ethylacrylic acid); PEG; polyethylene glycol; PEI; polyethylenimine (PEI); PET; positron emission tomography; PHPMA; poly[; N; -(2-hydroxypropyl)methacrylamide]; PIC; polyion complex; plk 1; polo-like kinase 1; PLL; poly-L-lysine; PMPC; poly(2-(methacryloyloxy)ethyl phosphorylcholine); POrn; poly(L-ornithine); PPAA; poly(propylacrylic acid); PSD; poly(methacryloyl sulfadimethoxine); RES; reticuloendothelial system; RGD; Arg-Gly-Asp peptide; RNAi; RNA interference; SDBS; sodium dodecylbenzenesulfonate; SDS; sodium dodecylsulfate; SPION; superparamagnetic iron oxide nanoparticle; TMAEMA; trimethyl aminoethyl methacrylate; US; ultrasoundNucleic acid delivery; Nonviral vectors; Barriers in nonviral gene delivery; Extra- and intracellular stimuli; Stimuli-responsive nanomaterials; Nanotheragnostics; Combined imaging and gene delivery

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Advanced Drug Delivery Reviews (v.64, #11)