Recent advances in medicine and biotechnology have prompted the need to develop nanoengineered delivery systems that can encapsulate a wide variety of novel therapeutics such as proteins, chemotherapeutics, and nucleic acids. Moreover, these delivery systems should be "intelligent", such that they can deliver their payload at a well-defined time, place, or after a specific stimulus. Polymeric multilayer capsules, made by layer-by-layer (LbL) coating of a sacrificial template followed by dissolution of the template, allow the design of microcapsules in aqueous conditions by using simple building blocks and assembly procedures, and provide a previously unmet control over the functionality of the microcapsules. Polymeric multilayer capsules have recently received increased interest from the life science community, and many interesting systems have appeared in the literature with biodegradable components and biospecific functionalities. In this Review we give an overview of the recent breakthroughs in their application for drug delivery.

Polymeric Multilayer Capsules in Drug Delivery

Nanoengineered multifunctional capsules with tailored structures and properties are of particular interest due to their multifunctions and potential applications as new colloidal structures in diverse fields. Among the available fabrication methods, the layer-by-layer (LbL) assembly of multilayer films onto colloidal particles followed by selective template removal has attracted extensive attention due to its advantages of precise control over the size, shape, composition, wall thickness and functions of the obtained capsules. The past decade has witnessed a rapid increase of research concerning the new fabrication strategies, functionalization and applications of this kind of capsules, particularly in the biomedical fields such as drug delivery, biosensors and bioreactors. In this critical review, the very recent progress of the multilayer capsules is summarized. First, the advances in assembly of capsules by the LbL technique are introduced with focus on tailoring the properties of hydrogen-bonded multilayer capsules by cross-linking, and fabrication of capsules based on covalent bonding and bio-specific interactions. Then the fabrication strategies which can speed up capsule fabrication are reviewed. In the following sections, the multi-compartmental capsules and the capsules that can transform their shape under stimulus are presented. Finally, the biomedical applications of multilayer capsules with particular emphasis on drug carriers, biosensors and bioreactors are described (306 references).

Layer-by-layer assembly of microcapsules and their biomedical applications

The advent of Layer-by-Layer (LbL) assembly to fabricate polymeric as well as hybrid multilayer thin films has opened exciting avenues for the design of multifunctional drug carriers with extreme control over their physico-chemical properties. These polymeric multilayer capsules (PMLC) are typically fabricated by sequential adsorption of polymers onto a spherical substrate with dimensions varying from 10 nm to several microns and larger. In this critical review, we give an overview of the recent advances in the field of PMLC with respect to drug delivery and point out how sophisticated capsule engineering can lead to well-defined drug carriers with unique properties (139 references).

Polymeric multilayer capsules for drug delivery.

Inspired by the simplicity and versatility of layer-by-layer (LbL) assembly, we applied multilayered polyelectrolyte assemblies on nanoparticles to create viable systemic delivery systems. Focusing on tumor-specific delivery, LbL nanoparticles that exhibit a pH-sensitive outer stealth layer are demonstrated to target and be retained in hypoxic tumor regions. The neutral layers shed in response to acidity to reveal a charged nanoparticle surface that is readily taken up by tumor cells. The first in vivo demonstration of this mechanism of targeting is presented, as well as an initial examination of the mechanism of uptake of the nanoparticles. We further demonstrate that this concept for tumor targeting is potentially valid for a broad range of cancers, with applicability for therapies that target hypoxic tumor tissue.

/pdf/layer-by-layer-nanoparticles-with-a-ph-sheddable-layer-for-1x6vm8di38.pdf

Layer-by-Layer Nanoparticles with a pH-Sheddable Layer for in Vivo Targeting of Tumor Hypoxia

Polymeric materials formed via layer-by-layer (LbL) assembly have promise for use as drug delivery vehicles. These multilayered materials, both as capsules and thin fi lms, can encapsulate a high payload of toxic or sensitive drugs, and can be readily engineered and functionalized with specific properties. This review highlights important and recent studies that advance the use of LbL-assembled materials as therapeutic devices. It also seeks to identify areas that require additional investigation for future development of the field. A variety of drug-loading methods and delivery routes are discussed. The biological barriers to successful delivery are identified, and possible solutions to these problems are discussed. Finally, state-of-the-art degradation and cargo release mechanisms are also presented.

/pdf/layer-by-layer-assembled-capsules-and-films-for-therapeutic-9cgtfynl45.pdf

Layer‐By‐Layer‐Assembled Capsules and Films for Therapeutic Delivery

Polyelectrolyte microcapsules are made by layer-by-layer (LbL) coating of a sacrificial template, followed by decomposition of the template, to produce hollow microcapsules. In this paper, we report on the in vivo cellular uptake, degradation and biocompatibility of polyelectrolyte microcapsules produced from alternating dextran sulphate and poly-L-arginine layers on a template of calcium carbonate microparticles. We show that a moderate tissue reaction is observed after subcutaneous injection of polyelectrolyte microcapsules in mice. Within sixteen days after subcutaneous injection, most of the microcapsules are internalized by the cells and start to get degraded. The number of polyelectrolyte layers determines the stability of the microcapsules after cellular uptake.

In vivo Cellular Uptake, Degradation, and Biocompatibility of Polyelectrolyte Microcapsules†

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In vivo Cellular Uptake, Degradation, and Biocompatibility of Polyelectrolyte Microcapsules†