Polymers at the Interface with Biology.

Biology in its broadest sense is an important model and inspiration for science and technology. In relation to polymers, biology uses a variety of complex macromolecules to accomplish a myriad of functions in living systems. These biopolymers incorporate many unique features that have inspired the polymer community, including sequence specificity, renewable feedstocks, catalytic activity, self-replication, and specific recognition. Bioinspired synthetic and biologically derived polymers are critical components of many innovative solutions aimed at addressing some of the most pressing problems related to human health and the environment. Challenges and opportunities for the polymer science community at large include both developing synthetic strategies toward such materials as well as studying and developing a fundamental understanding of their interactions with biological systems. Since its inception in 2000, Biomacromolecules has strived to become the leading forum for the dissemination of cutting-edge research at the interface of polymer science and biology. Articles published in Biomacromolecules contain strong elements of innovation in terms of macromolecular design, synthesis, and characterization or in new applications of polymers to biology and medicine. The aims of this Editorial are to review the evolution of research at the interface of polymer science and biology and to present a forward-looking view of this field. We do this by highlighting some areas of research that have been prominently featured in Biomacromolecules over the past years and by presenting some emerging topics that we consider of great relevance and interest to the polymer science community and the readership of Biomacromolecules. This Editorial is partly based on a symposium entitled “Polymers at the Interface with Biology” and an associated “round-table” discussion that took place during the 2017 American Chemical Society (ACS) Fall Meeting in Washington, DC. The participants of this discussion included the Editor-in-Chief and Associate Editors of Biomacromolecules as well as a group of 13 invited experts.

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[12]  Fan Yang,et al.  Covalently Adaptable Elastin‐Like Protein–Hyaluronic Acid (ELP–HA) Hybrid Hydrogels with Secondary Thermoresponsive Crosslinking for Injectable Stem Cell Delivery , 2017, Advanced functional materials.

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[16]  Jianhua Zhang,et al.  Facile Access to Multisensitive and Self-Healing Hydrogels with Reversible and Dynamic Boronic Ester and Disulfide Linkages. , 2017, Biomacromolecules.

[17]  Rodrigo L. Silveira,et al.  Effects of Xylan Side-Chain Substitutions on Xylan-Cellulose Interactions and Implications for Thermal Pretreatment of Cellulosic Biomass. , 2017, Biomacromolecules.

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[24]  Yi Yan Yang,et al.  Amphiphilic and Hydrophilic Block Copolymers from Aliphatic N-Substituted 8-Membered Cyclic Carbonates: A Versatile Macromolecular Platform for Biomedical Applications. , 2017, Biomacromolecules.

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[26]  H. Maynard,et al.  Substituted Polyesters by Thiol-Ene Modification: Rapid Diversification for Therapeutic Protein Stabilization. , 2017, Journal of the American Chemical Society.

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[29]  Lei Cai,et al.  Regulating Stem Cell Secretome Using Injectable Hydrogels with In Situ Network Formation , 2016, Advanced healthcare materials.

[30]  J. C. Barnes,et al.  Using an RNAi Signature Assay To Guide the Design of Three-Drug-Conjugated Nanoparticles with Validated Mechanisms, In Vivo Efficacy, and Low Toxicity. , 2016, Journal of the American Chemical Society.

[31]  Thomas H. Epps,et al.  Mechanistic Design of Polymer Nanocarriers to Spatiotemporally Control Gene Silencing. , 2016, ACS biomaterials science & engineering.

[32]  R. Nolte,et al.  Metal Ion-Induced Self-Assembly of a Multi-Responsive Block Copolypeptide into Well-Defined Nanocapsules. , 2016, Small.

[33]  E. Chen,et al.  Towards Truly Sustainable Polymers: A Metal-Free Recyclable Polyester from Biorenewable Non-Strained γ-Butyrolactone. , 2016, Angewandte Chemie.

[34]  L. Berglund,et al.  Optically Transparent Wood from a Nanoporous Cellulosic Template: Combining Functional and Structural Performance. , 2016, Biomacromolecules.

[35]  C. Park,et al.  In Situ Synthesis of Antimicrobial Silver Nanoparticles within Antifouling Zwitterionic Hydrogels by Catecholic Redox Chemistry for Wound Healing Application. , 2016, Biomacromolecules.

[36]  Kevin J. De France,et al.  Enhanced Mechanical Properties in Cellulose Nanocrystal-Poly(oligoethylene glycol methacrylate) Injectable Nanocomposite Hydrogels through Control of Physical and Chemical Cross-Linking. , 2016, Biomacromolecules.

[37]  Hong Shen,et al.  Facile Construction of pH- and Redox-Responsive Micelles from a Biodegradable Poly(β-hydroxyl amine) for Drug Delivery. , 2016, Biomacromolecules.

[38]  F. Cousin,et al.  Structural Description of the Interface of Pickering Emulsions Stabilized by Cellulose Nanocrystals. , 2016, Biomacromolecules.

[39]  Y. Lvov,et al.  Halloysite Clay Nanotubes for Enzyme Immobilization. , 2016, Biomacromolecules.

[40]  G. Schatz,et al.  Energy landscapes and function of supramolecular systems , 2015, Nature materials.

[41]  E. Chen,et al.  Completely recyclable biopolymers with linear and cyclic topologies via ring-opening polymerization of γ-butyrolactone. , 2016, Nature chemistry.

[42]  S. Heilshorn,et al.  Adaptable Hydrogel Networks with Reversible Linkages for Tissue Engineering , 2015, Advanced materials.

[43]  P. Gatenholm,et al.  3D Bioprinting Human Chondrocytes with Nanocellulose-Alginate Bioink for Cartilage Tissue Engineering Applications. , 2015, Biomacromolecules.

[44]  Stefan Tenzer,et al.  Protein corona of nanoparticles: distinct proteins regulate the cellular uptake. , 2015, Biomacromolecules.

[45]  Thomas H. Epps,et al.  Light‐Mediated Activation of siRNA Release in Diblock Copolymer Assemblies for Controlled Gene Silencing , 2015, Advanced healthcare materials.

[46]  Liqing Wei,et al.  Grafting of bacterial polyhydroxybutyrate (PHB) onto cellulose via in situ reactive extrusion with dicumyl peroxide. , 2015, Biomacromolecules.

[47]  K. Neoh,et al.  Tea stains-inspired initiator primer for surface grafting of antifouling and antimicrobial polymer brush coatings. , 2015, Biomacromolecules.

[48]  J. D. de Pablo,et al.  Chirality-selected phase behaviour in ionic polypeptide complexes , 2015, Nature Communications.

[49]  Lin Yu,et al.  Thermogelling polymer-platinum(IV) conjugates for long-term delivery of cisplatin. , 2015, Biomacromolecules.

[50]  D. Jo,et al.  Bioreducible shell-cross-linked hyaluronic acid nanoparticles for tumor-targeted drug delivery. , 2015, Biomacromolecules.

[51]  Thomas H. Epps,et al.  Light-Mediated Activation of siRNA Release in Diblock Copolymer Assemblies for Controlled Gene Silencing. , 2015, Advanced healthcare materials.

[52]  Jianhua Zhang,et al.  PEG-b-PCL copolymer micelles with the ability of pH-controlled negative-to-positive charge reversal for intracellular delivery of doxorubicin. , 2014, Biomacromolecules.

[53]  En-Wei Lin,et al.  Therapeutic protein-polymer conjugates: advancing beyond PEGylation. , 2014, Journal of the American Chemical Society.

[54]  Boxin Zhao,et al.  Dual responsive pickering emulsion stabilized by poly[2-(dimethylamino)ethyl methacrylate] grafted cellulose nanocrystals. , 2014, Biomacromolecules.

[55]  S. Sharma,et al.  Aerogel microspheres from natural cellulose nanofibrils and their application as cell culture scaffold. , 2014, Biomacromolecules.

[56]  Paula T. Hammond,et al.  A Convergent Synthetic Platform for Single-Nanoparticle Combination Cancer Therapy: Ratiometric Loading and Controlled Release of Cisplatin, Doxorubicin, and Camptothecin , 2014, Journal of the American Chemical Society.

[57]  Jeong Hyun Seo,et al.  Mussel-mimetic protein-based adhesive hydrogel. , 2014, Biomacromolecules.

[58]  Gregory L. Szeto,et al.  Structure-based programming of lymph-node targeting in molecular vaccines , 2014, Nature.

[59]  Byeong‐Su Kim,et al.  Light-responsive micelles of spiropyran initiated hyperbranched polyglycerol for smart drug delivery. , 2014, Biomacromolecules.

[60]  G. Vunjak‐Novakovic,et al.  Electrically Conductive Chitosan/Carbon Scaffolds for Cardiac Tissue Engineering , 2014, Biomacromolecules.

[61]  Lichen Yin,et al.  Redox-responsive, core-cross-linked micelles capable of on-demand, concurrent drug release and structure disassembly. , 2013, Biomacromolecules.

[62]  En-Wei Lin,et al.  Trehalose glycopolymers as excipients for protein stabilization. , 2013, Biomacromolecules.

[63]  Xuesi Chen,et al.  pH-Triggered charge-reversal polypeptide nanoparticles for cisplatin delivery: preparation and in vitro evaluation. , 2013, Biomacromolecules.

[64]  L. Kiessling,et al.  Glycopolymer probes of signal transduction. , 2013, Chemical Society reviews.

[65]  Qinglin Wu,et al.  Self-assembling behavior of cellulose nanoparticles during freeze-drying: effect of suspension concentration, particle size, crystal structure, and surface charge. , 2013, Biomacromolecules.

[66]  E. J. Foster,et al.  Isolation of thermally stable cellulose nanocrystals by phosphoric acid hydrolysis. , 2013, Biomacromolecules.

[67]  Henrik Birkedal,et al.  Self-healing mussel-inspired multi-pH-responsive hydrogels. , 2013, Biomacromolecules.

[68]  Akira Isogai,et al.  An ultrastrong nanofibrillar biomaterial: the strength of single cellulose nanofibrils revealed via sonication-induced fragmentation. , 2013, Biomacromolecules.

[69]  L. Kiessling,et al.  Noncarbohydrate glycomimetics and glycoprotein surrogates as DC-SIGN antagonists and agonists. , 2012, ACS chemical biology.

[70]  F. Caruso,et al.  Immobilization and intracellular delivery of an anticancer drug using mussel-inspired polydopamine capsules. , 2012, Biomacromolecules.

[71]  Chun-Nan Wu,et al.  Ultrastrong and high gas-barrier nanocellulose/clay-layered composites. , 2012, Biomacromolecules.

[72]  H. Maynard,et al.  Trehalose glycopolymers for stabilization of protein conjugates to environmental stressors. , 2012, Journal of the American Chemical Society.

[73]  Chang‐Ming Dong,et al.  Photoresponsive poly(S-(o-nitrobenzyl)-L-cysteine)-b-PEO from a L-cysteine N-carboxyanhydride monomer: synthesis, self-assembly, and phototriggered drug release. , 2012, Biomacromolecules.

[74]  A. Isogai,et al.  Relationship between length and degree of polymerization of TEMPO-oxidized cellulose nanofibrils. , 2012, Biomacromolecules.

[75]  H. Bizot,et al.  Modulation of cellulose nanocrystals amphiphilic properties to stabilize oil/water interface. , 2012, Biomacromolecules.

[76]  J. Risbo,et al.  Transparent films based on PLA and montmorillonite with tunable oxygen barrier properties. , 2012, Biomacromolecules.

[77]  Olli Ikkala,et al.  Strong and tough cellulose nanopaper with high specific surface area and porosity. , 2011, Biomacromolecules.

[78]  Yaling Zhang,et al.  Synthesis of multiresponsive and dynamic chitosan-based hydrogels for controlled release of bioactive molecules. , 2011, Biomacromolecules.

[79]  Hua Yue,et al.  Surface charge affects cellular uptake and intracellular trafficking of chitosan-based nanoparticles. , 2011, Biomacromolecules.

[80]  B. Simmons,et al.  Transition of cellulose crystalline structure and surface morphology of biomass as a function of ionic liquid pretreatment and its relation to enzymatic hydrolysis. , 2011, Biomacromolecules.

[81]  Jin-Kyu Lee,et al.  Bioinspired polymerization of dopamine to generate melanin-like nanoparticles having an excellent free-radical-scavenging property. , 2011, Biomacromolecules.

[82]  O. Ikkala,et al.  Clay nanopaper with tough cellulose nanofiber matrix for fire retardancy and gas barrier functions. , 2011, Biomacromolecules.

[83]  Andong Liu,et al.  Fast preparation procedure for large, flat cellulose and cellulose/inorganic nanopaper structures. , 2010, Biomacromolecules.

[84]  Zhaoxia Jin,et al.  Fabrication, mechanical properties, and biocompatibility of graphene-reinforced chitosan composites. , 2010, Biomacromolecules.

[85]  A. Isogai,et al.  Entire surface oxidation of various cellulose microfibrils by TEMPO-mediated oxidation. , 2010, Biomacromolecules.

[86]  Ru Cheng,et al.  Shell-sheddable micelles based on dextran-SS-poly(epsilon-caprolactone) diblock copolymer for efficient intracellular release of doxorubicin. , 2010, Biomacromolecules.

[87]  V. Vergaro,et al.  Cytocompatibility and uptake of halloysite clay nanotubes. , 2010, Biomacromolecules.

[88]  O. Rojas,et al.  Nanofiber composites of polyvinyl alcohol and cellulose nanocrystals: manufacture and characterization. , 2010, Biomacromolecules.

[89]  Akira Isogai,et al.  Elastic modulus of single cellulose microfibrils from tunicate measured by atomic force microscopy. , 2009, Biomacromolecules.

[90]  Akira Isogai,et al.  Individualization of nano-sized plant cellulose fibrils by direct surface carboxylation using TEMPO catalyst under neutral conditions. , 2009, Biomacromolecules.

[91]  Ivan Donati,et al.  Non-cytotoxic silver nanoparticle-polysaccharide nanocomposites with antimicrobial activity. , 2009, Biomacromolecules.

[92]  A. Dufresne,et al.  Cellulose whiskers versus microfibrils: influence of the nature of the nanoparticle and its surface functionalization on the thermal and mechanical properties of nanocomposites. , 2009, Biomacromolecules.

[93]  Yi Liu,et al.  Investigation of the interaction between Berberine and human serum albumin. , 2009, Biomacromolecules.

[94]  Akira Isogai,et al.  Transparent and high gas barrier films of cellulose nanofibers prepared by TEMPO-mediated oxidation. , 2009, Biomacromolecules.

[95]  Abhishek Sahu,et al.  Fluorescence study of the curcumin-casein micelle complexation and its application as a drug nanocarrier to cancer cells. , 2008, Biomacromolecules.

[96]  Marielle Henriksson,et al.  Cellulose nanopaper structures of high toughness. , 2008, Biomacromolecules.

[97]  Shaoyi Jiang,et al.  Zwitterionic polymers exhibiting high resistance to nonspecific protein adsorption from human serum and plasma. , 2008, Biomacromolecules.

[98]  Kentaro Abe,et al.  The effect of hemicelluloses on wood pulp nanofibrillation and nanofiber network characteristics. , 2008, Biomacromolecules.

[99]  H. Tajmir-Riahi,et al.  Interaction of β-Lactoglobulin with Resveratrol and its Biological Implications , 2008 .

[100]  J. Putaux,et al.  The shape and size distribution of crystalline nanoparticles prepared by acid hydrolysis of native cellulose. , 2008, Biomacromolecules.

[101]  H. Yano,et al.  Obtaining cellulose nanofibers with a uniform width of 15 nm from wood. , 2007, Biomacromolecules.

[102]  Akira Isogai,et al.  Cellulose nanofibers prepared by TEMPO-mediated oxidation of native cellulose. , 2007, Biomacromolecules.

[103]  Peter Fredericks,et al.  Interactions between alginate and chitosan biopolymers characterized using FTIR and XPS. , 2007, Biomacromolecules.

[104]  Jeffrey A Hubbell,et al.  PEG-SS-PPS: reduction-sensitive disulfide block copolymer vesicles for intracellular drug delivery. , 2007, Biomacromolecules.

[105]  O. Ikkala,et al.  Enzymatic hydrolysis combined with mechanical shearing and high-pressure homogenization for nanoscale cellulose fibrils and strong gels. , 2007, Biomacromolecules.

[106]  Hua Dong,et al.  New nanocomposite materials reinforced with flax cellulose nanocrystals in waterborne polyurethane. , 2007, Biomacromolecules.

[107]  H. Ohno,et al.  Superior solubility of polysaccharides in low viscosity, polar, and halogen-free 1,3-dialkylimidazolium formates. , 2006, Biomacromolecules.

[108]  A. Mikos,et al.  Electrospun poly(epsilon-caprolactone) microfiber and multilayer nanofiber/microfiber scaffolds: characterization of scaffolds and measurement of cellular infiltration. , 2006, Biomacromolecules.

[109]  Akira Isogai,et al.  Homogeneous suspensions of individualized microfibrils from TEMPO-catalyzed oxidation of native cellulose. , 2006, Biomacromolecules.

[110]  S. Ramakrishna,et al.  Coaxial electrospinning of (fluorescein isothiocyanate-conjugated bovine serum albumin)-encapsulated poly(epsilon-caprolactone) nanofibers for sustained release. , 2006, Biomacromolecules.

[111]  Thommey P. Thomas,et al.  PAMAM dendrimer-based multifunctional conjugate for cancer therapy: synthesis, characterization, and functionality. , 2006, Biomacromolecules.

[112]  M. Wolcott,et al.  Study of biodegradable polylactide/poly(butylene adipate-co-terephthalate) blends. , 2006, Biomacromolecules.

[113]  Lu Shen,et al.  Preparation and mechanical properties of chitosan/carbon nanotubes composites. , 2005, Biomacromolecules.

[114]  S. Ramakrishna,et al.  Characterization of the surface biocompatibility of the electrospun PCL-collagen nanofibers using fibroblasts. , 2005, Biomacromolecules.

[115]  Kam W Leong,et al.  Sustained release of proteins from electrospun biodegradable fibers. , 2005, Biomacromolecules.

[116]  S. Eichhorn,et al.  Elastic modulus and stress-transfer properties of tunicate cellulose whiskers. , 2005, Biomacromolecules.

[117]  M. Roman,et al.  Effect of reaction conditions on the properties and behavior of wood cellulose nanocrystal suspensions. , 2005, Biomacromolecules.

[118]  Robert Langer,et al.  Controlled degradation and mechanical behavior of photopolymerized hyaluronic acid networks. , 2005, Biomacromolecules.

[119]  Akira Isogai,et al.  TEMPO-mediated oxidation of native cellulose. The effect of oxidation conditions on chemical and crystal structures of the water-insoluble fractions. , 2004, Biomacromolecules.

[120]  M. Roman,et al.  Effect of sulfate groups from sulfuric acid hydrolysis on the thermal degradation behavior of bacterial cellulose. , 2004, Biomacromolecules.

[121]  Ung-Jin Kim,et al.  Structure and properties of silk hydrogels. , 2004, Biomacromolecules.

[122]  R. Koepsel,et al.  Permanent, nonleaching antibacterial surfaces. 1. Synthesis by atom transfer radical polymerization. , 2004, Biomacromolecules.

[123]  Jun Zhang,et al.  Homogeneous acetylation of cellulose in a new ionic liquid. , 2004, Biomacromolecules.

[124]  David L Kaplan,et al.  Porous 3-D scaffolds from regenerated silk fibroin. , 2004, Biomacromolecules.

[125]  Benjamin Thierry,et al.  Bioactive coatings of endovascular stents based on polyelectrolyte multilayers. , 2003, Biomacromolecules.

[126]  K. Healy,et al.  Synthesis and characterization of injectable poly(N-isopropylacrylamide-co-acrylic acid) hydrogels with proteolytically degradable cross-links. , 2003, Biomacromolecules.

[127]  J. Hubbell,et al.  Synthesis and physicochemical characterization of end-linked poly(ethylene glycol)-co-peptide hydrogels formed by Michael-type addition. , 2003, Biomacromolecules.

[128]  R. de Vries,et al.  Complex coacervation of whey proteins and gum arabic. , 2003, Biomacromolecules.

[129]  C. Tribet,et al.  Ionic strength dependence of protein-polyelectrolyte interactions. , 2003, Biomacromolecules.

[130]  Allon I Hochbaum,et al.  Rational design of cytophilic and cytophobic polyelectrolyte multilayer thin films. , 2003, Biomacromolecules.

[131]  Glenn D Prestwich,et al.  Disulfide cross-linked hyaluronan hydrogels. , 2002, Biomacromolecules.

[132]  Changyou Gao,et al.  Surface modification of polycaprolactone membrane via aminolysis and biomacromolecule immobilization for promoting cytocompatibility of human endothelial cells. , 2002, Biomacromolecules.

[133]  David L Kaplan,et al.  Electrospinning Bombyx mori silk with poly(ethylene oxide). , 2002, Biomacromolecules.

[134]  Bruce P. Lee,et al.  Synthesis and gelation of DOPA-modified poly(ethylene glycol) hydrogels. , 2002, Biomacromolecules.

[135]  Ashutosh Chilkoti,et al.  Genetically encoded synthesis of protein-based polymers with precisely specified molecular weight and sequence by recursive directional ligation: examples from the elastin-like polypeptide system. , 2002, Biomacromolecules.

[136]  David G Simpson,et al.  Electrospinning of collagen nanofibers. , 2002, Biomacromolecules.

[137]  S. Pérez,et al.  Molecular basis of C(2+)-induced gelation in alginates and pectins: the egg-box model revisited. , 2001, Biomacromolecules.

[138]  A. Domard,et al.  Relation between the degree of acetylation and the electrostatic properties of chitin and chitosan. , 2001, Biomacromolecules.

[139]  K. Kataoka,et al.  Glutathione-sensitive stabilization of block copolymer micelles composed of antisense DNA and thiolated poly(ethylene glycol)-block-poly(L-lysine): a potential carrier for systemic delivery of antisense DNA. , 2001, Biomacromolecules.

[140]  P. Langan,et al.  X-ray structure of mercerized cellulose II at 1 a resolution. , 2001, Biomacromolecules.

[141]  J. Hubbell,et al.  Conjugate addition reactions combined with free-radical cross-linking for the design of materials for tissue engineering. , 2001, Biomacromolecules.

[142]  P. Dubois,et al.  Mechanisms and Kinetics of Thermal Degradation of Poly(ε-caprolactone) , 2001 .

[143]  V. Normand,et al.  New insight into agarose gel mechanical properties. , 2000, Biomacromolecules.

[144]  O. Abián,et al.  Multifunctional epoxy supports: a new tool to improve the covalent immobilization of proteins. The promotion of physical adsorptions of proteins on the supports before their covalent linkage. , 2000, Biomacromolecules.

[145]  R. Larossa,et al.  Quaternary ammonium functionalized poly(propylene imine) dendrimers as effective antimicrobials: structure-activity studies. , 2000, Biomacromolecules.

[146]  T. Kondo,et al.  Periodate oxidation of crystalline cellulose. , 2000, Biomacromolecules.

[147]  M Cornelissen,et al.  Structural and rheological properties of methacrylamide modified gelatin hydrogels. , 2000, Biomacromolecules.

[148]  R. Gross,et al.  Candida antartica lipase B catalyzed polycaprolactone synthesis: effects of organic media and temperature. , 2000, Biomacromolecules.