The Experts below are selected from a list of 297 Experts worldwide ranked by ideXlab platform
Daniela A Wilson - One of the best experts on this subject based on the ideXlab platform.
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Spatial control over catalyst positioning on biodegradable polymeric nanomotors
Nature Communications, 2019Co-Authors: B. Jelle Toebes, F. Cao, Daniela A WilsonAbstract:Scientists over the world are inspired by biological nanomotors and try to mimic these complex structures. In recent years multiple nanomotors have been created for various fields, such as biomedical applications or environmental remediation, which require a different design both in terms of size and shape, as well as material properties. So far, only relatively simple designs for synthetic nanomotors have been reported. Herein, we report an approach to create biodegradable polymeric nanomotors with a multivalent design. PEG-PDLLA (poly(ethylene glycol)-b-poly(D,L-lactide)) Stomatocytes with azide handles were created that were selectively reduced on the outside surface by TCEP (tris(2-carboxyethyl)phosphine) functionalized beads. Thereby, two different functional handles were created, both on the inner and outer surface of the Stomatocytes, providing spatial control for catalyst positioning. Enzymes were coupled on the inside of the Stomatocyte to induce motion in the presence of fuel, while fluorophores and other molecules can be attached on the outside.
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Spatial control over catalyst positioning on biodegradable polymeric nanomotors
Nature Communications, 2019Co-Authors: B. Jelle Toebes, F. Cao, Daniela A WilsonAbstract:Multiple nanomotors for application in various fields have been fabricated, but so far only relatively simple designs for synthetic nanomotors are reported. Here, the authors report on a biodegradable polymeric nanomotor and demonstrate spatial control for catalyst positioning. Scientists over the world are inspired by biological nanomotors and try to mimic these complex structures. In recent years multiple nanomotors have been created for various fields, such as biomedical applications or environmental remediation, which require a different design both in terms of size and shape, as well as material properties. So far, only relatively simple designs for synthetic nanomotors have been reported. Herein, we report an approach to create biodegradable polymeric nanomotors with a multivalent design. PEG-PDLLA (poly(ethylene glycol)-b-poly( D,L -lactide)) Stomatocytes with azide handles were created that were selectively reduced on the outside surface by TCEP (tris(2-carboxyethyl)phosphine) functionalized beads. Thereby, two different functional handles were created, both on the inner and outer surface of the Stomatocytes, providing spatial control for catalyst positioning. Enzymes were coupled on the inside of the Stomatocyte to induce motion in the presence of fuel, while fluorophores and other molecules can be attached on the outside.
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Nonequilibrium Reshaping of Polymersomes via Polymer Addition.
ACS Nano, 2019Co-Authors: Yongjun Men, Geertjan A Janssen, Roeland J. M. Nolte, Fei Peng, Daniela A WilsonAbstract:Polymersomes are a class of artificial liposomes, assembled from amphiphilic synthetic block copolymers, holding great promise toward applications in nanomedicine. The diversity in polymersome morphological shapes and, in particular, the precise control of these shapes, which is an important aspect in drug delivery studies, remains a great challenge. This is due to a lack of general methodologies that can be applied and the inability to capture the morphologies at the nanometer scale. Here, we present a methodology that can accurately control the shape of polymersomes via the addition of polyethylene glycol (PEG) under nonequilibrium conditions. Various shapes including spheres, ellipsoids, tubes, discs, Stomatocytes, nests, Stomatocyte-in-Stomatocytes, disc-in-discs, and large compound vesicles (LCVs) can be uniformly captured by adjusting the water content and the PEG concentration. Moreover, these shapes undergo nonequilibrium changes in time, which is reflected in their phase diagram changes. This research provides a universal tool to fabricate all shapes of polymersomes by controlling three variables: water content, PEG concentration, and time. The use of the biofriendly polymer PEG enables the application of this methodology in the field of nanomedicine.
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Motion Control of Polymeric Nanomotors Based on Host–Guest Interactions
Angewandte Chemie, 2019Co-Authors: Yingfeng Tu, Josje M. Heuvelmans, Roeland J. M. Nolte, Fei Peng, Daniela A WilsonAbstract:Controlling the motion of artificial self-propelled micro- and nanomotors independent of the fuel concentration is still a great challenge. Here we describe the first report of speed manipulation of supramolecular nanomotors via blue light-responsive valves, which can regulate the access of hydrogen peroxide fuel into the motors. Light-sensitive polymeric nanomotors are built up via the self-assembly of functional block copolymers, followed by bowl-shaped Stomatocyte formation and incorporation of platinum nanoparticles. Subsequent addition of β-cyclodextrin (β-CD) leads to the formation of inclusion complexes with the trans-isomers of the azobenzene derivatives grafted from the surfaces of the Stomatocytes. β-CDs attachment decreases the diffusion rate of hydrogen peroxide into the cavities of the motors because of partly blocking of the openings of the Stomatocyte. This results in a lowering of the speed of the nanomotors. Upon blue light irradiation, the trans-azobenzene moieties isomerize to the cis-form, which lead to the detachment of the β-CDs due to their inability to form complexes with the cis-isomer. As a result, the speed of the nanomotors increases accordingly. Such a conformational change provides us with the unique possibility to control the speed of the supramolecular nanomotor via light-responsive host-guest complexation. We envision that such artificial responsive nano-systems with controlled motion could have potential applications in drug delivery.
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Stomatocyte in Stomatocyte: A New Shape of Polymersome Induced via Chemical-Addition Methodology.
Nano Letters, 2018Co-Authors: Yongjun Men, Geertjan A Janssen, Roger S. M. Rikken, Daniela A WilsonAbstract:Accurate control of the shape transformation of polymersome is an important and interesting challenge that spans across disciplines such as nanomedicine and nanomachine. Here, we report a fast and facile methodology of shape manipulation of polymersome via out-of-equilibrium polymer self-assembly and shape change by chemical addition of additives. Due to its increased permeability, hydrophilicity, and fusogenic properties, poly(ethylene oxide) was selected as the additive for bringing the system out of equilibrium via fast addition into the polymersome organic solution. A new shape, Stomatocyte-in-Stomatocyte (sto-in-sto), is obtained for the first time. Moreover, fast shape transformation within less than 1 min to other relevant shapes such as Stomatocyte and large compound vesicles was also obtained and accurately controlled in a uniform dispersion. This methodology is demonstrated as a general strategy with which to push the assembly further out of equilibrium to generate unusual nanostructures in a co...
Fei Peng - One of the best experts on this subject based on the ideXlab platform.
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Nonequilibrium Reshaping of Polymersomes via Polymer Addition.
ACS Nano, 2019Co-Authors: Yongjun Men, Geertjan A Janssen, Roeland J. M. Nolte, Fei Peng, Daniela A WilsonAbstract:Polymersomes are a class of artificial liposomes, assembled from amphiphilic synthetic block copolymers, holding great promise toward applications in nanomedicine. The diversity in polymersome morphological shapes and, in particular, the precise control of these shapes, which is an important aspect in drug delivery studies, remains a great challenge. This is due to a lack of general methodologies that can be applied and the inability to capture the morphologies at the nanometer scale. Here, we present a methodology that can accurately control the shape of polymersomes via the addition of polyethylene glycol (PEG) under nonequilibrium conditions. Various shapes including spheres, ellipsoids, tubes, discs, Stomatocytes, nests, Stomatocyte-in-Stomatocytes, disc-in-discs, and large compound vesicles (LCVs) can be uniformly captured by adjusting the water content and the PEG concentration. Moreover, these shapes undergo nonequilibrium changes in time, which is reflected in their phase diagram changes. This research provides a universal tool to fabricate all shapes of polymersomes by controlling three variables: water content, PEG concentration, and time. The use of the biofriendly polymer PEG enables the application of this methodology in the field of nanomedicine.
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Motion Control of Polymeric Nanomotors Based on Host–Guest Interactions
Angewandte Chemie, 2019Co-Authors: Yingfeng Tu, Josje M. Heuvelmans, Roeland J. M. Nolte, Fei Peng, Daniela A WilsonAbstract:Controlling the motion of artificial self-propelled micro- and nanomotors independent of the fuel concentration is still a great challenge. Here we describe the first report of speed manipulation of supramolecular nanomotors via blue light-responsive valves, which can regulate the access of hydrogen peroxide fuel into the motors. Light-sensitive polymeric nanomotors are built up via the self-assembly of functional block copolymers, followed by bowl-shaped Stomatocyte formation and incorporation of platinum nanoparticles. Subsequent addition of β-cyclodextrin (β-CD) leads to the formation of inclusion complexes with the trans-isomers of the azobenzene derivatives grafted from the surfaces of the Stomatocytes. β-CDs attachment decreases the diffusion rate of hydrogen peroxide into the cavities of the motors because of partly blocking of the openings of the Stomatocyte. This results in a lowering of the speed of the nanomotors. Upon blue light irradiation, the trans-azobenzene moieties isomerize to the cis-form, which lead to the detachment of the β-CDs due to their inability to form complexes with the cis-isomer. As a result, the speed of the nanomotors increases accordingly. Such a conformational change provides us with the unique possibility to control the speed of the supramolecular nanomotor via light-responsive host-guest complexation. We envision that such artificial responsive nano-systems with controlled motion could have potential applications in drug delivery.
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Redox‐Sensitive Stomatocyte Nanomotors: Destruction and Drug Release in the Presence of Glutathione
Angewandte Chemie, 2017Co-Authors: Yingfeng Tu, Paul B White, Fei Peng, Daniela A WilsonAbstract:The development of artificial nanomotor systems that are stimuli-responsive is still posing many challenges. Herein, we demonstrate the self-assembly of a redox-responsive Stomatocyte nanomotor system, which can be used for triggered drug release under biological reducing conditions. The redox sensitivity was introduced by incorporating a disulfide bridge between the hydrophilic poly(ethylene glycol) block and the hydrophobic polystyrene block. When incubated with the endogenous reducing agent glutathione at a concentration comparable to that within cells, the external PEG shells of these stimuli-responsive nanomotors are cleaved. The specific bowl-shaped Stomatocytes aggregate after the treatment with glutathione, leading to the loss of motion and triggered drug release. These novel redox-responsive nanomotors can not only be used for remote transport but also for drug delivery, which is promising for future biomedical applications.
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Redox-Sensitive Stomatocyte Nanomotors: Destruction and Drug Release in the Presence of Glutathione.
Angewandte Chemie (International ed. in English), 2017Co-Authors: Yingfeng Tu, Paul B White, Fei Peng, Daniela A WilsonAbstract:The development of artificial nanomotor systems that are stimuli-responsive is still posing many challenges. Herein, we demonstrate the self-assembly of a redox-responsive Stomatocyte nanomotor system, which can be used for triggered drug release under biological reducing conditions. The redox sensitivity was introduced by incorporating a disulfide bridge between the hydrophilic poly(ethylene glycol) block and the hydrophobic polystyrene block. When incubated with the endogenous reducing agent glutathione at a concentration comparable to that within cells, the external PEG shells of these stimuli-responsive nanomotors are cleaved. The specific bowl-shaped Stomatocytes aggregate after the treatment with glutathione, leading to the loss of motion and triggered drug release. These novel redox-responsive nanomotors can not only be used for remote transport but also for drug delivery, which is promising for future biomedical applications.
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Self-destroyed Redox-sensitive Stomatocyte Nanomotor
Angewandte Chemie, 2017Co-Authors: Fei Peng, Paul B White, Daniela A WilsonAbstract:The development of artificial nanomotor systems capable of stimuli responsiveness is still posing many challenges. Here we demonstrate the self-assembly of a redox-responsive Stomatocyte nanomotor system, which can be used for triggered drug release under biological reducing conditions. The redox sensitivity was introduced via the disulfide bridge between hydrophilic poly(ethylene glycol) block and hydrophobic polystyrene block. When incubating with endogenous reducing agent glutathione at a concentration comparable to the one within cells, the external PEG shells of these stimuli-responsive nanomotors were cleaved. The specific bowl-shaped Stomatocyte aggregated after the treatment with glutathione, leading to the loss of motion and triggered drug release. These novel bio-redox responsive nanomotors achieve not only remote transport but also potential drug delivery, which is promising for future biomedical applications.
Jan C. M. Van Hest - One of the best experts on this subject based on the ideXlab platform.
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atp mediated transient behavior of Stomatocyte nanosystems
Angewandte Chemie, 2019Co-Authors: Hailong Che, Loai K. E. A. Abdelmohsen, Jianzhi Zhu, Shidong Song, Alexander F. Mason, Shoupeng Cao, Imke A. B. Pijpers, Jan C. M. Van HestAbstract:In nature, dynamic processes are ubiquitous and often characterized by adaptive, transient behavior. Herein, we present the development of a transient bowl-shaped nanoreactor system, or Stomatocyte, the properties of which are mediated by molecular interactions. In a stepwise fashion, we couple motility to a dynamic process, which is maintained by transient events; namely, binding and unbinding of adenosine triphosphate (ATP). The surface of the nanosystem is decorated with polylysine (PLL), and regulation is achieved by addition of ATP. The dynamic interaction between PLL and ATP leads to an increase in the hydrophobicity of the PLL-ATP complex and subsequently to a collapse of the polymer; this causes a narrowing of the opening of the Stomatocytes. The presence of the apyrase, which hydrolyzes ATP, leads to a decrease of the ATP concentration, decomplexation of PLL, and reopening of the Stomatocyte. The competition between ATP input and consumption gives rise to a transient state that is controlled by the out-of-equilibrium process.
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ATP‐Mediated Transient Behavior of Stomatocyte Nanosystems
Angewandte Chemie, 2019Co-Authors: Hailong Che, Loai K. E. A. Abdelmohsen, Jianzhi Zhu, Shidong Song, Alexander F. Mason, Shoupeng Cao, Imke A. B. Pijpers, Jan C. M. Van HestAbstract:In nature, dynamic processes are ubiquitous and often characterized by adaptive, transient behavior. Herein, we present the development of a transient bowl-shaped nanoreactor system, or Stomatocyte, the properties of which are mediated by molecular interactions. In a stepwise fashion, we couple motility to a dynamic process, which is maintained by transient events; namely, binding and unbinding of adenosine triphosphate (ATP). The surface of the nanosystem is decorated with polylysine (PLL), and regulation is achieved by addition of ATP. The dynamic interaction between PLL and ATP leads to an increase in the hydrophobicity of the PLL-ATP complex and subsequently to a collapse of the polymer; this causes a narrowing of the opening of the Stomatocytes. The presence of the apyrase, which hydrolyzes ATP, leads to a decrease of the ATP concentration, decomplexation of PLL, and reopening of the Stomatocyte. The competition between ATP input and consumption gives rise to a transient state that is controlled by the out-of-equilibrium process.
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Biomorphic Engineering of Multifunctional Polylactide Stomatocytes toward Therapeutic Nano-Red Blood Cells.
Advanced Science, 2019Co-Authors: Jingxin Shao, Loai K. E. A. Abdelmohsen, David S. Williams, Shoupeng Cao, Imke A. B. Pijpers, Xuehai Yan, Jan C. M. Van HestAbstract:Morphologically discrete nanoarchitectures, which mimic the structural complexity of biological systems, are an increasingly popular design paradigm in the development of new nanomedical technologies. Herein, engineered polymeric Stomatocytes are presented as a structural and functional mimic of red blood cells (RBCs) with multifunctional therapeutic features. Stomatocytes, comprising biodegradable poly(ethylene glycol)-block-poly(D,L-lactide), possess an oblate-like morphology reminiscent of RBCs. This unique dual-compartmentalized structure is augmented via encapsulation of multifunctional cargo (oxygen-binding hemoglobin and the photosensitizer chlorin e6). Furthermore, Stomatocytes are decorated with a cell membrane isolated from erythrocytes to ensure that the surface characteristics matched those of RBCs. In vivo biodistribution data reveal that both the uncoated and coated nano-RBCs have long circulation times in mice, with the membrane-coated ones outperforming the uncoated stomatoctyes. The capacity of nano-RBCs to transport oxygen and create oxygen radicals upon exposure to light is effectively explored toward photodynamic therapy, using 2D and 3D tumor models; addressing the challenge presented by cancer-induced hypoxia. The morphological and functional control demonstrated by this synthetic nanosystem, coupled with indications of therapeutic efficacy, constitutes a highly promising platform for future clinical application.
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Morphology Under Control: Engineering Biodegradable Stomatocytes.
ACS Macro Letters, 2017Co-Authors: Imke A. B. Pijpers, Loai K. E. A. Abdelmohsen, David S. Williams, Jan C. M. Van HestAbstract:Biodegradable nanoarchitectures, with well-defined morphological features, are of great importance for nanomedical research; however, understanding (and thereby engineering) their formation is a substantial challenge. Herein, we uncover the supramolecular potential of PEG–PDLLA copolymers by exploring the physicochemical determinants that result in the transformation of spherical polymersomes into Stomatocytes. To this end, we have engineered blended polymersomes (comprising copolymers with varying lengths of PEG), which undergo solvent-dependent reorganization inducing negative spontaneous membrane curvature. Under conditions of anisotropic solvent composition across the PDLLA membrane, facilitated by the dialysis methodology, we demonstrate osmotically induced Stomatocyte formation as a consequence of changes in PEG solvation, inducing negative spontaneous membrane curvature. Controlled formation of unprecedented, biodegradable Stomatocytes represents the unification of supramolecular engineering with t...
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Sub‐Micron Polymeric Stomatocytes as Promising Templates for Confined Crystallization and Diffraction Experiments
Small, 2017Co-Authors: Alaa Adawy, Jan C. M. Van Hest, Zakariae Amghouz, Daniela A WilsonAbstract:The possibility of using sub-micrometer polymeric Stomatocytes is investigated to effectuate confined crystallization of inorganic compounds. These bowl-shaped polymeric compartments facilitate confined crystallization while their glassy surfaces provide their crystalline cargos with convenient shielding from the electron beam's harsh effects during transmission electron microscopy experiments. Stomatocytes host the growth of a single nanocrystal per nanocavity, and the electron diffraction experiments reveal that their glassy membranes do not interfere with the diffraction patterns obtained from their crystalline cargos. Therefore, it is expected that the encapsulation and crystallization within these compartments can be considered as a promising template (nanovials) that hold and protect nanocrystals and protein clusters from the direct radiation damage before data acquisition, while they are examined by modern crystallography methodologies such as serial femtosecond crystallography.
Sei Kwang Hahn - One of the best experts on this subject based on the ideXlab platform.
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light guided nanomotor systems for autonomous photothermal cancer therapy
ACS Applied Materials & Interfaces, 2018Co-Authors: Hyunsik Choi, Sei Kwang HahnAbstract:Machines have greatly contributed to the human civilization, enabling tasks beyond our capacities for improved quality of life. Recently, the progress in nanotechnology has triggered to build a miniaturized machine of nanoscale. In this context, synthetic nanomotors have gained considerable interest because of their great promise for diverse applications. Currently, the movement control of these nanomotors has been widely investigated using various stimuli. Here, we demonstrate near-infrared (NIR) light controlled on/off motion of Stomatocyte nanomotors powered by the conversion of hydrogen peroxide. The nanomotors encapsulating naphthalocyanine (NC) are aggregated or separated (collective motion) with or without near-IR light illumination, resulting in the well-controlled movement. Remarkably, the nanomotors can move directionally toward hydrogen peroxide released from cancer cells and photothermally ablate the cancer cells. Taken together, our Stomatocyte nanomotor systems can be effectively harnessed f...
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Light-Guided Nanomotor Systems for Autonomous Photothermal Cancer Therapy
2017Co-Authors: Hyunsik Choi, Geon-hui Lee, Ki Su Kim, Sei Kwang HahnAbstract:Machines have greatly contributed to the human civilization, enabling tasks beyond our capacities for improved quality of life. Recently, the progress in nanotechnology has triggered to build a miniaturized machine of nanoscale. In this context, synthetic nanomotors have gained considerable interest because of their great promise for diverse applications. Currently, the movement control of these nanomotors has been widely investigated using various stimuli. Here, we demonstrate near-infrared (NIR) light controlled on/off motion of Stomatocyte nanomotors powered by the conversion of hydrogen peroxide. The nanomotors encapsulating naphthalocyanine (NC) are aggregated or separated (collective motion) with or without near-IR light illumination, resulting in the well-controlled movement. Remarkably, the nanomotors can move directionally toward hydrogen peroxide released from cancer cells and photothermally ablate the cancer cells. Taken together, our Stomatocyte nanomotor systems can be effectively harnessed for autonomous photothermal cancer therapy
Loai K. E. A. Abdelmohsen - One of the best experts on this subject based on the ideXlab platform.
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atp mediated transient behavior of Stomatocyte nanosystems
Angewandte Chemie, 2019Co-Authors: Hailong Che, Loai K. E. A. Abdelmohsen, Jianzhi Zhu, Shidong Song, Alexander F. Mason, Shoupeng Cao, Imke A. B. Pijpers, Jan C. M. Van HestAbstract:In nature, dynamic processes are ubiquitous and often characterized by adaptive, transient behavior. Herein, we present the development of a transient bowl-shaped nanoreactor system, or Stomatocyte, the properties of which are mediated by molecular interactions. In a stepwise fashion, we couple motility to a dynamic process, which is maintained by transient events; namely, binding and unbinding of adenosine triphosphate (ATP). The surface of the nanosystem is decorated with polylysine (PLL), and regulation is achieved by addition of ATP. The dynamic interaction between PLL and ATP leads to an increase in the hydrophobicity of the PLL-ATP complex and subsequently to a collapse of the polymer; this causes a narrowing of the opening of the Stomatocytes. The presence of the apyrase, which hydrolyzes ATP, leads to a decrease of the ATP concentration, decomplexation of PLL, and reopening of the Stomatocyte. The competition between ATP input and consumption gives rise to a transient state that is controlled by the out-of-equilibrium process.
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ATP‐Mediated Transient Behavior of Stomatocyte Nanosystems
Angewandte Chemie, 2019Co-Authors: Hailong Che, Loai K. E. A. Abdelmohsen, Jianzhi Zhu, Shidong Song, Alexander F. Mason, Shoupeng Cao, Imke A. B. Pijpers, Jan C. M. Van HestAbstract:In nature, dynamic processes are ubiquitous and often characterized by adaptive, transient behavior. Herein, we present the development of a transient bowl-shaped nanoreactor system, or Stomatocyte, the properties of which are mediated by molecular interactions. In a stepwise fashion, we couple motility to a dynamic process, which is maintained by transient events; namely, binding and unbinding of adenosine triphosphate (ATP). The surface of the nanosystem is decorated with polylysine (PLL), and regulation is achieved by addition of ATP. The dynamic interaction between PLL and ATP leads to an increase in the hydrophobicity of the PLL-ATP complex and subsequently to a collapse of the polymer; this causes a narrowing of the opening of the Stomatocytes. The presence of the apyrase, which hydrolyzes ATP, leads to a decrease of the ATP concentration, decomplexation of PLL, and reopening of the Stomatocyte. The competition between ATP input and consumption gives rise to a transient state that is controlled by the out-of-equilibrium process.
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Biomorphic Engineering of Multifunctional Polylactide Stomatocytes toward Therapeutic Nano-Red Blood Cells.
Advanced Science, 2019Co-Authors: Jingxin Shao, Loai K. E. A. Abdelmohsen, David S. Williams, Shoupeng Cao, Imke A. B. Pijpers, Xuehai Yan, Jan C. M. Van HestAbstract:Morphologically discrete nanoarchitectures, which mimic the structural complexity of biological systems, are an increasingly popular design paradigm in the development of new nanomedical technologies. Herein, engineered polymeric Stomatocytes are presented as a structural and functional mimic of red blood cells (RBCs) with multifunctional therapeutic features. Stomatocytes, comprising biodegradable poly(ethylene glycol)-block-poly(D,L-lactide), possess an oblate-like morphology reminiscent of RBCs. This unique dual-compartmentalized structure is augmented via encapsulation of multifunctional cargo (oxygen-binding hemoglobin and the photosensitizer chlorin e6). Furthermore, Stomatocytes are decorated with a cell membrane isolated from erythrocytes to ensure that the surface characteristics matched those of RBCs. In vivo biodistribution data reveal that both the uncoated and coated nano-RBCs have long circulation times in mice, with the membrane-coated ones outperforming the uncoated stomatoctyes. The capacity of nano-RBCs to transport oxygen and create oxygen radicals upon exposure to light is effectively explored toward photodynamic therapy, using 2D and 3D tumor models; addressing the challenge presented by cancer-induced hypoxia. The morphological and functional control demonstrated by this synthetic nanosystem, coupled with indications of therapeutic efficacy, constitutes a highly promising platform for future clinical application.
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Morphology Under Control: Engineering Biodegradable Stomatocytes.
ACS Macro Letters, 2017Co-Authors: Imke A. B. Pijpers, Loai K. E. A. Abdelmohsen, David S. Williams, Jan C. M. Van HestAbstract:Biodegradable nanoarchitectures, with well-defined morphological features, are of great importance for nanomedical research; however, understanding (and thereby engineering) their formation is a substantial challenge. Herein, we uncover the supramolecular potential of PEG–PDLLA copolymers by exploring the physicochemical determinants that result in the transformation of spherical polymersomes into Stomatocytes. To this end, we have engineered blended polymersomes (comprising copolymers with varying lengths of PEG), which undergo solvent-dependent reorganization inducing negative spontaneous membrane curvature. Under conditions of anisotropic solvent composition across the PDLLA membrane, facilitated by the dialysis methodology, we demonstrate osmotically induced Stomatocyte formation as a consequence of changes in PEG solvation, inducing negative spontaneous membrane curvature. Controlled formation of unprecedented, biodegradable Stomatocytes represents the unification of supramolecular engineering with t...
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Morphology Under Control: Engineering Biodegradable Stomatocytes
2017Co-Authors: Imke A. B. Pijpers, Loai K. E. A. Abdelmohsen, David S. Williams, Jan C. M. Van HestAbstract:Biodegradable nanoarchitectures, with well-defined morphological features, are of great importance for nanomedical research; however, understanding (and thereby engineering) their formation is a substantial challenge. Herein, we uncover the supramolecular potential of PEG–PDLLA copolymers by exploring the physicochemical determinants that result in the transformation of spherical polymersomes into Stomatocytes. To this end, we have engineered blended polymersomes (comprising copolymers with varying lengths of PEG), which undergo solvent-dependent reorganization inducing negative spontaneous membrane curvature. Under conditions of anisotropic solvent composition across the PDLLA membrane, facilitated by the dialysis methodology, we demonstrate osmotically induced Stomatocyte formation as a consequence of changes in PEG solvation, inducing negative spontaneous membrane curvature. Controlled formation of unprecedented, biodegradable Stomatocytes represents the unification of supramolecular engineering with the theoretical understanding of shape transformation phenomena
