Publications by authors named "Dongyuan Zhao"

294 Publications

Sulfur-Based Aqueous Batteries: Electrochemistry and Strategies.

J Am Chem Soc 2021 Sep 12. Epub 2021 Sep 12.

Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, School of Chemistry and Materials, Fudan University, Shanghai 200433, P.R. China.

While research interest in aqueous batteries has surged due to their intrinsic low cost and high safety, the practical application is plagued by the restrictive capacity (less than 600 mAh g) of electrode materials. Sulfur-based aqueous batteries (SABs) feature high theoretical capacity (1672 mAh g), compatible potential, and affordable cost, arousing ever-increasing attention and intense efforts. Nonetheless, the underlying electrochemistry of SABs remains unclear, including complicated thermodynamic evolution and insufficient kinetics metrics. Consequently, multifarious irreversible reactions in various application systems imply the systematic complexity of SABs. Herein, rather than simply compiling recent progress, this Perspective aims to construct a theory-to-application methodology. Theoretically, attention has been paid to a critical appraisal of the aqueous-S-related electrochemistry, including fundamental properties evaluation, kinetics metrics with transient and steady-state analyses, and thermodynamic equilibrium and evolution. To put it into practice, current challenges and promising strategies are synergistically proposed. Practically, the above efforts are employed to evaluate and develop the device-scale applications, scilicet flow-SABs, oxide-SABs, and metal-SABs. Last, chemical and engineering insights are rendered collectively for the future development of high-energy SABs.
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http://dx.doi.org/10.1021/jacs.1c06923DOI Listing
September 2021

Precisely Designed Mesoscopic Titania for High-Volumetric-Density Pseudocapacitance.

J Am Chem Soc 2021 Sep 11;143(35):14097-14105. Epub 2021 Aug 11.

Laboratory of Advanced Materials, Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, People's Republic of China.

Surface redox pseudocapacitance, which enables short charging times and high power delivery, is very attractive in a wide range of sites. To achieve maximized specific capacity, nanostructuring of active materials with high surface area is indispensable. However, one key limitation for capacitive materials is their low volumetric capacity due to the low tap density of nanomaterials. Here, we present a promising mesoscale TiO structure with precisely controlled mesoporous frameworks as a high-density pseudocapacitive model system. The dense-packed mesoscopic TiO in micrometer size offers a high accessible surface area (124 m g) and radially aligned mesopore channels, but high tap density (1.7 g cm) that is much higher than TiO nanoparticles (0.47 g cm). As a pseudocapacitive sodium-ion storage anode, the precisely designed mesoscopic TiO model achieved maximized gravimetric capacity (240 mAh g) and volumetric capacity (350 mAh cm) at 0.025 A g. Such a designed pseudocapacitive mesostructure further realized a commercially comparable areal capacity (2.1 mAh cm) at a high mass loading of 9.47 mg cm. This mesostructured electrode that enables fast sodiation in dense nanostructures has implications for high-power applications, fast-charging devices, and pseudocapacitive electrode design.
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http://dx.doi.org/10.1021/jacs.1c03433DOI Listing
September 2021

A hybrid erbium(III)-bacteriochlorin near-infrared probe for multiplexed biomedical imaging.

Nat Mater 2021 Jul 29. Epub 2021 Jul 29.

Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials and iChem, Fudan University, Shanghai, People's Republic of China.

Spectrally distinct fluorophores are desired for multiplexed bioimaging. In particular, monitoring biological processes in living mammals needs fluorophores that operate in the 'tissue-transparent' near-infrared (NIR) window, that is, between 700 and 1,700 nm. Here we report a fluorophore system based on molecular erbium(III)-bacteriochlorin complexes with large Stokes shift (>750 nm) and narrowband NIR-to-NIR downconversion spectra (full-width at half-maximum ≤ 32 nm). We have found that the fast (2 × 10 s¹) and near-unity energy transfer from bacteriochlorin triplets to the erbium(III) I level overcomes the notorious vibrational overtones quenching, resulting in bright and long-lived (1.73 μs) 1,530 nm luminescence in water. We demonstrate the excitation/emission-multiplexed capability of the complexes in the visualization of dynamic circulatory and metabolic processes in living mice, and through skull tracking of cancer cell metastases in mouse brain. This hybrid probe system facilitates robust multiplexed NIR imaging with high contrast and spatial resolution for applications ranging from fluorescence-guided surgery, diagnostics and intravital microscopy.
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http://dx.doi.org/10.1038/s41563-021-01063-7DOI Listing
July 2021

Imparting multi-functionality to covalent organic framework nanoparticles by the dual-ligand assistant encapsulation strategy.

Nat Commun 2021 07 27;12(1):4556. Epub 2021 Jul 27.

Department of Chemistry, Laboratory of Advanced Materials and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, State Key Laboratory of Molecular Engineering of Polymers, Fudan University, Shanghai, PR China.

The potential applications of covalent organic frameworks (COFs) can be further developed by encapsulating functional nanoparticles within the frameworks. However, the synthesis of monodispersed [email protected] structured COF nanocomposites without agglomeration remains a significant challenge. Herein, we present a versatile dual-ligand assistant strategy for interfacial growth of COFs on the functional nanoparticles with abundant physicochemical properties. Regardless of the composition, geometry or surface properties of the core, the obtained [email protected] structured nanocomposites with controllable shell-thickness are very uniform without agglomeration. The derived bowl-shape, [email protected], [email protected]@shell nanostructures can also be fabricated delicately. As a promising type of photosensitizer for photodynamic therapy (PDT), the porphyrin-based COFs were grown onto upconversion nanoparticles (UCNPs). With the assistance of the near-infrared (NIR) to visible optical property of UCNPs core and the intrinsic porosity of COF shell, the [email protected] nanocomposites can be applied as a nanoplatform for NIR-activated PDT with deep tissue penetration and chemotherapeutic drug delivery.
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http://dx.doi.org/10.1038/s41467-021-24838-7DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8316466PMC
July 2021

Streamlined Mesoporous Silica Nanoparticles with Tunable Curvature from Interfacial Dynamic-Migration Strategy for Nanomotors.

Nano Lett 2021 07 16;21(14):6071-6079. Epub 2021 Jul 16.

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, State Key Laboratory of Molecular Engineering of Polymers, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, People's Republic of China.

Streamlined architectures with a low fluid-resistance coefficient have been receiving great attention in various fields. However, it is still a great challenge to synthesize streamlined architecture with tunable surface curvature at the nanoscale. Herein, we report a facile interfacial dynamic migration strategy for the synthesis of streamlined mesoporous nanotadpoles with varied architectures. These tadpole-like nanoparticles possess a big streamlined head and a slender tail, which exhibit large inner cavities (75-170 nm), high surface areas (424-488 m g), and uniform mesopore sizes (2.4-3.2 nm). The head curvature of the streamlined mesoporous nanoparticles can be well-tuned from ∼2.96 × 10 to ∼5.56 × 10 nm, and the tail length can also be regulated from ∼30 to ∼650 nm. By selectively loading the FeO catalyst in the cavity of the streamlined silica nanotadpoles, the HO-driven mesoporous nanomotors were designed. The mesoporous nanomotors with optimized structural parameters exhibit outstanding directionality and a diffusion coefficient of 8.15 μm s.
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http://dx.doi.org/10.1021/acs.nanolett.1c01404DOI Listing
July 2021

X-ray-activated persistent luminescence nanomaterials for NIR-II imaging.

Nat Nanotechnol 2021 09 10;16(9):1011-1018. Epub 2021 Jun 10.

Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers and iChem, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, China.

Persistent luminescence is not affected by background autofluorescence, and thus holds the promise of high-contrast bioimaging. However, at present, persistent luminescent materials for in vivo imaging are mainly bulk crystals characterized by a non-uniform size and morphology, inaccessible core-shell structures and short emission wavelengths. Here we report a series of X-ray-activated, lanthanide-doped nanoparticles with an extended emission lifetime in the second near-infrared window (NIR-II, 1,000-1,700 nm). Core-shell engineering enables a tunable NIR-II persistent luminescence, which outperforms NIR-II fluorescence in signal-to-noise ratios and the accuracy of in vivo multiplexed encoding and multilevel encryption, as well as in resolving mouse abdominal vessels, tumours and ureters in deep tissue (~2-4 mm), with up to fourfold higher signal-to-noise ratios and a threefold greater sharpness. These rationally designed nanoparticles also allow the high-contrast multiplexed imaging of viscera and multimodal NIR-II persistent luminescence-magnetic resonance-positron emission tomography imaging of murine tumours.
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http://dx.doi.org/10.1038/s41565-021-00922-3DOI Listing
September 2021

Quantized doping of CdS quantum dots with twelve gold atoms.

Chem Commun (Camb) 2021 Jun;57(52):6448-6451

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, China.

Through a bottom-up strategy, CdS quantum dots (QDs) doped with 12 gold atoms in each nanocrystal (NC) were prepared by cation exchange reactions. The (Au12) dopants inside the CdS matrix were directly observed using Cs-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images and quantitatively confirmed using the inductively coupled plasma atomic emission spectroscopy (ICP-AES) data. With a photoluminescence quantum yield (PLQY) of 37.5%, the as-prepared (Au12)@CdS QDs emitted light at 635 nm. Due to the injection of excited electrons from the lowest unoccupied molecular orbital (LUMO) of dopants to the conduction band (CB) of CdS, multiple fine peaks were observed in the photoluminescence excitation (PLE) spectra. By using clusters as starting materials, we demonstrate a universal approach for the precise tailoring of dopants and provide a pathway for band energy engineering of doped QDs.
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http://dx.doi.org/10.1039/d1cc02460dDOI Listing
June 2021

Inorganic-organic competitive coating strategy derived uniform hollow gradient-structured ferroferric oxide-carbon nanospheres for ultra-fast and long-term lithium-ion battery.

Nat Commun 2021 May 20;12(1):2973. Epub 2021 May 20.

Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, and Laboratory of Advanced Materials, Fudan University, Shanghai, P. R. China.

The gradient-structure is ideal nanostructure for conversion-type anodes with drastic volume change. Here, we demonstrate an inorganic-organic competitive coating strategy for constructing gradient-structured ferroferric oxide-carbon nanospheres, in which the deposition of ferroferric oxide nanoparticles and polymerization of carbonaceous species are competitive and well controlled by the reaction thermodynamics. The synthesized gradient-structure with a uniform size of ~420 nm consists of the ferroferric oxide nanoparticles (4-8 nm) in carbon matrix, which are aggregated into the inner layer (~15 nm) with high-to-low component distribution from inside to out, and an amorphous carbon layer (~20 nm). As an anode material, the volume change of the gradient-structured ferroferric oxide-carbon nanospheres can be limited to ~22% with ~7% radial expansion, thus resulting in stable reversible specific capacities of ~750 mAh g after ultra-long cycling of 10,000 cycles under ultra-fast rate of 10 A g. This unique inorganic-organic competitive coating strategy bring inspiration for nanostructure design of functional materials in energy storage.
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http://dx.doi.org/10.1038/s41467-021-23150-8DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8137936PMC
May 2021

Sequential Superassembly of Nanofiber Arrays to Carbonaceous Ordered Mesoporous Nanowires and Their Heterostructure Membranes for Osmotic Energy Conversion.

J Am Chem Soc 2021 May 30;143(18):6922-6932. Epub 2021 Apr 30.

Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai 200438, P. R. China.

The capture of sustainable energy from a salinity gradient, in particular, using renewable biomass-derived functional materials, has attracted significant attention. In order to convert osmotic energy to electricity, many membrane materials with nanofluidic channels have been developed. However, the high cost, complex preparation process, and low output power density still restrict the practical application of traditional membranes. Herein, we report the synthesis of highly flexible and mechanically robust nanofiber-arrays-based carbonaceous ordered mesoporous nanowires (CMWs) through a simple and straightforward soft-templating hydrothermal carbonization approach. This sequential superassembly strategy shows a high yield and great versatility in controlling the dimensions of CMWs with the aspect ratio changes from about 3 to 39. Furthermore, these CMWs can be used as novel building blocks to construct functional hybrid membranes on macroporous alumina. This nanofluidic membrane with asymmetric geometry and charge polarity exhibits low resistance and high-performance energy conversion. This work opens a solution-based route for the one-pot preparation of CMWs and functional heterostructure membranes for various applications.
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http://dx.doi.org/10.1021/jacs.1c00547DOI Listing
May 2021

General Synthesis of Ultrafine Monodispersed Hybrid Nanoparticles from Highly Stable Monomicelles.

Adv Mater 2021 Jun 29;33(23):e2100820. Epub 2021 Apr 29.

Department of Chemistry, Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM and State Key Laboratory of Molecular Engineering of Polymers, Fudan University, Shanghai, 200433, P. R. China.

Ultrafine nanoparticles with organic-inorganic hybridization have essential roles in myriad applications. Over the past three decades, although various efforts on the formation of organic or inorganic ultrasmall nanoparticles have been made, ultrafine organic-inorganic hybrid nanoparticles have scarcely been achieved. Herein, a family of ultrasmall hybrid nanoparticles with a monodisperse, uniform size is synthesized by a facile thermo-kinetics-mediated copolymer monomicelle approach. These thermo-kinetics-mediated monomicelles with amphiphilic ABC triblock copolymers are structurally robust due to their solidified polystyrene core, endowing them with ultrahigh thermodynamic stability, which is difficult to achieve using Pluronic surfactant-based micelles (e.g., F127). This great stability combined with a core-shell-corona structure makes the monodispersed monomicelles a robust template for the precise synthesis of ultrasmall hybrid nanoparticles with a highly uniform size. As a demonstration, the obtained micelles/SiO hybrid nanoparticles display ultrafine sizes, excellent uniformity, monodispersity, and tunable structural parameters (diameters: 24-47 nm and thin shell thickness: 2.0-4.0 nm). Notably, this approach is universal for creating a variety of multifunctional ultrasmall hybrid nanostructures, involving organic/organic micelle/polymers (polydopamine) nanoparticles, organic/inorganic micelle/metal oxides (ZnO, TiO , Fe O ), micelle/hydroxides (Co(OH) ), micelle/noble metals (Ag), and micelle/TiO /SiO hybrid composites. As a proof of concept, the ultrasmall micelle/SiO hybrid nanoparticles demonstrate superior toughness as biomimetic materials.
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http://dx.doi.org/10.1002/adma.202100820DOI Listing
June 2021

Ligand-Mediated Spatially Controllable Superassembly of Asymmetric Hollow Nanotadpoles with Fine-Tunable Cavity as Smart HO-Sensitive Nanoswimmers.

ACS Nano 2021 Apr 16. Epub 2021 Apr 16.

Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200438, China.

Ligand-mediated interface control has been broadly applied as a powerful tool in constructing sophisticated nanocomposites. However, the resultant morphologies are usually limited to solid structures. Now, a facile spatially controllable ligand-mediated superassembly strategy is explored to construct monodispersed, asymmetric, hollow, open Au-silica (SiO) nanotadpoles (AHOASTs). By manipulating the spatial density of ligands, the degree of diffusion of silica can be precisely modulated; thus the diameters of the cavity can be continuously tuned. Due to their highly anisotropic, hollow, open morphologies, we construct a multicompartment nanocontainer with enzymes held and isolated inside the cavity. Furthermore, the resulting enzyme-AHOASTs are used as biocompatible smart HO-sensitive nanoswimmers and demonstrate a higher diffusion coefficient than other nanoscaled swimmers. We believe that this strategy is critical not only in designing sophisticated hollow nanosystem but also in providing great opportunities for applications in nanomaterial assembly, catalysis, sensors, and nanoreactors.
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http://dx.doi.org/10.1021/acsnano.1c01159DOI Listing
April 2021

Precisely Controlled Vertical Alignment in Mesostructured Carbon Thin Films for Efficient Electrochemical Sensing.

ACS Nano 2021 Apr 6;15(4):7713-7721. Epub 2021 Apr 6.

Laboratory of Advanced Materials, Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, People's Republic of China.

Two-dimensional carbon materials, incorporating a large mesoporosity, are attracting considerable research interest in various fields such as catalysis, electrochemistry, and energy-related technologies owing to their integrated functionalities. However, their potential applications, which require favorable mass transport within mesopore channels, are constrained by the undesirable and finite mesostructural configurations due to the immense synthetic difficulties. Herein, we demonstrate an oriented monomicelle assembly strategy, for the facile fabrication of highly ordered mesoporous carbon thin films with vertically aligned and permeable mesopore channels. Such a facile and reproducible approach relies on the swelling and fusion effect of hydrophobic benzene homologues for directional monomicelle assembly. The orientation assembly process shows precise controllability and great universality, affording mesoporous carbon films with a cracking-free structure over a centimeter in size, highly tunable thicknesses (13 to 85 nm, an interval of ∼12 nm), mesopore size (8.4 to 13.5 nm), and switchable growth substrates. Owing to their large permeable mesopore channels, electrochemical sensors based on vertical mesoporous carbon films exhibit an ultralow limit of detection (50 nmol L) and great sensitivity in dopamine detection.
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http://dx.doi.org/10.1021/acsnano.1c01367DOI Listing
April 2021

Membrane Interactions of Virus-like Mesoporous Silica Nanoparticles.

ACS Nano 2021 04 16;15(4):6787-6800. Epub 2021 Mar 16.

Department of Pharmacy, University of Copenhagen, DK-2100 Copenhagen, Denmark.

In the present study, we investigated lipid membrane interactions of silica nanoparticles as carriers for the antimicrobial peptide LL-37 (LLGDFFRKSKEKIGKEFKRIVQRIKDFLRNLVPRTES). In doing so, smooth mesoporous nanoparticles were compared to virus-like mesoporous nanoparticles, characterized by a "spiky" external surface, as well as to nonporous silica nanoparticles. For this, we employed a combination of neutron reflectometry, ellipsometry, dynamic light scattering, and ζ-potential measurements for studies of bacteria-mimicking bilayers formed by palmitoyloleoylphosphatidylcholine/palmitoyloleoylphosphatidylglycerol. The results show that nanoparticle topography strongly influences membrane binding and destabilization. We found that virus-like particles are able to destabilize such lipid membranes, whereas the corresponding smooth silica nanoparticles are not. This effect of particle spikes becomes further accentuated after loading of such particles with LL-37. Thus, peptide-loaded virus-like nanoparticles displayed more pronounced membrane disruption than either peptide-loaded smooth nanoparticles or free LL-37. The structural basis of this was clarified by neutron reflectometry, demonstrating that the virus-like nanoparticles induce trans-membrane defects and promote incorporation of LL-37 throughout both bilayer leaflets. The relevance of such effects of particle spikes for bacterial membrane rupture was further demonstrated by confocal microscopy and live/dead assays on bacteria. Taken together, these findings demonstrate that topography influences the interaction of nanoparticles with bacteria-mimicking lipid bilayers, both in the absence and presence of antimicrobial peptides, as well as with bacteria. The results also identify virus-like mesoporous nanoparticles as being of interest in the design of nanoparticles as delivery systems for antimicrobial peptides.
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http://dx.doi.org/10.1021/acsnano.0c10378DOI Listing
April 2021

Laser Cladding Induced Spherical Graphitic Phases by Super-Assembly of Graphene-Like Microstructures and the Antifriction Behavior.

ACS Cent Sci 2021 Feb 27;7(2):318-326. Epub 2020 Dec 27.

Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, P. R. China.

Laser cladding coatings with excellent wear resistance behaviors are prepared on a titanium alloy substrate with a new precursor material system comprising nanoscale BC and Ni60A self-fluxing alloy powder. Structural analysis reveals the existence of micron-size spherical or nearly spherical graphitic phases in the prepared coatings, which are composed of graphene-like microstructures closely associated with other reinforcement phases of high hardness such as TiC and CrB. The formation mechanism of these graphitic phases involves superassembly of uncombined C atoms via repeated growth and reorientation of the graphene-like microstructures and is closely related to the laser processing parameters as well as the precursor compositions. The coexistence of these heterogeneous phases enable the obtained coatings with high wear resistance and low friction coefficient. It was found that the wear resistance of the coating has a remarkable 43.67 times enhancement than that of the titanium alloy while simultaneously showing a low friction coefficient (∼0.35). The understanding of the formation mechanism on the graphene-related novel microstructures with significantly improved mechanical properties is expected to lay the foundation for future developments and applications of graphene and its related carbon materials, such as large-scale production and further incorporation into composite materials with desired local structures.
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http://dx.doi.org/10.1021/acscentsci.0c01365DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7908040PMC
February 2021

Surface-Confined Winding Assembly of Mesoporous Nanorods.

J Am Chem Soc 2020 Nov 3. Epub 2020 Nov 3.

Department of Chemistry and Laboratory of Advanced Materials, State Key Laboratory of Molecular Engineering of Polymers, Collaborative Innovation Center of Chemistry for Energy Materials (2011-iChEM), Fudan University, Shanghai 200433, P. R. China.

Bending and folding are important stereoscopic geometry parameters of one-dimensional (1D) nanomaterials, yet the precise control of them has remained a great challenge. Herein, a surface-confined winding assembly strategy is demonstrated to regulate the stereoscopic architecture of uniform 1D mesoporous SiO (mSiO) nanorods. Based on this brand-new strategy, the 1D mSiO nanorods can wind on the surface of 3D premade nanoparticles (sphere, cube, hexagon disk, spindle, rod, etc.) and inherit their surface topological structures. Therefore, the mSiO nanorods with a diameter of ∼50 nm and a variable length can be bent into arc shapes with variable radii and radians, as well as folded into 60, 90, 120, and 180° angular convex corners with controllable folding times. Additionally, in contrast to conventional [email protected] structures, this winding structure induces partial exposure and accessibility of the premade nanoparticles. The functional nanoparticles can exhibit large accessible surface and efficient energy exchanges with the surroundings. As a proof of concept, winding-structured CuS&mSiO nanocomposites are fabricated, which are made up of a 100 nm CuS nanosphere and the 1D mSiO nanorods with a diameter of ∼50 nm winding the nanosphere in the perimeter. The winding structured nanocomposites are demonstrated to have fourfold photoacoustic imaging intensity compared with the conventional [email protected] nanostructure with an inaccessible core because of the greatly enhanced photothermal conversion efficiency (increased by ∼30%). Overall, our work paves the way to the design and synthesis of 1D nanomaterials with controllable bending and folding, as well as the formation of high-performance complex nanocomposites.
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http://dx.doi.org/10.1021/jacs.0c08277DOI Listing
November 2020

An Aqueous Route Synthesis of Transition-Metal-Ions-Doped Quantum Dots by Bimetallic Cluster Building Blocks.

J Am Chem Soc 2020 09 14;142(38):16177-16181. Epub 2020 Sep 14.

Department of Chemistry, Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai 200438, China.

Water-soluble doped quantum dots have unique photophysical properties and functionalities as optical labels for bioimaging and chemo-/biosensing. However, doping in quantum dots is not easy due to the dopant-ion size mismatch and "self-purification" effect. Here, we demonstrate a successful preparation of Mn-, Cu-, and Ni-doped CdS quantum dots with bimetallic clusters instead of ions as building blocks under mild aqueous conditions up to gram scale. The representative Mn-doped quantum dots have uniform size, about 3.2 ± 0.5 nm, and emit at 620 nm. The doping concentration can be adjusted in the range 6.4%-25.7%. On the premise of good water solubility, they are stable and nontoxic so as to be directly used for cell imaging. Copper and nickel doping have similar results. Because of the close sizes of bimetallic clusters and the low reaction temperature, the challenges posed by dopant size mismatch and ion diffusion are ignored. X-ray absorption fine structure analysis proves that dopants are inside the quantum dots rather than on the surface, indicating that the "self-purification" effect can be effectively overcome. Furthermore, codoped ZnS quantum dots with adjustable emission are achieved, which validates the versatility of our new approach.
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http://dx.doi.org/10.1021/jacs.0c07274DOI Listing
September 2020

Stable Ti Defects in Oriented Mesoporous Titania Frameworks for Efficient Photocatalysis.

Angew Chem Int Ed Engl 2020 Sep 12;59(40):17676-17683. Epub 2020 Aug 12.

Laboratory of Advanced Materials, Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai, 200433, P. R. China.

By introducing a compatible reducing agent (2-ethylimidazole) into a mono-micelle assembly process, we present a type of ordered mesoporous TiO microspheres that combines radially aligned mesostructure with Ti defects in mesoporous frameworks. Such reductant acts as a building block of mesostructured frameworks and reduces Ti in situ to generate defects during calcination, giving rise to the coexistence of bulk Ti defects and an ordered mesostructure. The mesoporous TiO has both excellent mesoporosity (a high surface area of 106 m  g , a mean pore size of 18.4 nm) and stable defects with an extended photoresponse. Such integration of unique mesoscopic architecture and atomic vacancies provide both effective mass transportation and enhanced light utilization, leading to a remarkable increase in H generation rate. A maximum H evolution rate of 19.8 mmol g  h can be achieved, along with outstanding stability under solar light.
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http://dx.doi.org/10.1002/anie.202007859DOI Listing
September 2020

Organic NIR-II molecule with long blood half-life for in vivo dynamic vascular imaging.

Nat Commun 2020 06 18;11(1):3102. Epub 2020 Jun 18.

Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials and iChem, Fudan University, Shanghai, 200433, PR China.

Real-time monitoring of vessel dysfunction is of great significance in preclinical research. Optical bioimaging in the second near-infrared (NIR-II) window provides advantages including high resolution and fast feedback. However, the reported molecular dyes are hampered by limited blood circulation time (~ 5-60 min) and short absorption and emission wavelength, which impede the accurate long-term monitoring. Here, we report a NIR-II molecule (LZ-1105) with absorption and emission beyond 1000 nm. Thanks to the long blood circulation time (half-life of 3.2 h), the fluorophore is used for continuous real-time monitoring of dynamic vascular processes, including ischemic reperfusion in hindlimbs, thrombolysis in carotid artery and opening and recovery of the blood brain barrier (BBB). LZ-1105 provides an approach for researchers to assess vessel dysfunction due to the long excitation and emission wavelength and long-term blood circulation properties.
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http://dx.doi.org/10.1038/s41467-020-16924-zDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7303218PMC
June 2020

Emerging trends in porous materials for CO capture and conversion.

Chem Soc Rev 2020 Jul;49(13):4360-4404

Global Innovative Centre for Advanced Nanomaterials, Faculty of Engineering & Built Environment, University of Newcastle, Callaghan, 2308, Australia.

The presence of an excessive concentration of CO2 in the atmosphere needs to be curbed with suitable measures including the reduction of CO2 emissions at stationary point sources such as power plants through carbon capture technologies and subsequent conversion of the captured CO2 into non-polluting clean fuels/chemicals using photo and/or electrocatalytic pathways. Porous materials have attracted much attention for carbon capture and in the recent past; they have witnessed significant advancements in their design and implementation for CO2 capture and conversion. In this context, the emerging trends in major porous adsorbents such as MOFs, zeolites, POPs, porous carbons, and mesoporous materials for CO2 capture and conversion are discussed. Their surface texture and chemistry, and the influence of various other features on their efficiency, selectivity, and recyclability for CO2 capture and conversion are explained and compared thoroughly. The scientific and technical advances on the material structure versus CO2 capture and conversion provide deep insights into designing effective porous materials. The review concludes with a summary, which compiles the key challenges in the field, current trends and critical challenges in the development of porous materials, and future research directions combined with possible solutions for realising the deployment of porous materials in CO2 capture and conversion.
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http://dx.doi.org/10.1039/d0cs00075bDOI Listing
July 2020

Scalable Synthesis of Uniform Mesoporous Aluminosilicate Microspheres with Controllable Size and Morphology and High Hydrothermal Stability for Efficient Acid Catalysis.

ACS Appl Mater Interfaces 2020 May 30;12(19):21922-21935. Epub 2020 Apr 30.

Particle Engineering Laboratory (PEL), School of Chemical and Environmental Engineering, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, Jiangsu 215123, P. R. China.

Mesoporous aluminosilicates are promising solid acid catalysts. They are also excellent supports for transition metal catalysts for various catalytic applications. Synthesis of mesoporous aluminosilicates with controllable particle size, morphology, and structure, as well as adjustable acidity and high hydrothermal stability, is very desirable. In this work, we demonstrate the scalable synthesis of Al-SBA-15 microspheres with controllable physicochemical properties by using the microfluidic jet-spray-drying technology. The productivity is up to ∼30 g of dried particles per nozzle per hour. The Al-SBA-15 microspheres possess uniform controllable micron sizes (27.5-70.2 μm), variable surface morphologies, excellent hydrothermal stability (in pure steam at 800 °C), high surface areas (385-464 m/g), ordered mesopore sizes (5.4-5.8 nm), and desirable acid properties. The dependence of various properties, including particle size, morphology, porosity, pore size, acidity, and hydrothermal stability, of the obtained Al-SBA-15 microspheres on experimental parameters including precursor composition (Si/Al ratio and solid content) and processing conditions (drying and calcination temperatures) is established. A unique morphology transition from smooth to wrinkled microsphere triggered by control of the Si/Al ratio and solid content is observed. The particle formation and morphology-evolution mechanism are discussed. The Al-SBA-15 microspheres exhibit high acid catalytic performance for aldol-condensation reaction between benzaldehyde and ethyl alcohol with a high benzaldehyde conversion (∼56.3%), a fast pseudo-first-order reaction rate (∼0.1344 h), and a high cyclic stability, superior to the commercial zeolite acid (H-ZSM-5). Several influencing factors on the catalytic performance of the obtained Al-SBA-15 microspheres are also studied.
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http://dx.doi.org/10.1021/acsami.0c04998DOI Listing
May 2020

Size and charge dual-transformable mesoporous nanoassemblies for enhanced drug delivery and tumor penetration.

Chem Sci 2020 Feb 3;11(10):2819-2827. Epub 2020 Feb 3.

Department of Chemistry, Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, State Key Laboratory of Molecular Engineering of Polymers, Collaborative Innovation Center of Chemistry for Energy Materials (2011-iChEM), Fudan University Shanghai 200433 P. R. China

A series of biological barriers in a nanoparticle-formulated drug delivery process inevitably result in the current low delivery efficiency, limited tumor penetration and insufficient cellular internalization of drugs. These multiple biological barriers are intimately related to the physicochemical properties of nanoparticles, especially the contradictory demand on size and surface charge for long blood circulation (larger and negative) and deep tumor penetration (smaller) as well as efficient cellular internalization (positive). Herein, we report tumor microenvironment triggered size and charge dual-transformable nanoassemblies. The nanoassembly is realized by immobilizing positive up/downconverting luminescent nanoparticles (U/DCNPs) onto large mesoporous silica nanoparticles (MSNs) acid-labile bonds to form [email protected] structured [email protected]/DCNPs nanoassemblies, and subsequent capping of charge reversible polymers. At physiological pH, the integrated nanoassemblies with a larger size (∼180 nm) and negative charge can effectively achieve a prolonged blood circulation and high tumor accumulation. While under an acidic tumor microenvironment, the charge reversal of outer polymers and cleavage of linkers between MSNs and U/DCNPs can induce disintegration of the nanoassemblies into isolated MSNs and smaller U/DCNPs, both with a positively charged surface, which thereby potentiate the tumor penetration and cell uptake of dissociated nanoparticles. Combined with the independent near-infrared (NIR)-to-visible and NIR-to-NIR luminescence of U/DCNPs and high surface area of MSNs, the nanoassemblies can implement NIR bioimaging guided chemo- and photodynamic combined therapy with remarkable antitumor efficiency because of the high accumulation and deep tumor penetration induced by the dual transformability of the nanoassemblies.
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http://dx.doi.org/10.1039/c9sc06260bDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8157500PMC
February 2020

A Universal Lab-on-Salt-Particle Approach to 2D Single-Layer Ordered Mesoporous Materials.

Adv Mater 2020 Mar 29;32(10):e1906653. Epub 2020 Jan 29.

Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai, 200433, China.

The advantages of existing ordered mesoporous materials have not yet been fully realized, due to their limited accessibility of in-pore surface and long mass-diffusion length. A general, controllable, and scalable synthesis of a family of two-dimensional (2D) single-layer ordered mesoporous materials (SOMMs) with completely exposed mesopore channels, significantly improved mass diffusion, and diverse framework composition is reported here. The SOMMs are synthesized via a surface-limited cooperative assembly (SLCA) on water-removable substrates of inorganic salts (e.g., NaCl), combined with vacuum filtration. As a proof of concept, the obtained CeO -based SOMMs show superior catalytic performance in CO oxidation with high conversion efficiency, ≈33 times higher than that of conventional bulk mesoporous CeO . This SLCA is a promising approach for developing next-generation porous materials for various applications.
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http://dx.doi.org/10.1002/adma.201906653DOI Listing
March 2020

Three-Dimensional Hierarchical Porous Nanotubes Derived from Metal-Organic Frameworks for Highly Efficient Overall Water Splitting.

iScience 2020 Jan 10;23(1):100761. Epub 2019 Dec 10.

Department of Chemical Engineering, Monash University, Clayton, VIC 3800, Australia. Electronic address:

Effective design of bifunctional catalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is important but remains challenging. Herein, we report a three-dimensional (3D) hierarchical structure composed of homogeneously distributed Ni-Fe-P nanoparticles embedded in N-doped carbons on nickel foams (denoted as [email protected]/NF) as an excellent bifunctional catalyst. This catalyst was fabricated by an anion exchange method and a low-temperature phosphidation of nanotubular Prussian blue analogue (PBA). The [email protected]/NF displayed exceptional catalytic activity toward both HER and OER and delivered an ultralow cell voltage of 1.47 V to obtain 10 mA cm with extremely excellent durability for 100 h when assembled as a practical electrolyser. The extraordinary performance of [email protected]/NF is attributed to the abundance of unsaturated active sites, the well-defined hierarchical porous structure, and the synergistic effect between multiple components. Our work will inspire more rational designs of highly active non-noble electrocatalysts for industrial energy applications.
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http://dx.doi.org/10.1016/j.isci.2019.100761DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6941879PMC
January 2020

Sequential Chemistry Toward Core-Shell Structured Metal Sulfides as Stable and Highly Efficient Visible-Light Photocatalysts.

Angew Chem Int Ed Engl 2020 Feb 9;59(8):3287-3293. Epub 2020 Jan 9.

Department of Chemistry, Laboratory of Advanced Materials, State Key Laboratory of Molecular Engineering of Polymers, and, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433, P. R. China.

A universal sequential synthesis strategy in aqueous solution is presented for highly uniform core-shell structured photocatalysts, which consist of a metal sulfide light absorber core and a metal sulfide co-catalyst shell. We show that the sequential chemistry can drive the formation of unique core-shell structures controlled by the constant of solubility product of metal sulfides. A variety of metal sulfide core-shell structures have been demonstrated, including [email protected] , [email protected] , [email protected] , [email protected] , [email protected], and more complexed [email protected] @CoS . The obtained strawberry-like [email protected] core-shell structures exhibit a high photocatalytic H production activity of 3.92 mmol h and an impressive apparent quantum efficiency of 67.3 % at 420 nm, which is much better than that of pure CdS nanoballs (0.28 mmol h ), CdS/CoS composites (0.57 mmol h ), and 5 %wt Pt-loaded CdS photocatalysts (1.84 mmol h ).
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http://dx.doi.org/10.1002/anie.201913600DOI Listing
February 2020

Synthesis of orthogonally assembled 3D cross-stacked metal oxide semiconducting nanowires.

Nat Mater 2020 Feb 2;19(2):203-211. Epub 2019 Dec 2.

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, State Key Laboratory of Molecular Engineering of Polymers, and iChEM, Fudan University, Shanghai, China.

Assemblies of metal oxide nanowires in 3D stacks can enable the realization of nanodevices with tailored conductivity, porous structure and a high surface area. Current fabrication methods require complicated multistep procedures that involve the initial preparation of nanowires followed by manual assembly or transfer printing, and thus lack synthesis flexibility and controllability. Here we report a general synthetic orthogonal assembly approach to controllably construct 3D multilayer-crossed metal oxide nanowire arrays. Taking tungsten oxide semiconducting nanowires as an example, we show the spontaneous orthogonal packing of composite nanorods of poly(ethylene oxide)-block-polystyrene and silicotungstic acid; the following calcination gives rise to 3D cross-stacked nanowire arrays of Si-doped metastable ε-phase WO. This nanowire stack framework was also tested as a gas detector for the selective sensing of acetone. By using other polyoxometallates, this fabrication method for woodpile-like 3D nanostructures can also be generalized to different doped metal oxide nanowires, which provides a way to manipulate their physical properties for various applications.
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http://dx.doi.org/10.1038/s41563-019-0542-xDOI Listing
February 2020

Two-Dimensional Mesoporous Heterostructure Delivering Superior Pseudocapacitive Sodium Storage via Bottom-Up Monomicelle Assembly.

J Am Chem Soc 2019 Oct 11;141(42):16755-16762. Epub 2019 Oct 11.

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) , Fudan University , Shanghai 200433 , PR China.

Two-dimensional (2D) heterostructures endowed with mesoporosities offer exciting opportunities in electrocatalysis, photocatalysis, energy storage, and conversion technologies due to their integrated functionalities, abundant active sites and shortened diffusion distance. However, layered mesostructures have not been combined due to the immense difficulties by conventional chemical, mechanical exfoliation or self-assembly approaches. Herein, we explore a bottom-up strategy, carried out under mild conditions, for the facile synthesis of monolayered mesoporous-titania-mesoporous-carbon vertical heterostructure with uniform mesopore size, which enables ultrahigh rate capability and cycling longevity for pseudocapacitive sodium-ion storage in nonaqueous electrolyte. Such a brand-new type of heterostructure consists of well-ordered monolayered mesoporous titania nanosheets and surrounding two mesoporous carbon monolayers assembled at both sides. Remarkably, the combination of interconnected large mesoporosity and heterointerface leads to highly promoted reversible pseudocapacitance (96.4% of total charge storage at a sweep rate of 1 mV s), and it enables the material to retain strong mechanical stability during the rapid sodiation and desodiation processes. This study reveals the importance of incorporating mesopores into heterointerface as a strategy for enhancing charge storage kinetics of electroactive materials.
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http://dx.doi.org/10.1021/jacs.9b06962DOI Listing
October 2019

Surface-kinetics mediated mesoporous multipods for enhanced bacterial adhesion and inhibition.

Nat Commun 2019 09 26;10(1):4387. Epub 2019 Sep 26.

Department of Chemistry and Laboratory of Advanced Materials, State Key Laboratory of Molecular Engineering of Polymers, Collaborative Innovation Center of Chemistry for Energy Materials (2011-iChEM), Fudan University, Shanghai, 200433, PR China.

Despite the importance of nanoparticle's multipods topology in multivalent-interactions enhanced nano-bio interactions, the precise manipulation of multipods surface topological structures is still a great challenge. Herein, the surface-kinetics mediated multi-site nucleation strategy is demonstrated for the fabrication of mesoporous multipods with precisely tunable surface topological structures. Tribulus-like tetra-pods [email protected]@RF&PMOs (RF = resorcinol-formaldehyde resin, PMO = periodic mesoporous organosilica) nanocomposites have successfully been fabricated with a centering [email protected] [email protected]@RF nanoparticle, and four surrounding PMO nanocubes as pods. By manipulating the number of nucleation sites through mediating surface kinetics, a series of multipods mesoporous nanocomposites with precisely controllable surface topological structures are formed, including Janus with only one pod, nearly plane distributed dual-pods and tri-pods, three-dimensional tetrahedral structured tetra-pods, etc. The multipods topology endows the mesoporous nanocomposites enhanced bacteria adhesion ability. Particularly, the tribulus-like tetra-pods mesoporous nanoparticles show ~100% bacteria segregation and long-term inhibition over 90% after antibiotic loading.
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http://dx.doi.org/10.1038/s41467-019-12378-0DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6763480PMC
September 2019

Spherical Mesoporous Materials from Single to Multilevel Architectures.

Acc Chem Res 2019 Oct 19;52(10):2928-2938. Epub 2019 Sep 19.

Department of Chemistry, Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM and State Key Laboratory of Molecular Engineering of Polymers , Fudan University , Shanghai 200433 , China.

Mesoporous materials with various structures have attracted considerable attention due to their distinctive properties such as large pore sizes, high surface areas, tunable pore structures, and controllable framework compositions. Among them, spherical mesoporous materials (SMMs) are of great interest owing to the unique spherical shape, which show the closed packing nature and lowest surface energy. The open mesopores and short channels of SMMs not only increase the density of high accessible active sites but also facilitate the mass diffusion with short length. These characteristics are particularly useful for applications in catalysis, adsorption, energy storage and conversion, biomedicine, and so on. In addition, the creation of a spherical shape is conformable to the law of natural selection because objects in nature tend to minimize energy, while the sphere is one of the most perfect matter structures. Therefore, the design and synthesis of SMMs are very important from both fundamental and technological viewpoints. Compared to the simple single-level, SMMs with more complex multilevel structures inevitably bring unusual mechanical, electrical, and optical properties, which are highly desired for practical applications. For example, the construction of core-shell structured SMMs has inspired great attention as they can combine multiple components into one functional unit, exhibiting ameliorated or new physicochemical properties, which cannot be obtained from the isolated one. The presence of a hollow cavity in the yolk-shell structure allows sufficient exposure of the core while maintaining the protective ability of the shell, which is conducive to retaining the distance-dependent properties of the core. Multishelled hollow structures consisting of two or more mesoporous shells are expected to show superior activities in various applications compared to their bulk counterparts because more active interfaces and unique compartmentation environments can be provided. Therefore, SMMs from single to multilevel structure represent a class of advanced nanostructured materials with unique structures and fascinating properties. In this Account, we highlight the progresses on the synthesis and applications of SMMs from single to multilevel architectures. The synthetic strategies have been summarized and categorized into (i) the modified Stöber method, (ii) the hydrothermal strategy, (iii) the biphase stratification approach, (iv) the nanoemulsion assembly method, (v) the evaporation induced aggregating assembly (EIAA) method, and (vi) the confined self-assembly strategy. Special emphasis is placed on the synthetic principles and underlying mechanisms for precise control of SMMs over the particle sizes, pore sizes, pore structures and functionalities as well as different levels of architectures. Moreover, the implementation performances in catalysis, drug delivery, and energy related fields have been highlighted. Finally, the opportunities and challenges for the future development of SMMs in terms of synthesis and applications are proposed.
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http://dx.doi.org/10.1021/acs.accounts.9b00357DOI Listing
October 2019

Spray-drying water-based assembly of hierarchical and ordered mesoporous silica microparticles with enhanced pore accessibility for efficient bio-adsorption.

J Colloid Interface Sci 2019 Nov 24;556:529-540. Epub 2019 Aug 24.

Department of Chemical Engineering, Monash University, Clayton Campus, Victoria 3800, Australia. Electronic address:

The fast and scalable spray-drying-assisted evaporation-induced self-assembly (EISA) synthesis of hierarchically porous SBA-15-type silica microparticles from a water-based system is demonstrated. The SBA-15-type silica microparticles has bowl-like shapes, uniform micro-sizes (∼90 µm), large ordered mesopores (∼9.5 nm), hierarchical meso-/macropores (20-100 nm) and open surfaces. In the synthesis, soft- and hard-templating approaches are combined in a single rapid drying process with a non-ionic tri-block copolymer (F127) and a water-insoluble polymer colloid (Eudragit RS, 120 nm) as the co-templates. The RS polymer colloid plays three important roles. First, the RS nanoparticles can be partially dissolved by in-situ generated ethanol to form RS polymer chains. The RS chains swell and modulate the hydrophilic-hydrophobic balance of F127 micelles to allow the formation of an ordered mesostructure with large mesopore sizes. Without RS, only worm-like mesostructure with much smaller mesopore sizes can be formed. Second, part of the RS nanoparticles plays a role in templating the hierarchical pores distributed throughout the microparticles. Third, part of the RS polymer forms surface "skins" and "bumps", which can be removed by calcination to enable a more open surface structure to overcome the low pore accessibility issue of spray-dried porous microparticles. The obtained materials have high surface areas (315-510 m g) and large pore volumes (0.64-1.0 cm g), which are dependent on RS concentration, HCl concentration, silica precursor hydrolysis time and drying temperature. The representative materials are promising for the adsorption of lysozyme. The adsorption occurs at a >three-fold faster rate, in a five-fold larger capacity (an increase from 20 to 100 mg g) and without pore blockage compared with the adsorption of lysozyme onto spray-dried microparticles of similar physicochemical properties obtained without the use of RS.
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http://dx.doi.org/10.1016/j.jcis.2019.08.084DOI Listing
November 2019
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