Publications by authors named "Chengzhong Yu"

173 Publications

Superstructured Macroporous Carbon Rods Composed of Defective Graphitic Nanosheets for Efficient Oxygen Reduction Reaction.

Adv Sci (Weinh) 2021 Sep 29;8(18):e2100120. Epub 2021 Jul 29.

School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, P. R. China.

Rationally designed carbon materials with superstructures are promising candidates in applications such as electrocatalysis. However, the synthesis of highly porous carbon superstructures with macropores and carbon defects from a simple crystalline solid remains challenging. In this work, superstructured macroporous carbon rods composed of defective graphitic nanosheets are synthesized by direct carbonization of crystalline poly tannic acid (PTA) rods as precursors. During carbonization, PTA rods with a highly ordered lamellar structure induce a spatially confined two-step localized contraction that takes place in different dimensions and directions in each step. The unexpected contraction behavior results in the sponge-like macroporous carbon superstructure with large surface area, high porosity, and abundant defects, thus showing a superior electrocatalytic performance with high activity and selectivity for oxygen reduction reaction. The study provides new understandings in the design of functional carbon materials with distinctive structures and applications.
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http://dx.doi.org/10.1002/advs.202100120DOI Listing
September 2021

Ferroptosis-Strengthened Metabolic and Inflammatory Regulation of Tumor-Associated Macrophages Provokes Potent Tumoricidal Activities.

Nano Lett 2021 08 22;21(15):6471-6479. Epub 2021 Jul 22.

School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200241, People's Republic of China.

Modulation of tumor-associated macrophages (TAMs) holds promise for cancer treatment, mainly relying on M1 signaling activation and pro-inflammatory promotion. Nevertheless, the antitumor activity is often limited by the anti-inflammatory factors in the tumor microenvironment. Moreover, the metabolic function of TAMs is also critical to tumor progression. However, there are a few strategies that can simultaneously regulate both inflammatory and metabolic functions to achieve safe and potent antitumor activation of TAMs. Herein, we demonstrate that an iron-based metal organic framework nanoparticle and a ferroptosis-inducing agent synergistically induce mitochondrial alternation in TAMs, resulting in a radical metabolic switch from mitochondrial oxidative phosphorylation to glycolysis, which is resistant to anti-inflammatory stimuli challenge. The ferroptosis stress strengthened by the nanoformulation also drives multiple pro-inflammatory signaling pathways, enabling macrophage activation with potent tumoricidal activities. The ferroptosis-strengthened macrophage regulation strategy present in this study paves the way for TAM-centered antitumoral treatment to overcome the limitations of conventional methods.
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http://dx.doi.org/10.1021/acs.nanolett.1c01401DOI Listing
August 2021

Post translational modification-assisted cancer immunotherapy for effective breast cancer treatment.

Chem Sci 2020 Sep 10;11(38):10421-10430. Epub 2020 Sep 10.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland QLD 4072 Australia

Post translational modifications (PTM) such as phosphorylation are often correlated with tumorigenesis and malignancy in breast cancer. Herein, we report a PTM-assisted strategy as a simplified version of a personalized cancer vaccine for enhanced cancer immunotherapy. Titanium modified dendritic mesoporous silica nanoparticles (TiDMSN) are applied to assist the specific enrichment of phosphorylated tumor antigens released upon immunogenic cell death. This strategy significantly improved the tumor inhibition efficacy in a bilateral breast cancer model and the expansion of both CD8 and CD4 T cells in the distant tumor site. The nanotechnology based PTM-assisted strategy provides a simple and generalizable methodology for effective personalized cancer immunotherapy.
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http://dx.doi.org/10.1039/d0sc02803gDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8162284PMC
September 2020

Synthesis of dendritic mesoporous organosilica nanoparticles under a mild acidic condition with homogeneous wall structure and near-neutral surface.

Chem Commun (Camb) 2021 May;57(36):4416-4419

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD 4072, Australia. and School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200241, P. R. China.

Dendritic mesoporous organosilica nanoparticles were synthesized under a mild acidic condition (pH 6.2), featuring a molecularly homogeneous wall structure and an unusual near-neutral charged surface, consequently enabling reduced protein fouling property.
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http://dx.doi.org/10.1039/d0cc08017aDOI Listing
May 2021

Rational Design of Dendritic Mesoporous Silica Nanoparticles' Surface Chemistry for Quantum Dot Enrichment and an Ultrasensitive Lateral Flow Immunoassay.

ACS Appl Mater Interfaces 2021 May 3;13(18):21507-21515. Epub 2021 May 3.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland 4072, Australia.

Lateral flow immunoassays (LFIAs) have drawn much attention in point-of-care diagnostic applications, and the development of high-performance label materials is the key. In this study, the impact of the surface chemistry of dendritic mesoporous silica nanoparticles (DMSNs) on their enrichment performance toward quantum dots (QDs) and signal amplification of the resultant DMSNs-QDs as label materials have been investigated. A series of DMSNs with controllable amino/thiol group densities have been synthesized. It is demonstrated that the amino groups are beneficial for QD fluorescence preservation, owing to the amino-based surface passivation, while the thiol groups are responsible for increasing the loading capacity of QDs due to the thiol-metal coordination. The optimized DMSNs-QDs labels with an amino density of 153 μmol g and a thiol density of 218 μmol g displayed sufficient QD fluorescence preservation (89.4%) and high QD loading capacity (1.55 g g). Ultrasensitive detection of serum amyloid A (SAA) with a detection limit of 10 pg mL with the naked eye was achieved, which is 1 order of magnitude higher than that reported in the literature. This study provides insights into the development of advanced label materials and an ultrasensitive LFIA for future bioassay applications.
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http://dx.doi.org/10.1021/acsami.1c02149DOI Listing
May 2021

Nanochemistry Modulates Intracellular Decomposition Routes of S-Nitrosothiol Modified Silica-Based Nanoparticles.

Small 2021 05 15;17(21):e2007671. Epub 2021 Apr 15.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD, 4072, Australia.

Cellular delivery of nitric oxide (NO) using NO donor moieties such as S-nitrosothiol (SNO) is of great interest for various applications. However, understandings of the intracellular decomposition routes of SNO toward either NO or ammonia (NH ) production are surprisingly scarce. Herein, the first report of SNO modified mesoporous organosilica nanoparticles with tetrasulfide bonds for enhanced intracellular NO delivery, ≈10 times higher than a commercial NO donor, is presented. The tetrasulfide chemistry modulates the SNO decomposition by shifting from NH to NO production in glutathione rich cancer cells. This study provides a new strategy to control the NO level in biological systems.
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http://dx.doi.org/10.1002/smll.202007671DOI Listing
May 2021

Designer Anticancer Nanoprodrugs with Self-Toxification Activity Realized by Acid-triggered Biodegradation and In Situ Fragment Complexation.

Angew Chem Int Ed Engl 2021 05 6;60(20):11504-11513. Epub 2021 Apr 6.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St. Lucia, Brisbane, QLD, 4072, Australia.

Prodrugs that allow in situ chemical conversion of less toxic precursors into active drugs in response to certain stimuli are promising anticancer candidates. Herein, we present a novel design of nanoprodrugs with a "degradation-mediated self-toxification" strategy, which realizes intracellular synthesis of anticancer agents using the nanoparticles' own degradation fragments as the precursors. To fulfill this concept, a metal complexing dicyclohexylphosphine (DCP) organosilane is carefully screened out from various ligands to conjugate onto Pd(OH) nanodots confined hollow silica nanospheres (PD-HSN). This constructed nanoprodrug shows acid-triggered degradation in lysosomes and neutralizes protons to induce lysosomes rupturing, generating predesigned less toxic fragments (Pd and DCP-silicates) that complex into DCP/Pd complex in situ for inducing DNA damage, leading to enhanced anticancer activity against various cancer cell lines as well as in a xenograft tumour model.
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http://dx.doi.org/10.1002/anie.202102704DOI Listing
May 2021

MnO Nanoflowers Induce Immunogenic Cell Death under Nutrient Deprivation: Enabling an Orchestrated Cancer Starvation-Immunotherapy.

Adv Sci (Weinh) 2021 Feb 31;8(4):2002667. Epub 2020 Dec 31.

Australian Institute for Bioengineering and Nanotechnology The University of Queensland St. Lucia Brisbane QLD 4072 Australia.

MnO nanoparticles have been widely employed in cancer immunotherapy, playing a subsidiary role in assisting immunostimulatory drugs by improving their pharmacokinetics and/or creating a favorable microenvironment. Here, the stereotype of the subsidiary role of MnO nanoparticles in cancer immunotherapy is challenged. This study unravels an intrinsic immunomodulatory property of MnO nanoparticles as a unique nutrient-responsive immunogenic cell death (ICD) inducer, capable of directly modulating immunosurveillance toward tumor cells. MnO nanoflowers (MNFs) constructed via a one pot self-assembly approach selectively induce ICD to nutrient-deprived but not nutrient-replete cancer cells, which is confirmed by the upregulated damage associated molecular patterns in vitro and a prophylactic vaccination in vivo. The underlying mechanism of the MNFs-mediated selective ICD induction is likely associated with the concurrently upregulated oxidative stress and autophagy. Built on their unique immunomodulatory properties, an innovative nanomaterials orchestrated cancer starvation-immunotherapy is successfully developed, which is realized by the in situ vaccination with MNFs and vascular disrupting agents that cut off intratumoral nutrient supply, eliciting potent efficacy for suppressing local and distant tumors. These findings open up a new avenue toward biomedical applications of MnO materials, enabling an innovative therapeutics paradigm with great clinical significance.
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http://dx.doi.org/10.1002/advs.202002667DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7887587PMC
February 2021

Benzene-Bridged Organosilica Modified Mesoporous Silica Nanoparticles via an Acid-Catalysis Approach.

Langmuir 2021 Mar 16;37(8):2780-2786. Epub 2021 Feb 16.

School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200241, P. R. China.

Surface functionalization of mesoporous silica nanoparticles is important for their applications but fairly challenging using benzene-bridged organosilane as the precursor through the postsynthesis approach. Herein, we report an acid-catalysis approach for the postmodification of benzene-bridged organosilica onto the surface of large-pore mesoporous silica nanoparticles. By using HCl (∼1 M) as the acid catalyst in a tetrahydrofuran solvent, the self-assembly of the bridged organosilica precursor is avoided, while surface modification of mesoporous silica nanoparticles is promoted with controllable organic contents and retained large pore sizes. This strategy can also be applied to the postmodification of organosilica with end benzene groups. The strategy developed in this study is expected to be applied for the postmodification of other organosilica precursors with various functions.
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http://dx.doi.org/10.1021/acs.langmuir.0c03541DOI Listing
March 2021

Biomimetic inorganic-organic hybrid nanoparticles from magnesium-substituted amorphous calcium phosphate clusters and polyacrylic acid molecules.

Bioact Mater 2021 Aug 23;6(8):2303-2314. Epub 2021 Jan 23.

Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning, 110016, China.

Amorphous calcium phosphate (ACP) has been widely found during bone and tooth biomineralization, but the meta-stability and labile nature limit further biomedical applications. The present study found that the chelation of polyacrylic acid (PAA) molecules with Ca ions in Mg-ACP clusters (~2.1 ± 0.5 nm) using a biomineralization strategy produced inorganic-organic Mg-ACP/PAA hybrid nanoparticles with better thermal stability. Mg-ACP/PAA hybrid nanoparticles (~24.0 ± 4.8 nm) were pH-responsive and could be efficiently digested under weak acidic conditions (pH 5.0-5.5). The internalization of assembled Mg-ACP/PAA nanoparticles by MC3T3-E1 cells occurred through endocytosis, indicated by laser scanning confocal microscopy and cryo-soft X-ray tomography. Our results showed that cellular lipid membranes remained intact without pore formation after Mg-ACP/PAA particle penetration. The assembled Mg-ACP/PAA particles could be digested in cell lysosomes within 24 h under weak acidic conditions, thereby indicating the potential to efficiently deliver encapsulated functional molecules. Both the and results preliminarily demonstrated good biosafety of the inorganic-organic Mg-ACP/PAA hybrid nanoparticles, which may have potential for biomedical applications.
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http://dx.doi.org/10.1016/j.bioactmat.2021.01.005DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7841502PMC
August 2021

Characterization of the Biodistribution of a Silica Vesicle Nanovaccine Carrying a Protective Antigen With Live Animal Imaging.

Front Bioeng Biotechnol 2020 18;8:606652. Epub 2021 Jan 18.

Queensland Alliance for Agriculture and Food Innovation, The University of Queensland, Brisbane, QLD, Australia.

Development of veterinary subunit vaccines comes with a spectrum of challenges, such as the choice of adjuvant, antigen delivery vehicle, and optimization of dosing strategy. Over the years, our laboratory has largely focused on investigating silica vesicles (SVs) for developing effective veterinary vaccines for multiple targets. (cattle tick) are known to have a high impact on cattle health and the livestock industry in the tropical and subtropical regions. Development of vaccine using Bm86 antigen against has emerged as an attractive alternative to control ticks. In this study, we have investigated the biodistribution of SV in a live animal model, as well as further explored the SV ability for vaccine development. Rhodamine-labeled SV-140-C (Rho-SV-140-C) vesicles were used to adsorb the Cy5-labeled Bm86 antigen (Cy5-Bm86) to enable detection and characterization of the biodistribution of SV as well as antigen in a small animal model for up to 28 days using optical fluorescence imaging. We tracked the biodistribution of SVs and Bm86 antigen at different timepoints (days 3, 8, 13, and 28) in BALB/c mice. The biodistribution analysis by live imaging as well as by measuring the fluorescent intensity of harvested organs over the duration of the experiment (28 days) showed greater accumulation of SVs at the site of injection. The Bm86 antigen biodistribution was traced in lymph nodes, kidney, and liver, contributing to our understanding how this delivery platform successfully elicits antibody responses in the groups administered antigen in combination with SV. Selected tissues (skin, lymph nodes, spleen, kidney, liver, and lungs) were examined for any cellular abnormalities by histological analysis. No adverse effect or any other abnormalities were observed in the tissues.
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http://dx.doi.org/10.3389/fbioe.2020.606652DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7848120PMC
January 2021

Manganese-Doped Silica-Based Nanoparticles Promote the Efficacy of Antigen-Specific Immunotherapy.

J Immunol 2021 03 27;206(5):987-998. Epub 2021 Jan 27.

The University of Queensland Diamantina Institute, Translational Research Institute, Woolloongabba, Queensland 4102, Australia;

Prophylactic human papillomavirus (HPV) vaccines are commercially available for prevention of infection with cancerogenic HPV genotypes but are not able to combat pre-existing HPV-associated disease. In this study, we designed a nanomaterial-based therapeutic HPV vaccine, comprising manganese (Mn)-doped silica nanoparticles (Mn-SNPs) and the viral neoantigen peptide GF001 derived from the HPV16 E7 oncoprotein. We show in mice that Mn-SNPs act as self-adjuvants by activating the inflammatory signaling pathway via generation of reactive oxygen species, resulting in immune cell recruitment to the immunization site and dendritic cell maturation. Mn-SNPs further serve as Ag carriers by facilitating endo/lysosomal escape via depletion of protons in acidic endocytic compartments and subsequent Ag delivery to the cytosol for cross-presentation. The Mn-SNPs+GF001 nanovaccine induced strong E7-specific CD8 T cell responses, leading to remission of established murine HPV16 E7-expressing solid TC-1 tumors and E7-expressing transgenic skin grafts. This vaccine construct offers a simple and general strategy for therapeutic HPV and potentially other cancer vaccines.
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http://dx.doi.org/10.4049/jimmunol.2000355DOI Listing
March 2021

Synergistic Effect of Two Nanotechnologies Enhances the Protective Capacity of the Sporozoite p67C Antigen in Cattle.

J Immunol 2021 02 8;206(4):686-699. Epub 2021 Jan 8.

Animal and Human Health Program, International Livestock Research Institute, Nairobi 00100, Kenya.

East Coast fever (ECF), caused by , is the most important tick-borne disease of cattle in sub-Saharan Africa. Practical disadvantages associated with the currently used live-parasite vaccine could be overcome by subunit vaccines. An 80-aa polypeptide derived from the C-terminal portion of p67, a sporozoite surface Ag and target of neutralizing Abs, was the focus of the efforts on subunit vaccines against ECF and subjected to several vaccine trials with very promising results. However, the vaccination regimen was far from optimized, involving three inoculations of 450 μg of soluble p67C (s-p67C) Ag formulated in the Seppic adjuvant Montanide ISA 206 VG. Hence, an improved formulation of this polypeptide Ag is needed. In this study, we report on two nanotechnologies that enhance the bovine immune responses to p67C. Individually, HBcAg-p67C (chimeric hepatitis B core Ag virus-like particles displaying p67C) and silica vesicle (SV)-p67C (s-p67C adsorbed to SV-140-C, octadecyl-modified SVs) adjuvanted with ISA 206 VG primed strong Ab and T cell responses to p67C in cattle, respectively. Coimmunization of cattle () with HBcAg-p67C and SV-p67C resulted in stimulation of both high Ab titers and CD4 T cell response to p67C, leading to the highest subunit vaccine efficacy we have achieved to date with the p67C immunogen. These results offer the much-needed research depth on the innovative platforms for developing effective novel protein-based bovine vaccines to further the advancement.
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http://dx.doi.org/10.4049/jimmunol.2000442DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7851744PMC
February 2021

Nitrogen-Doped Mesoporous Carbon Microspheres by Spray Drying-Vapor Deposition for High-Performance Supercapacitor.

Front Chem 2020 10;8:592904. Epub 2020 Nov 10.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD, Australia.

Nitrogen-doped mesoporous carbon microspheres have been successfully synthesized via a spray drying-vapor deposition method for the first time, using commercial Ludox silica nanoparticles as hard templates. Compared to freeze-drying and air-drying methods, mesoporous carbon with a higher packing density can be achieved through the spray drying method. Vapor deposition of polypyrrole followed by carbonization and etching is beneficial for the generation of ultra-thin carbon network. The mesoporous carbon microspheres possess a mesopore-dominate (95%) high surface area of 1528 m g, a wall thickness of 1.8 nm, and a nitrogen content of 8 at% in the framework. Benefiting from the increased apparent density, high mesopore surface area, and considerable nitrogen doping, the resultant mesoporous carbon microspheres show superior gravimetric/volumetric capacitance of 533.6 F g and 208.1 F cm, good rate performance and excellent cycling stability in electric double-layer capacitors.
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http://dx.doi.org/10.3389/fchem.2020.592904DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7683435PMC
November 2020

Ternary MOF-on-MOF heterostructures with controllable architectural and compositional complexity via multiple selective assembly.

Nat Commun 2020 Oct 2;11(1):4971. Epub 2020 Oct 2.

School of Chemistry and Molecular Engineering, East China Normal University, 200241, Shanghai, P. R. China.

Assembly of different metal-organic framework (MOF) building blocks into hybrid MOF-on-MOF heterostructures is promising in chemistry and materials science, however the development of ternary MOF-on-MOF heterostructures with controllable architectural and compositional complexity is challenging. Here we report the synthesis of three types of ternary MOF-on-MOF heterostructures via a multiple selective assembly strategy. This strategy relies on the choice of one host MOF with more than one facet that can arrange the growth of a guest MOF, where the arrangement is site-selective without homogenous growth of guest MOF or homogenous coating of guest on host MOF. The growth of guest MOF on a selected site of host MOF in each step provides the opportunity to further vary the combinations of arrangements in multiple steps, leading to ternary MOF-on-MOF heterostructures with tunable complexity. The developed strategy paves the way towards the rational design of intricate and unprecedented MOF-based superstructures for various applications.
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http://dx.doi.org/10.1038/s41467-020-18776-zDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7532534PMC
October 2020

Dendritic Mesoporous Silica Nanoparticle Adjuvants Modified with Binuclear Aluminum Complex: Coordination Chemistry Dictates Adjuvanticity.

Angew Chem Int Ed Engl 2020 10;59(44):19610-19617

Australian Institute for Bioengineering and Nanotechnology, UQ-JLU Joint Research Centre for Future Materials, The University of Queensland, St Lucia, Brisbane, QLD, 4072, Australia.

Aluminum-containing adjuvants used in vaccine formulations suffer from low cellular immunity, severe aggregation, and accumulation in the brain. Conventional aluminosilicates widely used in the chemical industry focus mainly on acidic sites for catalytic applications, but they are rarely used as adjuvants. Reported here is an innovative "ligand-assisted steric hindrance" strategy to create a high density of six-coordinate Al-OH groups with basicity on dendritic mesoporous silica nanoparticles as new nanoadjuvants. Compared to four-coordinate Al-modified counterparts, Al-OH-rich aluminosilicate nanoadjuvants enhance cellular delivery of antigens and provoke stronger cellular immunity. Moreover, the aluminum accumulation in the brain is more reduced than that with a commercial adjuvant. These results show that coordination chemistry can be used to control the adjuvanticity, providing new understanding in the development of next-generation vaccine adjuvants.
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http://dx.doi.org/10.1002/anie.202006861DOI Listing
October 2020

Eliciting Immunogenic Cell Death via a Unitized Nanoinducer.

Nano Lett 2020 09 14;20(9):6246-6254. Epub 2020 Aug 14.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, Brisbane, QLD 4072, Australia.

Utilizing chemotherapeutics to induce immunogenic cell death (ICD) is a promising strategy to sensitize tumor cells and induce anticancer immunity. However, the application of traditional ICD inducers, such as chemodrugs, is largely hindered by their low tumor selectivity and severe side effects. Here, a new unitized ICD nanoinducer with high potency and cancer cell specificity is reported to achieve effective cancer immunotherapy. This nanoinducer is composed of disulfide-bond-incorporated organosilica nanoparticles, curcumin (CUR), and iron oxide nanoparticles, which can deplete intracellular glutathione, produce hydroxyl radicals, and induce cancer-cell-specific Ca depletion as well as thioredoxin reductase inhibition. While the components are unable to induce ICD individually, their complementary pharmaceutical activities significantly elevate intracellular oxidative stress and endoplasmic reticulum stress in parallel. Consequently, ICD and systemic antitumor immunity can be elicited. Compared to the conventional ICD inducer doxorubicin, the unitized nanoinducer exhibits significantly improved ICD-inducing activity and cancer cell selectivity.
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http://dx.doi.org/10.1021/acs.nanolett.0c00713DOI Listing
September 2020

[email protected] Mesoporous Silica Nanoparticles for Lactate Depletion and Tumor Microenvironment Regulation.

Angew Chem Int Ed Engl 2020 12 7;59(49):22054-22062. Epub 2020 Oct 7.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, Brisbane, QLD, 4072, Australia.

The direct depletion of lactate accumulated in the tumor microenvironment holds promise for cancer therapy but remains challenging. Herein, we report a one-pot synthesis of [email protected] dendritic mesoporous silica nanoparticles (ODMSNs) to address this problem. ODMSNs self-assembled through a time-resolved lamellar growth mechanism feature an openworked core and a dendritic shell, both constructed by silica nanosheets of ≈3 nm. With a large pore size, high surface area and pore volume, ODMSNs exhibited a high loading capacity (>0.7 g g ) of lactate oxidase (LOX) and enabled intratumoral lactate depletion by >99.9 %, leading to anti-angiogenesis, down-regulation of vascular endothelial growth factor, and increased tumor hypoxia. The latter event facilitates the activation of a co-delivered prodrug for enhancing anti-tumor and anti-metastasis efficacy. This study provides an innovative nano-delivery system and demonstrates the first example of direct lactate-depletion-enabled chemotherapy.
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http://dx.doi.org/10.1002/anie.202001469DOI Listing
December 2020

Shaping Nanoparticles for Interface Catalysis: Concave Hollow Spheres via Deflation-Inflation Asymmetric Growth.

Adv Sci (Weinh) 2020 Jul 19;7(13):2000393. Epub 2020 May 19.

Australian Institute for Bioengineering and Nanotechnology The University of Queensland Brisbane Queensland 4072 Australia.

Hollow spheres are charming objects in nature. In this work, an unexpected deflation-inflation asymmetric growth (DIAG) strategy is reported, generating hollow nanoparticles with tailored concave geometry for interface catalysis. Starting from aminophenol-formaldehyde (APF) nanospheres where the interior crosslinking degree is low, fully deflated nanobowls are obtained after etching by acetone. Due to APF etching and repolymerization reactions occuring asymmetrically within a single particle, an autonomous inflation process is observed similar to a deflated basketball that inflates back to a "normal" ball, which is rare at the nanoscale. A nucleophilic addition reaction between acetone and APF is elucidated to explain the chemistry origin of the DIAG process. Interestingly, the deflated APF hollow spheres enable preferential immobilization of lipase in the concave domain, which facilitates the stabilization of Pickering emulsion droplets for enhanced enzymatic catalysis at the oil-water interface. The study provides new understandings in the designable synthesis of hollow nanoparticles and paves the way toward a wide range of applications of asymmetric architectures.
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http://dx.doi.org/10.1002/advs.202000393DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7341089PMC
July 2020

Silica-Based Nanoparticles for Biomedical Applications: From Nanocarriers to Biomodulators.

Acc Chem Res 2020 08 15;53(8):1545-1556. Epub 2020 Jul 15.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland 4072, Australia.

Silica-based nanoparticles (SNPs) are a classic type of material employed in biomedical applications because of their excellent biocompatibility and tailorable physiochemical properties. Typically, SNPs are designed as nanocarriers for therapeutics delivery, which can address a number of intrinsic drawbacks of therapeutics, including limited bioavailability, short circulation lifetime, and unfavorable biodistribution. To improve the delivery efficiency and spatiotemporal precision, tremendous efforts have been devoted to engineering the physiochemical properties of SNPs, including particle size, morphology, and mesostructure, as well as conjugating targeting ligands and/or "gatekeepers" to endow improved cell selectivity and on demand release profiles. Despite significant progress, the biologically inert nature of the bare silica framework has largely restricted the functionalities of SNPs, rendering conventional SNPs mainly as nanocarriers for targeted delivery and controlled release. To meet the requirements of next generation nanomedicines with improved efficacy and precision, new insights on the relationship between the physiochemical properties of SNPs and their biological behavior are highly valuable. Meanwhile, a conceptual shift from a simple spatiotemporal control mechanism to a more sophisticated biochemistry and signaling pathway modulation would be of great importance.In this Account, an overview of our recent contribution to the field is presented, wherein SNPs with rationally designed nanostructures and nanochemistry are applied as nanocarriers (defined as "nanomaterials being used as a transport module for another substance" according to Wikipedia) and/or biomodulators (defined as "any material that modifies a biological response" according to Wiktionary). This Account encompasses two main sections. In the first section, we focus on the conventional nanocarriers concept with new insights on the design principles of the nanostructures. We present examples to demonstrate the engineering of pore geometry, surface topology, and asymmetry of nanoparticles to achieve enhanced drug, gene, and protein delivery efficiency. The contribution of surface roughness of SNPs on improving the cellular uptake efficiency, adhesion property, and DNA transfection capacity is particularly highlighted. In the second section, we discuss novel SNPs designed as biomodulators to regulate intracellular microenvironment and cell signaling, such as the oxidative stress and glutathione levels for improving the anticancer efficacy of therapeutics and mRNA transfection in specific cell lines. The interplay between the nanoparticles, biological system, and drugs is discussed. We further discuss how to engineer the composition of SNPs to modulate metal hemostasis to realize inherent anticancer activity. Two typical examples, including modulating copper signaling for tumor vasculature targeted therapy and controlling iron signaling for macrophage polarization based immunotherapy, are presented to highlight the unique advantages of SNPs as nanosized therapeutics in comparison to molecular drugs. Moreover, utilizing these two examples, we showcase the possibility of designing SNPs with intrinsic pharmaceutical activity to indirectly control tumor growth without inducing significant cytotoxicity, thus alleviating the biosafety concerns of nanomedicines. At the end of this Account, we discuss our personal perspectives on the promises, opportunities, and issues in engineered SNPs as nanocarriers as well as their transition toward biomodulators. With a major focus on the latter scenario, the current status and possible future directions are outlined.
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http://dx.doi.org/10.1021/acs.accounts.0c00280DOI Listing
August 2020

Synthesis of cube-rod-tube triblock asymmetric nanostructures for enhanced heterogeneous catalysis.

Chem Commun (Camb) 2020 Jul;56(57):7973-7976

School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200241, P. R. China. and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland 4072, Australia.

A triblock asymmetric nanostructure composed of a core-shell [email protected] cube as the head, SiO2 rod as the body and SiO2 tube as the tail is fabricated via a sequential growth process combining solution-liquid-solid and droplet soft templating mechanisms, which can be used as a nano stir bar with accelerated catalytic performance.
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http://dx.doi.org/10.1039/d0cc03198dDOI Listing
July 2020

Emerging Concepts of Nanobiotechnology in mRNA Delivery.

Angew Chem Int Ed Engl 2020 12 9;59(52):23374-23385. Epub 2020 Sep 9.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD, 4072, Australia.

Introducing mRNA into cells has attracted intense interest for diverse applications; however, success requires delivery solutions. Engineered nanomaterials have been applied as mRNA nanocarriers; their functions are designed mainly as delivery vehicles, but rarely in regulation of the protein translation. Recently, progress in nanobiotechnology has shifted the design principle of mRNA nanocarriers from simple delivery tools to translation modulators. Here, we review the emerging concepts of nanomaterials regulating mRNA translation and recent progress in mRNA delivery. Designer nanomaterials providing integrated functions for specific mRNA applications are also reviewed to provide insights for the design of next-generation nanomaterials to revolutionize mRNA technology.
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http://dx.doi.org/10.1002/anie.202003545DOI Listing
December 2020

Lyophilization enabled disentanglement of polyethylenimine on rambutan-like silica nanoparticles for enhanced plasmid DNA delivery.

J Mater Chem B 2020 06 11;8(21):4593-4600. Epub 2020 May 11.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD 4072, Australia.

Polyethylenimine (PEI) functionalization onto nanoparticles is a widely used strategy for constructing particulate vectors for gene delivery. However, how to control the conformation of PEI chains and the resultant impact on gene transfection efficiency remains largely unexplored. Herein, we report that drying methods dramatically affect the conformation of PEI chains modified on the surface of silica nanoparticles and consequently the plasmid DNA transfection performance. Specifically, lyophilization renders less entangled PEI compared to commonly used vacuum drying as evidenced by an elevated glass transition temperature. The lyophilization induced disentangled conformation is likely associated with the solid-to-gas phase transition drying mechanism, which removes the bound crystal water content and thus reduces hydrogen bonding between amines. Moreover, we find that the stretched PEI chains on the surface of rambutan-like silica nanoparticles promote their binding capacity towards plasmid DNA molecules and thereby enhanced gene delivery and transfection efficiency. Our findings have provided new understanding about amine based polymers modified on nanoparticles, and have significant implications on the design of efficient particulate vectors for gene delivery.
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http://dx.doi.org/10.1039/d0tb00720jDOI Listing
June 2020

Materials Science in Australia.

Adv Mater 2020 05;32(18):e2001629

Centre for Clean Environment and Energy, Griffith University, Gold Coast Campus, Southport, Queensland, 4222, Australia.

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http://dx.doi.org/10.1002/adma.202001629DOI Listing
May 2020

MOFs derived Co/Cu bimetallic nanoparticles embedded in graphitized carbon nanocubes as efficient Fenton catalysts.

J Hazard Mater 2020 07 19;394:122567. Epub 2020 Mar 19.

School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, PR China; Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland, 4072, Australia. Electronic address:

In this work, Cu-Co bimetallic nanoparticles embedded carbon nanocubes (CuCo/CNC) are synthesized by direct carbonization of Cu-Co bimetal ZIF. The ratio of Cu and Co nanoparticles in CuCo/CNC as well as morphology, pore structure and graphitization degree of carbon substrates can be tuned by adjusting the molar ratio of Cu/Co (0:10, 1:9, 2:8, 3:7, 4:6 and 5:5) in ZIF precursors. The Fenton catalytic performances of CuCo/CNC are further studied by degrading a typical azo dye, Acid Orange II (AOII). The results show the CuCo/CNC with a Cu/Co ratio of 4/6 display the highest catalytic activity with faster dye degradation rate than other catalysts, which may be ascribed to the synergetic effects of optimized ratio of Cu/Co bimetals, high surface area and graphitized carbon framework. The stability and reusability of the catalyst has been investigated, showing a good performance after five consecutive runs. The catalysts prepared in this study can be used as an attractive alternative in heterogeneous Fenton chemistry and wastewater treatment.
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http://dx.doi.org/10.1016/j.jhazmat.2020.122567DOI Listing
July 2020

Site-specific growth of MOF-on-MOF heterostructures with controllable nano-architectures: beyond the combination of MOF analogues.

Chem Sci 2020 Mar 5;11(14):3680-3686. Epub 2020 Mar 5.

School of Chemistry and Molecular Engineering, East China Normal University Shanghai 200241 P. R. China

The integration of different metal-organic frameworks (MOFs) into one system has led to the recent combinatorial innovation of various MOF-on-MOF hybrids; however control over their site-specific growth beyond MOF analogues remains challenging. In this work, a site-specific epitaxial-growth strategy is developed to synthesize MOF-on-MOF heterostructures comprised of two MOFs with totally different compositions. A guest MOF (ZIF-8) is epitaxially grown on the specific {110} facets of a host MOF (MIL-125). Moreover, the position of ZIF-8 growth on MIL-125 is also selectable by using MIL-125 hosts with {110} facets exposed on either the corner or side surface. Consequently, two [email protected] heterostructures with elaborately designed different architectures are synthesized. Benefiting from the high adsorption capacity of ZIF-8 and the photocatalytic activity of MIL-125, the [email protected] heterostructures demonstrate synergistically enhanced photocatalytic performance compared to single MOF subunits. Moreover, the corner growth leads to higher activity than the side growth of the [email protected] heterostructures. Our contribution paves the way for the rational design of composite MOFs with tunable compositions and nanostructures using the crystal engineering approach.
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http://dx.doi.org/10.1039/d0sc00417kDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8152623PMC
March 2020

Bottom-up self-assembly of heterotrimeric nanoparticles and their secondary Janus generations.

Chem Sci 2019 Nov 19;10(44):10388-10394. Epub 2019 Sep 19.

Australian Institute for Bioengineering and Nanotechnology , The University of Queensland , St Lucia , Brisbane , QLD 4072 , Australia . Email: ; Email:

A bottom-up self-assembly approach is developed for the synthesis of type heterotrimeric nanoparticles, which can be converted into secondary Janus-type silica derivatives. Compared to spherical ones, Janus silica nanoparticles stimulate stronger phagocytosis and transcytosis through intestinal epithelial microfold cells and exhibit higher cargo transport across an epithelial monolayer model mimicking the human intestinal epithelium.
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http://dx.doi.org/10.1039/c9sc02961cDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6988604PMC
November 2019

A General Approach to Direct Growth of Oriented Metal-Organic Framework Nanosheets on Reduced Graphene Oxides.

Adv Sci (Weinh) 2020 Feb 3;7(4):1901480. Epub 2020 Jan 3.

School of Chemistry and Molecular Engineering East China Normal University Shanghai 200241 P. R. China.

Ultrathin metal-organic framework nanosheets (UMOFNs) deposited on graphene are highly attractive, however direct growth of UMOFNs on graphene with controlled orientations remains challenging. Here, a low-concentration-assisted heterogeneous nucleation strategy is reported for the direct growth of UMOFNs on reduced graphene oxides (rGO) surface with controllable orientations. This general strategy can be applied to construct various UMOFNs on rGO, including Co-ZIF, Ni-ZIF, Co, Cu-ZIF and Co, Fe-ZIF. When UMOFNs are mostly attached perpendicularly on rGO, a 3D foam-like hierarchical architecture (named [email protected]) is formed with an open pore structure and excellent conductivity, showing excellent performance as electrode materials for Li-ion batteries and oxygen evolution. The contribution has provided a strategy for improving the electrochemical performance of MOFs in energy storage applications.
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http://dx.doi.org/10.1002/advs.201901480DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7029658PMC
February 2020

Functional Nanoparticles with a Reducible Tetrasulfide Motif to Upregulate mRNA Translation and Enhance Transfection in Hard-to-Transfect Cells.

Angew Chem Int Ed Engl 2020 02 9;59(7):2695-2699. Epub 2020 Jan 9.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD, 4072, Australia.

Effective messenger RNA (mRNA) transfection in hard-to-transfect cells delivered by vectors is a long-standing challenge. Now it is hypothesized that the high intracellular glutathione level is associated with suppressed mRNA translation. This theory leads to a new design principle of next-generation mRNA vectors: nanoparticles with glutathione depletion chemistry upregulate mRNA translation and enhance transfection, which is beneficial for mRNA delivery in hard-to-transfect cells in vitro and in vivo.
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http://dx.doi.org/10.1002/anie.201914264DOI Listing
February 2020

Antibiotic-Free Antibacterial Strategies Enabled by Nanomaterials: Progress and Perspectives.

Adv Mater 2020 May 3;32(18):e1904106. Epub 2019 Dec 3.

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD, 4072, Australia.

Bacterial infection is one of the top ten leading causes of death globally and the worst killer in low-income countries. The overuse of antibiotics leads to ever-increasing antibiotic resistance, posing a severe threat to human health. Recent advances in nanotechnology provide new opportunities to address the challenges in bacterial infection by killing germs without using antibiotics. Antibiotic-free antibacterial strategies enabled by advanced nanomaterials are presented. Nanomaterials are classified on the basis of their mode of action: nanomaterials with intrinsic or light-mediated bactericidal properties and others that serve as vehicles for the delivery of natural antibacterial compounds. Specific attention is given to antibacterial mechanisms and the structure-performance relationship. Practical antibacterial applications employing these antibiotic-free strategies are also introduced. Current challenges in this field and future perspectives are presented to stimulate new technologies and their translation to fight against bacterial infection.
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http://dx.doi.org/10.1002/adma.201904106DOI Listing
May 2020
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