Publications by authors named "Yen Wei"

328 Publications

State-of-art review on preparation, surface functionalization and biomedical applications of cellulose nanocrystals-based materials.

Int J Biol Macromol 2021 Jul 14;186:591-615. Epub 2021 Jul 14.

Department of Chemistry and the Tsinghua Center for Frontier Polyer Research, Tsinghua University, Beijing 100084, China. Electronic address:

Cellulose nanocrystals (CNCs) are a class of sustainable nanomaterials that are obtained from plants and microorganisms. These naturally derived nanomaterials are of abundant hydroxyl groups, well biocompatibility, low cost and biodegradable potential, making them suitable and promising candidates for various applications, especially in biomedical fields. In this review, the recent advances and development on the preparation, surface functionalization and biomedical applications of CNCs-based materials have been summarized and outlined. The main context of this paper could be divided into the following three parts. In the first part, the preparation strategies based on physical, chemical, enzymatic and combination techniques for preparation of CNCs have been summarized. The surface functionalization methods for synthesis CNCs-based materials with designed properties and functions were outlined in the following section. Finally, the current state about applications of CNCs-based materials for tissue engineering, medical hydrogels, biosensors, fluorescent imaging and intracellular delivery of biological agents have been highlighted. Moreover, current issues and future directions about the above aspects have also pointed out and discussed. We believe this review will attract great research attention of scientists from materials, chemistry, biomedicine and other disciplines. It will also provide some important insights on the future development of CNCs-based materials especially in biomedical fields.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.ijbiomac.2021.07.066DOI Listing
July 2021

Rapid synthesis of polyimidazole functionalized MXene via microwave-irradiation assisted multi-component reaction and its iodine adsorption performance.

J Hazard Mater 2021 Jul 6;420:126580. Epub 2021 Jul 6.

Department of Chemistry and the Tsinghua Center for Frontier Polymer Research, Tsinghua University, Beijing 100084, China.

The adsorption applications of MXene-based adsorbents have intensively investigated recently. However, the performance of MXene-based adsorbents has been largely limited owing to their lack of functional groups and adsorptive sites. Therefore, surface functionalization of MXene is an important route to achieve better performance for environmental adsorption. Herein, polyionic liquid functionalized MXene (named as MXene-PIL) was prepared through a multi-component reaction and adsorptive removal of iodine by MXene-PIL was also evaluated. The successful generation of PIL on MXene was confirmed by a series of characterization measurements. Furthermore, the effects of contact time, iodine concentration, environmental temperature and other factors on the adsorption performance of MXene-PIL were investigated. Adsorption kinetic analysis including pseudo-first-order dynamic model, pseudo-second-order dynamic model and Weber-Morris model, adsorption thermodynamic analysis such as Langmuir and Freundlich models and Van't Hoff equation were used for further analysis the adsorption behavior of iodine by MXene-PIL. We demonstrated that the adsorption capacity could be as high as about 170 mg/g, which is obviously larger than the unmodified MXene and most of other reported adsorbents. Taken together, a simple strategy has been developed for in-situ generation of PIL on MXene and the resultant composites show potential application for adsorptive removal of iodine.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.jhazmat.2021.126580DOI Listing
July 2021

Revealing the Distribution of Aggregation-Induced Emission Nanoparticles via Dual-Modality Imaging with Fluorescence and Mass Spectrometry.

Research (Wash D C) 2021 19;2021:9784053. Epub 2021 Jun 19.

The Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing 100084, China.

Aggregation-induced emission nanoparticles (AIE NPs) are widely used in the biomedical field. However, understanding the biological process of AIE NPs via fluorescence imaging is challenging because of the strong background and poor penetration depth. Herein, we present a novel dual-modality imaging strategy that combines fluorescence imaging and label-free laser desorption/ionization mass spectrometry imaging (LDI MSI) to map and quantify the biodistribution of AIE NPs (TPAFN-F127 NPs) by monitoring the intrinsic photoluminescence and mass spectrometry signal of the AIE molecule. We discovered that TPAFN-F127 NPs were predominantly distributed in the liver and spleen, and most gradually excreted from the body after 5 days. The accumulation and retention of TPAFN-F127 NPs in tumor sites were also confirmed in a tumor-bearing mouse model. As a proof of concept, the suborgan distribution of TPAFN-F127 NPs in the spleen was visualized by LDI MSI, and the results revealed that TPAFN-F127 NPs were mainly distributed in the red pulp of the spleen with extremely high concentrations within the marginal zone. The toxicity test demonstrated that TPAFN-F127 NPs are nontoxic for a long-term exposure. This dual-modality imaging strategy provides some insights into the fine distribution of AIE NPs and might also be extended to other polymeric NPs to evaluate their distribution and drug release behaviors .
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.34133/2021/9784053DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8237597PMC
June 2021

Simultaneous surface functionalization and drug loading: A novel method for fabrication of cellulose nanocrystals-based pH responsive drug delivery system.

Int J Biol Macromol 2021 Jul 2;182:2066-2075. Epub 2021 Jun 2.

Department of Chemistry and the Tsinghua Center for Frontier Polymer Research, Tsinghua University, Beijing 100084, China.

Herein, a novel strategy for surface functionalization and drug loading of cellulose nanocrystals (CNCs) through formation of hydrazone bonds between functionalized CNCs and aldehyde group containing polyethylene glycol (CHO-PEG)/anticancer drug doxorubicin (DOX) was reported for the first time. DOX could be loaded on PEGylated CNCs with high capacity and released from drug complexes (P-CNCs-D) with pH dependent behavior. The biological evaluation results demonstrated that drug carriers (CNCs-EBO-NH) showed negative cytotoxicity while DOX could be transported into cells and exhibits desirable anticancer effects. As compared with other method, the method developed in this work is rather simple and effective and can be achieved for simultaneous for surface functionalization and drug loading in a one-pot route. This work will open a new avenue for fabrication of various multifunctional composites based on other carbohydrate polymers or materials and to explore their applications in biomedical fields.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.ijbiomac.2021.05.193DOI Listing
July 2021

Gold-iron selenide nanocomposites for amplified tumor oxidative stress-augmented photo-radiotherapy.

Biomater Sci 2021 Jun;9(11):3979-3988

Key Laboratory of Advanced Materials, Ministry of Education of China, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China. and State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China.

The radio-resistance of tumor tissues has been considered a great challenge for cancer radiotherapy (RT).The development of nanoparticle (NP)-based radio-sensitizers can enhance the radio-sensitization of tumor tissues while reducing the side effects to surrounding tissues. However, most of the nano-radiosensitizers show increased radiation deposition with a high-Z element but achieve limited enhancement. Herein, we investigated polyethylene glycol (PEG)-modified gold-iron selenide nanocomposites (Au-FeSe2 NCs) for simultaneously enhancing therapeutic effects in multiple ways. In this study, the high-Z element Au (Z = 79) endows Au-FeSe2 NCs with enhanced X-ray deposition and thus causes more DNA damage. On the other hand, Au-FeSe2 exhibits the ability to produce reactive oxygen species (ROS) by catalyzing endogenous hydrogen peroxide in tumor sites as well as improve the hydrogen peroxide level during ionizing irradiation. Finally, combined with photothermal therapy (PTT), Au-FeSe2 NCs could exhibit a remarkable RT/PTT synergistic effect on tumor treatment.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1039/d1bm00306bDOI Listing
June 2021

Construction of ionic liquid functionalized MXene with extremely high adsorption capacity towards iodine via the combination of mussel-inspired chemistry and Michael addition reaction.

J Colloid Interface Sci 2021 May 20;601:294-304. Epub 2021 May 20.

Department of Chemistry and the Tsinghua Center for Frontier Polymer Research, Tsinghua University, Beijing 100084, PR China. Electronic address:

In this work, a highly efficient adsorbent based on ionic liquid functionalized MXene has been fabricated through the combination of mussel-inspired chemistry and Michael addition reaction. The surface of MXene was first coated with polydopamine (PDA) through self-polymerization of dopamine and the amino groups were introduced on the surface of MXene simultaneously. After that, the ene bond-containing ionic liquid was further immobilized on the surface of MXene-PDA to obtain MXene-PDA-IL. As a concept, the adsorptive removal of iodine using MXene-PDA-IL was conducted and the effects of various factors on the adsorption behavior were examined. The experimental data were analyzed by intermittent adsorption experiments, the adsorption kinetics, adsorption isotherm, adsorption thermodynamics, and cyclic adsorption experiments. We found that the adsorption procedure could reach equilibrium within 10 min after mixing adsorbent and iodine. The maximum adsorption capacity of MXene-PDA-IL towards iodine was as high as 695.4 mg g, which is greater than most of reported adsorbents. Considered the advantages of mussel-inspired chemistry for surface functionalization and the adsorption capacity of ionic liquids, the method could be used for construct a number of composites with potential for adsorption applications.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.jcis.2021.05.096DOI Listing
May 2021

Promotion of Color-Changing Luminescent Hydrogels from Thermo to Electrical Responsiveness toward Biomimetic Skin Applications.

ACS Nano 2021 06 1;15(6):10415-10427. Epub 2021 Jun 1.

Key Laboratory of Marine Materials and Related Technologies, Zhejiang Key Laboratory of Marine Materials and Protective Technologies, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China.

The active color-changing ability of many living species has inspired scientists to replicate the optical property into soft wet and tissue-like hydrogel materials. However, the color-changing processes of most reported examples are controlled by the traditional stimuli (, pH, temperature, and ions), which may suffer from the residual chemical product accumulation, and have difficulty in achieving local control and integration into the commercial robots, especially when applied as biomimetic skins. Herein, inspired by the nervous (bioelectricity) control of skin color change in cephalopods, we present an electrically powered multicolor fluorescent hydrogel system with asymmetric configuration that couples thermoresponsive fluorescent hydrogel with stacked graphene assembly (SGA)-based conductive paper through luminous paint as the middle layer. Owing to the highly controllable electrical stimulus in terms of amplitude and duration, the Joule heat supplied by SGA film can be regulated locally and in real time, leading to precise and local emission color control at low voltage. It also avoids the addition of any chemicals. Furthermore, the electrically powered color-changing hydrogel system can be conveniently integrated into the commercial robots as biomimetic skins that help them achieve desirable camouflage, display, or alarming functions.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1021/acsnano.1c02720DOI Listing
June 2021

Metal-phenolic networks: facile assembled complexes for cancer theranostics.

Theranostics 2021 19;11(13):6407-6426. Epub 2021 Apr 19.

The Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China.

In recent years, metal-phenolic networks (MPNs) have attracted increasing attention for the engineering of multi-functional platforms because of their easy fabrication processes, excellent physicochemical properties, outstanding biocompatibility, and promising theranostic applications. In this review, we summarize recent progress in the design, synthesis, shape-control, biocompatibility evaluation, and potential theranostic applications of MPNs, especially for cancer theranostics. First, we provide an overview of various MPN systems, relevant self-assembly procedures, and shape-controllable preparation. The and biocompatibility evaluation of MPNs is also discussed, including co-incubation viability, adhesion, bio-distribution, and inflammation. Finally, we highlight the significant achievements of various MPNs for cancer theranostics, such as tumor imaging, drug delivery, photothermal therapy, radiotherapy, and chemo- and photo-dynamic therapy. This review provides a comprehensive background on the design and controllable synthesis, and biocompatibility evaluation, applications of MPNs as cancer theranostic agents, and presents an overview of the most up-to-date achievements in this field.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.7150/thno.58711DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8120219PMC
July 2021

Recent advances in thermo-sensitive hydrogels for drug delivery.

J Mater Chem B 2021 04 22;9(13):2979-2992. Epub 2021 Mar 22.

Laboratory of Chemical Biology, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.

Hydrogels are cross-linked hydrophilic macromolecules that contain a certain amount of water. Due to their biocompatible, highly tunable and hydrophilic nature, hydrogels have attracted much attention in the applications of chemical, biomedical and pharmaceutical fields over the past twenty years. In particular, thermo-sensitive hydrogels, which can undergo phase transition or swell/deswell as ambient temperature changes, endow the drug delivery system with enhanced local drug penetration, desirable spatial and temporal control, and improved drug bioavailability. These merits facilitate their extensive applications in drug delivery. In this review, we focus on advances in the development of different thermo-sensitive polymers as a scaffold for drug delivery, including poly(N-isopropylacrylamide) (pNIPAAM), poloxamer, polyethylene glycol/poly(lactic acid)co-(glycolic acid) (PEG/PLGA), and chitosan. The state-of-the-art thermo-sensitive hydrogels for various pharmaceutical applications, such as anti-tumor drug delivery, transdermal drug delivery, ocular drug delivery, nasal drug delivery, and buccal drug delivery, are elaborated. Finally, the future research perspectives and challenges are also discussed, which could facilitate the translation of thermo-sensitive hydrogels for drug delivery from bench to bedside.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1039/d0tb02877kDOI Listing
April 2021

Poly(amino acid)s-based star AIEgens for cell uptake with pH-response and chiral difference.

Colloids Surf B Biointerfaces 2021 Jun 9;202:111687. Epub 2021 Mar 9.

Beijing Laboratory of Biomedical Materials, Beijing University of Chemical Technology, Beijing 100029, PR China. Electronic address:

Chiral aggregation-induced emission luminogens (AIEgens) are the new-generation chiral sensors that regulate chiral signals from the molecular level to the macroscopic assembly. Expanding applications of chiral AIEgens and in-depth understanding of their chiral recognition in biological systems are meaningful. Herein, two star chiral AIEgens, consisting of tetraphenylethene (TPE) as core and poly(N-acryloyl-L(D) valine) (PLV or PDV) as arms, were precisely synthesized via atom transfer radical polymerization (ATRP) technique and named TPE-PLV and TPE-PDV. They possessed typical AIE characteristics and exhibited an increase in concentration-dependent fluorescence intensity. The two AIEgens were pH-responsive and had strong AIE-related emission in acidic solution. Importantly, AIEgens can enter the living cells by ATP dependent endocytosis, then light them up. The interactions between the AIEgens and living human hepatocarcinoma (HepG2) cells revealed that the internalization process of TPE-PLV and TPE-PDV was both chiral-dependent and pH-responsive. This novel strategy for synthesizing poly(amino acid)s functionalized AIEgens could inspire the development of promising fluorescent materials with chirality.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.colsurfb.2021.111687DOI Listing
June 2021

and Study on an Injectable Glycol Chitosan/Dibenzaldehyde-Terminated Polyethylene Glycol Hydrogel in Repairing Articular Cartilage Defects.

Front Bioeng Biotechnol 2021 16;9:607709. Epub 2021 Feb 16.

Chinese PLA General Hospital, Institute of Orthopedics, Beijing, China.

The normal anatomical structure of articular cartilage determines its limited ability to regenerate and repair. Once damaged, it is difficult to repair it by itself. How to realize the regeneration and repair of articular cartilage has always been a big problem for clinicians and researchers. Here, we conducted a comprehensive analysis of the physical properties and cytocompatibility of hydrogels, and evaluated their feasibility as cell carriers for Adipose-derived mesenchymal stem cell (ADSC) transplantation. Concentration-matched hydrogels were co-cultured with ADSCs to confirm ADSC growth in the hydrogel and provide data supporting experiments, which comprised the hydrogel/ADSCs, pure-hydrogel, defect-placement, and positive-control groups. Rat models of articular cartilage defect in the knee joint region was generated, and each treatment was administered on the knee joint cartilage area for each group; in the positive-control group, the joint cavity was surgically opened, without inducing a cartilage defect. The reparative effect of injectable glycol chitosan/dibenzaldehyde-terminated polyethylene glycol (GCS/DF-PEG) hydrogel on injured articular cartilage was evaluated by measuring gross scores and histological score of knee joint articular-cartilage injury in rats after 8 weeks. The 1.5% GCS/2% DF-PEG hydrogels degraded quickly . Then, We perform and experiments to evaluate the feasibility of this material for cartilage repair and .
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.3389/fbioe.2021.607709DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7928325PMC
February 2021

Multifunctional Organic Fluorescent Probe with Aggregation-Induced Emission Characteristics: Ultrafast Tumor Monitoring, Two-Photon Imaging, and Image-Guide Photodynamic Therapy.

ACS Appl Mater Interfaces 2021 Feb 9;13(7):7987-7996. Epub 2021 Feb 9.

MOE Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology, Department of Chemistry, Tsinghua University, Beijing 100084, China.

The development of multifunctional photosensitizers (PSs) with aggregation-induced emission (AIE) properties plays a critical role in promoting the progress of the photodynamic therapy (PDT). In this work, a multifunctional PS (named DSABBT NPs) with AIE activity has been designed and prepared to carry out ultrafast staining, excellent two-photon bioimaging, and high-efficiency image-guided PDT. Simply, DSABBT with AIE characteristic was synthesized by one-step Schiff reaction of 4-(diethylamino)-salicylaldehyde (DSA) and 4,7-bis(4-aminophenyl)-2,1,3-benzothiadiazole (BBT). Then, DSABBT and DSPE-PEG-cRGD generate nanoparticles (NPs) easily in an ultrapure water/tetrahydrofuran mixture through a facile nanoprecipitation at room temperature. We found that DSABBT NPs exhibit bright solid-state fluorescence with large stokes shifts (180 nm) and two-photon absorption cross-section (1700 GM). Importantly, DSABBT NPs exhibited excellent ability of ultrafast staining and two-photon imaging, which can readily label suborganelles by subtly shaking the living cells for 5 s under mild conditions. Moreover, DSABBT NPs displayed high singlet oxygen (O) generation capacity and remarkable image-guided PDT efficiency. Therefore, DSABBT NPs can act as the promising candidate for multifunctional PSs, which can destroy cancer cells and block malignant tumor growth via the production of reactive oxygen species upon irradiation conditions. These outcomes provide us with a selectable strategy for developing multifunctional theranostic systems.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1021/acsami.0c21309DOI Listing
February 2021

Recent Advances on Fabrication of Polymeric Composites Based on Multicomponent Reactions for Bioimaging and Environmental Pollutant Removal.

Macromol Rapid Commun 2021 Mar 4;42(6):e2000563. Epub 2021 Feb 4.

Department of Chemistry and the Tsinghua Center for Frontier Polymer Research, Tsinghua University, Beijing, 100084, P. R. China.

As the core of polymer chemistry, manufacture of functional polymers is one of research hotspots over the past several decades. Various polymers are developed for diverse applications due to their tunable structures and unique properties. However, traditional step-by-step preparation strategies inevitably involve some problems, such as separation, purification, and time-consuming. The multicomponent reactions (MCRs) are emerging as environmentally benign synthetic strategies to construct multifunctional polymers or composites with pendant groups and designed structures because of their features, such as efficient, fast, green, and atom economy. This mini review summarizes the latest advances about fabrication of multifunctional fluorescent polymers or adsorptive polymeric composites through different MCRs, including Kabachnik-Fields reaction, Biginelli reaction, mercaptoacetic acid locking imine reaction, Debus-Radziszewski reaction, and Mannich reaction. The potential applications of these polymeric composites in biomedical and environmental remediation are also highlighted. It is expected that this mini-review will promote the development preparation and applications of functional polymers through MCRs.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1002/marc.202000563DOI Listing
March 2021

Universal and tunable liquid-liquid separation by nanoparticle-embedded gating membranes based on a self-defined interfacial parameter.

Nat Commun 2021 Jan 4;12(1):80. Epub 2021 Jan 4.

Department of Chemistry, Tsinghua University, 100084, Beijing, P.R. China.

Superwetting porous membranes with tunable liquid repellency are highly desirable in broad domains including scientific research, chemical industry, and environmental protection. Such membranes should allow for controllable droplet bouncing or spreading, which is difficult to achieve for low surface energy organic liquids (OLs). Here we develop an interfacial physical parameter to regulate the OL wettability of nanoparticle-embedded membranes by structuring synergistic layers with reconfigurable surface energy components. Under the tunable solid-liquid interaction in the aggregation-induced process, the membranes demonstrate positive/negative liquid gating regularity for polar protic liquids, polar aprotic liquids, and nonpolar liquids. Such a membrane can be employed as self-adaptive gating for various immiscible liquid mixtures with superior separation efficiency and permeation flux, even afford successive achievement of high-performance in situ extraction-back extraction coupling. This study should provide distinctive insights into intrinsic wetting behaviors and have pioneered a rational strategy to design high-performance separation materials for diverse applications.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1038/s41467-020-20369-9DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7782719PMC
January 2021

Improving Chronic Diabetic Wound Healing through an Injectable and Self-Healing Hydrogel with Platelet-Rich Plasma Release.

ACS Appl Mater Interfaces 2020 Dec 1;12(50):55659-55674. Epub 2020 Dec 1.

Key Laboratory for Biomechanics and Mechanobiology of Ministry of Education, School of Biological Science and Medical Engineering, Beijing Advanced Innovation Centre for Biomedical Engineering, Beihang University, Xue Yuan Road No. 37, Haidian District, Beijing 100191, People's Republic of China.

Diabetic skin ulcer is one of the severe complications of diabetes mellitus, which has a high incidence and may cause death or disability. Platelet-rich plasma (PRP) is widely used in the treatment of diabetic wounds due to the effect of growth factors (GFs) derived from it. However, the relatively short half-life of GFs limits their applications in clinics. In addition, the presence of a large amount of proteases in the diabetic wound microenvironment results in the degradation of GFs, which further impedes angiogenesis and diabetic wound healing. In our study, we fabricated a self-healing and injectable hydrogel with a composite of chitosan, silk fibroin, and PRP ([email protected]) for promoting diabetic wound healing. [email protected] could protect PRP from enzymatic hydrolysis, release PRP sustainably, and enhance the chemotaxis of mesenchymal stem cells. The results showed that it could promote the proliferation of repair cells . Moreover, it could enhance wound healing by expediting collagen deposition, angiogenesis, and nerve repair in a type 2 diabetic rat model and a rat skin defect model. We hope that this study will offer a new treatment for diabetic nonhealing wounds in clinics.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1021/acsami.0c17142DOI Listing
December 2020

High-throughput preparation of radioprotective polymers via Hantzsch's reaction for in vivo X-ray damage determination.

Nat Commun 2020 12 4;11(1):6214. Epub 2020 Dec 4.

The Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing, 100084, China.

Radioprotectors for acute injuries caused by large doses of ionizing radiation are vital to national security, public health and future development of humankind. Here, we develop a strategy to explore safe and efficient radioprotectors by combining Hantzsch's reaction, high-throughput methods and polymer chemistry. A water-soluble polymer with low-cytotoxicity and an excellent anti-radiation capability has been achieved. In in vivo experiments, this polymer is even better than amifostine, which is the only approved radioprotector for clinical applications, in effectively protecting zebrafish embryos from fatally large doses of ionizing radiation (80 Gy X-ray). A mechanistic study also reveals that the radioprotective ability of this polymer originates from its ability to efficiently prevent DNA damage due to high doses of radiation. This is an initial attempt to explore polymer radioprotectors via a multi-component reaction. It allows exploiting functional polymers and provides the underlying insights to guide the design of radioprotective polymers.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1038/s41467-020-20027-0DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7718248PMC
December 2020

Fabrication of claviform fluorescent polymeric nanomaterials containing disulfide bond through an efficient and facile four-component Ugi reaction.

Mater Sci Eng C Mater Biol Appl 2021 Jan 25;118:111437. Epub 2020 Aug 25.

Department of Chemistry and the Tsinghua Center for Frontier Polymer Research, Tsinghua University, Beijing 100084, China; Department of Chemistry and Center for Nanotechnology and Institute of Biomedical Technology, Chung-Yuan Christian University, Chung-Li 32023, Taiwan. Electronic address:

Multicomponent reactions (MCRs) have attracted broad interest for preparation of functional nanomaterials especially for the synthesis of functional polymers. Herein, we utilized an "old" MCR, the four-component Ugi reaction, to synthesize disulfide bond containing poly(PEG-TPE-DTDPA) amphiphilic copolymers with aggregation-induced emission (AIE) feature. This four-component Ugi reaction was carried out under rather mild reaction conditions, such as room temperature, no gas protection and absent of catalysts. The amphiphilic poly(PEG-TPE-DTDPA) copolymers with high number-average molecular weight (up to 86,440 Da) can self-assemble into claviform fluorescent polymeric nanoparticles (FPNs) in aqueous solution, and these water-dispersed nanoparticles exhibited strong emission, large Stokes shift (142 nm), low toxicity and remarkable ability in cellular imaging. Moreover, owing to the introduction of 3,3'-dithiodipropionic acid with disulfide bond, the resultant AIE-active poly(PEG-TPE-DTDPA) could display reduction-responsiveness and be utilized for synthesis of photothermal agents in-situ. Therefore, the AIE-active poly(PEG-TPE-DTDPA) could be promising for controlled intracellular delivery of biological activity molecules and fabrication of multifunctional AIE-active materials. Therefore, these novel AIE-active polymeric nanoparticles could be of great potential for various biomedical applications, such as biological imaging, stimuli-responsive drug delivery and theranostic applications.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.msec.2020.111437DOI Listing
January 2021

Hollow Au/Polypyrrole Capsules to Form Porous and Neural Network-Like Nanofibrous Film for Wearable, Super-Rapid, and Ultrasensitive NH Sensor at Room Temperature.

ACS Appl Mater Interfaces 2020 Dec 24;12(49):55056-55063. Epub 2020 Nov 24.

Institute for Frontier Materials, Deakin University, Locked Bag 2000, Geelong, Victoria 3220, Australia.

Wearable conducting polymer-based NH sensors are highly desirable in real-time environmental monitoring and human health protection but still a challenge for their relatively long response/recovery time and moderate sensitivity at room temperature. Herein, we present an effective route to fulfill this challenge by constructing porous and neural network-like Au/polypyrrole (Au/PPy) electrospun nanofibrous film with hollow capsular units for NH sensor. Taking the unique architecture and synergistic effect between Au and PPy, our sensor exhibits not only super-rapid response/recovery time (both ∼7 s), faster than all reported sensors, but also stable and ultrahigh sensitivity (response reaches ∼2.3 for 1 ppm NH) at room temperature even during repeated deformation. Furthermore, good selectivity has been also achieved. These outstanding properties make our sensor hold great potential in real-time NH-related disease diagnosis and environmental monitoring at room temperature.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1021/acsami.0c15585DOI Listing
December 2020

An Adaptable Cryptosystem Enabled by Synergies of Luminogens with Aggregation-Induced-Emission Character.

Adv Mater 2020 Dec 27;32(48):e2004616. Epub 2020 Oct 27.

The Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology, Department of Chemistry, Tsinghua University, Beijing, 100084, China.

The strong emission in the solid state and the feasibility of introducing stimuli responsiveness make aggregation-induced-emission luminogens promising for optical information encryption. Yet, the vast majority of previous reports rely on subtle changes in the molecular conformation or intermolecular interactions, limiting the robustness, multiplicity, capacity, and security of the resulting cryptosystems. Herein, a versatile cryptographic system is presented based on three interconnected and orthogonal covalent transformations concerning a tetraphenylethylene-maleimide conjugate. The cryptosystem is adapted into four configurations with different functionalities by organizing the reactions and molecules in different ways. These variants either balance the accessibility and security of the encrypted information or improve the security and density in data encryption. Significantly, they allow variable decryption from a single encryption and reconstruction of the chemical nature hidden in the fluorescent pattern can only be accessed through given algorithms. These results highlight the importance of multi-component synergies in advancing information encryption systems, which is enabled by the robustness and diversity stemming from the covalent nature of these transformations.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1002/adma.202004616DOI Listing
December 2020

Aggregation-induced Emission Based Fluorogens for Mitochondria-targeted Tumor Imaging and Theranostics.

Chem Asian J 2020 Dec 19;15(23):3942-3960. Epub 2020 Oct 19.

Department of Nuclear Medicine and PET-CT Center, The Second Hospital of Zhejiang University School of Medicine, Hangzhou, Zhejiang Province, 310009, P. R. China.

Occurrence and development of cancer are multifactorial and multistep processes which involve complicated cellular signaling pathways. Mitochondria, as the energy producer in cells, play key roles in tumor cell growth and division. Since mitochondria of tumor cells have a more negative membrane potential than those of normal cells, several fluorescent imaging probes have been developed for mitochondria-targeted imaging and photodynamic therapy. Conventional fluorescent dyes suffer from aggregation-caused quenching effect, while novel aggregation-induced emission (AIE) probes are ideal candidates for biomedical applications due to their large stokes shift, strong photo-bleaching resistance, and high quantum yield. This review aims to introduce the recent advances in the design and application of mitochondria-targeted AIE probes. The comprehensive review focuses on the structure-property relationship of these imaging probes, expecting to inspire the development of more practical and versatile AIE fluorogens (AIEgens) as tumor imaging and therapy agents for preclinical and clinical use.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1002/asia.202001100DOI Listing
December 2020

The Hantzsch Reaction in Polymer Chemistry: From Synthetic Methods to Applications.

Macromol Rapid Commun 2021 Mar 1;42(6):e2000459. Epub 2020 Oct 1.

The Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.

The Hantzcsh reaction is a robust four-component reaction for the efficient generation of 1,4-dihydropyridine (1,4-DHP) derivatives. Recently, this reaction has been introduced into polymer chemistry in order to develop polymers having 1,4-DHP structures in the main and/or side chains. The 1,4-DHP groups confer new properties/functions to the polymers. This mini-review summarizes the recent studies on the development of new functional polymers by using the Hantzsch reaction. Several synthetic approaches, including polycondensation, post-polymerization modification (PPM), monomer to polymer strategy, and one-pot strategy are introduced; different applications (protein conjugation, formaldehyde detection, drug carrier, and anti-bacterial adhesion) of the resulting polymers are emphasized. Meanwhile, the future development of the Hantzsch reaction in exploring new functional polymers is also discussed.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1002/marc.202000459DOI Listing
March 2021

Antioxidant Polymers via the Kabachnik-Fields Reaction to Control Cellular Oxidative Stress.

Macromol Biosci 2020 12 28;20(12):e1900419. Epub 2020 Sep 28.

Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.

Small molecular antioxidants are almost ineffective in regulating harmful oxidative stress in vivo because of their poor bioavailability. Polymer antioxidants are a promising alternative to address this issue, but their laborious synthetic routes limit their development. In this study, aliphatic and aromatic aldehydes are used to synthesize a family of polymers containing different α-aminophosphonate pendant groups via a facile one-pot method that combines the Kabachnik-Fields (KF) reaction and free radical polymerization. The structure-property relationship study of these polymers reveals the KF moieties in polymer structures confer radical scavenging ability on polymers. The radical scavenging ability and cytotoxicity of these polymers are evaluated in a stepwise manner to identify a biocompatible polymer antioxidant that can effectively protect the cells from H O -induced oxidative damage. This is the first attempt to develop antioxidative polymers by the KF reaction. It highlights the feasibility of synthesizing new functional polymers using multicomponent reactions, which has important implications for organic and polymer chemistry.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1002/mabi.201900419DOI Listing
December 2020

A magnetic solder for assembling bulk covalent adaptable network blocks.

Chem Sci 2020 Aug 2;11(29):7694-7700. Epub 2020 Jun 2.

The Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology (Ministry of Education) , Department of Chemistry , Tsinghua University , Beijing 100084 , China . Email: ; Email:

Covalent adaptable networks (CANs) represent a novel covalently cross-linked polymer that is capable of being reprocessed and recycled relying on reversible covalent bond structures and present exceptional opportunities in a wide range of prospective applications. However, it is genuinely difficult to fabricate bulk CAN blocks with solid-core geometries that possess complex shapes or multiple materials, which are crucial in cutting-edge fields such as soft robotics, flexible electronic devices and biomedical engineering. Here we report a welding technique to strategically construct complex and heterogeneous 3D CAN structures by utilizing a solder doped with magnetic nanoparticles. The solder is able to induce a bond exchange reaction at the interface between the to-be-welded pieces. Using this method, not only CAN bulks with the same materials can be welded to form complex geometries, distinctive bulks with different physical properties and chemical compositions can also be connected to fabricate multimaterial devices. Besides, this method can be used to repair damaged CAN materials and efficiently recycle scrap CAN materials, which can effectively save resources and protect the environment. The universality and robustness of this strategy is expected to promote CAN application in broader functional polymer fields.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1039/d0sc01678kDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7473190PMC
August 2020

Cryogenic 3D printing of dual-delivery scaffolds for improved bone regeneration with enhanced vascularization.

Bioact Mater 2021 Jan 12;6(1):137-145. Epub 2020 Aug 12.

Department of Chemistry, Tsinghua University, Beijing, PR China.

Three-dimensional (3D) printing has been increasingly employed to produce advanced bone tissue engineering scaffolds with biomimetic structures and matched mechanical strengths, in order to induce improved bone regeneration in defects with a critical size. Given that the successful bone regeneration requires both excellent osteogenesis and vascularization, endowing scaffolds with both strong bone forming ability and favorable angiogenic potential would be highly desirable to induce improved bone regeneration with required vascularization. In this investigation, customized bone tissue engineering scaffolds with balanced osteoconductivity/osteoinductivity were produced via cryogenic 3D printing of β-tricalcium phosphate and osteogenic peptide (OP) containing water/poly(lactic--glycolic acid)/dichloromethane emulsion inks. The fabricated scaffolds had a hierarchically porous structure and were mechanically comparable to human cancellous bone. Angiogenic peptide (AP) containing collagen I hydrogel was then coated on scaffold surface to further provide scaffolds with angiogenic capability. A sequential release with a quick AP release and a slow but sustained OP release was obtained for the scaffolds. Both rat endothelial cells (ECs) and rat bone marrow derived mesenchymal stem cells (MSCs) showed high viability on scaffolds. Improved migration and angiogenesis of ECs were obtained for scaffolds delivered with AP while enhanced osteogenic differentiation was observed in scaffolds containing OP. The results showed that, toward scaffolds containing both AP and OP, the quick release of AP induced obvious angiogenesis , while the sustained OP release significantly improved the new bone formation. This study provides a facile method to produce dual-delivery scaffolds to achieve multiple functions.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.bioactmat.2020.07.007DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7426490PMC
January 2021

Advanced reconfigurable scaffolds fabricated by 4D printing for treating critical-size bone defects of irregular shapes.

Biofabrication 2020 08 18;12(4):045025. Epub 2020 Aug 18.

School of Mechanical Engineering, Dongguan University of Technology, Dongguan, Guangdong, People's Republic of China. Contributed equally. Author to whom any correspondence should be addressed.

While scaffold-based tissue engineering has been widely used to treat bone critical-size defects, challenges such as implantation of scaffolds in defects with irregular shapes and implantation of scaffolds through minimally invasive surgery remain in the tissue engineering field. Customized bioactive bone tissue engineering scaffolds with reconfigurable capability for both easy scaffold implantation and perfect shape fitting in irregularly shaped bone defects are therefore needed. Herein, applying 4D printing, photothermal-responsive shape memory bone tissue engineering scaffolds are constructed by incorporating black phosphorus nanosheets and osteogenic peptide into β-tricalcium phosphate/poly(lactic acid-co-trimethylene carbonate) (TCP/P(DLLA-TMC)) nanocomposite scaffolds. When near-infrared irradiation is applied to customized scaffolds on-demand, scaffold temperature rapidly increases to 45 °C, enabling scaffold shape reconfiguration for easy scaffold implantation and precise fitting in irregular bone defects. Once the implantation is finished, scaffold temperature rapidly decreases to 37 °C and scaffolds display mechanical properties comparable to those of human cancellous bone. The improved osteogenesis in bone defect sites is then initiated through pulsed peptide release from scaffolds. Compact integration of reconfigurable scaffolds in rat cranial bone defects and improved new bone formation are demonstrated through micro-computed tomography and histochemical analyses. This study shows a facile method to clinically treat bone defects of irregular shapes.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1088/1758-5090/abab5bDOI Listing
August 2020

A bifunctional β-MnO mesh for expeditious and ambient degradation of dyes in activation of peroxymonosulfate (PMS) and simultaneous oil removal from water.

J Colloid Interface Sci 2020 Nov 26;579:412-424. Epub 2020 Jun 26.

Department of Chemistry, Tsinghua University, Beijing 100084, PR China. Electronic address:

Dual functional membranes that can simultaneously remove water-insoluble oil and degrade water-soluble dyes have received considerable attention. Nevertheless, there remain arduous challenges due to the critical restriction of slow degradation rate and the heavy dependence on external stimuli like light, electricity or heat. Herein, we report a superwetting and rapidly catalytic β-MnO mesh prepared by one-step hydrothermal method. In activation of peroxymonosulfate (PMS), this β-MnO mesh can expeditiously degrade dyes without any external stimuli and simultaneously remove oils. The removal efficiencies were all > 99% and the filtrates were proved eco-friendly through leaching test and toxic experiment. Furthermore, a mechanism on the excellent catalytic ability of β-MnO mesh was proposed, i.e. H was immobilized in 1 × 1 tunnel of β-MnO, which made the mesh surface a positive zeta potential and attract more negative sulfate radicals, as a result inducing an improved degradation efficiency. Therefore, we anticipate this bifunctional and ingenious β-MnO mesh can contribute a lot to prompt and mild sewage purifications.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1016/j.jcis.2020.06.073DOI Listing
November 2020

Volatile-Organic-Compound-Intercepting Solar Distillation Enabled by a Photothermal/Photocatalytic Nanofibrous Membrane with Dual-Scale Pores.

Environ Sci Technol 2020 07 8;54(14):9025-9033. Epub 2020 Jul 8.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

Solar distillation is emerging as a robust and energy-effective tool for water purification and freshwater production. However, many water sources contain harmful volatile organic compounds (VOCs), which can evaporate through the photothermal evaporators and be collected together with distilled water, or even be enriched in the distilled water. In view of the penetration of volatile organic compounds, herein, we rationally demonstrate a dual-scale porous, photothermal/photocatalytic, flexible membrane for intercepting volatile organic compounds during solar distillation, which is based on a mesoporous oxygen-vacancy-rich TiO nanofibrous membrane (m-TiO NFM). The dual-scale porous structure was constructed by micrometer-sized interconnected tortuous pores formed by the accumulation of m-TiO nanofibers and nanometer-sized pores in the m-TiO individual nanofibers. Consequently, the membrane can sustainably in situ intercept VOCs by providing more photocatalytic reactive sites for collision (mainly by mesopores) and longer tortuous channels for prolonging VOC retention (mainly by micrometer-sized pores); thus, it results in less than 5% of phenol residual in distilled water. As a proof of concept, when the m-TiO NFM is employed to purify practical river water in an evaporation prototype under real solar irradiation, complex volatile natural organic contaminants can be effectively intercepted and the produced distilled water meets the drinking water standards of China. This development will promote the application prospects of solar distillation.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1021/acs.est.9b07903DOI Listing
July 2020

Robust Multiscale-Oriented Thermoresponsive Fibrous Hydrogels with Rapid Self-Recovery and Ultrafast Response Underwater.

ACS Appl Mater Interfaces 2020 Jul 10;12(29):33152-33162. Epub 2020 Jul 10.

Department of Chemistry, Tsinghua University, Beijing 100084, China.

Hydrogels with ultrafast response to environmental stimuli, possessing robust structural integrity and rapid self-recovery, have been considered as promising platforms for numerous applications, for example, in biomimetic materials and nanomedicine. Inspired by the bundled fibrous structure of actin, we developed a robust and ultrafast thermoresponsive fibrous hydrogel (TFH) by fully utilizing the weak noncovalent bonds and strong covalently cross-linked semiflexible electrospun fibrous nets. The TFH exhibits an ultrafast response (within 10 s), rapid self-recovery rate (74% within 10 s), tunable tensile strength (3-380 kPa), and high toughness (∼1560 J/m) toward temperature. A multiscale orientation is considered to play a key role in the excellent mechanical properties at the fibrous mesh, fiber, and molecular scales. Furthermore, to take advantage of this TFH adequately, a novel kind of noodle-like hydrogel for thermo-controlled protein sorption based on the TFH is prepared, which exhibits high stability and ultrafast sorption properties. The bioinspired platforms hold promise as artificial skins and "smart" sorption membrane carriers, which provide a unique bioactive environment for tissue engineering and nanomedicine.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1021/acsami.0c06164DOI Listing
July 2020

Preparation recombination human-like collagen/fibroin scaffold and promoting the cell compatibility with osteoblasts.

J Biomed Mater Res A 2021 03 6;109(3):346-353. Epub 2020 Jul 6.

School of Materials Science and Engineering, Tsinghua University, Beijing, China.

On this basis, a novel recombinant human-like collagen (RHLC)/silk fibroin scaffold material with high porosity and controllable aperture was prepared. The compatibility of osteoblasts (OB) with the blends was tested in vitro. The morphology, adhesion and growth of scaffold cells were observed by scanning electron microscope and laser confocal microscope. Extensive measurements, including 3-[4, 5-dimethylthiazole-2-acyl]-2, 5-diphenyl tetrabrominate assays, intracellular total protein content, and alkaline phosphatase activity assays were performed after 7 days of culture. Survival and protein content increased in RHLC/fibroin stents. LSCM and SEM results confirmed that the cells grew better in the mixed scaffolds than in the pure silk scaffolds, and showed that the cells were easy to adhere and diffuse in the RHLC/silk scaffolds. RHLC/silk fibroin scaffolds are promising biomaterials for bone tissue engineering.
View Article and Find Full Text PDF

Download full-text PDF

Source
http://dx.doi.org/10.1002/jbm.a.37027DOI Listing
March 2021
-->