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1. Recent Advances on Fabrication of Polymeric Composites Based on Multicomponent Reactions for Bioimaging and Environmental Pollutant Removal
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.
Figure 1 The preparation of fluorescent copolymers with AIE feature and adsorptive polymeric composites through different MCRs and their potential applications for biomedical and environmental applications
Paper link：
https://onlinelibrary.wiley.com/doi/abs/10.1002/marc.202000563
2. Multifunctional Organic Fluorescent Probe with Aggregation-Induced Emission Characteristics: Ultrafast Tumor Monitoring, Two-Photon Imaging, and Image-Guide Photodynamic Therapy
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− PEG2000−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(1O2) 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.
Figure 2 Multifunctional Organic Fluorescent Probe with Aggregation-Induced Emission Characteristics
Paper link：
https://pubs.acs.org/doi/abs/10.1021/acsami.0c21309
3. Spatiotemporal Magnetocaloric Microenvironment for Guiding the Fate of Biodegradable Polymer Implants
The degradation behavior of implants is significantly important for bone repair. However, it is still unprocurable to spatiotemporally regulate the degradation of the implants to match bone ingrowth. In this paper, a magneto‐controlled biodegradation model is established to explore the degradation behavior of magnetic scaffolds in a magnetothermal microenvironment generated by an alternating magnetic field (AMF). The results demonstrate that the scaffolds can be heated by magnetic nanoparticles (NPs) under AMF, which dramatically accelerated scaffold degradation. Especially, magnetic NPs modified by oleic acid with a better interface compatibility exhibit a greater heating efficiency to further facilitate the degradation. Furthermore, the molecular dynamics simulations reveal that the enhanced motion correlation between magnetic NPs and polymer matrix can accelerate the energy transfer. As a proof‐of‐concept, the feasibility of magneto‐controlled degradation for implants is demonstrated, and an optimizing strategy for better heating efficiency of nanomaterials is provided, which may have great instructive significance for clinical medicine.
Figure 3 Schematic illustration of magneto-controlled degradation in polymer implants
Paper link：
https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202009661
4.Rational Design of Carbon Layer-Decorated Metal Oxide/Nickel Cobalt Sulfide-Based Composite with Faster Energy Storage and Long Cyclic Life
We have prepared hybrid supercapacitors (HSCs) based on metal oxide/nickel cobalt sulfide composite electrodes decorated with an ultrathin carbon layer (Co3O4@C@CoNi2S4). This ultrathin carbon layer serves as an “expressway” for enhanced electron and ion transport, and the horizontally aligned nanosheet structure prevents the electrodes from structural collapse during electrochemical reaction processes. The obtained Co3O4@C@CoNi2S4 hierarchical composites exhibit a higher gravimetric specific discharge capacity (400.6 mA h·g–1 at 1 A·g–1). More importantly, as a HSC based on Co3O4@C@CoNi2S4//active carbon (AC), a high specific energy of 46.5 W h·kg–1 at a specific power of 1052.8 W h·kg–1 was obtained (95.6% capacitance retention after 10,000 charge/discharge cycles). The result indicates that such Co3O4@C@CoNi2S4 heterostructures may show significant promise for application of electrochemistry in the energy field.
Figure 4 The performance of Carbon Layer-Decorated Metal Oxide/Nickel Cobalt Sulfide-Based Composite
Paper link：
https://pubs.acs.org/doi/abs/10.1021/acsaem.0c02633
5.In vitro and in vivo Study on an Injectable Glycol Chitosan/Dibenzaldehyde-Terminated Polyethylene Glycol Hydrogel in Repairing Articular Cartilage Defects
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 in vivo 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 in vitro. Then, we perform in vivo and in vitro experiments to evaluate the feasibility of this material for cartilage repair in vivo and in vitro.
Figure 5 Test results 8 weeks postoperatively
Paper link：
https://www.frontiersin.org/articles/10.3389/fbioe.2021.607709/full
6.DOPA-derived electroactive copolymer and IGF-1 immobilized poly(lactic-co-glycolic acid)/hydroxyapatite biodegradable microspheres for synergistic bone repair
Owing to defect features (irregular shape and size) and local environments (e.g., pulsation of dura matter and proximity of the brain), the skull is one of the most difficult to repair. Electroactive microsphere systems with good injectability, adjustable size, high surface-to-volume ratio and surface modifiability, exhibit excellent bone regeneration potential. Herein, the electroactive microspheres were prepared by immobilizing aniline tetramer (AT) on poly(lactic-co-glycolic acid)/hydroxyapatite (PLGA/HA) microspheres. Subsequently, the 3,4-hydroxyphenalyalanine-containing recombinant insulin-like growth-factor-1 (DOPA-IGF-1) inspired by bioorthogonal chemistry was designed by combining the recombinant DNA technology and tyrosinase treatment, and modified on electroactive scaffolds surface. The as-prepared microspheres exhibited excellent sphericity and homogeneity with an average diameter of 329.2 ± 16.5 μm. The electroactive microsphere exhibits significant cell proliferation and enhanced osteogenic differentiation, and combining with DOPA-IGF-1 can further synergistically induce mineralization and osteogenic differentiation. Rat calvarial defect repair experiments showed excellent repairability in forming mineralized collagen deposition within the transplanted composite microspheres scaffold in the bone defect site. Thus, biomimetic composite microsphere with electroactivity and bioactivity exhibits considerable potential for calvarial defect repair.
Figure 6 Biodegradable microspheres for synergistic bone repair
Paper link：
https://www.sciencedirect.com/science/article/abs/pii/S1385894721007208
