Nature Communications
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2024
·Vol. 15
·期 1
·1-13
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IF 14.7
Li Yongqiang,Yang Siwei,Bao Wancheng,Tao Quan,Jiang Xiuyun,Li Jipeng,He Peng,Wang Gang,Qi Kai,Dong Hui,Ding Guqiao,Xie Xiaoming
Investigating proton transport at the interface in an excited state facilitates the mechanistic investigation and utilization of nanomaterials. However, there is a lack of suitable tools for in-situ and interfacial analysis. Here we addresses this gap by in-situ observing the proton transport of graphene quantum dots (GQDs) in an excited state through reduction of magnetic resonance relaxation time. Experimental results, utilizing 0.1 mT ultra-low-field nuclear magnetic resonance relaxometry compatible with a light source, reveal the light-induced proton dissociation and acidity of GQDs’ microenvironment in the excited state (Hammett acidity function: –13.40). Theoretical calculations demonstrate significant acidity enhancement in –OH functionalized GQDs with light induction ( \({{\mathrm{p}}}{K}_{{\text{a}}}^{*}\) = –4.62, stronger than that of H 2 SO 4 ). Simulations highlight the contributions of edge and phenolic –OH groups to proton dissociation. The light-induced superacidic microenvironment of GQDs benefits functionalization and improves the catalytic performances of GQDs. Importantly, this work advances the understanding of interfacial properties of light-induced sp 2 – sp 3 carbon nanostructure and provides a valuable tool for exploring catalyst interfaces in photocatalysis.
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Journal of Materials Chemistry C
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2024
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IF 5.7
Tonghui Zhao,Yuqing Zhang,Lifei Wu,Qitong Zhong,Wei Xie,Bo Li,Dongling Geng,Haibo Zeng
In this research, we present an innovative, environmentally friendly, and cost-effective alcohothermal method for synthesizing Mn2+ and Mn2+–Cu+ doped 0D Cs3ZnCl5, a green luminescent material, marking the first time this approach has been reported. An exhaustive analysis of the luminescence properties of both undoped and doped Cs3ZnCl5 was conducted, with a particular emphasis on the energy transfer mechanisms in the Mn2+ mono-doped and Mn2+–Cu+ co-doped systems. The results demonstrate the successful construction of an efficient energy transfer pathway that significantly enhances the luminescence efficiency of Cs3ZnCl5:Mn2+. Specifically, the photoluminescence quantum yield of Mn2+ within the Cs3ZnCl5 matrix has been improved from 51.6% to 71.1%, thanks to the Cu+ codopant acting as an effective energy transfer mediator. A mechanism for the luminescence and energy transfer phenomena observed in the Mn2+–Cu+ co-doped Cs3ZnCl5 system has been also proposed. Furthermore, to assess the practical applicability of the synthesized materials, their structural and photoluminescent stability were evaluated. In essence, our study presents a promising solution to current challenges in the synthesis of advanced luminescent materials and opens up new possibilities for harnessing the potential of Mn2+-activated 0D metal halides in optoelectronic applications.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Linlin Song,Zhihui Liu,Xiujing He,Tianyue Xu,Meixu Chen,Zihan Xu,Haina Zhao,Jiaojiao Suo,Hong Wang,Zhankun Yang,Shenglan You,Xiaoting Chen,Guang Yang,Jing Jing,Yulan Peng,Hubing Shi
Synchronizing therapy and diagnosis is an ideal mode for clinical treatment of localized disease, e.g., tumor. Here, we develop a diagnosis-therapy coupled sonodynamic nano delivery system ZSMT which is constructed with a TiO 2 embedding hollow Mn-MOF. Loaded with perfluorohexane, the ZSMT nanoparticle is not only capable for carrying ozone as a ROS donor but also endowed with double modes of imaging, namely ultrasound and magnetic resonance imaging. The TiO 2 -Mn-MOF can efficiently generate ROS by sonodynamic catalyzing ozone. Moreover, fluorescent tracer indicates the ZSMT particle can be internalized by tumor cells. With the stimulation of ultrasound, ozone carried ZSMT potently inhibits cell proliferation and promotes immunogenic cell death in vitro and in vivo by inducing a mitochondrial related cell death. Remarkably, combination of ultrasound-responsive ozone catalytic nano system and PD-1 blockade systematically suppresses the tumor growth by reprogramming the immune microenvironment. In conclusion, our sonodynamic nano system not only proves the principle of drug administration strategy on “treat-as-you-see” but also provides a combo regimen of improving PD-1 blockade with precision localized antigen boosting.
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Materials Today Energy
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2024
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IF 9
Yaqi Hong,Song Zhang,Hu Shen,Xingyuan Tian,Bin Zhang,Xin Zhou,Rong Liu,Ying Liu,Yicong Gao,Ruirui Cao,Huilin Li,Fumin Li,Zhitao Shen,Chong Chen
Perovskite solar cells (PSCs) have demonstrated extensive prospects for future applications. However, defects remain as the crucial factor that impedes their further advancement in performance, and passivation of the interfaces (such as the buried and/or top interfaces) is regarded as one of the most effective approaches. Herein, we aim to address another important interface, namely, the indium tin oxide/electron transport layer (ITO/ETL) interface in n-i-p structured devices. Since electron transport layers are typically fabricated using commercial nano tin dioxide, which often display insufficient density. To combat this, we employ the most commonly used bathocuproine (BCP) material to treat the ITO/ETL interface. The incorporation of BCP diminishes the direct contact between the perovskite and ITO layers, while also passivating buried interface and adjusting the crystal orientation of perovskites. Furthermore, the substrate layer exhibits improved transparency, consequently elevating the utilization rate of light by perovskite. As a result, the BCP-based PSC exhibits an impressive efficiency greater than 22%, surpassing the control one of 19.91%, and which simultaneously demonstrates excellent stability. Notably, the optimization of this interface has universal applicability in the improvement of PSCs performance.
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Journal of Physical Chemistry C
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2024
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IF 3.3
Qi Liu,Wenrou Yu,Anping Liu,Zhaoxian Chen,Xuliang Xia,Yingzhou Huang,Haiyang Shi
By harnessing the capture of target molecules at the metal surface via a highly confined electromagnetic field induced by surface plasmons, surface-enhanced Raman spectroscopy (SERS) has emerged as a sensitive technique for spectral analysis. However, the precise identification of biomarkers in urine using SERS remains a formidable challenge due to the low concentration of biomarkers and the complex nature of the urine composition. In this investigation, we developed an optoplasmonic film SERS substrate comprising silver nanowires (AgNWs) and silicon dioxide (SiO2) to tackle this issue. The AgNWs produce robust SERS signals, while SiO2 enhances laser focusing, facilitating the efficient detection of levothyroxine sodium (LS) in urine with an ultralow detection limit of 1 × 10–9 M. Leveraging artificial intelligence (AI) algorithms, this optoplasmonic substrate achieved precise LS identification in urine with a remarkable accuracy rate. This pioneering substrate holds substantial promise for the noninvasive, swift detection of target molecules in biofluids, heralding advancements in disease diagnostics and health monitoring.
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Heliyon
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2024
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IF 3.4
Feifei Sun,Yao Xiao,Lili Kong,Haibo Mu,Xing Wang,Jinyou Duan
The consequences caused by bacterial resistance are becoming more and more serious. The rate of antibiotic development is far behind the rate of bacterial resistance, so it is urgent to develop a new drug system. In this study, photoresponsive nanogels based on hyaluronic acid were prepared and loaded with ciprofloxacin as a model molecule. The results showed that the nanogels had the advantages of high stability and good cytocompatibility. The inhibition effect of drug-loaded nanogels after light irradiation on the growth of Staphylococcus aureus and Salmonella typhimurium was significantly better than that before light irradiation, and ciprofloxacin could be released on demand and in control. This strategy is of great significance to reduce the unnecessary use of antibiotics and weaken bacterial resistance.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Kai Han,Jian Liu,Fukang Hao,Jianlong Wang,Jinfeng Yuan,Zhicheng Pan,Mingwang Pan
Waterborne fluorocarbon coatings are gaining popularity as a more environmentally friendly replacement for traditional solvent-based coatings because of its corrosion resistance and antibiofouling properties. However, the environmental unfriendliness of small molecular emulsifiers used, the occurrence of flash rusting, and the inability to self-repair after accidental damage restrict its application in the marine industry. Here, a redox-responsive copolymer (PM x ) was synthesized by the amphiphilic nature of waterborne polyurethane as microreactors, which was employed as coatings (PM x /WPU) with anti-flashing rust, antibiofouling, and self-repairing functions. The copolymer was polymerized from chlorotrifluoroethylene (CTFE), vinyl acetate (VA), and a special monomer conjugated to the corrosion inhibitor 2-benzothiazolethiol (MBT) through disulfide bonds, in which MBT can be released through disulfide bond breaking in a reducing environment, effectively preventing the occurrence of flash rusting. The combination of the repelling properties of the fluorinated groups and the bactericidal action of the MBT results in PM x /WPU coatings with excellent antibiofouling properties. Additionally, the reversible hydrogen bonds in the polyurethane provide the PM x /WPU coatings with excellent self-repairing ability (93.9%). Our study presents a new approach to polymerize fluoro-substituted ethylene monomers using polyurethane as microreactors, enabling the preparation of waterborne fluorocarbon coatings with anti-flashing rust, antibiofouling, and self-repairing properties for practical applications.
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Acta Pharmaceutica Sinica B
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2024
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IF 14.7
Yongkang Lai,Tinglin Zhang,Xiaojing Yin,Chunping Zhu,Yiqi Du,Zhaoshen Li,Jie Gao
Helicobacter pylori ( H. pylori) infection remains the leading cause of gastric adenocarcinoma, and its eradication primarily relies on the prolonged and intensive use of two antibiotics. However, antibiotic resistance has become a compelling health issue, leading to H. pylori eradication treatment failure worldwide. Additionally, the powerlessness of antibiotics against biofilms, as well as intracellular H. pylori and the long-term damage of antibiotics to the intestinal microbiota, have also created an urgent demand for antibiotic-free approaches. Herein, we describe an antibiotic-free, multifunctional copper-organic framework (HKUST-1) platform encased in a lipid layer comprising phosphatidic acid (PA), rhamnolipid (RHL), and cholesterol (CHOL), enveloped in chitosan (CS), and loaded in an ascorbyl palmitate (AP) hydrogel: AP@CS@Lip@HKUST-1. This platform targets inflammatory sites where H. pylori aggregates through electrostatic attraction. Then, hydrolysis by matrix metalloproteinases (MMPs) releases CS-encased nanoparticles, disrupting bacterial urease activity and membrane integrity. Additionally, RHL disperses biofilms, while PA promotes lysosomal acidification and activates host autophagy, enabling clearance of intracellular H. pylori . Furthermore, AP@CS@Lip@HKUST-1 alleviates inflammation and enhances mucosal repair through delayed Cu 2+ release while preserving the intestinal microbiota. Collectively, this platform presents an advanced therapeutic strategy for eradicating persistent H. pylori infection without inducing drug resistance.
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JOURNAL OF MEDICINAL CHEMISTRY
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2024
·
IF 6.8
Chao Zhao,Wanlu Sun,Yanyan Zhu,Xiaoyan Huang,Ye Sun,Hai-Yan Wang,Yi Pan,Yi Liu
Photodynamic therapy (PDT) is an innovative and promising method for treating tumors that has attracted significant interest but still faces several challenges, such as a lack of selectivity, deep penetration of light, and efficient ROS generation. To address these challenges, we optimized and synthesized a series of photosensitizers and successfully developed a heavy-atom-free near-infrared FUCL photosensitizer NFh-NMe-2. This photosensitizer can generate singlet oxygen (1O2) and induce cellular apoptosis under 808 nm light. For the safe ablation of microtumors in vivo, an activatable FUCL photosensitizer NFh-NTR was developed based on the overexpression of nitroreductase (NTR). NFh-NTR could be activated by NTR, leading to the release of the photosensitizer NFh-NMe-2, restoring the fluorescence signal, and effectively killing tumor cells under 808 nm light irradiation. This work opens new possibilities in the chemical design of an FUCL photosensitizer for cancer treatment.
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BIOTECHNOLOGY AND BIOENGINEERING
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2024
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IF 3.5
Chunyu Han,Zhenxu Wu,Yuqi Gao,Shuang Yang,Yu Wang,Min Guo,Yueyue Li,Wanzhong Yin,Ling Liu,Wenzhi Song,Peibiao Zhang,Liqiang Wang
The repair process of bone tissue includes the early inflammatory response period and the late tissue repair period. It has been widely approved to be beneficial to the repair of bone injury by procedurally inhibiting the inflammatory response in the early stage and promoting bone regeneration in the late stage. In this study, the nano-hydroxyapatite/Poly(glycolide-co-caprolactone) (n-HA/PGCL) scaffold loaded with icariin was fabricated by fused deposition modeling technique, and the quercetin-loaded GelMA was further filled into the scaffold pores via light-curing methods to form a biphasic scaffold loaded with dual molecules (PHI + GQ scaffold). The releases of icariin and quercetin were sequential due to different degradation rates of GelMA and PGCL. In vitro, the scaffold not only scavenged reactive oxygen species production, but also promoted osteogenic differentiation of the MC-3T3-E1 cells. Furthermore, in vivo bone reconstruction of PHI + GQ scaffold was better than other groups by assessment of micro-CT data. In addition, the immunofluorescence staining of Arg-1 and iNOS indicated that PHI + GQ scaffold created an immune microenvironment conducive to bone repair due to the release of quercetin in the early stage, and HE and Masson staining suggested that PHI + GQ scaffold induced more new bone formation. These results demonstrated that the biphasic scaffold loaded with icariin and quercetin had both antioxidants in the early stage and osteogenesis properties in the late stage, obtaining satisfactory bone repair outcomes. Thus, the biphasic scaffold loaded with icariin and quercetin for sequential release could provide a promising solution for the restoration of bone defects and represent a potential strategy for bone regeneration.
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GREEN CHEMISTRY
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2024
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IF 9.3
Yunjian Wu,Yiran Hu,Hui Lin,Xiaoxing Zhang
Anhydride-cured epoxy is a common insulating material used in electrical equipment, but recycling it effectively is difficult, which results in the overall abandonment of the equipment after decommissioning and serious environmental pollution. In order to make anhydride cured epoxy degradable while maintaining its electrical performance, we synthesized a high-performance epoxy insulating material that can be recycled and reused using triethanolamine as a transesterification catalyst co-accelerator. Results show that the new epoxy has the lowest dielectric loss of 0.0012, the highest breakdown strength of 42.26 kV mm−1, and the highest tensile strength of 93.7 MPa. The degradable epoxy can be recovered via mechanical hot pressing and regenerated through chemical degradation. Degradation products can be directly used as curing accelerators to complete the re-preparation of the insulating material. Even after recovery, the properties of the epoxy resin meet the application requirements of insulating materials.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Lei Li,Haoze Li,Junrong Wang,Yulin Xie,Minghong Gao,Zhongjun Yang,Chunxia Li
Damaged skin compromises its ability to effectively prevent the invasion of harmful bacteria into the tissue, leading to bacterial infection of the wound and hindering the healing process. To address this challenge, we have developed a multifunctional asymmetric wound dressing (CuPt-Cur-ABC) that effectively addresses the lack of bactericidal activity and the release of active ingredients in conventional bacterial cellulose (BC), which can be employed to create a barrier of defense between the wound and its surrounding environment. Compared with BC, asymmetric bacterial cellulose (ABC) used starch as a pore-causing agent, forming holes of different sizes at the top and bottom, which enhanced the ability of ABC to load and moderate-release drugs. First, as-synthesized CuPt nanozymes with an octopod nanoframe structure had multiple enzymatic activities including peroxidase-like, catalase-like, and glutathione peroxidase-like activities. Then, CuPt and curcumin (Cur) were loaded into ABC under ultrasound. Under 808 nm laser irradiation, the nanocomposites possessed good photothermal properties. So the photothermal therapy combined with chemodynamic therapy and inherent antibacterial performance of Cur achieved 99.3% and 99.6% in vitro bactericidal efficacy against Staphylococcus aureus and Escherichia coli, respectively. Moderate release of Cur can clear the excess reactive oxygen species and promote the polarization of macrophages toward the M2 type. In vivo experiments additionally confirmed that the constructed wound dressing achieved multiple functions, including effective antibacterial activity, reversing the inflammatory microenvironment, and promoting wound healing.
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