ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Haifeng Lu,Qi Lu,Hongwu Sun,Zhongkun Wang,Xiang Shi,Yuling Ding,Xiang Ran,Jing Pei,Yubo Pan,Qunlin Zhang
Intracellular reactive oxygen species (ROS) are closely associated with cancer cell types. Therefore, ROS-based pattern recognition is a promising strategy for precise diagnosis of cancer, but such a possibility has never been reported yet. Herein, we proposed an ROS-responsive fluorescent sensor array based on pH-controlled histidine-templated gold nanoclusters (AuNCs@His) to distinguish cancer cell types and their proliferation states. In this strategy, three types of AuNCs@His with diverse fluorescence profiles were first synthesized by only adjusting the pH value. Upon the addition of various ROS, fluorescence quenching of three types of AuNCs@His occurred with different degrees, thereby forming unique optical “fingerprints”, which were well-clustered into several separated groups without overlap by principal component analysis (PCA). The sensing mechanism was attributable to the oxidation of AuNCs@His by ROS, as revealed by X-ray photoemission spectroscopy, Fourier transform infrared spectroscopy, 1H nuclear magnetic resonance spectroscopy, and electrospray ionization mass spectrometry. Based on the ROS-responsive sensing pattern, cancer cell types were successfully differentiated via PCA with 100% accuracy. Additionally, the proposed sensor array exhibited excellent performance in distinguishing the proliferation states of cancer cells, which was supported by the results of the Ki-67 immunohistochemistry assay. Overall, the ROS-responsive fluorescent sensor array can serve as a promising tool for precise diagnosis of cancer, indicating great potential for clinical application.
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Biomaterials Science
·
2023
·
IF 6.6
Muse Ji,Hongbing Liu,Hanxun Wang,Xinxin Liang,Mingli Wei,Dongmei Shi,Jingxin Gou,Tian Yin,Haibing He,Xing Tang,Yu Zhang
Chemodynamic therapy (CDT) is an emerging oncological treatment that can kill tumor cells by generating lethal hydroxyl radical (•OH) via Fenton or Fenton-like reaction inside tumors. However, the overexpression of glutathione (GSH) and low reaction efficiency in the tumor microenvironment (TME) limited the therapeutic efficacy of CDTs. Herein, CDT agents (Cu2+) and chemotherapeutic agent (Axitinib, AXB) were employed to fabricate a novel pH-activatable metal ion-drug coordinated nanoparticles (Cu-AXB NPs) for enhancing the treatment of tumors. The obtained nanoparticles exhibited ultrahigh drug loading capacity of 87.55% and had an average size of 180 nm. Moreover, the characteristics of excellent plasma stability and pH-responsive drug release contribute to the long circulation in the blood and targeted therapy at the weakly acidic tumor site. The released AXB could play a chemotherapeutic role in killing tumor cells and Cu2+ ion could be reduced to Cu+ by GSH, further generating toxic •OH with hydrogen peroxide (H2O2) for CDT through Fenton-like reaction. Cu-AXB NPs could also efficiently break copper metabolic balances and increase the intracellular Cu content, thus amplifying CDT. In vitro research results of cytotoxicity and apoptosis confirmed the optimal tumor cell killing efficacy of the Cu-AXB NPs, which was attributed to the synergistic effect of CDT with chemotherapy. What is more, Cu-AXB NPs exhibited good tumor targeting and potent tumor inhibition effect (77.53% inhibition), while exhibiting good biocompatibility in tumor bearing mice. In conclusion, this work provided a promising strategy for safe and efficient cancer therapy through the combination of CDT with chemotherapy.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
·
IF 4.4
Simin Lin,Chunmei Lai,Zejie Huang,Wei Liu,Lei Xiong,Yuxin Wu,Yanqiao Jin
Synthesis of lignin-based carbon dots (LCDs) with high quantum yield (QY), stable fluorescence properties and biocompatibility has been a challenge. Here, we propose an improved two-step strategy for producing high-quality LCDs from enzymatic hydrolysis lignin (EHL). The p-aminobenzenesulfonic acid used in the strategy not only provides nitrogen and sulfur elements, but also tailors the disordered three-dimensional structure of EHL. The successful co-doping of N and S elements favors the reduction of the optical energy bandgap (E g ), resulting in a high QY of 45.05% for LCDs. The LCDs exhibited superior selectivity and sensitivity for Fe 3+ with a limit of detection (LOD) of 0.15 μM when Fe 3+ concentration was 50–500 μM. In addition, LCDs demonstrated significant fluorescence in HepG2 cells and HepG2 cells loaded with LCDs at a concentration of 80 μg/mL showed good viability, suggesting that they are suitable for in vivo applications. The luminescent centers of LCDs change during pH regulation and thus show a special visual response to pH changes, making them have great potential for detecting metabolism in living cells. This work provides a novel and low-cost method for fabricating sustainable fluorescent probes for chemical sensing and bioimaging.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2023
·Vol. 39
·期 4
·647-653
·
IF 3.1
Li Miao,Hao Yashi,Yang Zuobo,Yun Jimmy,Liang Xin
Ruthenium(Ru) and its derivatives have been widely studied as oxygen evolution reaction(OER) electrocatalysts in acidic water electrolysis due to their inherent electronic properties and high oxygen evolution activity. A facile pH-induced size regulation approach for Ru nanocrystals has been developed by introducing NaOH and CH 3 COOH in a polyol system. The size of Ru particles decreases with the increase of the dosage of NaOH and increases at a certain dosage of CH 3 COOH. The formation mechanism of ruthenium nanocrystals was investigated through a series of characterizations and kinetic experiments. The electrocatalytic activities of the electrocatalysts derived from these Ru particles were studied toward OER to investigate the influence of particle size on their electrocatalytic properties. Moreover, the prepared electrocatalysts were applied as anodic materials in the proton exchange membrane(PEM) electrolysis cell and demonstrated excellent performance.
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ACS Nano
·
2023
·
IF 17.1
Chaojie Ren,Danni Zhong,Yuchen Qi,Chaoyi Liu,Xingyu Liu,Shihong Chen,Sheng Yan,Min Zhou
The oral form of insulin is more convenient and has better patient compliance than subcutaneous or intravenous insulin. Current oral insulin preparations, however, cannot overcome the enzyme barrier, chemical barrier, and epithelial barrier of the gastrointestinal tract completely. In this study, a microalgae-based oral insulin delivery strategy (CV@INS@ALG) was developed using Chlorella vulgaris (CV)-based insulin delivery system cross-linking with sodium alginate (ALG). CV@INS@ALG could overcome the gastrointestinal barrier, protect insulin from harsh gastric conditions, and achieve a pH-responsive drug release in the intestine. CV@INS@ALG might contribute to two mechanisms of insulin absorption, including direct insulin release from the delivery system and endocytosis by M cells and macrophages. In the streptozotocin (STZ)-induced type 1 diabetic mouse model, CV@INS@ALG showed a more effective and long-lasting hypoglycemic effect than direct insulin injection and did not cause any damage to the intestinal tract. Additionally, the long-term oral administration of the carrier CV@ALG effectively ameliorated gut microbiota disorder, and significantly increased the abundance of probiotic Akkermansia in db/db type 2 diabetic mice, thereby enhancing the insulin sensitivity of mice. Microalgal insulin delivery systems could be degraded and metabolized in the intestinal tract after oral administration, showing good biodegradability and biosafety. This insulin delivery strategy based on microalgal biomaterials provides a natural, efficient, and multifunctional solution for oral insulin delivery.
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FOOD HYDROCOLLOIDS
·
2023
·
IF 10.7
Hanyu Li,Minghui Zhao,Sijie Zhou,Huajiang Zhang,Jing Wang,Ning Xia,Yujia Liu,Shihui Hua,Guixin Tan
Curcumin is a hydrophobic polyphenol with various health benefits, but its poor water solubility and stability limit its application in the food and pharmaceutical industries. In this study, a pH-driven method was developed to prepare ovalbumin (OVA)-curcumin nanocomplexes without organic solvents, reducing the environmental impact. The results showed that curcumin was encapsulated in OVA with a high efficiency of over 95% and remained in an amorphous state within the protein molecules. Molecular docking and spectroscopic analyses revealed that curcumin was mainly bound and stabilized by hydrogen bonds and hydrophobic interactions in the hydrophobic core of OVA. The binding strength of the intermediate stage of the pH-driven method was stronger than that of the final stage, due to the exposure of OVA molecular binding sites and the involvement of electrostatic attraction. Furthermore, the potential of polysaccharide blending to enhance the stability of the nanocomplexes was investigated. The results showed that sodium alginate effectively enhanced the photostability and thermal stability of the OVA-curcumin nanocomplexes by co-solubilization and electrostatic complex formation. In addition, simulated in vitro digestion also demonstrated that the pH-driven method combined with polysaccharide blending increased the bioaccessibility of curcumin in nanocomplexes from 17.79% to 52.54%. Therefore, the pH-driven method coupled with polysaccharide blending ensures the encapsulation and stabilization of hydrophobic bioactive substances for use in their delivery systems to improve bioaccessibility.
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TALANTA
·
2023
·
IF 6.1
Xiaohui Wen,Chenghui Li,Zexi Zhou,Yujing He,Juan He,Xiandeng Hou
With the increasing demand for on-site detection, the current approach of building dual-emission or multi-emission luminescence sensors based on metal-organic frameworks (MOFs) which possess the capacity of self-reference for numerous non-analyte factors falls short of meeting sensing requirements. Therefore, we have designed a novel strategy for constructing wavelength shift-based luminescence sensor named Eu/Gd(TCPP), which exhibits dual-emitting from metal ions Eu 3+ and flexible rotating aggregation-induced emission (AIE) ligands H 4 TCPP (2,3,5,6-tetrakis(4-carboxyphenyl)pyrazine). This sensor was prepared by a simple, green and fast plasma synthesis method. It's worth noting that the fluorescence emission of Eu/Gd(TCPP) shows a specific wavelength shift from ligand peak, and a visual color change from red to blue within a pH range of 4 to 3. Moreover, various characterization data verified that the luminescence switching mechanism of Eu/Gd(TCPP) was attributed to the H + -induced collapse of the Eu/Gd(TCPP) crystal structure, followed by untwisting of free ligands that lose rigid MOFs confinement. This hindered the antenna effect from H 4 TCPP to Ln 3+ ions and restricted the rotation emission of ligand, resulting in the red-shifting of the ligand emission and corresponding luminescence switching. By tactfully utilizing the short-range pH response property of Eu/Gd(TCPP), highly sensitive and selective on-site visual detection of acidic aspartic acid can be achieved.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Chen Jiadong,Chen Chunhong,Qin Minkai,Li Ben,Lin Binbin,Mao Qing,Yang Hongbin,Liu Bin,Wang Yong
Noble metal electrocatalysts (e.g., Pt, Ru, etc.) suffer from sluggish kinetics of water dissociation for the electrochemical reduction of water to molecular hydrogen in alkaline and neutral pH environments. Herein, we found that an integration of Ru nanoparticles (NPs) on oxygen-deficient WO 3-x manifested a 24.0-fold increase in hydrogen evolution reaction (HER) activity compared with commercial Ru/C electrocatalyst in neutral electrolyte. Oxygen-deficient WO 3-x is shown to possess large capacity for storing protons, which could be transferred to the Ru NPs under cathodic potential. This significantly increases the hydrogen coverage on the surface of Ru NPs in HER and thus changes the rate-determining step of HER on Ru from water dissociation to hydrogen recombination.
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WATER RESEARCH
·
2022
·
IF 13.4
Jun Liang,Kexin Chen,Xiaoguang Duan,Ling Zhao,Hao Qiu,Xiaoyun Xu,Xinde Cao
The impacts of pH on purification efficiency can be phenomenal in advanced oxidation processes (AOPs), because solution pH affects persulfate (PS) activation processes. However, consensus has not been reached on the regimes of pH-regulated oxidation in persulfate-based AOPs (PS-AOPs). Particularly, the impacts of pH on carbon-catalyzed generation of radical and nonradical species remain unclear. In this work, we evaluated three typical carbonaceous materials including pyrolytic carbon (PC), activated carbon (AC), and carbon nanotube (CNT) to activate PS for sulfamethoxazole (SMX) degradation within a pH range from 4 to 9. The experiment revealed pH-dependent SMX removal in PC/PS, AC/PS, and CNT/PS, and the kinetics followed an order of pH 4 > pH 7 > pH 9. Solution pH simultaneously affected SMX adsorption and degradation, but the latter was more profound. Chemical quenching experiment, electrochemical measurement, kinetics calculation, and ATR-FTIR tests collectively revealed that high pH was not favorable for both radical and nonradical oxidation. In the PC/PS system, increased pH decreased the amount of phenolic –OH on PC surface, thereby restraining the generation of SO 4 •− and • OH due to the lack of electron donors. For AC/PS system, elevated pH hindered the interactions between AC and PS, thus suppressing the formation of surface-bound radicals. CNT/PS initiated an electron-transfer pathway, and increased pH reduced the oxidation potential of surface CNT-PS* complex, which was not favorable for nonradical oxidation of adsorbed pollutants. Therefore, outcomes of this work will advance the current knowledge on the intrinsic impacts of pH in PS-AOPs catalyzed by carbonaceous materials for wastewater purification.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Wanfeng Wu,Yanan Qin,Yan Fang,Yukun Zhang,Shuxuan Shao,Fanxing Meng,Minwei Zhang
Currently, graphene quantum dots (GQDs) are widely used as antibacterial agents, and their effects are dependent on the reactive oxygen species (ROS) generated by photodynamic and peroxidase activities. Nevertheless, the supply of substrates or light greatly limits GQDs application. Besides, due to compensatory mechanisms in bacteria, comprehensive analysis of the molecular mechanism underlying the effects of GQDs based on cellular-level experiments is insufficient. Therefore, N-GQDs with inherent excellent, broad-spectrum antibacterial efficacy under acidic conditions were successfully synthesized. Then, via multi-omics analyses, the antibacterial mechanisms of the N-GQDs were found to not only involve generation ROS but also be associated with changes in osmotic pressure , interference with nucleic acid synthesis and inhibition of energy metabolism. More surprisingly, the N-GQDs could destroy intracellular acid-base homeostasis , causing bacterial cell death. In conclusion, this study provides important insights into the antibacterial mechanism of GQDs, offering a basis for the engineering design of antibacterial nanomaterials .
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2022
·
IF 5.999
Xiaowei Yang,Zhihui Kuang,Xinmin Yang,Xin Hu,Peng Luo,Qi Lai,Bin Zhang,Xiaoyong Zhang,Yen Wei
Osteoporosis is an age-related metabolic disease of bone, resulting in bone pain and even bone fragility and brittle fracture . Inhibiting overactive osteoclasts while promoting osteoblast activity is an ideal way to treat osteoporosis. Previous studies have demonstrated that natural compounds , such as curcumin (Cur) have dual roles both in promoting bone formation and inhibiting bone resorption , making them promising candidates for osteoporosis treatment . However, their poor water solubility, high dosage of curative effect and significant toxicity to other organs have largely limited their clinical translations. In this study, a novel method was reported to conjugate Cur and poly(amidoamine) dendrimers (PAD) using hexachlorocyclotriphosphazene (HCCP) as the linkage through a one-pot reaction, forming stable and uniform Cur loaded nanospheres (HCCP-Cur-PAD, HCP NPs). Owing to the hydrophilicity of PAD and hydrophobicity of Cur, HCP NPs can self-assemble into nanoparticles with particle size of 138.8 ± 78.7 nm and display excellent water dispersity . The loading capacity of Cur can reach 27.2% and it can be released from HCP NPs with pH-responsiveness. In vitro experimental results demonstrated that the HCP NPs entered lysosomes by endocytosis and proved dual anti-osteoporosis effects of inhibiting osteoclasts and promoting osteoblasts.
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ChemistrySelect
·
2022
·Vol. 7
·期 37
·e202202462
·
IF 2.307
Minmin Wang,Li Zhou,Mengke Zhang,Wenwu Song,Weiting Zhong,Xunyue Wang,Yanfeng Tang
Graphical A facile one-step phosphorization method to fabricate a 1D Ni 12 P 5 nanoneedle array was reported. The obtained Ni 12 P 5 requires overpotentials of 59, 117, and 148 mV to reach the current density of 10, 50 and 100 mA cm −2 toward HER in 1 mol/L KOH solution, respectively. Excellent electrochemical performances demonstrate that the nickel phosphide could be a candidate for high-performance water electrolysis over a wide pH range. Transition metal phosphides (TMP) with high conductivity and better H* intermediate adsorption energy have attracted great attention in hydrogen evolution process. Herein, a Ni 12 P 5 nanoneedle array was synthesized by a facile one-step phosphorization method. As expected, the obtained Ni 12 P 5 nanoneedle arrays exhibits high HER performance, and low overpotentials of 59, 117, and 148 mV are need to drive hydrogen evolution at current densities of 10, 50, and 100 mA cm −2 in 1 mol/L KOH electrolyte, respectively. Meanwhile, the obtained electrode exhibits excellent hydrogen evolution activity in both acidic and neutral media. Excellent electrochemical performances demonstrate that the nickel phosphide could be a candidate for high-performance water electrolysis over a wide pH range.
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