CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Zining Hao,Yuchu He,Jing Wang,Xuwu Zhang,Fei Ye,Ze Guan,Xiaokang Liu,Zhenhe Ma,Yi Yuan,Hongming Lou,Dawei Gao
Tumor interstitial solid phase-induced physical obstacles and fluid phase-induced hydrostatic pressure are regarded as the two main intractable barriers of drug delivery, leading to the survive of deep-seated tumor stem cells. Herein, a rational strategy is presented based on near-infrared light-stimuli enzymolysis and photocatalysis to decompose the tumor interstitial solid and fluid phases for boosting the tumor penetration of nanomedicine. In detail, a cuprous oxide/sliver nano-photocatalyst (Cu 2 O/Ag) is designed, which is covered with the thermosensitive papain-loaded tumor-homing homologous cytomembrane to form the nanomedicine (Cu 2 O/ [email protected] ). With the light irradiation, the heat generated by Cu 2 O/Ag promote the enzymolysis of extracellular matrix by papain, which eliminate the physical obstacles. Moreover, the photocatalytic water splitting of Cu 2 O/Ag reduce the volume of tumor interstitial fluid, which decrease the elevated hydrostatic pressure to boost the tumor penetration of nanomedicine. Additionally, during the intratumoral delivery, Cu 2 O/ [email protected] is able to realize anti-tumor photothermal therapy and chemotherapy. The results indicate that the Cu 2 O/ [email protected] decompose a majority of tumor extracellular matrix and interstitial fluid under light irradiation. The tumor interstitial hydrostatic pressure is reduced by 69.7%. The tumor penetration of Cu 2 O/ [email protected] + L treated group is 5.03-fold than the Cu 2 O/ [email protected] −L group, leading to the 95.19% of tumor inhibition rate.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 48
·72764-72776
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IF 5.19
Zhong Dan,Feng Weinan,Ma Wencheng,Liu Xinyue,Ma Jun,Zhou Ziyi,Du Xuan,He Fu
Goethite and lepidocrocite, as the main compositions of pipe deposits in the water distribution network, could be used as a catalyst for advanced oxidation processes (AOPs). This research utilizes them to activate PDS/H 2 O 2 and PMS/H 2 O 2 degrading the 2,4,6-trichlorophenol, respectively. To describe the incomplete degradation of pollutants and reflect the induction period, a modified first-order model has been proposed and used to analyze degradation differences under several key affecting factors. The results revealed that the PDS/H 2 O 2 system has a synergy effect in the 2,4,6-trichlorophenol degradation process. The possible degradation pathways and intermediate products were confirmed by gas chromatograph-mass spectrometry (GC–MS). The paper provides a new idea for the effective use of pipe deposits to remove chlorophenols from drinking water, which is of great significance to ensure water quality safety.
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Biochar
·
2022
·Vol. 4
·期 1
·1-16
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IF 11.452
Wang Zeyu,Hu Liyong,Zhao Min,Dai Luyao,Hrynsphan Dzmitry,Tatsiana Savitskaya,Chen Jun
The development of a multifunctional oil adsorbing material which could effectively and quickly separate oily wastewater is one of the focuses in water environment restoration. In this study, bamboo charcoal (BC) was used as an improver to modify polyurethane (PU) foam. The results of scanning electron microscope (SEM) and Fourier-transform infrared spectroscopy (FTIR) revealed that the addition of BC could effectively improve the mechanical properties of PU. The adsorption data exhibited that the BC-loaded PU (BC/PU) foam composites effectively removed seven organic solvents (OSs, including octane, petroleum ether, soybean oil, chlorobenzene, 1,2-dichloroethane, n-hexane, cyclohexane), and the maximum adsorption capacity of BC/PU was 23.6 g g −1 when BC content was 5%. The order of pseudo-second-order kinetic constants and maximum adsorption capacity of seven OSs was octane < petroleum ether < soybean oil < chlorobenzene < 1, 2-dichloroethane < cyclohexane < n -hexane. Based on the experimental data and density functional theory (DFT) simulation, the adsorption mechanism of OSs on BC/PU-5 was discussed. The E HOMO and μ of OSs calculated by DFT were highly correlated with absorption affinity (K 2 , Q e and Q max ). Hence, the contribution of OSs to the adsorption efficiency of BC/PU-5 may be mainly due to electron donor–acceptor (EDA) interaction and non-hydrophobic interaction. In addition, the adsorption capacity did not change significantly after repeated recycling 5 times. Overall, the prepared BC/PU foam composites could be used as a potential candidate for separating OSs in engineering applications. Graphical Abstract
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
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IF 9.221
Jiawei Gong,Tongtong Zhang,Peng Chen,Fei Yan,Jiyang Liu
Herein we reported the construction of dual-mode electrochemiluminescence (ECL) and electrochemical (EC) sensing platform using the bipolar silica nanochannel array (bp-SNA) confined with the bifunctional probe (tris(2,2′-bipyridyl) ruthenium , Ru(bpy) 3 2+ ) inside the nanochannels (designated as Ru@bp-SNA). With the asymmetric surface charges, bp-SNA on the indium tin oxide electrode can effectively function as electrostatic nanocage for the stable confinement of Ru(bpy) 3 2+ via dual electrostatic force , namely electrostatic attraction of inner negative surface and electrostatic repulsion of outer positive surface. Ru(bpy) 3 2+ immobilized into the nanospace acts as both highly efficient ECL luminophore and well-defined EC redox molecule to generate strong signal. Since the modification of bio-recognition units on the top of Ru@bp-SNA is able to confer excellent recognitive capacity and obtain the formation of complex in the presence of specific analyte, the decrease of ECL and EC signals enables the quantitative detection of this analyte. As proof-of-concept experiments, two tumor related biomarkers, CEA and CA15–3, have been successfully determined in aqueous solution and human serum by ECL and EC modes, respectively.
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Acta Biomaterialia
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2022
·
IF 10.633
Wenbao Zuo,Zhongxiong Fan,Luping Chen,Jinxue Liu,Zheng Wan,Zhimei Xiao,Weibin Chen,Liang Wu,Dengyue Chen,Xuan Zhu
ABSTRACT Chemodynamic therapy (CDT) has aroused extensive attention as a potent therapeutic modality. However, its practical application is severely restricted by the strong acidity requirement for Fenton reaction and upregulated antioxidant defense within metastatic breast cancer. Herein, a copper-based single-site nanocatalyst functionalized with carbonic anhydrase inhibitor (CAI) was constructed for magnetic resonance/photoacoustic imaging (MRI/PA)-guided synergetic photothermal therapy (PTT) and CDT. Once reaching tumor sites, the nanocatalyst can be recognized by tumor cell membranes-overexpressed carbonic anhydrase IX (CA IX). Subsequently, the single-site Cu II can be reduced to Cu I by the tumor-overexpressed glutathione (GSH), which simultaneously impaired the tumor antioxidant defense system and triggered CAI release for inducing intracellular H + accumulation. Further, the decreased intracellular pH can accelerate the nanocatalyst biodegradation to release more Cu II and CAI to participate in next-cycle GSH-depletion and cytoplasm acidification, respectively, thereby continuously supplying Cu I and H + for self-cyclically amplified CDT. Upon laser irradiation, the nanocatalyst can generate local heat, which not only permits PTT but also enhances the nanocatalyst-mediated CDT. Moreover, the suppression of CA IX can hinder the tumor extracellular matrix degradation to prevent tumor metastasis. Overall, this work highlighted the great application prospect in enhancing CDT via tumor acidic/redox microenvironment remodeling, and provides an insightful paradigm for inhibiting breast cancer metastasis. Statement of significance The practical application of chemodynamic therapy (CDT) is severely restricted by the strong acidity requirement for Fenton reaction and upregulated antioxidant defense within cancer. Herein, we developed a carbonic anhydrase inhibitor (CAI)-functionalized Cu-based nanocatalyst. Once reaching tumor sites, the Cu II can be reduced to Cu I by the tumor-overexpressed glutathione (GSH), which simultaneously impaired the tumor antioxidant system and triggered CAI release for inducing intracellular H + accumulation. Further, the decreased intracellular pH can accelerate the nanocatalyst biodegradation to release more Cu II and CAI to participate in next-cycle GSH-depletion and cytoplasm acidification, respectively, thus continuously supplying Cu I and H + for self-cyclically amplified CDT. Upon laser irradiation, the nanocatalyst not only permits PTT but also enhances the CDT.
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Water
·
2022
·Vol. 14
·期 18
·2811
·
IF 3.53
Zhixiong Liu,Wenlei Qin,Lei Sun,Huiyu Dong,Xiangjuan Yuan,Fei Pan,Dongsheng Xia
The degradation of acyclovir (ACY) and atenolol (ATL) in the UV/peroxydisulfate (UV/PDS) process has been systematically considered, focusing on the degradation kinetics, theoretical models, and reaction pathways via applying a microfluidic UV reaction system. The removal efficiencies of ACY and ATL were >94.8%, and the apparent degradation rate constants (kobs) were 0.0931 and 0.1938 min−1at pH 6.0 in the UV/PDS system. The sulfate radical (SO4•−) and hydroxyl radical (•OH) were identified as the major reactive radicals. The pH-dependent reaction rate constants of ACY and ATL with•OH and SO4•−were measured via the competing kinetics. Meanwhile, the contributions of•OH and SO4•−for ACY and ATL degradation were calculated by the radical steady-state hypothesis, and the results revealed that SO4•−occupied a decisive position (>84.5%) for the elimination of ACY and ATL. The contribution of•OH became more significant with the increasing pH, while SO4•−was still dominant. Moreover, ACY and ATL degradation performance were systematically evaluated via the experiments and Kintecus model under different operational parameters (Cl−, Br−, HCO3−, NOM, etc.) in the UV/PDS process. Furthermore, the plausible reaction pathways of ACY and ATL were elucidated based on the Fukui function theory and ultra-performance liquid chromatography-tandem quadrupole time-of-flight mass spectrometry (UPLC-QTOF-MS) analysis. The UV/PDS process has been demonstrated to be an efficient and potential application for micropollutants mitigation.Keywords:UV/PDS;micropollutants;radical contribution rates;kinetic models;degradation pathways
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ANALYTICAL CHEMISTRY
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2022
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IF 8.008
Chengjie Duan,Wenting Cheng,Yanheng Yao,Dayong Li,Zhongyun Wang,Yang Xiang
Aptamer-based methods have attracted increasing interest due to flexible engineering, but their generality is limited by the heterogeneity of signal transduction mechanisms. Given the fact that nonlinear and large molecules are more likely to make the nanosurface overloaded, we investigated a novel signal transduction process to extend the application of aptasensors. In this work, an aptamer complementary element (ACE) is designed with a primer region to serve as the signal probe, which can fully hybridize with an aptamer and be separated by magnetic beads (MBs). Upon target binding, the formed aptamer/target complex is much larger than the linear aptamer/ACE-primer dimer, causing overload of MBs on account of steric hindrance. An extra aptamer/ACE-primer can escape from the surface to the supernatant, which can be amplified by a catalytic hairpin assembly (CHA) circle. The size-dependent signal transduction and the modular design endow the method with high generality and flexibility for protein analysis. The proposed aptasensor was successfully applied to the detection of tau proteins ranging from 0.5 to 1000 ng mL–1 with a limit of detection (LOD) as low as 0.254 ng mL–1. The recovery tests in both human serum and cerebra spinal fluid confirmed the high accuracy and stability. Furthermore, a successful distinction was made between AD patients and healthy controls by the method, suggesting the possible applicability for practical analysis of tau proteins.
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ACS Nano
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2022
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IF 18.027
Yong Yan,Min Ni,Fan Wang,Yue Yu,Xin Gong,Yue Huang,Wei Tao,Chao Li,Feng Wang
Plant biotic or abiotic stresses, such as pathogens, mechanical damage, or high temperature, can increase intracellular H2O2 concentration, damaging proteins, lipids, and DNA. Most current H2O2 detection methods require the separation or grinding of plant samples, inducing plant stresses, and the process is complicated and time-consuming. This paper constructed a metal–organic framework (MOF)-based biosensor for real-time, remote, and in situ detection of exogenous/endogenous H2O2 in plant organs through color-to-thermal signal conversion. By simply spraying horseradish peroxidase, 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), and the precursor of zeolite imidazolate frameworks-8 (ZIF-8), ZIF-8 biosensors were formed in situ on a plant root, petiole, or leaf. This biosensor could report sub-micromolar H2O2 in plants since the oxidation products, ABTS• +, emitted heat when they absorbed energy from near-infrared (NIR) light. Due to the plant’s low absorption in the NIR region, the ZIF-8 biosensor allowed for remote thermal sensing of H2O2 transport or biotic/abiotic stresses in plants with a high signal-to-noise ratio combining NIR laser and thermometer. Our biosensor can be used for the future development of plant sensors for monitoring plant signaling pathways and metabolism that are nondestructive, minimally invasive, and capable of real-time, in situ analysis.
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ATMOSPHERIC ENVIRONMENT
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2022
·
IF 5.755
Jinwen Li,Qingcai Chen,Dongjie Guan
Atmospheric aerosols contain organic compounds that can form triplet organics ( 3 C*) excited by sunlight, which plays a significant role in the aging process of aerosols. The formation characteristics of 3 C* of aerosol components with different polarities were investigated, including highly polar water-soluble matter (HP-WSM), humic-like substances (HULIS), and methanol-soluble matter (MSM). Carbon analysis, probe method and electron paramagnetic resonance were used to investigate the photochemical properties of ambient samples. The coupling effect of generation of 3 C* and reactive oxygen species (ROS) between different aerosol components was also examined. The results showed that the 3 C* generation characteristics are strongly dependent on the polarity of these components. HULIS has the strongest generation ability of 3 C*, and the MSM contributes the most to the total generation of 3 C*. It was found that the high-energy triplet states ( E T ≥ 250 kJ mol −1 ) of HULIS and HP-WSM components account for up to 80% of the water soluble components. These 3 C* have an important contribution to the photochemically generation of ROS, and the generated ROS of different components are also different, which is determined by the chromophore composition of complex organic compounds. A tyrosine-like chromophore is the main substance leading to the formation of water-soluble 3 C*, while the highly oxidized HULIS chromophore plays a leading role in the water-insoluble component. This study also found that there is a coupling effect between HP-WSM and HULIS on 3 C* and ROS generation. The generation rate of 3 C* increases by about 40% after mixing, but the generation of 1 O 2 is severely reduced. In general, this study provided deep insights into the generation characteristics and aging impact of the triplet state on atmospheric aerosols.
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MOLECULAR MEDICINE
·
2022
·Vol. 28
·期 1
·1-15
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IF 6.376
Wang Bingwu,Gao Jian,Zhao Zhongjun,Zhong Xuefei,Cui Hao,Hou Hui,Zhang Yanping,Zheng Junnian,Di Jiehui,Liu Yong
Background Targeting ribosome biogenesis to activate p53 has recently emerged as a therapeutic strategy in human cancer. Among various ribosomal proteins, RPL11 centralizes the nucleolar stress-sensing pathway by binding MDM2, leading to MDM2 inactivation and p53 activation. Therefore, the identification of MDM2-binding RPL11-mimetics would be valuable for anti-cancer therapeutics.Methods Based on the crystal structure of the interface between RPL11 and MDM2, we have identified 15 potential allosteric modulators of MDM2 through the virtual screening.Results One of these compounds, named S9, directly binds MDM2 and competitively inhibits the interaction between RPL11 and MDM2, leading to p53 stabilization and activation. Moreover, S9 inhibits cancer cell proliferation in vitro and in vivo. Mechanistic study reveals that MDM2 is required for S9-induced G2 cell cycle arrest and apoptosis, whereas p53 contributes to S9-induced apoptosis.Conclusion sPutting together, S9 may serve as a lead compound for the development of an anticancer drug that specifically targets RPL11-MDM2-p53 pathway.
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MOLECULES
·
2022
·Vol. 27
·期 18
·5742
·
IF 4.927
Yang Liu,Xue Zhou,Dan Zhou,Yongxing Jian,Jingfu Jia,Fahuan Ge
Diabetes is a chronic metabolic disease, whereas α-glucosidases are key enzymes involved in the metabolism of starch and glycogen. There is a long history of the use of mulberry leaf (the leaf ofMorus alba) as an antidiabetic herb in China, and we found that chalcomoracin, one of the specific Diels–Alder adducts in mulberry leaf, had prominent α-glucosidase inhibitory activity and has the potential to be a substitute for current hypoglycemic drugs such as acarbose, which have severe gastrointestinal side effects. In this study, chalcomoracin was effectively isolated from mulberry leaves, and its α-glucosidase inhibition was studied via enzymatic kinetics, isothermal titration (ITC) and molecular docking. The results showed that chalcomoracin inhibited α-glucosidase through both competitive and non-competitive manners, and its inhibitory activity was stronger than that of 1-doxymycin (1-DNJ) but slightly weaker than that of acarbose. ITC analysis revealed that the combination of chalcomoracin and α-glucosidase was an entropy-driven spontaneous reaction, and the molecular docking results also verified this conclusion. During the binding process, chalcomoracin went into the “pocket” of α-glucosidase via hydrophobic interactions, and it is linked with residues Val544, Asp95, Ala93, Gly119, Arg275 and Pro287 by hydrogen bonds. This study provided a potential compound for the prevention and treatment of diabetes and a theoretical basis for the discovery of novel candidates for α-glycosidase inhibitors.Keywords:mulberry leaf;chalcomoracin;α-glucosidase inhibitor;enzymatic kinetics;molecular docking
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BIOMATERIALS
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2022
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IF 15.304
Xiaohui Xiao,Yupeng Wang,Jieyao Chen,Peng Qin,Peiyao Chen,Dongfang Zhou,Yue Pan
Chemoradiotherapy is a widely used treatment for patients with malignancies such as hepatocellular carcinoma (HCC). However, it remains challenging to realize safe and synergistic chemotherapy and radiation sensitization . Herein, we design a self-targeting nano-assembly (STNA) based on platinum(IV)-lactose amphiphilic prodrug for synergistic and safe chemoradiotherapy of HCC. The Pt STNA would improve the tumor accumulation due to the targeting ability of lactose to HCC cells. After receptor-mediated endocytosis , Pt STNA would release cisplatin(II) in cancer cells to form DNA-binding, thus inducing DNA damage and cell apoptosis. Meanwhile, the DNA-binding also causes cell cycle arrest in the radiation-sensitive G2/M phase by the up-regulation of phosphorylated checkpoint kinase 1 (p-Chk1) expression. Furthermore, under X-ray irradiation, Pt STNA as radiosensitizer possesses a strong X-ray attenuation ability to deposit more energy, thus elevating the level of reactive oxygen species (ROS) to amplify the cell-killing effect of radiotherapy in the G2/M phase with increased DNA damage. As a result, Pt STNA exhibits significant synergistic therapeutic effects in chemoradiotherapy with no adverse effects in vitro and in vivo . Overall, we present a novel self-targeting nano-assembly strategy based on widely used Pt drugs for synergistic chemotherapy and radiation sensitization of HCC treatment.
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