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WATER RESEARCH · 2022 · IF 13.4

Integrating anodic sulfate activation with cathodic H2O2 production/activation to generate the sulfate and hydroxyl radicals for the degradation of emerging organic contaminants

Chaozhi Kuang,Guoshen Zeng,Yangjian Zhou,Yaoyao Wu,Dexuan Li,Yingfei Wang,Chuanhao Li

Conventional electrocatalytic degradation of pollutants involves either cathodic reduction or anodic oxidation process, which caused the low energy utilization efficiency. In this study, we successfully couple the anodic activation of sulfates with the cathodic H 2 O 2 production/activation to boost the generation of sulfate radical (SO 4 ·− ) and hydroxyl radical (·OH) for the efficient degradation of emerging contaminants. The electrocatalysis reactor is composed of a modified-graphite-felt (GF) cathode, in-situ prepared by the carbonization of polyaniline (PANI) electrodeposited on a GF substrate, and a boron-doped diamond (BDD) anode. In the presence of sulfates, the electrocatalysis system shows superior activities towards the degradation of pharmaceutical and personal care products (PPCPs), with the optimal performance of completely degrading the representative pollutant carbamazepine (CBZ, 0.2 mg L −1 ) within 150 s. Radicals quenching experiments indicated that ·OH and SO 4 ·− act as the main reactive oxygen species for CBZ decomposition. Results from the electron paramagnetic resonance (EPR) and chronoamperometry studies verified that the sulfate ions were oxidized to SO 4 ·− radicals at the anode, while the dissolve oxygen molecules were reduced to H 2 O 2 molecules which were further activated to produce ·OH radicals at the cathode. It was also found that during the catalytic reactions SO 4 ·− radicals could spontaneously convert into peroxydisulfate (PDS) which were subsequently reduced back to SO 4 ·− at the cathodes. The quasi-steady-state concentrations of ·OH and SO 4 ·− were estimated to be 0.51×10 −12  M and 0.56×10 −12  M, respectively. This study provides insight into the synergistic generation of ·OH/SO 4 ·− from the integrated electrochemical anode oxidation of sulfate and cathode reduction of dissolved oxygen, which indicates a potential practical approach to efficiently degrade the emerging organic water contaminants.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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ACS ES&T Water · 2022 · IF 0

Polyamide Thin-Film Composite Janus Membranes Avoiding Direct Contact between Feed Liquid and Hydrophobic Pores for Excellent Wetting Resistance in Membrane Distillation

Tengjing Gong,Danting Shi,Zhigao Zhu,Bin Liu,Senlin Shao

Hydrophobic membranes are very susceptible to pore wetting when they contact the feed water containing surfactants or low-surface-tension liquids in membrane distillation (MD). Avoiding direct contact between feed water and hydrophobic membrane pores is a potential strategy to control membrane pore wetting. In this study, we successfully fabricated a polyamide thin-film composite (TFC) Janus membrane through interfacial polymerization, with a hydrophobic microporous membrane as the substrate. The fabricated TFC Janus membrane showed a super antiwetting ability when treating the hypersaline water containing surfactants (>0.4 mM sodium dodecyl sulfate) or ethanol (>40% v/v). The optical coherence tomography (OCT) observation revealed that no liquid water was present at the distillate-facing side of the polyamide layer. Therefore, we ascribed the super antiwetting ability to the fact that the polyamide layer could prevent the feed liquid from directly contacting hydrophobic pores. The TFC Janus membrane could also avoid the wetting induced by gypsum scaling because the polyamide layer could act as a barrier to hinder the intrusion of gypsum crystals into hydrophobic pores. In addition to the antiwetting ability, the TFC Janus membrane showed 10–20% increases in vapor flux, despite the existence of a dense polyamide layer. Because interfacial polymerization is the most commonly used method for the fabrication of commercial TFC membranes, this study provides a facile and scalable method to fabricate membranes with robust antiwetting ability.

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Biomaterials Advances · 2022 · IF 0

Novel ROS-scavenging hydrogel with enhanced anti-inflammation and angiogenic properties for promoting diabetic wound healing

Lianghua Jiang,Xufeng Yang,Yijian Zhang,Dawei He,Yijun Gao,Ke Lu,Yanming Hao,Yan Gao,Daming Lu,Xiangyun Jin,Chong Li

Accelerating angiogenesis of diabetic wounds is crucial to promoting wound healing. Currently, vascular endothelial growth factor (VEGF), an angiogenesis-related bioactive molecule, is widely used in clinic to enhance wound angiogenesis, but it faces problems of inactivation and low utilization due to harsh microenvironment. Here, we developed a novel reactive oxygen species (ROS)-scavenging hydrogel aimed to polarize macrophages toward an anti-inflammatory phenotype, inducing efficient angiogenesis in diabetic wounds. This composite hydrogel with good biosafety and mechanical properties showed sustainable release of bioactive VEGF. Importantly, it could significantly reduce ROS level and rapidly improve wound microenvironment, which ensured the activity of VEGF in vitro and in vivo and successful healing eventually. At the same time, the composite hydrogel exhibited excellent antibacterial properties. In vivo results confirmed good anti-inflammatory, stimulated vascularization and accelerated wound healing attributed to the novel ROS-scavenging hydrogel, which might serve as a promising wound dressing in diabetic wound healing.

CAS / MDL: 90-80-2 28211-04-3
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2022 · IF 5.999

Hyaluronic acid mediated Fe3O4 nanocubes reversing the EMT through targeted cancer stem cell

Yuhui Wang,Shilong Ma,Xuanyu Liu,Yan Wei,Haofeng Xu,Ziwei Liang,Yinchun Hu,Xiaojie Lian,Di Huang

Hepatocellular carcinoma (HCC) is one of the deadliest tumors in the world with a high rate of recurrence and metastasis. Therefore, the most pressing issue today is the development of new drugs, diagnostic and therapeutic approaches for effective cancer treatment. Cancer stem cells (CSCs) play a pivotal role in tumor recurrence, tumor resistance, and tumor metastasis, which provides a new perspective on the development of liver cancer. In the study, a high-temperature thermal breakdown approach was used to create composite magnetic nanocubes modified by polyethyleneimine (PEI) and hyaluronic acid (HA). The Fe 3 O 4 nanocubes can recognize HCC stem cells via receptor−ligand binding of HA and CD44 (HA receptor). While loading a small molecule LDN193189 inhibited the expression of stemness-related genes OCT4 and Nanog . More crucially, the Fe 3 O 4 nanocubes significantly suppressed HCC cell proliferation and migration by regulating the expression of epithelial-mesenchymal transition (EMT) process markers E-cadherin, Vimentin , and N-cadherin. Dual targeting using magnetic and receptor-mediated targeting improved the uptake of the drug delivery system. Our findings imply that the medication delivery method might be a potential therapeutic strategy for HCC.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMISTRY & BIODIVERSITY · 2022 ·Vol. 20 ·期 1 ·e202200867 · IF 2.745

Design, Synthesis, Calculation and Biological Activity Studies Based on Privileged Coumarin Derivatives as Multifunctional Anti-AD Lead Compound

Huiyan Wang,Mengyang Su,Xuli Shi,Xiangyu Li,Xinyu Zhang,Aihong Yang,Rui Shen

Coumarins and their derivatives possessed a variety of biological activities and some of coumarin-based drugs have been approved by the US Food and Drug Administration. Alzheimer's disease (AD) has caused great losses to human society. However, due to its complex pathogenesis, the ideal therapeutic approach has not been found yet. Free radical scavenging activity which is one of the main activities of coumarin core structure is closely related to other anti-AD activities. Therefore, in this work coumarins were chosen as privileged lead compounds for the development of anti-AD drugs based on strategy of multi-target directed ligands (MTDLs). Derivatives 1 – 3 which could modulate multiple targets simultaneously, including ROS, cholinesterase, βamyloid (Aβ) aggregation, and metal dyshomeostasis were designed and for the first time synthesized. Their anti-AD activities were studied both in vitro and in silico . Results showed that 1 – 3 possessed potent antioxidant activities and 7-OH group did change the electron distribution of the molecule and enhance the antioxidant activities. They also have good inhibition activities on acetylcholinesterase (AChE) and Aβ aggregation and compound 1 had the strongest AChE inhibitory effect among the three compounds (AChE IC 50 =11.15 μM). Compound 1 – 3 could also selectively chelate with Cu 2+ and Al 3+ to regulate the metal homeostasis. In silico simulations, including molecular docking and prediction of ADMET performance, indicated that 1 – 3 could interact with target proteins and cross the blood brain barrier. In conclusion, 1 – 3 could be promising MTDLs applied as anti-AD candidate drugs. Graphical

✓ 已验证 产品关联 DOI PubMed 高影响因子
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2022 · IF 11.357

Visible Light Accelerates Cr(III) Release and Oxidation in Cr–Fe Chromite Residues: An Overlooked Risk of Cr(VI) Reoccurrence

Dashi Lei,Chunli Gou,Chunli Wang,Juanqin Xue,Zhongshen Zhang,Weizhen Liu,Zhang Lin,Jing Zhang

The reduced chromite ore processing residue (rCOPR) deposited in environments is susceptible to surrounding factors and causes reoccurrence of Cr(VI). However, the impact of natural sunlight on the stability of rCOPR is still unexplored. Herein, we investigated the dissolution and transformation behaviors of Cr(III)–Fe(III) hydroxide, a typical Cr(III)-containing component in rCOPR, under visible light. At acidic conditions, the release rate of Cr(III) under illumination markedly increased, up to 7 times higher than that in the dark, yet no Cr(VI) was produced. While at basic conditions, only Cr(VI) was obtained by photo-oxidation, with an oxidation rate of ∼7 times higher than that by δ-MnO2 under dark conditions at pH 10, but no reactive oxygen species was generated. X-ray absorption near-edge structure and density functional theory analyses reveal that coexisting Fe in the solid plays a critical role in the pH-dependent release and transformation of Cr(III), where photogenerated Fe(II) accelerates Cr(III) produced at acidic conditions. Meanwhile, at basic conditions, the production of intermediate Cr(III)–Fe(III) clusters by light leads to the oxidation of Cr(III) into Cr(VI) through the nonradical “metal-to-metal charge transfer” mechanism. Our study provides a new insight into Cr(VI) reoccurrence in rCOPR and helps in predicting its environmental risk in nature.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Constructing abundant phase interfaces of the sulfides/metal-organic frameworks p-p heterojunction array for efficient overall water splitting and urea electrolysis

Tao Zhao,Dazhong Zhong,Lu Tian,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao

Designing efficient electrocatalysts to improve the overall water splitting and urea electrolysis efficiency for hydrogen generation can greatly solve the dilemma of energy shortage and environmental pollution. In this work, Co 8 FeS 8 @CoFe–MOF/NF heterojunction arrays were fabricated by embedding sulfides into the surface of metal-organic frameworks (MOFs) nanosheets as multifunctional electrocatalyst. The introduction of sulfide on CoFe–MOF/NF can not only adjust the electronic structure (electron-rich state) and change the surface properties (more hydrophilic), but also increase the active area to enhance the catalytic activity. The in situ Raman shows Co 8 FeS 8 @CoFe–MOF/NF is more easily to generate active species at low potentials and generates a higher content of active β-MOOH phase than CoFe–MOF/NF. Therefore, the Co 8 FeS 8 @CoFe–MOF/NF exhibits excellent oxygen evolution reaction (OER) performance with an overpotential of 213 mV at 10 mA cm −2 . Furthermore, when used as a urea oxidation reaction (UOR), only an ultralow potential of 1.311 V at 10 mA cm −2 . More importantly, the assembled two-electrode drives overall water splitting and urea electrolysis with cell voltages of 1.62 V and 1.55 V at 10 mA cm −2 , respectively. This work provides insights into the preparation of electrocatalysts with multifunctional heterostructure arrays for hydrogen production.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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BIOMATERIALS · 2022 · IF 15.304

Self-intensified synergy of a versatile biomimetic nanozyme and doxorubicin on electrospun fibers to inhibit postsurgical tumor recurrence and metastasis

Yongwei Hu,Yanteng Xu,Rachel L. Mintz,Xing Luo,Youqiang Fang,Yeh-Hsing Lao,Hon Fai Chan,Kai Li,Shixian Lv,Guojun Chen,Yu Tao,Yun Luo,Mingqiang Li

Tumor-positive resection margins after surgery can result in tumor recurrence and metastasis. Although adjuvant postoperative radiotherapy and chemotherapy have been adopted in clinical practice, they lack efficacy and result in unavoidable side effects. Herein, a self-intensified in-situ therapy approach using electrospun fibers loaded with a biomimetic nanozyme and doxorubicin (DOX) is developed. The fabricated PEG-coated zeolite imidazole framework-67 (PZIF67) is demonstrated as a versatile nanozyme triggering reactions in cancer cells based on endogenous H 2 O 2 and •O 2 − . The PZIF67-generated •OH induces reactive oxygen species (ROS) overload, implementing chemodynamic therapy (CDT). The O 2 produced by PZIF67 inhibits the expression of hypoxia-up-regulated proteins, thereby suppressing tumor progression. PZIF67 also catalyzes the degradation of glutathione , further disturbing the intracellular redox homeostasis and enhancing CDT. Furthermore, the introduced DOX not only kills cancer cells individually, but also replenishes the continuously consumed substrates for PZIF67-catalyzed reactions. The PZIF67-weakened drug resistance strengthens the cytotoxicity of DOX. The combined application of PZIF67 and DOX also suppresses metastasis-associated genes. Both in vitro and in vivo results demonstrate that the self-intensified synergy of PZIF67 and DOX on electrospun fibers efficiently prevents postsurgical tumor recurrence and metastasis, offering a feasible therapeutic regimen for operable malignant tumors.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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MOLECULAR PHARMACEUTICS · 2022 · IF 5.364

Synthesis of Novel Pentacyclic Triterpenoid Derivatives that Induce Apoptosis in Cancer Cells through a ROS-dependent, Mitochondrial-Mediated Pathway

Boyang Cheng,Xindang Chu,Ruiwen Liu,Xinyuan Ma,Mengyang Wang,Jiayi Zhang,Pingxuan Jiao,Qianqian Gao,Wenxiao Ma,Yongmin Zhang,Chuanke Zhao,Demin Zhou,Sulong Xiao

Betulinic acid (BA) and oleanolic acid (OA) are plant-derived conjugates found in various medicinal plants that have emerged as potential antitumor agents. Herein, a series of novel BA and OA derivatives were synthesized by conjugation with per-O-methylated-β-cyclodextrin (PM-β-CD), and their anticancer properties against a panel of three human cancer cell lines were evaluated. Two OA-PM-β-CD conjugates (48 and 50) were observed to be the most potent conjugates against the three cell lines (MCF-7, BGC-823, and HL-60), with a 15- to 20-fold decrease in the IC50 values (IC50: 6.06–8.47 μM) compared with their parental conjugate (OA). Annexin V-FITC/propidium iodide staining and Western blot analysis revealed that both conjugates induced apoptosis in HL-60 cells. Additionally, in the representative conjugate 48-treated HL-60 cells, a decrease in mitochondrial membrane potential and subsequent release of cytochrome c into the cytosol were observed, indicating the activation of the intrinsic apoptosis pathway. Furthermore, 48 dramatically induced the generation of reactive oxygen species (ROS) in HL-60 cells, and the corresponding effect could be reversed using the ROS scavenger N-acetylcysteine. Collectively, these results suggest that the novel pentacyclic triterpenoid derivatives trigger the intrinsic apoptotic pathways via the ROS-mediated activation of caspase-3 signaling, inducing cell death in human cancer cells.

CAS / MDL: 111689-03-3
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ANALYTICAL CHEMISTRY · 2022 · IF 8.008

Dense Conductive Metal–Organic Frameworks as Robust Electrocatalysts for Biosensing

Kai Niu,Pengcheng Sun,Jiping Chen,Xianbo Lu

Due to the fascinating properties such as high porosity, large surface areas, and tunable chemical components, metal–organic frameworks (MOFs) have emerged in many fields including catalysis, energy storage, and gas separation. However, the intrinsic electrical insulation of MOFs severely restricts their application in electrochemistry. Here, we synthesize a series of 2D conductive MOFs (cMOFs) through tuning the structure with atomic precision using simple hydrothermal methods. Various electroactive probes are used to reveal the structure–property relationships in 2D cMOFs. Then, we demonstrate the first exploration and implementation of 2D cMOFs toward the construction of electrochemical biosensors. In particular, the biosensor based on Cu3(tetrahydroxy-1,4-quinone)2 [Cu3(THQ)2] displays a remarkably improved electrocatalytic performance at a much lower potential. The mechanism study reveals the essential role of charge-transfer interactions between the dense catalytic sites of Cu3(THQ)2 and analytes. Furthermore, the Cu3(THQ)2-based biosensor demonstrates robust anti-interference capability, good stability, fast response speed, and an ultralow detection limit for paraoxon. These promising results indicate the great potential of cMOFs in biomedical, food safety, and environmental sensing applications.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF MATERIALS SCIENCE · 2022 ·Vol. 57 ·期 47 ·21693-21708 · IF 4.682

Red emission B, N, S-co-doped carbon dots with pH-responsive functionality for colorimetric and fluorescent dual-mode detection of Ag+ ions

Du Jinyan,Xu Na,Wang Chaofeng,Shu Qin,Xu Qidi,Zhang Ping,Zhuo Shujuan,Zhu Changqing

Novel red-emitting B, N, S-co-doped carbon dots (B,N,S-CDs) were prepared via a one-step hydrothermal carbonization. The obtained B,N,S-CDs are found to be responsive to the pH changes, i.e., the fluorescence intensities obviously change with the watershed of pH 7.4, accompanied by a blue-shift of the fluorescence emission wavelengths with the pH from 1 to 13. The surface state and size of the B, N, S-CDs are responsible for the fantastic responses. Furthermore, introduction of Ag + into the B, N, S-CDs resulted in fluorescence quenching and apparent changes of extinction value, thereby the quantitative assay can be successfully realized where a linear range of 0.1–400 and 0–700 μM with a detection limit of 38 and 107 nM is obtained, respectively. The mechanism might be due to static quenching and induced electron/energy transfer (ET) resulted from the formation of non-fluorescent complex. Strikingly, Ag + can be visualized via evident color changes from red to navy blue under UV light and from maroon to dark brown under sunlight, respectively. These findings indicate that the as-obtained B, N, S-CDs possess a great potential as a dual probe of pH and Ag + ions for biosensing. Graphical Abstract The red-emitting fluorescent B, N, S-CDs with a fantastic pH-sensitive feature, as a dual-mode nanosensor via colorimetric and fluorescence outputs, were applied to detect Ag + ions with the LOD of 107 and 38 nM, respectively.

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MATERIALS CHEMISTRY AND PHYSICS · 2022 · IF 4.778

The preparation of chiral carbon dots and the study on their antibacterial abilities

Dan Zhao,Mengyu Xu,Kang Dai,Huan Liu,Yan Jiao,Xincai Xiao

Chirality is one of the most widespread properties in nature. After the successful application of non-optical active carbon dots (CDs) in the fields of detection, imaging, and antibacterial, the researchers turned more attention to the preparation and applications of chiral CDs. This paper reports the preparation of several chiral CDs with chiral amino acids as carbon sources through two different methods (one-step hydrothermal route and two-step coupling route), and further explores the difference in antibacterial abilities of these chiral CDs prepared by different carbon sources and synthesis methods. The experiments results showed that chiral D/LGU which are prepared through one-step method and with glutamic acid (Glu), are superior to those prepared by two-step method (NLDU/NDGU), or those prepared with cysteine as raw material (D/LCS). For D/LCS, the antibacterial ability of the L type is superior to that of the D type, proving that the synthesis method and the chirality of raw material are both important in the antibacterial behavior of prepared CDs. The chirality and optical properties of prepared CDs have been characterized by UV–vis spectrophotometer , fluorescence spectrology, and circular dichroism. Through MurA enzyme inhibition tests, SEM, and molecular docking design, the antibacterial mechanism of chiral CDs has been investigated. The research provides a sound foundation for the preparation, characterization, and application of chiral CDs, as well as the novel targeting antibacterial applications.

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