通讯机构:
[Yi Liu; Peng Jiang] C;College of Chemistry and Molecular Sciences & School of Pharmaceutical Sciences, Department of Orthopedics Trauma and Microsurgery (Zhongnan Hospital of Wuhan University), Wuhan University, Wuhan 430072, P. R. China<&wdkj&>Key Laboratory of Coal Conversion and New Carbon Materials of Hubei Province & Institute of Advanced Materials and Nanotechnology, College of Chemical and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China<&wdkj&>School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, P. R. China<&wdkj&>College of Chemistry and Molecular Sciences & School of Pharmaceutical Sciences, Department of Orthopedics Trauma and Microsurgery (Zhongnan Hospital of Wuhan University), Wuhan University, Wuhan 430072, P. R. China<&wdkj&>Key Laboratory of Combinatorial Biosynthesis and Drug Discovery, Ministry of Education, Wuhan University, Wuhan 430071, P. R. China<&wdkj&>Hubei Jiangxia Laboratory, Wuhan 430200, P. R. China
摘要:
Tumor-specific targeting and tumor visualization are major obstacles for clinical diagnosis and treatment. Herein, a dual-targeted "all-in-one" nanoplatform (FAA@CM) for trimodal imaging-guided photothermal/chemodynamic synergistic therapy was successfully synthesized by encapsulating Fe(3)O(4), Ag(2)S, and ascorbic acid with the 4T1 cell membrane. The dual-targeting capability derived from 4T1 cell membrane cloaking and magnetic targeting enables the highly precise tumor-specific delivery of FAA@CM. Fe(2+) released from FAA@CM in a weakly acidic tumor microenvironment can trigger the Fenton reaction to achieve chemodynamic therapy (CDT). The photothermal performance of FAA@CM not only enables photothermal therapy but also promotes the CDT effect. In order to relieve H(2)O(2) deficiency, a biosafe H(2)O(2) prodrug, ascorbic acid, was introduced to greatly increase the H(2)O(2) concentration in tumors, promoting the Fenton reaction to produce more (•)OH to enhance the oxidative damage to tumors. Interestingly, FAA@CM exhibits trimodal imaging capabilities, including second near-infrared (NIR-II, 1000-1700 nm) fluorescence imaging, photoacoustic imaging, and magnetic resonance imaging, which can guide the laser irradiation, achieving complete elimination of 4T1 tumors in BALB/c mice. This work provided a novel dual-targeted, multifunctional theranostic nanoplatform for highly effective tumor therapy.
关键词:
Lithium aluminum layered double hydroxides;Lithium extraction;Phosphate intercalation;Deactivation;Density functional theory
摘要:
Lithium aluminum layered double hydroxides (LiAl-LDHs) have emerged as the most promising adsorbent for lithium extraction from salt lake brines. However, the development of LiAl-LDHs is impeded by their susceptibility to structural collapse and deactivation during desorption process. Herein, an interlayer anion regulation strategy was proposed to endow LiAl-LDHs with superior resistance to deactivation induced by excessive Li+ deintercalation through strengthening the interlayer interactions. Consequently, a novel LiAl-LDH with interlayer Cl− partially replaced by PO43− (LiAl-LDH-P) was synthesized by coupling PO43− intercalation with Li+ insertion during co-precipitation. Combining DFT calculations and elution strength experiments, it was revealed that the intercalated PO43− could anchor Li+ into the vacancies of Al-O octahedron via high interlayer binding energy and strong electrostatic interaction, which imparted LiAl-LDH-P with an excellent anti-elution deactivation ability. Moreover, LiAl-LDH-P presented distinctly advanced compared to commercialized and reported LiAl-LDHs, with extraordinary Li+ adsorption capacity (9.35 mg/g), selectivity (separation factors of 270.3, 450.3, 453.7 for Li+/Na+, Li+/K+, Li+/Mg2+, respectively), and reusability in Lop Nor brine, even at the ultra-high eluent consumption. Furthermore, the physicochemical properties and Li+-extraction mechanism of the LiAl-LDH-P were investigated as well. This work provides a promising strategy to solve the current deactivation of LiAl-LDHs and offers a prospective adsorbent for Li+ extraction from brine.
通讯机构:
[Ya Sun; Juntao Yan] C;College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan, China<&wdkj&>College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan, China
关键词:
Li1.2Ni0.2Mn0.6O2;Li3PO4;Surface coating;Density functional theory (DFT);Cathode materials;Lithium-ion batteries
摘要:
Layered lithium-rich oxide materials are regarded as one of the most promising cathode materials. However, inferior cycling stability and poor rate performance hinder their practical application prospect. In this study, Li3PO4-coated Li1.2Ni0.2Mn0.6O2 cathode materials have been synthesized by sol-gel method together with a facile liquid-evaporation process. The results suggested that the Li3PO4 coating layer, which could not only facilitate the lithium-ion diffusion rate and accelerate the diffusion kinetics but also act as a protective layer to protect it from corrosion by HF and other side reactions. Density functional theory (DFT) calculations confirmed the essence effect on lithium-ion diffusion coefficient and electronic conductivity. After modifying with an appropriate amount of Li3PO4, the Li-rich layered oxides showed enhanced electrochemical performance. Especially, the capacity retention of 5 wt% Li3PO4-coated Li1.2Ni0.2Mn0.6O2 was significantly enhanced from 17.7% of the bare Li1.2Ni0.2Mn0.6O2 to 73.8%. In terms of rate capabilities, 5 wt% Li3PO4-coated Li1.2Ni0.2Mn0.6O2 retained capacities of 181.0, 165.9, 128.8, and 107.8 mAh g(-1), while the bare Li1.2Ni0.2Mn0.6O2 were only 137.4, 109.3, 75.6, and 45.9 mAh g(-1), respectively, at rates of 0.5 C, 1 C, 2 C, and 5 C. Our research findings show that coating with an appropriate amount of lithium-ion conductor material is one of the effective measures to obtain improved performance of Li-rich and Mn-rich layered oxide materials.
通讯机构:
[Liu, Y ; Jiang, P] W;[Jiang, P ] H;Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China.;Hubei Univ Sci & Technol, Hubei Key Lab Radiat Chem & Funct Mat, Xianning 437100, Peoples R China.;Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.
摘要:
Nanocatalytic therapy (NCT) has made great achievements in tumor treatments due to its remarkable enzyme-like activities and high specificity. Nevertheless, the limited types of nanozymes and undesirable tumor microenvironments (TME) greatly weaken the therapeutic efficiency. Developing a combination therapy integrating NCT and other strategies is of great significance for optimal treatment outcomes. Herein, a AuPt-loaded Cu-doped polydopamine nanocomposite (AuPt@Cu-PDA) with multiple enzyme-like activities was rationally designed, which integrated photothermal therapy (PTT) and NCT. The peroxidase (POD)-like activity of AuPt@Cu-PDA can catalyze hydrogen peroxide (H(2)O(2)) into ·OH, and the catalase (CAT)-mimic activity can decompose H(2)O(2) into O(2) to alleviate hypoxia of TME, and O(2) can be further converted into toxic ·O(2)(-) by its oxidase (OXD)-mimic activity. In addition, Cu(2+) in AuPt@Cu-PDA can effectively consume GSH overexpressed in tumor cells. The boosting of reactive oxygen species (ROS) and glutathione (GSH) depletion can lead to severe oxidative stress, which can be enhanced by its excellent photothermal performance. Most importantly, the accumulation of Cu(2+) can disrupt copper homeostasis, promote the aggregation of lipoylated dihydrolipoamide S-acetyltransferase (DLAT), disrupt the mitochondrial tricarboxylic acid (TCA) cycle, and finally result in cuproptosis. Collectively, photothermal and photoacoustic imaging (PTI/PAI)-guided cuproptosis-enhanced NCT/PTT can be achieved. This work may expand the application of nanozymes in synergistic therapy and provide new insights into cuproptosis-related therapeutic strategies.
摘要:
Balancing ion conductivity, mechanical strength, and alkali stability is a significant challenge in the application of anion exchange membranes (AEMs) in anion exchange membrane fuel cells (AEMFCs). In this study, rigid poly (4-vinylbiphenyl chloride) (PVB) and flexible polystyrene-b-poly(ethylene-co-butylene)-b-polystyrene (SEBS) are selected as the polymer backbones to create semi-interpenetrating network (SIPN) AEMs. To achieve high ionic conductivity, quaternary ammonium groups are grafted onto each PVB structural unit, and TMHDA reacts with CMSEBS to construct a cross-linking network while also generating quaternary ammonium groups. This approach, along with well-defined micro-morphology, result in SIPN-SEBS/PVB-10 exhibiting an impressive ionic conductivity of 105.7 mS cm(-1) at 80degree celsius. The SIPN structure, formed by the linear quaternary ammonium PVB and cross-linked SEBS, enhances the compatibility between the rigid and flexible components, resulting in good tensile strength (>14.5 Mpa) and elongation at break (>31.8%) for SIPN-SEBS/PVB AEMs at 25degree celsius in the wet state. Furthermore, SIPN-SEBS/PVB AEMs exhibit excellent chemical stability, in addition to the restricted swelling behavior, which can be attributed to the stable PVB and SEBS main chains. After immersion in a 1 M NaOH solution at 80degree celsius for 30 days, the degradation of backbones and cations in all membranes is less than 10% and 20%, respectively. Moreover, the peak power density of SIPN-SEBS/PVB-10 in an H-2/O-2 single fuel cell reaches an impressive value of 379 mW cm(- 2). Based on these excellent properties, the developed SIPN AEMs hold great promise as candidates for AEMFCs.
通讯机构:
[Likun Li; Lei Zhang] A;Authors to whom correspondence should be addressed.<&wdkj&>China-Ukraine Institute of Welding, Guangdong Academy of Sciences, Guangzhou 510650, China<&wdkj&>Authors to whom correspondence should be addressed.<&wdkj&>School of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China
关键词:
acidic wastewater;heavy metal ions;pyridine-modified chitosan adsorbent;adsorption mechanism
摘要:
A novel pyridine-modified chitosan (PYCS) adsorbent was prepared in a multistep procedure including the successive grafting of 2-(chloromethyl) pyridine hydrochloride and crosslinking with glutaraldehyde. Then, the as-prepared materials were used as adsorbents for the removal of metal ions from acidic wastewater. Batch adsorption experiments were carried out to study the impact of various factors such as solution pH value, contact time, temperature, and Fe (III) concentration. The results showed that the absorbent exhibited a high capacity of Fe (III) and the maximum adsorption capacity was up to 66.20 mg/g under optimal experimental conditions (the adsorption time = 12 h, pH = 2.5, and T = 303 K). Adsorption kinetics and isotherm data were accurately described by the pseudo-second-order kinetic model and Sips model, respectively. Thermodynamic studies confirmed that the adsorption was a spontaneous endothermic process. Moreover, the adsorption mechanism was investigated using Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results revealed the pyridine group forms a stable chelate with iron (III) ions. Therefore, this acid-resistant adsorbent exhibited excellent adsorption performance for heavy metal ions from acidic wastewater compared to the conventional adsorbents, helping realize direct decontamination and secondary utilization.
作者机构:
[Qi, Zheng; Zhang, Sushu; Zhou, Weichuang; Lv, Kangle] South Cent Minzu Univ, State Ethn Affairs Commiss, Key Lab Catalysis & Mat Sci, Wuhan 430074, Peoples R China.;[Qi, Zheng; Zhang, Sushu; Zhou, Weichuang; Lv, Kangle] South Cent Minzu Univ, Minist Educ, Coll Resources & Environm, Wuhan 430074, Peoples R China.;[Fan, Jiajie; Chen, Jinbao] Zhengzhou Univ, Sch Mat Sci & Engn, Zhengzhou 450001, Peoples R China.;[Li, Yuhan] Chongqing Technol & Business Univ, Engn Res Ctr Waste Oil Recovery Technol & Equipmen, Chongqing Key Lab Catalysis & New Environm Mat, Minist Educ, Chongqing 400067, Peoples R China.;[Li, Xiaofang] Wuhan Polytech Univ, Coll Chem & Environm Engn, Wuhan 430023, Peoples R China.
通讯机构:
[Yuhan Li] E;[Kangle Lv] K;Engineering Research Center for Waste Oil Recovery Technology and Equipment, Ministry of Education, Chongqing Key Laboratory of Catalysis and New Environmental Materials, Chongqing Technology and Business University, Chongqing 400067, China<&wdkj&>Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission & Ministry of Education, College of Resources and Environment, South-Central Minzu University, Wuhan 430074, China
通讯机构:
[Huang Dai; Xiaodan Liu] C;College of Food Science and Engineering, Wuhan Polytechnic University, Wuhan 430023, China<&wdkj&>Key Laboratory for Deep Processing of Major Grain and Oil (Wuhan Polytechnic University), Ministry of Education, Wuhan 430023, China<&wdkj&>Food Safety Research Center, Key Research Institute of Humanities and Social Sciences of Hubei Province, Wuhan 430023, China<&wdkj&>College of Food Science and Engineering, Wuhan Polytechnic University, Wuhan 430023, China<&wdkj&>Key Laboratory for Deep Processing of Major Grain and Oil (Wuhan Polytechnic University), Ministry of Education, Wuhan 430023, China
关键词:
Curcumin;UiO-66(Zr);Electrochemical sensor;Methyl parathion;Vegetables and fruits
摘要:
As a typical organophosphorus pesticide, the widespread abuse of methyl parathion (MP) has seriously threat-ened the environment and human health. To realize the sensitive detection of MP, an electrochemical sensor based on Metal-Organic Framework UiO-66(Zr) loaded curcumin(CCM) was designed. UiO-66 with high porosity for adsorption property and CCM with unique electrochemical activity conspired to improve the sensitivity of the electrochemical sensor. The result indicated that the CCM/UiO-66 electrode was well fabricated and exhibited an enhanced electrochemical response to MP. Under optimal conditions, the CCM/UiO-66 electrode extended a wide linear range from 20 ng mL-1 to 20000 ng mL-1 and a low limit of detection of 0.98 ng mL-1. The fabricated electrode also showed excellent reproducibility and stability. Additionally, the electrode demonstrated outstanding sensing capabilities in the electrochemical detection of MP in vegetables and fruits samples.
通讯机构:
[Bo Chai] S;School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China
关键词:
Built-in electric field;CoOOH/BC composites;Peroxymonosulfate;Radical and non-radical
摘要:
The strong electron interaction between metal oxide-carbon-based catalyst components plays a vital role in the peroxymonosulfate (PMS) activation for pollutant degradation. Herein, a novel CoOOH nanosheets anchored on rape straw-derived biochar (BC) surface (labeled as CoOOH/BC) as an efficient PMS activator toward degrading sulfamethoxazole (SMX) was synthesized. Experimental results indicated that integrating CoOOH nanosheets on the BC surface could inhibit CoOOH aggregation to increase the specific surface areas, exert a component synergistic effect to enhance activation degradation activity, and improve the catalyst stability. As a result, a 96 % degradation efficiency of SMX was achieved within 20 min over 20 wt% CoOOH/BC composite catalyst under the optimal conditions. Density functional theory (DFT) calculations disclosed that a built-in electric field (BIEF) pointing from BC to CoOOH was constructed at their interface, which could mediate PMS activation for reactive oxygen species (ROS) generation and induce direct electron transfer from SMX to PMS, resulting in efficient SMX degradation via both radical and non-radical pathways. Moreover, quenching experiments and electron paramagnetic resonance (EPR) measurements confirmed that single oxide (O-1(2)) and superoxide radical (O-2(center dot-)) are the dominant active species in the current system. Additionally, the possible SMX degradation routes were reasonably proposed based on liquid chromatography-mass spectrometry (LC-MS) results. This work provides an in-depth understanding of the role of BIEF in PMS activation, and expands the application of biochar-based materials in the field of environmental remediation. (c) 2023 Elsevier Inc. All rights reserved.
通讯机构:
[Likun Li; Lei Zhang] A;Authors to whom correspondence should be addressed.<&wdkj&>China-Ukraine Institute of Welding, Guangdong Academy of Sciences, Guangzhou 510650, China<&wdkj&>Authors to whom correspondence should be addressed.<&wdkj&>School of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China
摘要:
In this study, high-performance modified biochar/alginate composite bead (MCB/ALG) adsorbents were prepared from recycled agricultural waste corncobs by a high-temperature pyrolysis and KOH/FeCl3 activation process. The prepared MCB/ALG beads were tested for the adsorption of methylene blue (MB) dye from wastewater. A variety of analytical methods, such as SEM, BET, FTIR and XRD, were used to investigate the structure and properties of the as-prepared adsorbents. The effects of solution pH, time, initial MB concentration and adsorption temperature on the adsorption performance of MCB/ALG beads were discussed in detail. The results showed that the adsorption equilibrium of MB dye was consistent with the Langmuir isothermal model and the pseudo-second-order kinetic model. The maximum adsorption capacity of MCB/ALG-1 could reach 1373.49 mg/g at 303 K. The thermodynamic studies implied endothermic and spontaneous properties of the adsorption system. This high adsorption performance of MCB/ALG was mainly attributed to pore filling, hydrogen bonding and electrostatic interactions. The regeneration experiments showed that the removal rate of MB could still reach 85% even after five cycles of experiments, indicating that MCB/ALG had good reusability and stability. These results suggested that a win-win strategy of applying agricultural waste to water remediation was feasible.
通讯机构:
[Huaxiang Fang] W;[Huan He] S;School of Pharmaceutical Sciences, Guizhou University, Guiyang 550025, P. R. China<&wdkj&>Key Laboratory of Coal Conversion and New Carbon Materials of Hubei Province, College of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China<&wdkj&>Wuhan Yuxiang Pharmaceutical Technology Company, Limited, Wuhan 430200, P. R. China<&wdkj&>Wuhan Yuxiang Pharmaceutical Technology Company, Limited, Wuhan 430200, P. R. China
摘要:
Inhibition of methionine adenosyltransferase 2A (MAT2A) in cancers with a deletion of methylthioadenosine phosphorylase (MTAP) gene leads to synthetic lethality, thus receiving significant interest in the field of precise cancer treatment. Herein, we report the discovery of a tetrahydrobenzo[4,5]imidazo-[1,2-a]pyrazine fragment which occupies the MAT2A allosteric pocket. The lead compound 8 exhibited extremely high potency to inhibit MAT2A enzymatic activity (IC50 = 18 nM) and proliferation of MTAP-null cancer cells (IC50 = 52 nM). 8 had a favorable pharmacokinetic profile with a bioavailability of 116% in mice. More importantly, introducing an amide motif (28) to the core structure raised the plasma drug exposure from 11718 to 41 192 ng center dot h center dot mL-1. 28 displayed a significantly better in vivo potency than AG-270, which is being evaluated in clinical trails, and induced -52% tumor regression in a xenograft MTAP-depleted colon tumor model.
摘要:
In this paper, carbon‐based acid–base bifunctional catalyst was synthesized and employed for producing fuel precursor 5‐hydroxymethylfurfural from glucose, displaying excellent catalytic performance and stability. Abstract Carbon‐based acid–base bifunctional catalyst was synthesized by the functionalization of activated carbon (AC) with 3‐mercaptopropyl trimethoxysilane, 3‐aminopropyl trimethoxysilane, and H2SO4 via sulfhydrylation, ammonifiation, and sulfonation successively. The as‐prepared catalyst of NH2‐AC‐SO3H was characterized by infrared spectroscopy, X‐ray diffraction, thermogravimetric analysis and Brunauer–Emmet–Teller specific area analysis, and it was further used for producing fuel precursor 5‐hydroxymethylfurfural (5‐HMF) from glucose. The influences of the catalyst type, ratio of acid–base groups, catalyst amount, reaction temperature, and reaction time were investigated. It was found that NH2‐AC‐SO3H revealed excellent activity, and the yield of 5‐HMF reached 71.8% under the optimized reaction conditions with a 1.3:1 mass ratio of NH2‐AC‐SO3H to glucose at 140°C for 6 h in γ‐valerolactone. The reusability of NH2‐AC‐SO3H was also performed, and only slight decreases in the conversion of glucose and the yield of 5‐HMF were observed, still giving 65.3% yield of 5‐HMF after 4 runs.
通讯机构:
[Feng-Lei Jiang] S;Sauvage Center for Molecular Sciences, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan430072, P. R. China
摘要:
InP quantum dots (QDs) attract growing interest in recent years, owing to their environmental advantages upon applications in display and lighting. However, compared to Cd-based QDs and Pb-based perovskites, the synthesis of InP QDs with high optical quality is relatively more difficult. Here, we established a mid-synthetic modification approach to improve the optical properties of InP-based QDs. Tris(dimethylamino)phosphine ((DMA)(3)P) and indium iodide were used to prepare InP QDs with a green emission (∼527 nm). By introducing zinc halides (ZnX(2)) during the mid-synthetic process, the photoluminescence quantum yield (PLQY) of the resulting InP/ZnSeS/ZnS core/shell/shell QDs was increased to >70%, and the full-width-at-half-maximum (FWHM) could be narrowed to ∼40 nm. Transmission electron microscopy clearly showed the improvement of the QDs particle size distribution after introducing ZnX(2). It was speculated that ZnX(2) was bound to the surface of QDs as a Z-type ligand, which not only passivated surface defects and suppressed the emission of defect states but also prevented Ostwald ripening. The InP cores were also activated by ZnX(2), which made the growth of the ZnSeS shell more favorable. The photoluminescence properties started to be improved significantly only when the amount of ZnX(2) exceeded 0.5 mmol. As the amount increased, more ZnX(2) was distributed around the QDs to form a ligand layer, which prevented the shell precursor from crossing the ligand layer to the surface of the InP core, thus reducing the size of the InP/ZnSeS/ZnS QDs. This work revealed a new role of ZnX(2) and found a method for InP QDs with high brightness and low FWHM by the mid-synthetic modification, which would inspire the synthesis of even better InP QDs.
通讯机构:
[Huimin Hu; Qiwu Zhang] S;School of Resources and Environmental Engineering, Wuhan University of Technology, Luoshi Road 122, Wuhan, Hubei, 430070, China