通讯机构：
[Qingsong Zhang; Lin Cheng; Qingyi Zeng] S;School of Resource & Environment and Safety Engineering, University of South China, Hengyang 421001, China<&wdkj&>School of Chemistry and Chemical Engineering, Southeast University, Nanjing 210009, China
摘要：
An interfacial Cd-S bond modulated hierarchical Z-scheme heterostructure composed by indium vacancies-rich In2-xS3 and Cd-rich Cd1+xIn2-xS4 (In2-xS3/Cd1+xIn2-xS4) is rationally designed and fabricated by using MIL-68 (In) as precursor and template, and used for efficient photocatalytic wastewater treatment and CO2 reduction. The in -situ ion-exchange derived Cd-S bond at the heterointerface induced the Z-scheme charge transfer mechanism in hierarchical In2-xS3/Cd1+xIn2-xS4 photocatalyst, which is verified by the X-ray photoelectron spectroscopy, electron paramagnetic resonance and density functional theory calculations. Moreover, the hierarchical ultrathin and loose two-dimensional nanosheet structure is conducive to expose more active sites and adsorb more re-actants. By integrating the efficient adsorption capacity and Z-scheme mechanism, the In2-xS3/Cd1+xIn2-xS4 photocatalyst shows superior photocatalytic CO2 reduction activity and high removal efficiency of dyes and heavy metal. For example, under visible light illumination, it removed almost 100 % of various dyes within 10 min operation, and reduced 100 % Cr(VI) within 1 h, and it also manifested state-of-the-art production rates of 132.5 and 392.1 mu mol h-1 g-1 for CH4 and CO, respectively, in reducing CO2 without co-catalyst. A useful inspiration on purposive modulating Z-scheme charge transfer by atomic-level interface engineering was pro-posed to significantly promote the photocatalytic performance.
作者机构：
[Pan, Ai-Qun; Tang, Shuai; Wang, Huamin; Lin, Ying-Wu; Wang, HM; Huang, Jun] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Sun, Li-Juan; Lin, Ying-Wu] Univ South China, Hengyang Med Coll, Hengyang 421001, Peoples R China.;[Lin, Ying-Wu] Univ South China, Key Lab Prot Struct & Funct Univ Hunan Prov, Hengyang 421001, Peoples R China.
通讯机构：
[Lin, YW ; Wang, HM] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Hengyang Med Coll, Hengyang 421001, Peoples R China.;Univ South China, Key Lab Prot Struct & Funct Univ Hunan Prov, Hengyang 421001, Peoples R China.
摘要：
Significant efforts have been made in the design of artificial metalloenzymes. Myoglobin (Mb), an O2 carrier, has been engineered to exhibit different functions. Herein, we applied a series of engineered Mb mutants with peroxidase activity for biosynthesis of clofazimine (CFZ), a potential drug with a broad-spectrum antiviral activity, by integration with chemical synthesis. Two of those mutants, F43Y Mb and F43Y/T67R Mb, have been shown to efficiently catalyze the oxidative coupling of 2-N-(4-chlorophenyl) benzene-1,2-diamine (N-4-CPBDA) in the presence of H2O2, with 97% yields. The overall catalytic efficiency (kcat/Km) is 46-fold and 82-fold higher than that of WT Mb, respectively. By further combination of this reaction with chemical synthesis, the production of CFZ was accomplished with an isolated yield of 72%. These results showed that engineered Mbs containing the Tyr-heme cross-link (F43Y Mb and F43Y/T67R Mb) exhibit enhanced activity in the oxidative coupling reaction. This study also indicates that the combination of biocatalysis and chemical synthesis avoids the need for the separation of intermediate products, which offers a convenient approach for the total synthesis of the biological compound CFZ. Engineered myoglobins (Mbs), such as F43Y/T67R Mb, were applied to catalyze the oxidative coupling of N-4-CPBDA to produce N-5-CCPIPA in the presence of H2O2, which was further combined with chemical synthesis for the total synthesis of CFZ.
期刊：
CLINICAL AND EXPERIMENTAL MEDICINE,2023年23(7):3113-3124 ISSN：1591-8890
通讯作者：
She, MH
作者机构：
[Zeng, Qun; Zhang, Jiawei; She, Meihua; She, MH] Univ South China, Hengyang Med Sch, Dept Biochem & Mol Biol, Changsheng West Rd 28, Hengyang 421001, Peoples R China.
通讯机构：
[She, MH ] U;Univ South China, Hengyang Med Sch, Dept Biochem & Mol Biol, Changsheng West Rd 28, Hengyang 421001, Peoples R China.
关键词：
Four and a half LIM protein 2 (FHL2);LIM-only protein family;Tumor progression;Cancer treatment;Signaling pathways
摘要：
LIM domain protein 2, also known as LIM protein FHL2, is a member of the LIM-only family. Due to its LIM domain protein characteristics, FHL2 is capable of interacting with various proteins and plays a crucial role in regulating gene expression, cell growth, and signal transduction in muscle and cardiac tissue. In recent years, mounting evidence has indicated that the FHLs protein family is closely associated with the development and occurrence of human tumors. On the one hand, FHL2 acts as a tumor suppressor by down-regulating in tumor tissue and effectively inhibiting tumor development by limiting cell proliferation. On the other hand, FHL2 serves as an oncoprotein by up-regulating in tumor tissue and binding to multiple transcription factors to suppress cell apoptosis, stimulate cell proliferation and migration, and promote tumor progression. Therefore, FHL2 is considered a double-edged sword in tumors with independent and complex functions. This article reviews the role of FHL2 in tumor occurrence and development, discusses FHL2 interaction with other proteins and transcription factors, and its involvement in multiple cell signaling pathways. Finally, the clinical significance of FHL2 as a potential target in tumor therapy is examined.
摘要：
This work describes the electrochemical selenylation of alkynyl aryl ketones, which shows high efficiency in the synthesis of 3‐selenylated chromones under transition‐metal‐free and chemical‐oxidant‐free conditions. This method features mild conditions, easy operation, and wide substrate scope. Abstract An electrochemical synthesis of various 3‐selenylated chromones via selenylation of alkynyl aryl ketones without the employment of catalyst and chemical‐oxidant is described here. This method features mild conditions, high efficiency, and wide substrate scope. Furthermore, the scale‐up reaction runs smoothly which indicates the practicability of this electrosynthesis strategy.
作者机构：
[Lei, Xia-Ping; Nie, Chang-Ming] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Wu, Qun-Yan; Chai, Zhi-Fang; Wang, Cong-Zhi; Lan, Jian-Hui; Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
通讯机构：
[Qun-Yan Wu; Wei-Qun Shi] L;[Chang-Ming Nie] S;Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
摘要：
Graphene quantum dots are the latest addition to the low-dimensional nanomaterial family, which have drawn growing attention due to their unique physiochemical properties and potential applications in many fields. However, their practical application is hindered by the high fabrication cost and environmental concerns regarding unsustainable carbon sources and routes. This work demonstrates a universal approach to fabricate various heteroatom(s) doped lignin-derived graphene quantum dots (LGQDs) for utilization in the photoelectrochemical-type photodetectors (PDs). The results indicate that LGQDs are endowed with relatively dopant-rich chemical states and tailorable broadband photoluminescence. Based on these advantages, these novel LGQDs-based PDs present obvious and fast photo-response within the visible region, as well as good long-term stability in the mild neutral environment, suggesting their great practical significance. It is believed that this work paves a new way for developing PDs based on the photochemically active species from sustainable and cheap biomass-derived lignin.
通讯机构：
[Zeng, F.] C;[Wang, X.] S;College of Chemical and Biological Engineering, Hunan, China;School of Chemistry and Chemical Engineering, Hunan, China
通讯机构：
[Mingfei Shao; Mingfei Shao Mingfei Shao Mingfei Shao] S;State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100029 China
关键词：
chemical confinement;dendrite-free;liquid anode;NaK alloy;single-atom
摘要：
The design and tailoring of the cathode material for a supercapacitor are of enormous importance in achieving its high performance. A composite cathode material, composed of 2D BP coated on a 3D CoPBA, has been systematically developed and created through self-assembly using electrostatic adsorption. The structure and components of the CoPBA/BP composites were studied and analyzed using XRD, XPS, SEM, and TEM. The 2D BP wrappers can serve as conductive additives, facilitating charge transport and enhancing the electrochemical performance. The morphologies and electrochemical performances of CoPBA/BP were systematically investigated with increasing BP content. CoPBA-6BP is found to have a maximum specific capacitance of 755F/g at 1 A/ g, which is 2.6 times greater than pure CoPBA. This makes the 2D/3D structured composite a strong candidate for cathode material applications.
摘要：
To improve the recognition ability and the controlled release of andrographolide (ADR), it is necessary to prepare a better intelligent drug delivery carrier. In this paper, the magnetic andrographolide imprinted polymer (ADR-MMIP) with pH/redox/light triple stimulus response was successfully prepared by reverse atom transfer radical polymerization (RATRP), where ADR was as the template, beta-Cyclodextrin (beta-CD) and 4-amino-4 '-meth-acrylamide azobenzene (AMAB) as the bi-functional monomers, and both of N, N '-bis (acryloyl) cystamine (BAC) and ethylene glycol dimethacrylate (EGDMA) as cross-linkers. A series of adsorption experiments indicated that ADR-MMIP had excellent adsorption and selectivity capacities with the maximum adsorption capacity 41.43 mg g-1 and the factors alpha 4.256 and beta 1.940 for the selectivity and relative selectivity, respectively. The adsorption mechanism of ADR-MMIP was investigated the multiphase adsorption with the chemical action on heteroge-neous material surface by the linear fitting with the isothermal and kinetic adsorption models, and the in-vitro ADR release showed ADR-MMIP was sensitive to the triple-stimuli of pH/redox/light with the maximum cu-mulative drug release rate 91.53% when the above three conditions were applied concurrently. The above in-formation demonstrated the ADR-MMIP should be of great application potential in the ADR extraction and isolation from mixture and the intelligent drug delivery system.
作者机构：
[Lu, Yu-Han] Univ South China, Hengyang Med Sch, Hengyang 421001, Peoples R China.;[Wu, Chao; Zhou, Min-Hang; Hou, Jia-Cheng; Wu, Zhi-Lin; He, Wei-Min; Huang, Xiao-Jun; He, WM] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[He, WM ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
关键词：
semiheterogeneous;polycrystalline metal chalcogenide;ferrocene;redox catalyst;cascade reaction
摘要：
A merger of heterogeneous polycrystalline WSe2 semiconductor photocatalysis and homogeneous ferrocene redox catalysis for the cascade radical coupling-annulation reactions was established. In the redox-mediated photocatalysis, ferrocene can improve the separation of photogenerated hole-electron pairs on WSe2 by consuming the hole via the formation of a ferrocene cation, which triggered the molecular transformations. Various benzo[e]imidazo[1,5-c][1,2,3]oxathiazine 5,5-dioxides were formed through semiheterogeneous three-component reaction of N-sulfonyl ketimines, N-arylglycines, and formaldehyde.
摘要：
This Review focuses on the very recent advances (from 2021 to the beginning of 2023) in the field of three‐component reactions of quinoxalin‐2(1H)‐ones at the C3 position. According to the kind of radical types involved, some representative examples and detailed reaction mechanism have been categorized and discussed. Abstract The multicomponent reactions of quinoxalin‐2(1H)‐ones has attracted considerable interest due to their significant biological and chemical activities. The very recent advances (from 2021 to the beginning of 2023) on the radical three‐component cascade reaction of quinoxalin‐2(1H)‐one derivatives at the C3 position were summarized in this mini‐review. According to the kind of radical types involved, some representative examples and detailed reaction mechanism have been categorized and discussed. The red front was covered by Figure 1.
摘要：
For uranium adsorption in water, a new uranium adsorbent was synthesized by preparing poly(tetraethylenepentamine-trimesoyl chloride). The samples were characterized using SEM, EDS, TGA, FTIR and XPS. The removal ability and adsorption mechanism of uranium (VI) in an aqueous solution by poly(tetraethylenepentamine-trimesoyl chloride) were systematically studied. The results showed that the adsorption equilibrium was completed within 80 min, the adsorption capacity reached 189.82 mg g(-1), and the removal rate reached 94.91%. The adsorption process fitted well with the pseudo-second-order model and the Langmuir isotherm model. The thermodynamic analysis indicated that the adsorption was an endothermic and spontaneous process. This study proved that poly(tetraethylenepentamine-trimesoyl chloride) could be considered a highly efficient and sustainable material for the removal of uranium (VI) from aqueous solutions.
摘要：
In this study, the potential applications of perfect boron carbide (BC3) nanosheet and single-vacancy defect BC3 nanosheets (SVBC3-B and SVBC3-C), as the drug delivery vehicle for 6-mercaptopurine (6-MP), are investigated based on the calculation of the density functional theory (DFT). The interactions of the 6-MP drug with the BC3 nanosheet, SVBC3-B and SVBC3-C are simulated in the gas phase, water solvent and acidic solvent, respectively. The results demonstrated that the 6-MP drug tends to adsorb parallel on the surface of the BC3 nanosheet, and the adsorption energy on SVBC3-B is the largest, followed by the perfect BC3. The interactions between the 6-MP drug and the perfect BC3 nanosheet, SVBC3-B and SVBC3-C will be weakened in a water solvent. Furthermore, the interaction force between the 6-MP drug and the perfect BC3 nanosheet or SVBC3-B nanosheet in an acidic solvent is more significant than that in a water solvent, which is not conducive to separating the 6-MP drug from the two kinds of BC3 nanosheets. But, the adsorption energy of the 6-MP drug on SVBC3-C in the acidic solvent is much lesser than that in the water solvent, which indicates that the 6-MP drug can be easily separated from SVBC3-C in the acidic environment. The PH value of cancer tissue is just acidic, which provides an ideal environment for separating 6-MP. Generally, the results confirmed the possibility of SVBC3-C as a delivery vehicle for the 6-MP drug.
期刊：
Journal of Membrane Science,2022年645:120186 ISSN：0376-7388
通讯作者：
Hong Wu<&wdkj&>Yawei Liu
作者机构：
[You, Xinda; Jiang, Zhongyi; Yang, Chao; Cao, Li; Wu, Hong; Wang, Xiaoyao; Kong, Yan; Fan, Chunyang] Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China.;[You, Xinda; Jiang, Zhongyi; Yang, Chao; Cao, Li; Wu, Hong; Wang, Xiaoyao; Kong, Yan; Fan, Chunyang] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China.;[Wu, Hong] Tianjin Univ, Tianjin Key Lab Membrane Sci & Desalinat Technol, Tianjin 300072, Peoples R China.;[Jiang, Zhongyi] Natl Univ Singapore, Joint Sch, Binhai New City 350207, Fujian, Peoples R China.;[Jiang, Zhongyi] Tianjin Univ, Int Campus, Binhai New City 350207, Fujian, Peoples R China.
通讯机构：
[Hong Wu] K;[Yawei Liu] B;Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China<&wdkj&>Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China<&wdkj&>Tianjin Key Laboratory of Membrane Science and Desalination Technology, Tianjin University, Tianjin, 300072, China<&wdkj&>Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
摘要：
Covalent organic frameworks (COFs) with long-range ordered, rigid, and tailor-made nanochannels hold great promise for energy-related applications. Here, we fabricate COF membranes with one-dimensional charged nanochannels using ionic COF nanosheets decorated with sulfonic acid groups. The free-standing and robust COF membrane exhibits enhanced proton conductivity and suppressed methanol permeability compared to the benchmark Nafion membrane. More interestingly, the methanol permeability of the COF membrane remains almost constant in a wide range of methanol concentrations (5.35 x 10(-7) cm(2) s(-1) for the 2 M methanol/water mixture and 5.44 x 10(-7) cm(2 & nbsp;& nbsp;)s(-1) for the neat methanol). All-atomistic dynamics simulations indicate that the diffusio-osmotic effect arising from the charged nanochannels can account for the low and nearly constant methanol permeability of the COF membranes. These findings suggest that the ionic COF membranes can find potential applications in direct methanol fuel cell with high methanol concentrations, and meanwhile shed light on the mass transport mechanism in the charged, rigid and ordered nanochannels.
通讯机构：
[Prof. Dr. Ying-Wu Lin] S;School of Chemistry and Chemical Engineering, University of South China, Hengyang, 421001 China<&wdkj&>Key Lab of Protein Structure and Function of Universities in Hunan Province, University of South China, Hengyang, 421001 China
摘要：
A double mutant of human H64M/V71C neuroglobin (Ngb) was engineered, which formed a single thioether bond as that in atypical cytochrome c, whereas the heme distal Met64 was oxidized to both sulfoxide (SO-Met) and sulfone (SO2-Met). By contrast, no Cys-heme cross-link was formed in V71C Ngb with His64/His96 coordination, as shown by the X-ray crystal structure, which indicates that an open distal site facilitates the activation of heme iron for structural modifications.
摘要：
Tetracyclines are one class of widely used antibiotics. Meanwhile, due to abuse and improper disposal, they are often detected in wastewater, which causes a series of environmental problems and poses a threat to human health and safety. As an efficient and environmentally friendly method, enzymatic catalysis has attracted much attention. In previous studies, we have designed an efficient peroxidase (F43Y/P88W/F138W Mb, termed YWW Mb) based on the protein scaffold of myoglobin (Mb), an O-2 carrier, by modifying the heme active center and introducing two Trp residues. In this study, we further applied it to degrade the tetracycline antibiotics. Both UV-Vis and HPLC studies showed that the triple mutant YWW Mb was able to catalyze the degradation of tetracycline, oxytetracycline, doxycycline, and chlortetracycline effectively, with a degradation rate of similar to 100%, similar to 98%, similar to 94%, and similar to 90%, respectively, within 5 min by using H2O2 as an oxidant. These activities are much higher than those of wild-type Mb and other heme enzymes such as manganese peroxidase. As further analyzed by UPLC-ESI-MS, we identified multiple degradation products and thus proposed possible degradation mechanisms. In addition, the toxicity of the products was analyzed by using in vitro antibacterial experiments of E. coli. Therefore, this study indicates that the engineered heme enzyme has potential applications for environmental remediation by degradation of tetracycline antibiotics.
