作者机构:
[Zhao, Wei; Fu, Chao; Hu, Rong; Hu, R; Yin, Yuli; Yin, YL] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Tang, Ben Zhong] Chinese Univ Hong Kong, Shenzhen Inst Aggregate Sci & Technol, Sch Sci & Engn, Shenzhen CUHK Shenzhen, Shenzhen 518172, Guangdong, Peoples R China.;[Yan, Caihong] Univ South China, Affiliated Hosp 2, Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.;[Zhou, Yizhao] Hunan Normal Univ, Hunan Prov Peoples Hosp, Affiliated Hosp 1, Dept Orthoped, Changsha 410005, Peoples R China.;[Gao, Hanyi] Univ South China, Affiliated Hosp 7, Hunan Prov Vet Adm Hosp, Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.
通讯机构:
[Tang, BZ ] C;[Hu, R ; Yin, YL] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Chinese Univ Hong Kong, Shenzhen Inst Aggregate Sci & Technol, Sch Sci & Engn, Shenzhen CUHK Shenzhen, Shenzhen 518172, Guangdong, Peoples R China.
摘要:
Ultrasound-triggered sonodynamic therapy (SDT) presents growing promise in deep-seated or unresectable tumor inhibition because of the perfect tissue penetration ability. However, its therapeutic efficacy is always restricted by the limited reactive oxygen species (ROS) generation ability of sonosensitizers. In this work, based on molecular engineering, we have fabricated aggregation-induced emission (AIE)-active organic sonosensitizers bearing efficient ROS generation with US irradiation for tumor treatment. By enhancing the intramolecular charge transfer strength and intermolecular interaction, an organic sonosensitizer with reduced energy gap and AIE features was developed, presenting enhanced oxygen sensitization behavior to produce ROS upon an ultrasound trigger compared to Ce 6. Moreover, the excellent mitochondrial enrichment of the obtained sonosensitizer enables effective tumor cell eradication via apoptotic and ferroptosis pathways with ultrasound irradiation. The efficient in vivo tumor inhibition was also achieved based on the SDT approach. Therefore, this work provided a generalized and promising strategy for deep-seated or unresectable tumor treatment in the clinic. An organic sonosensitizer bearing a low-energy gap and aggregation-induced emission features was constructed for efficient tumor therapy based on ultrasound irradiation triggered-ROS generation.
期刊:
International Journal of Molecular Sciences,2023年24(3) ISSN:1422-0067
通讯作者:
Jiakun Xu<&wdkj&>Osami Shoji
作者机构:
[Li, Yanqing] Shanghai Ocean Univ, Coll Food Sci & Technol, Shanghai 201306, Peoples R China.;[Li, Yanqing; Wang, Fang; Wang, Jinghan; Xu, Jiakun] Chinese Acad Fishery Sci, Yellow Sea Fisheries Res Inst, Key Lab Sustainable Dev Polar Fisheries, Lab Marine Drugs & Byprod,Minist Agr & Rural Affai, Qingdao 266071, Peoples R China.;[Lin, Yingwu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Wang, Jinghan] Ocean Univ China, Coll Food Sci & Engn, Qingdao 266003, Peoples R China.;[Shoji, Osami] Nagoya Univ, Grad Sch Sci, Dept Chem, Furo Cho,Chikusa Ku, Nagoya 4648602, Japan.
通讯机构:
[Jiakun Xu] K;[Osami Shoji] D;Department of Chemistry, Graduate School of Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8602, Japan<&wdkj&>Key Lab of Sustainable Development of Polar Fisheries, Ministry of Agriculture and Rural Affairs, Yellow Sea Fisheries Research Institute, Chinese Academy of Fishery Sciences, Lab for Marine Drugs and Byproducts of Pilot National Lab for Marine Science and Technology, Qingdao 266071, China
关键词:
cytochromes P450BM3;dual-functional small molecule co-catalysis;hydroxylated indole;indigo;directed evolution
摘要:
With the increasing demand for blue dyes, it is of vital importance to develop a green and efficient biocatalyst to produce indigo. This study constructed a hydrogen peroxide-dependent catalytic system for the direct conversion of indole to indigo using P450BM3 with the assistance of dual-functional small molecules (DFSM). The arrangements of amino acids at 78, 87, and 268 positions influenced the catalytic activity. F87G/T268V mutant gave the highest catalytic activity with k(cat) of 1402 min(-1) and with a yield of 73%. F87A/T268V mutant was found to produce the indigo product with chemoselectivity as high as 80%. Moreover, F87G/T268A mutant was found to efficiently catalyze indole oxidation with higher activity (k(cat)/K-m = 1388 mM(-1) min(-1)) than other enzymes, such as the NADPH-dependent P450BM3 (2.4-fold), the Ngb (32-fold) and the Mb (117-fold). Computer simulation results indicate that the arrangements of amino acid residues in the active site can significantly affect the catalytic activity of the protein. The DFSM-facilitated P450BM3 peroxygenase system provides an alternative, simple approach for a key step in the bioproduction of indigo.
摘要:
The development of novel hydrogels with high biocompatibility is a vital and active topic of study. Here, we used a facile polycondensation approach to develop multifunctional poly (ether sulfone) (PES)-based hydrogels with diverse functional groups (−SO3Na, −COONa, −OH, and − NH2), as indicated by flourier transformed infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). The chemical structure of the PES-based hydrogels could be modulated by monomer selection and post-treatment, resulting in a wide range of biomolecule-mimic structures and matching biological functions. In the current investigation, heparin-mimic PES-based hydrogels demonstrated good hemocompatibility, as evident by reduced platelet adhesion and activation, delayed clotting times, suppressed blood-related complement activations, and CD11b expression on leukocytes in the blood. Moreover, hyper-sulfonated PES-based hydrogels showed exceptional cytocompatibility with human umbilical vein endothelial cells (HUVECs) and considerable antiproliferative activity against human umbilical artery smooth muscle cells (HUASMCs), as revealed by cell proliferation and cytotoxicity assay findings. Finally, chitosan-mimic PES-based hydrogels had marked anti-microbial properties against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), as shown by the number of colonies. The aforementioned bio-functions were attributed to the formation of various chemical structures on the surfaces of PES-based hydrogels. The distinctive PES-based hydrogels synthesized in this work would be of high utility not only in the synthesis of biomedical hydrogels but also in the rational design of various types of biocompatible materials.
通讯机构:
[Wei-Min He] S;School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
摘要:
A simple and practical electron donor–acceptor (EDA) strategy to synthesize various 3-alkylated coumarins from easily available coumarins and naturally abundant carboxylic acids under photocatalyst-, oxidant-, and additive-free and mild conditions is reported. Using Na2S as the catalytic electron donor, a series of primary, secondary, and tertiary carbon radicals can be efficiently generated, and the EDA complex can be regenerated without an alkaline additive.
通讯机构:
[Chuan-Wan Wei; 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<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
摘要:
In this study, we have synthesized a facile tyrosine derivative based compound (2-QY), which can act both as a gelator and a reducing agent. 2-QY can assemble to form a functional metallohydrogel (2-QY-Au) in the presence of HAuCl4 under mild conditions (room temperature, aqueous solution, and simple sonication treatment). Au nanoparticles (Au NPs) can be in situ formed and dispersed uniformly in the gel system, which did not require an external reducing agent and a stabilizing agent. The obtained 2-QY-Au NP@metallohydrogel can be used as a catalyst to degrade a variety of dyes, such as methyl orange, methyl green, reactive black 5, reactive orange 16, and p-nitrophenol. In particular, it exhibits excellent catalytic activity towards degradation of methylene blue in the presence of NaBH4, with a k(app) value (13.23 +/- 0.21 s(-1)) higher than those of most of the reported catalysts in the literature. Moreover, 2-QY-Au NPs have good biocompatibility and exhibit antibacterial activity against E. coli and B. subtilis. Therefore, the 2-QY-Au NP@metallohydrogel could be used as an effective catalyst for the degradation of pollution containing organic dyes, as well as for potential applications in the biomedical field.
期刊:
Chemical Communications,2023年59(94):14029-14032 ISSN:1359-7345
通讯作者:
He, WM;Ou, LJ
作者机构:
[Wu, Chao; Zhou, Min-Hang; Hou, Jia-Cheng; Lu, Yu-Han; He, Wei-Min; Ji, Hong-Tao; Ouyang, Wen-Tao; Jiang, Jun; He, WM] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Ou, Li-Juan] Hunan Inst Technol, Sch Mat Sci & Engn, Hengyang 421002, Peoples R China.
通讯机构:
[Ou, LJ ] H;[He, WM ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Hunan Inst Technol, Sch Mat Sci & Engn, Hengyang 421002, Peoples R China.
摘要:
With both ferrocene and air as the redox catalysts, for the first time, the low-cost natural ilmenite (FeTiO3) was successfully used for photocatalytic bond formations. Under the assistance of a traceless H-bond, and HCHO as the methylene reagent, a variety of imidazo[1,5-a]quinoxalinones were semi-heterogeneously photosynthesized in high yields with good functional group compatibility.
摘要:
Here we report a strategy for the facile assembly of fused 3-trifluoromethyl-1,2,4-triazoles, which are difficult to synthesize using traditional strategies, in 50-96% yields through a triethylamine-promoted intermolecular [3 + 2] cycloaddition pathway. This protocol features high efficiency, good functional group tolerance, mild conditions, and easy operation. Furthermore, a gram-scale reaction and product derivatizations were carried out smoothly to illustrate the practicability of this method.
期刊:
The Journal of Organic Chemistry,2023年88(21):15282-15287 ISSN:0022-3263
通讯作者:
Wang, Huamin;Lin, YW
作者机构:
[Wang, Huamin; Niu, Wenjing; He, Yongjun; Wei, Yibo; Li, Xianxian; Lin, Ying-Wu; Wang, HM] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Lin, Ying-Wu] Univ South China, Hengyang Med Coll, Hengyang 421001, Peoples R China.;[Lin, Ying-Wu] Univ South China, Med Sch, Lab Prot Struct & Funct, 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, Med Sch, Lab Prot Struct & Funct, Hengyang 421001, Peoples R China.
摘要:
We report herein a general and effective system achieving cyclization of β-trifluoromethyl enones with amidines in the presence of 1,3-diiodo-5,5-dimethylhydantoin (DIH), which affords a range of trifluoromethylated 2-imidazolines in synthetically useful yields with good diastereoselectivities (up to 95% yield, up to 98:2 dr) and good functional group tolerance. Furthermore, the one-pot synthesis of trifluoromethylated imidazoles via sequential cyclization and oxidation is demonstrated. More significantly, the reaction mechanism was verified by ESI-MS studies of possible intermediates, and a reasonable reaction mechanism was proposed.
摘要:
Existing technologies used to detect monosodium urate (MSU) crystals for gout diagnosis are not ideal due to their low sensitivity and complexity of operation. The purpose of this study was to explore whether aggregation-induced emission luminogens (AIEgens) can be used for highly specific imaging of MSU crystals to assist in the diagnosis of gout. First, we developed a series of luminogens (i.e., tetraphenyl ethylene (TPE)-NH2, TPE-2NH2, TPE-4NH2, TPE-COOH, TPE-2COOH, TPE-4COOH, and TPE-Ketoalkyne), each of which was then evenly mixed with MSU crystals. Next, optimal fluorescence imaging of each of the luminogens was characterized by a confocal laser scanning microscope (CLSM). This approach was used for imaging standard samples of MSU, hydroxyapatite (HAP) crystals, and mixed samples with 1:1 mass ratio of MSU/HAP. We also imaged samples from mouse models of acute gouty arthritis, HAP deposition disease, and comorbidities of interest. Subsequently, CLSM imaging results were compared with those of compensated polarized light microscopy, and we assessed the biosafety of TPE-Ketoalkyne in the RAW264.7 cell line. Finally, CLSM time series and three-dimensional imaging were performed on MSU crystal samples from human gouty synovial fluid and tophi. As a promising candidate for MSU crystal labeling, TPE-Ketoalkyne was found to detect MSU crystals accurately and rapidly in standard samples, animal samples, and human samples, and could precisely distinguish gout from HAP deposition disease. This work demonstrates that TPE-Ketoalkyne is suitable for highly specific and timely imaging of MSU crystals in gouty arthritis and may facilitate future research on MSU crystal-related diseases.
期刊:
Green Chemistry,2023年25(14):5539-5542 ISSN:1463-9262
通讯作者:
He, WM
作者机构:
[Li, Hong-Xia; Lu, Yu-Han; Mu, Si-Yu] Univ South China, Hengyang Med Sch, Hengyang 421001, Peoples R China.;[Wu, Chao; Zhou, Min-Hang; Lu, Yu-Han; He, Wei-Min; Ouyang, Wen-Tao; Jiang, 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.
摘要:
With formaldehyde as an atom-economical carbonyl synthon, the EtOH-catalyzed electrochemical multicomponent synthesis of various imidazolidine-fused sulfamidates was developed. A wide range of products were obtained in good to excellent yields under organic oxidant-free, energy-saving and mild conditions. The mechanistic study revealed that the in situ generated ethoxide played a crucial role in producing aminomethylene radicals at a lower voltage.
摘要:
The separation of thorium and uranium is an important guarantee for the fuel cycle of thorium-based molten salt reactors. Benzoxazole-based ligands have a wide range of applications and are also potential ligands for actinide separation. In this work, density functional theory (DFT) calculations were used to study the intrinsic properties of two ligands, 2,6-bis(benzo[d]oxazole-2-yl)pyridine (ligand a) and 1-(6-(4-acetylbenzo[d]oxazol-2-yl)pyridin2-yl)ethan-1-one (ligand b), revealing the structural characteristics and complexation behavior of their complexes with Th4+/UO5+. Quantum theory of atoms in molecules (QTAIM) and extended transition state - natural orbitals for chemical valence (ETS-NOCV) analyses show that the ligands form classical coordination bonds with Th4+/UO5+, with M- Noz bonds stronger than M- Npy bonds and partial electron acceptance by carbonyl O. The thermodynamic properties were used to evaluate the separation performance of these ligands for Th4+/UO5+ in four solvents (water, 1-hexanol, n-octanol and n-dodecane), with La more suitable for back extraction process and Lb having stronger binding with Th4+/UO5+. This work provides valuable theoretical insights into Th4+/UO5+ separation based on benzoxazole.
期刊:
International Journal of Biological Macromolecules,2023年253(Pt 4):127016 ISSN:0141-8130
通讯作者:
Liu, Jing-Jing;Lin, YW
作者机构:
[Liu, Jing-Jing; Lin, Ying-Wu; Liu, JJ; Wang, Zhan-Yi; Jiang, Bin-Bin] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Gao, Shu-Qin; Lin, Ying-Wu] Univ South China, Lab Prot Struct & Funct, Hengyang 421001, Peoples R China.;[Liu, Jing-Jing] Hunan Normal Univ, Key Lab Chem Biol & Tradit Chinese Med Res, Minist Educ, Changsha 410081, Hunan, Peoples R China.
通讯机构:
[Lin, YW ; Liu, JJ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
关键词:
Human myoglobin;Glycation sites;Thymoquinone
摘要:
Nonenzymatic glycation and the subsequent accumulation of advanced glycation end-products (AGEs) in proteins are factors underlying long-term pathogenesis in diabetes. The study of protein glycation is crucial for elucidating their relationship with diabetes mellitus and related disorders. This study explores the interaction between d-ribose and human myoglobin (HMb), as well as the protective effect of thymoquinone (TQ) on glycation. A time-dependent in-vitro glycation study was performed to investigate the mechanism of d-ribose-induced structural interference of HMb in the absence and presence of TQ. Spectroscopic and proteomic analysis indicated that the presence of TQ significantly reduced the total amount of AGEs while maintaining structural characteristics of HMb. 14 glycated sites on HMb were further identified via liquid chromatography-tandem mass spectrometry (LC-MS/MS) after incubation with d-ribose for 12h, predominantly interacting with lysine residues. TQ was found to disrupt this interaction, reducing the glycated sites from 14 to 12 sites and the percentage of glycated peptides from 26.50% to 12.97%. Additionally, there was a significant decrease in the degree of glycation at the same sites. In summary, our findings suggest that TQ has the potential to act as an anti-glycation agent and provide a comprehensive understanding underlying the inhibition mechanism of glycation.
通讯机构:
[Wei, CW; Lin, YW ] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Key Lab Prot Struct & Funct Univ Hunan Prov, Hengyang 421001, Peoples R China.
摘要:
The construction of smart materials, especially white light emitting (WLE) hydrogels with multi-stimuli responsive properties, has received widespread attention from researchers. In this study, a WLE hydrogel was obtained by the in situ doping of Eu3+ and Tb3+ into a blue emission low molecular weight gelator (MPF). Remarkably, the prepared WLE hydrogel possessed excellent stimuli responsiveness to pH, temperature and chemicals, and could be used as a soft thermometer and a selective sensor for Cu2+. The correlated color temperature of the WLE hydrogel was calculated to be 5063 K, suggesting a potential application in cool white light. Moreover, a series of metallohydrogels with different colors were obtained by modulating the ratio of MPF, Eu3+ and Tb3+ or changing the excitation wavelength, which was an excellent candidate to construct soft materials of a full-color system. Additionally, the WLE hydrogel could be used for constructing anti-counterfeiting materials. Therefore, this study provides a new approach for preparing smart WLE hydrogels with multiple functions.
通讯机构:
[Tao Gong; HongQing Wang] C;College of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
关键词:
wearable electronics;MXene;adhesive hydrogels;conductive nanocomposites;pressure and strain sensors
摘要:
To address the shortcomings of traditional filler-based wearable hydrogels, a new type of nanochannel hydrogel sensor is fabricated in this work through a combination of the unique structure of electrospun fiber textile and the properties of a double network hydrogel. Unlike the traditional Ti3C2Tx MXene-based hydrogels, the continuously distributed Ti3C2Tx MXene in the nanochannels of the hydrogel forms a tightly interconnected structure similar to the neuron network. As a result, they have more free space to flip and perform micromovements, which allows one to significantly increase the electrical conductivity and sensitivity of the hydrogel. According to the findings, the Ti3C2Tx MXene nanochannel hydrogel has excellent mechanical properties as well as self-adhesion and antifreezing characteristics. The hydrogel sensor successfully detects different human motions and physiological signals (e.g., low pulse signals) with high stability and sensitivity. Therefore, the proposed Ti3C2Tx MXene-based hydrogel with a unique structure and properties is very promising in the field of flexible wearable devices.
期刊:
RSC Chemical Biology,2023年4(5):330-333 ISSN:2633-0679
通讯作者:
Ying-Wu Lin
作者机构:
[Dai, Wei; Wang, Xiao-Juan] School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China;[Yuan, Hong; Tan, Xiangshi] Department of Chemistry & Institute of Biomedical Science, Fudan University, Shanghai 200433, China;[Gao, Shu-Qin] Key Lab of Protein Structure and Function of Universities in Hunan Province, University of South China, Hengyang 421001, China;[Lin, Ying-Wu] 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
通讯机构:
[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:
Myoglobin (Mb) was found to undergo self-oxidation when a cysteine residue was engineered at position 67 in the heme distal site. Both the X-ray crystal structure and mass spectrum confirmed the formation of a sulfinic acid (Cys-SO(2)H). Moreover, the self-oxidation could be controlled during protein purification to yield the unmodified form (T67C Mb). Importantly, both T67C Mb and T67C Mb (Cys-SO(2)H) were able to be labeled by chemicals, which provided useful platforms to generate artificial proteins.