Green Synthesis and Catalysis
·
2025
·
IF 6.3
Mengqian Song,Yu Li,Jinhui Feng,Shuhong Mao,Peiyuan Yao,Qiaqing Wu,Dunming Zhu
Chiral β-amino alcohols represent a significant structural motif in many biologically active molecules. Developing an efficient biocatalytic method for synthesizing chiral β-amino alcohols with structural diversity is highly desirable. In this study, enzymatic hydroxymethylation of aryl-aliphatic aldehydes by benzaldehyde lyases (BALs) enabled the synthesis of α-hydroxymethyl ketones at high substrate loadings (200 mmol/L - 300 mmol/L). And the reductive amination of diverse α-hydroxymethyl ketones by amine dehydrogenases (AmDHs) was conducted for synthesizing chiral β-amino alcohols in high isolated yields (60 %-79 %). Furthermore, a one-pot, two-step enzymatic process involving BAL-catalyzed hydroxymethylation of aldehydes and subsequent AmDH-catalyzed reductive amination was developed, enabling the synthesis of aromatic, aliphatic and aryl-aliphatic ( S )-β-amino alcohols from corresponding aldehydes in good to excellent isolated yields (56 %-96 %) and excellent enantioselectivity (>99 % ee ). The practical utility of this methodology was further demonstrated through the synthesis of key intermediates for antiviral drug Telaprevir or ATP competitive ERK inhibitor BVD-523.
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高影响因子
ACS Nano
·
2023
·
IF 17.1
Huiyi Liang,Yibo Du,Chenxu Zhu,Zhaoqiang Zhang,Guiqing Liao,Lixin Liu,Yongming Chen
Cancer metastasis that is resistant to conventional therapies has become a major cause of patient death. Recent reports indicate that the neutrophil extracellular trap (NET) is closely associated with cancer distant metastases, and the cell-free DNA of NETs has been identified as the ligand of the transmembrane protein CCDC25 of cancer cells, acting as a chemokine to induce cancer cell migration to distant organs. In this work, we present the poly(aspartic acid) based-cationic materials to interfere with the interaction between NET-DNA and CCDC25, and furthermore to inhibit NET-DNA-mediated cancer cell chemotaxis and migration. Because of a stronger binding affinity to DNA and favorable retention in the liver, nanoparticulate poly(aspartic acid) derivatives (cANP) efficiently reduce the level of hepatic NET-DNA infiltration, leading to a significant suppression of cancer metastases in mice and several human metastatic models. Moreover, the cANP exhibits no toxicity to organs of animals during the entire treatment. Thus, this work suggests a strategy for controlling cancer metastases, which will benefit patients in clinics.
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PubMed
高影响因子
PEST MANAGEMENT SCIENCE
·
2025
·
IF 3.8
Juncheng Wu,Zhengyuan Tao,Jingyi Cao,Wei Hu,Minghao Jiang,Yahui Li,Haiqun Cao,Min Liao,Ning Zhao
BACKGROUND Rice flatsedge ( Cyperus iria L.) is one of the most troublesome weeds infesting rice fields across China. Bensulfuron-methyl, an acetolactate synthase (ALS)-inhibiting herbicide, has been widely used for the control of Cyperaceae weeds in rice production. However, long-term and extensive use of this herbicide has resulted in the evolution of resistant C. iria populations. In this study, a suspected bensulfuron-methyl-resistant (R) population collected from a rice field that survived field-recommended applications was investigated to elucidate its resistance level and underlying mechanism. RESULTS Compared with a susceptible (S) population, the R population exhibited a high level of resistance to bensulfuron-methyl [resistance index (RI) = 12.88] and cross-resistance to metazosulfuron (RI = 11.66), bispyribac-sodium (RI = 9.10) and penoxsulam (RI = 6.35). No mutations were detected in the ALS gene, and ALS expression levels did not differ significantly between the R and S plants. Pretreatment with the cytochrome P450 inhibitor malathion and the glutathione S -transferase inhibitor 4-chloro-7-nitrobenzoxadiazole effectively reversed bensulfuron-methyl resistance in R plants. Liquid chromatography tandem mass spectrometry analysis showed that the R plants metabolized bensulfuron-methyl significantly faster than the S plants. RNA sequenccing analysis revealed remarkable upregulation of CYP97A3 and GSTF1 in the R population, while molecular docking indicated strong binding affinities between both enzymes and bensulfuron-methyl at their active sites. CONCLUSION These results reveal that enhanced expression of CYP97A3 and GSTF1 may contribute to bensulfuron-methyl resistance in C. iria , highlighting the role of metabolic detoxification in the evolution of non-target-site resistance in this species. © 2025 Society of Chemical Industry.
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2025
·Vol. 27
·期 1
·434
·
IF 4.9
Mingyuan Zhang,Jinru Wang,Caihan Zhu,Yuning Zhang,Dewei Li,Shuozhen Hu
Developing efficient and durable oxygen reduction reaction (ORR) catalysts is crucial for advancing fuel cell technology and sustainable energy conversion. In this study, a scalable strategy was employed to synthesize ZIF-derived nitrogen-sulfur co-doped carbon nanosheets embedded with in situ generated ZnS and Co9S8nanoparticles. The synergistic effect of heteroatom doping and metal sulfide modification effectively modulated the electronic structure, optimized charge transfer pathways, and enhanced structural stability. The optimized catalyst exhibited a half-wave potential of 0.83 V vs. RHE, close to that of commercial 20 wt% Pt/C (0.85 V), excellent 4e−ORR selectivity, and exceptional stability, with only a ~15 mV degradation after 10,000 cycles. These results demonstrate that the combination of nitrogen sulfur co-doping and in situ metal sulfide addition pro-vides an effective approach for designing highly active and durable non-precious metal catalysts for the ORR. This synthetic concept provides practical guidance for the scalable preparation of multifunctional nanomaterial-based catalysts for electrochemical energy applications.
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DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Jianwen Feng,Huan Yi,Zhiwen Lei,Jun Wang,Hongbo Zeng,Yonghong Deng,Chaoyang Wang
Poor cycling performance caused by the shuttle effect of polysulfides is the main obstacle in the development of advanced lithium–sulfur (Li–S) batteries. Functional polymer binders with polar groups can effectively adsorb polysulfides chemically, thereby suppressing the shuttle effect. Herein, a robust three-dimensional crosslinked polymer network, which demonstrates excellent mechanical property and strong affinity for polysulfides , is prepared by the aldimine condensation and coordination reactions. The crosslinked chitosan sulfate network (CCSN) significantly enhances the cycling performance and rate capability of the sulfur cathode. The CCSN-based sulfur cathode exhibits a high initial discharge capacity of 824 mAh g −1 with only 0.082% average capacity loss per cycle at 1 C. At a high rate of 4 C, the cathode exhibits a high capacity retention of 84.8% after 300 cycles. Moreover, the CCSN-based sulfur cathode exhibits an excellent cycling performance at a high sulfur loading of 2.5 mg cm −2 , which indicates the excellent mechanical strength and binding performance of the CCSN binder for high-energy density Li–S batteries. This study demonstrates a viable approach for developing high-performance Li–S batteries for practical application.
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高影响因子
Science Bulletin
·
2020
·
IF 9.511
Linbao Guo,Jiangjian Shi,Qing Yu,Biwen Duan,Xiao Xu,Jiazheng Zhou,Jionghua Wu,Yusheng Li,Dongmei Li,Huijue Wu,Yanhong Luo,Qingbo Meng
Aqueous precursors provide an alluring approach for low-cost and environmentally friendly production of earth-abundant Cu 2 ZnSn(S, Se) 4 (CZTSSe) solar cells. The key is to find an appropriate molecular agent to prepare a stable solution and optimize the coordination structure to facilitate the subsequent crystallization process . Herein, we introduce thioglycolic acid (TGA), which possesses strong coordination (SH) and hydrophilic (COOH) groups, as the agent and use deprotonation to regulate the coordination competition within the aqueous solution. Ultimately, metal cations are adequately coordinated with thiolate anions , and carboxylate anions are released to become hydrated to form an ultrastable aqueous solution. These factors have contributed to achieving CZTSSe solar cells with an efficiency as high as 12.3% (a certified efficiency of 12.0%) and providing an extremely wide time window for precursor storage and usage. This work represents significant progress in the non-toxic solution fabrication of CZTSSe solar cells and holds great potential for the development of CZTSSe and other metal sulfide solar cells.
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高影响因子
ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2020
·
IF 3.023
Hong-Yi Wang,Jia-Wei Tang,Peng Peng,Hai-Jun Yan,Fu-Li Zhang,Shao-Xin Chen
We first developed a novel and efficient chemoenzymatic process to prepare (S)-1-(pyridin-4-yl)-1,3-propanediol, a vital HepDirect prodrug intermediate, from inexpensive and commercially available isonicotinic acid. Through this process, we provide a creative way to obtain the key chiral intermediate, β-hydroxyester, with ketoreductase (KRED) EA. After optimization of the process, we performed the reaction on a 100 g scale with a substrate concentration of up to 150 g/L, a yield of 93%, and an ee value of up to 99.9%. Additionally, we used a simple and effective NaBH4/MgCl2 reduction system to obtain (S)-1-(pyridin-4-yl)-1,3-propanediol with >99.9% ee and an 80% yield. This novel chemoenzymatic process has the potential to be a cost-effective and environmentally friendly process suitable for industrial use.
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高影响因子
Water Cycle
·
2023
·
IF 0
Jiaolong Zhang,Shuting Gou,Zhe Yang,Chaolin Li,Wenhui Wang
The application of promising g-C 3 N 4 has been limited by poor photogenerated electron-hole separation and limited absorption for visible light. Sulfamethoxazole (SMX) is a typical antibiotic drug that is used worldwide and hard to be disposed through conventional wastewater treatment methods. Herein, S-scheme Fe 2 O 3 /g-C 3 N 4 heterojunction was successfully prepared via a facile one-step sintering method and applied to photodegrade SMX under visible light irradiation. The integration of Fe 2 O 3 and g-C 3 N 4 shows superior charge separation and light absorption ability. As a result, the removal efficiency of 11 wt% Fe 2 O 3 /g-C 3 N 4 reaches to 99.2% within 30 min, which is visibly higher than 59.5% of pure g-C 3 N 4 . ·O 2 − and ·OH are demonstrated to be the predominant active species for SMX photodegradation, and the possible degradation pathway is also proposed based on electronic band structure of Fe 2 O 3 /g-C 3 N 4 heterojunction. This study presents a facile construction of g-C 3 N 4 based S-scheme photocatalyst and offers an environmentally friendly approach to effectively remove organic pollutants using renewable solar energy.
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Functional Materials Letters
·
2024
·
IF 1.2
Kangjun Geng,Zhengdong Feng,Tingyu Zhang,Shan Huang,Honcheng Zhu,Bangzhi Shen,Boning Dong,Yan Yan,Sai Jiang,Jianhua Qiu,Huafei Guo
Antimony Selenide (Sb 2 Se 3 ) exhibits potential as a solar energy material owing to its optimal bandgap, lack of toxicity, and abundance of earth abundant elements. Currently, cadmium sulfide (CdS) serves as the predominant buffer layer for Sb 2 Se 3 solar cells. However, the use of CdS hinders environmentally friendly advancement due to the toxic properties of the element cadmium. Hence, the quest for non-toxic buffer layers poses a significant challenge to the further advancement of Sb 2 Se 3 solar cells. In prior research, tin oxide (SnO 2 ) has been explored as a buffer layer. Nonetheless, the efficiency of SnO 2 /Sb 2 Se 3 solar cells was hampered by the rough surface of SnO 2 films and the poor crystallinity of Sb 2 Se 3 films. In this investigation, we enhanced device efficiency by improving the uniformity of the SnO 2 surface and enhancing the crystallinity of Sb 2 Se 3 through spin-coating sulfur (S) onto the SnO 2 film. Detailed examinations were conducted on the structure, optical, and electrical properties of the respective SnO 2 and Sb 2 Se 3 thin films. Ultimately, an efficiency of 3.38% was achieved using the spin-coated S:SnO 2 film, marking an 85% enhancement compared to the baseline device.
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高影响因子
CELLULOSE
·
2017
·Vol. 24
·期 10
·4189-4203
·
IF 3.417
Zhang Xiuqiang,Zhang Jinlong,Dong Lili,Ren Suxia,Wu Qinglin,Lei Tingzhou
We report a series of thermoresponsive cellulose nanocrystals (CNCs) decorated with poly(poly(ethylene glycol) methylacrylate) copolymers (poly(PEGMA)- g -CNCs) synthesized by surface initiated-atom transfer radical polymerization (SI-ATRP). The chemical structures and surface morphologies were subsequently confirmed by FT-IR, XPS, and AFM measurements. With regard to thermally responsive behavior, poly(PEGMA)- g -CNCs show tunable lower critical solution temperature (LCST) values in the range of 34–66 °C by varying the feeding ratios of comonomers. The reversible morphological transformation from individual nano-rod structures to larger globule aggregates was further verified by AFM during the LCST transition. These functionalized CNCs have potential as smart film filters and biosensors.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 34
·18477-18487
·
IF 12.732
Menghua Yang,Xuewei Wang,Jinfeng Wu,Yue Tian,Xingyu Huang,Ping Liu,Xianyang Li,Xinru Li,Xiaoyan Liu,Hexing Li
Lithium sulfur (Li–S) batteries have been investigated as ideal candidates for future high-density energy storage systems with the advantages of abundant reserves, high energy density and competitive cost. The key issues are the severe shuttling of polysulfides and sluggish redox kinetics. Herein, we report a novel metal–organic framework-derived Co2P–ZnS/ZnS–C nanocomposite constructed from inner Co2P–ZnS and outer ZnS–C heterostructures. Both the experimental results and theoretical calculations demonstrated that these dual electrocatalytic heterostructures enabled strong affinity with polysulfides and facilitated the reaction kinetics. Meanwhile, the hollow carbon polyhedron provided fast electron/ion transfer channels and effectively buffered volume expansion during cycling. As anticipated, a high initial capacity of 1503 mA h g−1 was achieved at 0.2C with Co–Zn/Zn–C/S as a cathode, together with excellent stability after 500 cycles at 1C. Even a high reversible capacity of 540 mA h g−1 was achieved at 1C after 200 cycles under an elevated sulfur loading of 3.65 mg cm−2. This work presents a new strategy for designing dual electrocatalytic hosts for immobilization and conversion of polysulfides, which may offer more opportunities as cathodes in stable Li–S batteries with high energy density.
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高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 4
·655
·
IF 5.719
Wenjing Yu,Bo Liu,Xiaojiao Zhao
To develop high-performance microwave absorption materials with the features of lightweight, thin thickness, broad bandwidth, and strong absorption, an ultralight Ni3S2@N, S-codoped graphene aerogel with a density of 13.5 mg/cm3has been fabricated by the use of metal-organic frameworks (MOFs) to directly initiate the gelation of graphene oxide strategy. In such a strategy, dual-functional 1D Ni-MOF nanorods not only act as the gelation agent but also afford the doping elements (N and S) originated from the organic species and the precursor for metal sulfide. Due to the synergistic effects of good impedance matching and multiple losses, the optimal reflection loss (RL) of as-prepared Ni3S2@N, S-codoped graphene aerogel reaches −46.9 dB at 17.1 GHz with only 2.0 mm and ultralow filling content (1.75 wt%). The maximum effective absorption bandwidth (EAB) reaches 6.3 GHz (11.7–18.0 GHz) at 2.38 mm, covering the whole Ku band. Moreover, the value of EAB with the RL less than −30 dB can be tuned to 12.2 GHz (5.8–18 GHz) at the absorber thickness ranging from 1.9 to 5.0 mm. This work provides insight for rational design and fabrication of multicomponent-containing graphene aerogels, showing the potential application in lightweight and high-performance microwave absorption.
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高影响因子
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