通讯机构:
[Zhang, CH ] S;[Wang, HL; Liu, CR ] C;Shanxi Univ, Sch Chem & Chem Engn, Taiyuan 030006, Peoples R China.;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
Abnormal lipid droplets (LDs) are known to be intimately bound with the occurrence and development of cancer, allowing LDs to be critical biomarkers for cancers. Aggregation-induced emission luminogens (AIEgens), with efficient reactive oxygen species (ROS) production performance, are prime photosensitizers (PSs) for photodynamic therapy (PDT) with imaging. Therefore, the development of dual-functional fluorescent probes with aggregation-induced emission (AIE) characteristics that enable both simultaneous LD monitoring and imaging-guided PDT is essential for concurrent cancer diagnosis and treatment. Herein, we reported the development of a novel LD-targeting fluorescent probe (TDTI) with AIE performance, which was expected to realize the integration of cancer diagnosis through LD visualization and cancer treatment via PDT. We demonstrated that TDTI, with typical AIE characteristics and excellent photostability, could target LDs with high specificity, which enables the dynamic tracking of LDs in living cells, specific imaging of LDs in zebrafish, and the differentiation of cancer cells from normal cells for cancer diagnosis. Meanwhile, TDTI exhibited fast ROS generation ability (achieving equilibrium within 60 s) under white light irradiation (10 mW/cm(2)). The cell apoptosis assay revealed that TDTI effectively induced growth inhibition and apoptosis of HeLa cells. Further, the results of PDT in vivo indicated that TDTI had a good antitumor effect on the tumor-bearing mice model. Collectively, these results highlight the potential utility of the dual-functional fluorescent probe TDTI in the integrated diagnosis and treatment of cancer.
摘要:
Picolinamide fungicides, structurally related to UK-2A and antimycin-A, bind into the Qi-site in the bc(1) complex. However, the detailed binding mode of picolinamide fungicides remains unknown. In the present study, antimycin-A and UK-2A were selected to study the binding mode of picolinamide inhibitors with four protonation states in the Qi-site by integrating molecular dynamics simulation, molecular docking, and molecular mechanics Generalized Born surface area (MM/GBSA) calculations. Subsequently, a series of new picolinamide derivatives were designed and synthesized to further understand the effects of substituents on the tail phenyl ring. The computational results indicated that the substituted aromatic rings in antimycin-A and UK-2A were the pharmacophore fragments and made the primary contribution when bound to a protein. Compound 9g-hydrolysis formed H-bonds with Hie201 and Ash228 and showed an IC(50) value of 6.05 ± 0.24 μM against the porcine bc(1) complex. Compound 9c, with a simpler chemical structure, showed higher control effects than florylpicoxamid against cucumber downy mildew and expanded the fungicidal spectrum of picolinamide fungicides. The structural and mechanistic insights obtained from the present study will provide a valuable clue for the future designing of new promising Qi-site inhibitors.
通讯机构:
[Li, DF ] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
摘要:
The research on electron transfer coupled spin transition regulating the valence state and spin state transition of metal ions is promising and challenging. Herein, we report a cyano-bridged {(Fe2Fe2II)-Fe-III} molecular square complex, {[Fe(Tp)(CN)(3)](2) [Fe(bnbpen)](2)}(ClO4)(2)<middle dot>8CH(3)OH (1<middle dot>8CH(3)OH, bnbpen = N,N '-bis-(2-naphthylmethyl)-N,N '-bis(2-picolayl)-ethylenediamine), and its free of solvents form (1). Combined single-crystal X-ray diffraction, temperature-dependent infrared (IR) spectra, magnetic measurements, and M & ouml;ssbauer spectra reveal that 1<middle dot>8CH(3)OH and 1 exhibit reversible one-step and two-step electron transfer coupled spin transition (ETCST) with temperature change, between the low-temperature state {Fe-II,Fe-LS(mu-CN)Fe-III,Fe-LS}(2) (LS = low spin, HS = high spin) and the high-temperature state {Fe-III,Fe-LS(mu-CN)Fe-II,Fe-HS}(2), respectively.
期刊:
Sensors and Actuators B-Chemical,2024年406:135432 ISSN:0925-4005
通讯作者:
Feng, GQ
作者机构:
[Zheng, Zhoupeng; Feng, Guoqiang; Feng, GQ; Zhang, Jinzheng; Liu, Yijia; Gong, Shenyi] Cent China Normal Univ, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
通讯机构:
[Feng, GQ ] C;Cent China Normal Univ, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
关键词:
Dual -channel fluorescent probe;Viscosity;Peroxynitrite;Mitochondria;Diabetes;In vivo imaging
摘要:
Diabetes is a common metabolic disease worldwide, which often has serious complications and seriously threatens human health. Abnormal viscosity and peroxynitrite (ONOO-) concentration are closely related to diabetes. Herein, we report a fluorescent dual response probe AO, which can simultaneously detect the changes of viscosity and ONOO- in diabetes at dual fluorescence channels. AO sensitively responds to viscosity and ONOO- with significant emission signal changes at 710 nm and 645 nm, respectively. Moreover, AO selectively targets mitochondria and generates a new compound when detecting ONOO-, which can spontaneously target and light up another type of organelle (lipid droplets), thus showing spatially separated dual -channel fluorescence signals. More notably, AO was successfully used to simultaneously detect the viscosity and ONOO- variations in hyperglycemic cells, diabetes and its complications (using mice models) for the first time, which may lead to a better understanding of the physiological and pathological phenomena of diabetes.
期刊:
JOURNAL OF ORGANIC CHEMISTRY,2024年89(6):3941-3953 ISSN:0022-3263
通讯作者:
Wang, JG;Wu, AX
作者机构:
[Wang, Jun-Gang; Ma, Lin-Lin] Guizhou Minzu Univ, Sch Chem Engn, Guiyang 550025, Guizhou, Peoples R China.;[Wang, Zheng-Hao; Tang, Yong-Xing; Wu, An-Xin; Zhou, You; Chen, Ting; Wu, Yan-Dong] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构:
[Wu, AX ] C;[Wang, JG ] G;Guizhou Minzu Univ, Sch Chem Engn, Guiyang 550025, Guizhou, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要:
An efficient synthetic method for constructing 2,3- and 2,4-disubstituted pyrimidio[1,2-b]indazole skeletons through I(2)-DMSO-mediated and substrate-controlled regioselective [4 + 2] cyclization is reported. The reaction conditions are mild, its operation is simple, and the substrate scope is wide. More than 60 pyrimidio[1,2-b]indazole derivatives have been synthesized, providing a new methodology for constructing related molecules and potentially enriching bioactive-molecule libraries.
作者机构:
[Lin, Jinying] Jilin Univ, Sch Stomatol, Dept Oral Implantol, Jilin Prov Key Lab Tooth Dev & Bone Remodeling, Changchun 130021, Peoples R China.;[Ding, Qihang] Korea Univ, Dept Chem, Seoul 02841, South Korea.;[Sun, Yao] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构:
[Sun, Y ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
期刊:
Sensors and Actuators B-Chemical,2024年405 ISSN:0925-4005
通讯作者:
Xu, Miao;Gu, WL;Ye, HR
作者机构:
[Xu, Weiqing; Chen, Yifeng; Zhu, Chengzhou; Xu, Miao; Sha, Meng; Zou, Chufan; Gu, Wenling; Chen, Guo] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Ye, Huarong; Ye, HR] China Resources & Wisco Gen Hosp, Wuhan 430080, Peoples R China.;[Zhu, Chengzhou] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Key Lab Organosilicon Chem & Mat Technol, Minist Educ, Hangzhou 311121, Peoples R China.;[Gu, Wenling] Hubei Univ, Sch Life Sci, State Key Lab Biocatalysis & Enzyme Engn, Wuhan 430062, Peoples R China.
通讯机构:
[Xu, M; Gu, WL ; Ye, HR ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;China Resources & Wisco Gen Hosp, Wuhan 430080, Peoples R China.;Hubei Univ, Sch Life Sci, State Key Lab Biocatalysis & Enzyme Engn, Wuhan 430062, Peoples R China.
摘要:
The fragility inherent in enzymes can be overcome by immobilizing them within nano-carriers, which offer designability and controllability and serve as a promising strategy for overcoming the inherent fragility of enzymes. While enzyme immobilization enhances enzyme stability and reusability, it can potentially hinder their bioactivity and catalytic efficiency. In this study, we present an enzyme-directed biomimetic mineralization approach for the in situ encapsulation of horseradish peroxidase (HRP) within hydrogen-bonded organic frameworks (HOFs) to obtain HOF@HRP nanocomposites. Remarkably, the HOF@HRP nanocomposites exhibit an ultrahigh protein content and demonstrate comparable catalytic activity to that of the free enzyme. Moreover, the HOFs act as protective shields, safeguarding the internal enzymes against various environmental disturbances. Leveraging the unique properties of HOF@HRP, we propose a dual-modal enzyme-linked immunosorbent assay for the sensitive detection of prostate-specific antigen in human serum. The resultant biosensor exhibits a good linear range, excellent sensitivity, and selectivity, showcasing its promising potential and clinical application in the field of diagnostic medicine.
摘要:
CsPbBr(3) has received more and more attention in the field of optoelectronic devices due to its excellent stability. To address the cost and environmental concerns associated with the use of toxic methanol, water has been explored as a substitute solvent for CsBr in the preparation of CsPbBr(3) perovskite solar cells (PSCs). In this study, we utilized methanol as an anti-solvent of the CsBr/H(2)O solution to regulate the detrimental effects of water on the CsPbBr(3) film and control the crystallization process. From results of the experiment, it was found that methanol anti-solvent treatment greatly improved the crystallization of the CsPbBr(3) film, increased the grain size, and reduced the defect density. After the introduction of methanol anti-solvent treatment, the power conversion efficiency (PCE) increased from 6.09% to 7.91%, while the open-circuit voltage (V(oc)) increased from 1.18 V to 1.39 V. Furthermore, we incorporated 2-hydroxyethylurea into the CsPbBr(3) PSCs to improve the wettability of PbBr(2) towards the CsBr/H(2)O solution and ensure the formation of pure-phase CsPbBr(3) films. The introduction of 2-hydroxyethylurea resulted in an additional increase in V(oc) from 1.19 V to 1.42 V. The PCE further improved from 6.56% to 8.62% after methanol anti-solvent treatment. These results demonstrate that methanol treatment effectively addresses the low V(oc) issue observed in CsPbBr(3) PSCs prepared with water as a solvent. Importantly, this approach significantly reduces the reliance on methanol compared to conventional fabrication methods for CsPbBr(3) PSCs. Overall, this work presents a promising pathway for achieving high V(oc) and efficiency in CsPbBr(3) PSCs by utilizing water as a solvent.
作者机构:
[Zhao, Xia; Gu, Wenxin; Sun, Tengteng; Qin, Jingwen] Tianjin Normal Univ, Tianjin Key Lab Struct & Performance Funct Mol, Key Lab Inorgan Organ Hybrid Funct Mat Chem, Minist Educ,Coll Chem, Tianjin 300387, Peoples R China.;[Ye, Fei] Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;[Lu, Kui] Tianjin Univ Sci & Technol, Coll Biotechnol, China Int Sci & Technol Cooperat Base Food Nutr Sa, Tianjin 300457, Peoples R China.
通讯机构:
[Zhao, X ] T;[Ye, F ] C;Tianjin Normal Univ, Tianjin Key Lab Struct & Performance Funct Mol, Key Lab Inorgan Organ Hybrid Funct Mat Chem, Minist Educ,Coll Chem, Tianjin 300387, Peoples R China.;Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.
摘要:
A copper-catalyzed thiocyanation of cycloketone oxime esters with ammonium thiocyanate has been developed for the first time. This innovative approach allows access to cyano and thiocyano bifunctionally substituted alkanes, which can be further transformed into their respective trifluoromethylthiol-substituted or difluoromethylthiol-substituted alkylnitriles, alkynyl sulfides, and phosphorothioate esters. The readily available nature of ammonium thiocyanate and the cost-effectiveness of the copper catalyst make this method a promising strategy for the synthesis of sulfur-containing alkylnitriles.
期刊:
CHEMISTRY-A EUROPEAN JOURNAL,2024年30(18):e202303742 ISSN:0947-6539
通讯作者:
Li, HB
作者机构:
[Chen, Chunxiu; Li, Guang; Xu, Weiwei; Cai, Meng; Li, Haibing; Ma, Cuiguang; Li, HB; Zhang, Haifan; Noruzi, Ehsan Bahojb; Qu, Haonan] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Li, Haibing; Li, HB] Guangxi Univ, State Key Lab Featured MetaMat & Life Cycle Safety, Nanning 530004, Peoples R China.;[Wang, Miao] Xiamen Univ, Coll Mat, Xiamen 361005, Peoples R China.;[Hou, Xu] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China.
通讯机构:
[Li, HB ] C;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Guangxi Univ, State Key Lab Featured MetaMat & Life Cycle Safety, Nanning 530004, Peoples R China.
摘要:
Excess fluoride ions in groundwater accumulate through the roots of crops, affecting photosynthesis and inhibiting their growth. Long-term bioaccumulation also threatens human health because it is poorly degradable and toxic. Currently, one of the biggest challenges is developing a unique material that can efficiently remove fluoride ions from the environment. The excellent properties of functionalized pillar[5]arene polymer-filled nanochannel membranes were explored to address this challenge. Constructing a multistage porous nanochannel membrane, consisting of microscale etched nanochannels and nanoscale pillar[5]arene cross-linked polymer voids. A fluoride removal rate of 0.0088 mmol & sdot; L-1 & sdot; min-1 was achieved. Notably, this rate surpassed the rates observed with other control ions by a factor of 6 to 8.8. Our research provides a new direction for developing water fluoride ion removal materials. Fluoride contamination of groundwater has become one of the most serious problems in the world. Currently, excessive absorption of fluoride can be toxic to humans and crops. To address the challenge, we explored the excellent properties of functionalized pillar[5]arene polymer framework. By constructing a multistage porous nanochannel membrane, the pillar[5]arene polymer-filled nanochannel membrane achieves a fluoride removal. image
摘要:
An asymmetric cascade cyclization of enynamides and alpha-diazoketones to produce chiral bicyclic lactams bearing chiral all-carbon quaternary stereocenters is realized with up to 95% yield, 98% ee, and >19:1 dr. The combination of visible light photoactivation and the relay of gold and N-oxide catalysis in a cascade process enabled the facile generation and controlled assembly of two reactive intermediates, ketene and aza-o-quinone methide. Theoretical calculations revealed a stepwise [4 + 2] cycloaddition mechanism, with the stereochemistry controlled by the amide group of the catalyst. Remarkably, this study presents the first example of chiral N-oxides serving as catalysts for asymmetric ketene cycloaddition and illustrates how a cascade strategy could be a promising means to access significant chiral heterocyclic scaffolds.
摘要:
Water molecules are actively involved in many catalytic oxidation processes, which require the construction of highly active sites for their activation to accelerate the reaction rate, especially over non-noble metal catalysts. Herein, K species is embeded into the natural 2*2 channel of alpha-MnO2 by a hydrothermal coupled molten salt method, which would make these K species behave in an electron-rich state and provide more electrons for the activation of water molecules. Compared with surface K modification (namely, the electron-deficient K species), channel K confinement can lower the activation energy barrier of H2O dissociation on alpha-MnO2 to generate hydroxyl species with more nucleophilic oxygen atoms, contributing to the superior HCHO catalytic oxidation activity with a fourfold enhancement. The internal relationship among the confined channel, K species, and catalytic performance is systematically elucidated at the molecular level. This work offers a new ion confinement method and opens up new avenues to construct electron-rich metal sites with channel structures for the activation of water molecules.
作者机构:
[Yi, Yun-Ying; Liu, Yu-Ting; Song, Ying-Chun; Wang, Ming-Xuan; Zhang, Wen-Xin; Wang, Zi-Yue; Zhu, Yan-Ping; Sun, Yuan-Yuan] Yantai Univ, Minist Educ, Collaborat Innovat Ctr Adv Drug Delivery Syst & Bi, Sch Pharm,Key Lab Mol Pharmacol & Drug Evaluat, Yantai 264005, Shandong, Peoples R China.;[Wu, An-Xin] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构:
[Wu, AX ] C;[Zhu, YP ] Y;Yantai Univ, Minist Educ, Collaborat Innovat Ctr Adv Drug Delivery Syst & Bi, Sch Pharm,Key Lab Mol Pharmacol & Drug Evaluat, Yantai 264005, Shandong, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
关键词:
Total synthesis;Oxidative cyclization;Natural products;Switchable synthesis;Luotonin alkaloids
摘要:
A total synthesis strategy was developed for the synthesis of luotonin A, B and their analogues using synergistic FeCl3/KI-catalyzed oxidative cyclization. This protocol utilizes cheap and widely available N-propargyl 2-methyl-quinazolinones and arylamines under mild conditions, and it has a wide substrate scope and high atom economy. Different natural products (luotonin A, B and derivatives) can be synthesized via a unique switchable approach. Further transformations from luotonin B to luotonin E and structural modification of natural products demonstrate the potential applications of this method. Moreover, camptothecin can also be modified with the reported protocol to afford the hydroxyl-substituted product.
摘要:
Poly(ionic liquid)s (PILs) bearing high ionic densities are promising candidates for carbon dioxide (CO(2)) fixation. However, efficient and metal-free methods for boosting the catalytic efficiencies of PILs are still challenging. In this study, a novel family of poly(ionic liquid)-coated carbon nanotube nanoarchitectures (CNTs@PIL) were facilely prepared via a noncovalent and in-situ polymerization method. The effects of different carbon nanotubes (CNTs) and PILs on the structure, properties, and catalytic performance of the composite catalysts were systematically investigated. Characterizations and experimental results showed that hybridization of PIL with hydroxyl- or carboxyl-functionalized CNTs (CNT-OH, CNT-COOH) endows the composite catalyst with increased porosity, CO(2) capture capacity, swelling ability and diffusion rate with respect to individual PIL, and allows the CNTs@PIL to provide H-bond donors for the synergistic activation of epoxides at the interfacial layer. Benefiting from these merits, the optimal composite catalyst (CNT-OH@PIL) delivered a super catalytic efficiency in the cycloaddition of CO(2) to propylene oxide, which was over 4.5 times that of control PIL under metal- and co-catalyst free conditions. Additionally, CNT-OH@PIL showed high carbon dioxide/nitrogen (CO(2)/N(2)) adsorptive selectivity and could smoothly catalyze the cycloaddition reaction with a simulated flue gas (15% CO(2) and 85% N(2)). Furthermore, the CNT-OH@PIL exhibited broad substrate tolerance and could be readily recycled and efficiently reused at least 12 times. Hybridization of PIL with functionalized CNTs provides a feasible approach for boosting the catalytic performance of PIL-based solid catalysts for CO(2) fixation.
摘要:
A visible‐light‐driven four‐component radical relay aminocarbonylation reaction of unactivated alkenes using 4CzIPN as an organic photocatalyst is developed, providing robust access to β‐fluoroalkyl amides with good yields and selectivity under metal‐free conditions. Importantly, this strategy also shows good compatibility with tertiary carbon radicals. Comprehensive Summary Catalytic four‐component radical carbonylation of unactivated alkenes has recently been recognized as a robust protocol for rapid construction of various structurally diverse carbonyl compounds. Given the significance of fluorine‐containing groups, this reaction class has been extensively applied to assembly of a variety of perfluoroalkyl carboxylic acid derivatives by transition metal catalysis. Herein, we report a visible‐light‐driven radical relay 1,2‐perfluoroalkylation aminocarbonylation of unactivated alkenes using CO gas as carbonyl source and 4CzIPN as organic photocatalyst. A wide range of alkenes and amines were well tolerated, providing the valuable β‐perfluoroalkylated amides with generally good yields and high chemoselectivity.
摘要:
With increasingly stringent regulations, the reduction of NOx emissions during vehicle cold start is a major challenge. Pd-modified zeolites are considered as the most promising passive NOx adsorber (PNA) for cold start NOx control. Nevertheless, the scarcity and the high cost of Pd limit its practical application. Herein, a non-precious metal modified Co/Na-SSZ-13 zeolite for low-temperature NOx adsorption is reported. This one-pot synthesized Co/Na-SSZ-13 exhibits an extraordinary NOx storage capacity (212 mu mol g(cat)(-1)) under humid conditions (3% H2O v/v), which is more than double that of conventional Co or Pd-modified SSZ-13. This is attributed to the absence of the inert cobalt phyllosilicate commonly found in conventional Co-SSZ-13, as well as the highly dispersed Co and Na ions as the effective NOx adsorption sites in Co/Na-SSZ-13. Moreover, the presence of Na ions shields the negative charge generated by the Al center and weakens the local electric field strength of the Al and Co centers. This lowers the H2O adsorption energy and improves the zeolite hydrophobicity, which enhances the NO storage capacity of the Co/Na-SSZ-13 under humid conditions. This work highlights the Co/Na-SSZ-13, synthesize via a simple and high-efficiency method, as a promising substitute for noble metal PNA materials.
通讯机构:
[Peng, X ] C;[Quan, FJ ] W;Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.;Cent China Normal Univ, Inst Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
Recently, researchers have been paying much attention to zero-valent iron (ZVI) in the field of pollution remediation. However, the depressed electron transport from the iron reservoir to the iron oxide shell limited the wide application of ZVI. This study was aimed at promoting the performance of microscale ZVI (mZVI) for hexavalent chromium (Cr(vi)) removal by accelerating iron cycle with the addition of boron powder. It was found that the addition of boron powder enhanced the Cr(vi) removal rate by 2.1 times, and the proportion of Cr(iii) generation after Cr(vi) removal process also increased, suggesting that boron could promote the reduction pathway of Cr(vi) to Cr(iii). By further comparing the Cr(vi) removal percentage of Fe(iii) with or without the boron powder, we found that boron powder could promote the percentage removal of Cr(vi) with Fe(iii) from 10.1% to 33.6%. Moreover, the presence of boron powder could decrease the potential gap values (ΔE(p)) between Fe(iii) reduction and Fe(ii) oxidation from 0.668 V to 0.556 V, further indicating that the added boron powder could act as an electron sacrificial agent to promote the reduction process of Fe(iii) to Fe(ii), and thus enhancing the reduction of Cr(vi) with Fe(ii). This study shed light on the promoted mechanism of Cr(vi) removal with boron powder and provided an environmentally friendly and efficient approach to enhance the reactivity of the mZVI powder, which would benefit the wide application of mZVI technology in the environmental remediation field.
通讯机构:
[Zhang, ZH; Lei, HH ] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430083, Hubei, Peoples R China.
摘要:
Regioselective C-H amination of simple arenes is highly desirable, but accessing meta-sites of ubiquitous arenes has proven challenging due to the lack of both electronic and spatial preference. This study demonstrates the successful use of various privileged nitrogen-containing functionalities found in pharmaceutical compounds to direct meta-C-H amination of arenes, overcoming the long-standing requirement for a redundant directing group. The remarkable advancements in functional group accommodation for precise regiochemical control were achieved through the discovery of an unprecedented organo-initiator and the strategic utilization of non-covalent interactions. This protocol has been successfully applied in the concise synthesis and late-stage derivatization of drug molecules, which would have been otherwise challenging to achieve.