期刊:
PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2025年27(5):2828-2833 ISSN:1463-9076
通讯作者:
Liu, Xichun;Lin, YW
作者机构:
[Han, Hui; Pan, Aiqun; Lin, Ying-Wu; Liu, Xichun; Liu, XC] 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.
通讯机构:
[Lin, YW ; Liu, XC] U;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;Univ South China, Lab Prot Struct & Funct, Hengyang 421001, Peoples R China.
摘要:
Globin X is a newly discovered member of the globin family, while its structure and function are not fully understood. In this study, we performed protein modelling studies using Alphafold3 and molecular dynamics simulations, which suggested that the protein adopts a typical globin fold, with the formation of a potential disulfide bond of Cys65 and Cys141. To elucidate the role of this unique disulfide in protein structure and stability, we constructed a double mutant of C65S/C141S by mutating the two cysteine residues to serine. As suggested by protein mass, ultraviolet-visible (UV-Vis) and circular dichroism (CD) spectroscopy analyses, the potential disulfide bond has minimal effect on the overall protein structure, but its absence reduces the protein stability. Electron paramagnetic resonance (EPR) analysis also revealed an increase in the proportion of high-spin state heme iron, which accelerates the rate of heme degradation in reaction with H(2)O(2). This study highlights the critical role of the Cys65-Cys141 in maintaining the stability of globin X and the bis-His heme coordination state, providing insights into the structure-function relationship of the newly discovered globin.
摘要:
In this paper, a novel bifunctional molecule dialkyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DAHAOEP) containing both phosphoryl and hydroxamic groups was designed and synthesized, and used as a uranium extractant. The extraction properties of DAHAOEP were focused. Dihexyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DHHAOEP) was shown to have a better extraction effect on uranyl ions than dibutyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DBHAOEP) and diethyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DEHAOEP). Under the optimal extraction conditions, the extraction efficiency of DHHAOEP on uranyl ions could reach up to 98 %. Extraction saturation capacity, reusability and selectivity results indicated that the saturation capacity of DHHAOEP continuous extraction can reach 596 % after 10 times of extraction, DHHAOEP had been recycled more than 5 times, and exhibited a superior selectivity for uranyl ions. Slope method showed that DHHAOEP mainly coordinated with uranyl ions in a 1:2 coordination, i.e., monomolecular bidentate coordination M2L. FTIR and XPS analysis further confirmed that DHHAOEP combined with uranyl ions through it’s -C(=O)-NHOH and P = O groups to form a five-membered ring and P-O-U configuration, respectively.
In this paper, a novel bifunctional molecule dialkyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DAHAOEP) containing both phosphoryl and hydroxamic groups was designed and synthesized, and used as a uranium extractant. The extraction properties of DAHAOEP were focused. Dihexyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DHHAOEP) was shown to have a better extraction effect on uranyl ions than dibutyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DBHAOEP) and diethyl (2-(hydroxyamino)-2-oxoethyl) phosphonate (DEHAOEP). Under the optimal extraction conditions, the extraction efficiency of DHHAOEP on uranyl ions could reach up to 98 %. Extraction saturation capacity, reusability and selectivity results indicated that the saturation capacity of DHHAOEP continuous extraction can reach 596 % after 10 times of extraction, DHHAOEP had been recycled more than 5 times, and exhibited a superior selectivity for uranyl ions. Slope method showed that DHHAOEP mainly coordinated with uranyl ions in a 1:2 coordination, i.e., monomolecular bidentate coordination M2L. FTIR and XPS analysis further confirmed that DHHAOEP combined with uranyl ions through it’s -C(=O)-NHOH and P = O groups to form a five-membered ring and P-O-U configuration, respectively.
摘要:
In uranium(VI) (U(VI)) photoreduction, it is still a challenge to simultaneously degrade naturally coexisting organics and explore their impact on U(VI) photoreduction. Meanwhile, how to boost the separation and transport capability of photo-induced carriers is also a hot topic of current research. In this work, an ultrathin Bi 2 WO 6 /Bi 2 MoO 6 Z-type heterojunction was developed for the simultaneous treatment of U(VI) and its co-existing organics (tannic acid (TA)). Ultrathin interface engineering increased the contact area and shortened the transmission distance of photo-induced carriers. As a result, ultrathin Bi 2 WO 6 /Bi 2 MoO 6 exhibited highly efficient U(VI) removal rate (95.8 %) and TA degradation rate (97.2 %), which were much higher than those of bulk Bi 2 WO 6 /Bi 2 MoO 6 and single ultrathin Bi 2 WO 6 . In addition, the material possessed excellent stability and recyclability. Importantly, TA not only enhanced U(VI) removal by eliminating holes, but also favored U(VI) removal by serving as a bridge to the catalyst for U(VI) adsorption. Finally, a new mechanism was proposed.
In uranium(VI) (U(VI)) photoreduction, it is still a challenge to simultaneously degrade naturally coexisting organics and explore their impact on U(VI) photoreduction. Meanwhile, how to boost the separation and transport capability of photo-induced carriers is also a hot topic of current research. In this work, an ultrathin Bi 2 WO 6 /Bi 2 MoO 6 Z-type heterojunction was developed for the simultaneous treatment of U(VI) and its co-existing organics (tannic acid (TA)). Ultrathin interface engineering increased the contact area and shortened the transmission distance of photo-induced carriers. As a result, ultrathin Bi 2 WO 6 /Bi 2 MoO 6 exhibited highly efficient U(VI) removal rate (95.8 %) and TA degradation rate (97.2 %), which were much higher than those of bulk Bi 2 WO 6 /Bi 2 MoO 6 and single ultrathin Bi 2 WO 6 . In addition, the material possessed excellent stability and recyclability. Importantly, TA not only enhanced U(VI) removal by eliminating holes, but also favored U(VI) removal by serving as a bridge to the catalyst for U(VI) adsorption. Finally, a new mechanism was proposed.
摘要:
The rapid and selective identification of microorganisms is of great significance for clinical therapy applications. To develop high performance probes for microbe determination, we systemically constructed series aggregation-induced emission (AIE) luminogens by modulating the structural planarity, the basicity of functional group, the length of linker moiety and the hydrophobicity based on our previous work. The detail structure-property relationship study based on experimental and theoretical observation revealed that: i) the planar skeleton is essential for probe insertion towards the cell wall via van n der Waals' force. ii) the basic function group enable the anchoring on the membrane by binding with acidic biomolecules. iii) the shortened alkyl chain is in favor of the efficient binding of basic groups with microbes and endows the desirable hydrophobicity. Based on the developed probes, the successful detection of the pathogens in clinic samples was achieved in highly sensitive and simple way. This work provides a reliable strategy for designing intelligent luminogens for microorganism discrimination and identification in efficient and sensitive way for in vitro diagnosis applications, especially point-of-care testing (POCT).
The rapid and selective identification of microorganisms is of great significance for clinical therapy applications. To develop high performance probes for microbe determination, we systemically constructed series aggregation-induced emission (AIE) luminogens by modulating the structural planarity, the basicity of functional group, the length of linker moiety and the hydrophobicity based on our previous work. The detail structure-property relationship study based on experimental and theoretical observation revealed that: i) the planar skeleton is essential for probe insertion towards the cell wall via van n der Waals' force. ii) the basic function group enable the anchoring on the membrane by binding with acidic biomolecules. iii) the shortened alkyl chain is in favor of the efficient binding of basic groups with microbes and endows the desirable hydrophobicity. Based on the developed probes, the successful detection of the pathogens in clinic samples was achieved in highly sensitive and simple way. This work provides a reliable strategy for designing intelligent luminogens for microorganism discrimination and identification in efficient and sensitive way for in vitro diagnosis applications, especially point-of-care testing (POCT).
期刊:
Journal of Colloid and Interface Science,2025年679(Pt B):569-577 ISSN:0021-9797
通讯作者:
Ren, Xiaohui;Ni, Hongwei
作者机构:
[Cao, Wenzhe; Zou, Haoran; Jiang, Xingxin; Zhang, Hua; Zhang, Tian] The State Key Laboratory of Refractories and Metallurgy, Key Laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education & Hubei Provincial Key Laboratory for New Processes of Ironmaking and Steel Making, Faculty of Materials, Wuhan University of Science and Technology, Wuhan 430081, China;[Ren, Xiaohui] The State Key Laboratory of Refractories and Metallurgy, Key Laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education & Hubei Provincial Key Laboratory for New Processes of Ironmaking and Steel Making, Faculty of Materials, Wuhan University of Science and Technology, Wuhan 430081, China. Electronic address: xhren@wust.edu.cn;[Ma, Feng; Chen, Rongsheng] School of Chemical Engineering and Technology, Wuhan University of Science and Technology, Wuhan, Hubei 430081, China;[Qiao, Hui] Hunan Key Laboratory for Micro-Nano Energy Materials and Devices, and School of Physics and Optoelectronic, Xiangtan University, Hunan 411105, China;[Zhang, Ye] Lab of Optoelectronic Technology for Low Dimensional Nanomaterials, School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
通讯机构:
[Ren, Xiaohui; Ni, Hongwei] T;The State Key Laboratory of Refractories and Metallurgy, Key Laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education & Hubei Provincial Key Laboratory for New Processes of Ironmaking and Steel Making, Faculty of Materials, Wuhan University of Science and Technology, Wuhan 430081, China. Electronic address:
摘要:
The exploration of multiphases and 0D/2D heterojunction in transition metal phosphides (TMPs) and transition metal sulfides (TMDs) is of major interest for hydrogen evolution reaction (HER). Herein, a novel combination route where 0D mixed-phased 1T/2H molybdenum sulfide quantum dots (MoS 2 QDs) are uniformly anchored on the 2D CoP x nanosheets is developed. MoS 2 QDs and CoP x were prepared via hydrothermal method and mixed with different ratios (Mo:Co ratios of 2:1, 1:1, and 1:2) and annealed under different temperatures to modulate their application in acidic HER processes. Specifically, 2Mo/1Co exhibited advanced performance for HER in 0.5 M H 2 SO 4 solution and required 14 mV to deliver 10 mA cm −2 and revealed a descended Tafel slope of 75.42 mV dec −1 with 240 h stability except obvious deactivation. The successful design and construction of 0D/2D mixed-dimensional materials would broaden the application of MoS 2 and CoP x for electrocatalytic hydrogen evolution.
The exploration of multiphases and 0D/2D heterojunction in transition metal phosphides (TMPs) and transition metal sulfides (TMDs) is of major interest for hydrogen evolution reaction (HER). Herein, a novel combination route where 0D mixed-phased 1T/2H molybdenum sulfide quantum dots (MoS 2 QDs) are uniformly anchored on the 2D CoP x nanosheets is developed. MoS 2 QDs and CoP x were prepared via hydrothermal method and mixed with different ratios (Mo:Co ratios of 2:1, 1:1, and 1:2) and annealed under different temperatures to modulate their application in acidic HER processes. Specifically, 2Mo/1Co exhibited advanced performance for HER in 0.5 M H 2 SO 4 solution and required 14 mV to deliver 10 mA cm −2 and revealed a descended Tafel slope of 75.42 mV dec −1 with 240 h stability except obvious deactivation. The successful design and construction of 0D/2D mixed-dimensional materials would broaden the application of MoS 2 and CoP x for electrocatalytic hydrogen evolution.
作者机构:
[Tang, Cen; Wang, Hongqing; Fu, Chao; Yin, Yuting; Kong, Xianghe; Hu, Rong; Hu, Qinghua] School of Chemistry and Chemical Engineering, Hunan Key Laboratory for the Design and Application of Actinide Complexes, University of South China, 28 Changsheng West Road, Hengyang, Hunan 421001, P. R. China
摘要:
The sensitive detection of the radioactive thorium (Th) ion with an oxidation state of +4 (Th(4+)) is of great significance for environmental protection and life safety. In this study, five fluorescence sensors with regulated donor-acceptor (D-A) interactions were constructed for Th(4+) detection based on intramolecular charge transfer and aggregation-induced emission mechanisms. Among the developed sensors, TPE-D bearing electron-deficient π-bridge and weak D-A interactions presented ratiometric fluorescence detection behavior toward Th(4+) in aqueous solution due to its aggregation-induced emission characteristics and unique D-A-D structures. Moreover, TPE-D showed excellent selectivity and sensitivity for Th(4+) detection, and the detection limit was as low as 8.1 × 10(-8) M. The sensing mechanism observation revealed that Th(4+) could coordinate with the hydroxyl, imine, and carbonyl groups of TPE-D accompanied by an electron transfer process. In addition, TPE-D could selectively be enriched in the lysosome. Both the detection of Th(4+) in the lysosome and liver of mice and zebrafish were realized based on this strategy, and a mobile-assisted detection approach toward Th(4+) in actual water samples was also established with high sensitivity. This is the first report for Th(4+) detection in organelles and organs, which provides a great significance and reliable strategy for radionuclide toxicology detection and analysis applications.
作者:
Ji, Hong-Tao;Lu, Yu-Han;Liu, Yan-Ting;Huang, Yu-Lin;Tian, Jiang-Feng;...
期刊:
中国化学快报:英文版,2025年36(2):412-416 ISSN:1001-8417
通讯作者:
Zhang, YH;He, WM
作者机构:
[Liu, Yan-Ting; Liu, Feng; Ji, Hong-Tao; Huang, Yu-Lin; Zhang, Yong-Hong] Univ South China, Affiliated Nanhua Hosp, Hengyang Med Sch, Dept Ophthalmol, Hengyang 421001, Peoples R China.;[Zeng, Yan-Yan; Lu, Yu-Han; He, Wei-Min; Tian, Jiang-Feng; Ji, Hong-Tao; He, WM] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Yang, Hai-Yan] Cent South Univ, Hunan Canc Hosp, Affiliated Canc Hosp,Xiangya Sch Med, Dept Lung Canc & Gastroenterol, Changsha 410013, Peoples R China.
通讯机构:
[Zhang, YH ; He, WM ] U;Univ South China, Affiliated Nanhua Hosp, Hengyang Med Sch, Dept Ophthalmol, Hengyang 421001, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
关键词:
Dual catalysis;Semiconductor;Chlorine;Redox catalyst;Hydrogen atom transfer
摘要:
The first example of Nd@C3N4-photoredox/chlorine dual catalyzed alkylation with unactivated alkanes as the alkyl sources has been developed, which allows for the synthesis of various 4-alkylated cyclic sulfonyl ketimines. In this process, chlorine functions as both a redox and hydrogen atom transfer catalyst. The synergism of the reversible Nd2+/Nd3+ and Cl¯/Cl˙ redox pairs significantly enhances overall photocatalytic efficiency. The in vitro anticancer activity of 4-alkylated products was evaluated by using the CCK8 assay against both human choroidal melanoma (MUM-2B) and lung cancer (A549) cell. Compound 3da showed approximately triple the potency of 5-fluorouracil.
The first example of Nd@C3N4-photoredox/chlorine dual catalyzed alkylation with unactivated alkanes as the alkyl sources has been developed, which allows for the synthesis of various 4-alkylated cyclic sulfonyl ketimines. In this process, chlorine functions as both a redox and hydrogen atom transfer catalyst. The synergism of the reversible Nd2+/Nd3+ and Cl¯/Cl˙ redox pairs significantly enhances overall photocatalytic efficiency. The in vitro anticancer activity of 4-alkylated products was evaluated by using the CCK8 assay against both human choroidal melanoma (MUM-2B) and lung cancer (A549) cell. Compound 3da showed approximately triple the potency of 5-fluorouracil.
摘要:
Chloroanilines represent a class of persistent and highly toxic environmental pollutants, posing significant challenges for green remediation strategies. While P450BM3 monooxygenases are renowned for their ability to catalyze the monooxidation of inert C-H bonds, costly NAD(P)H and complex electron transport systems required for P450BM3 catalysis limit their practical applications. This study pioneers the development of innovative artificial biocatalysts by strategically engineering the active site of P450BM3. Specifically, the substitution of the highly conserved threonine 268 with aspartic acid effectively induces peroxygenase activity, allowing for enhanced catalytic efficiency. Remarkably, the engineered P450BM3 mutants achieved degradation rates of 98.38–99.18 % for five chloroanilines (4-chloroaniline, 2-chloroaniline, 2,4-dichloroaniline, 3,4-dichloroaniline, and 3,5-dichloroaniline) in just 10–15 min, all without the need for NAD(P)H or dual-functional small molecules. Comprehensive degradation mechanism analysis via UPLC-MS corroborated the remarkable performance of these biocatalysts. This research not only demonstrates a novel approach for engineering P450 monooxygenases to exhibit peroxygenase activity but also significantly broadens their potential applications in synthetic chemistry and synthetic biology, paving the way for greener and more sustainable remediation technologies.
Chloroanilines represent a class of persistent and highly toxic environmental pollutants, posing significant challenges for green remediation strategies. While P450BM3 monooxygenases are renowned for their ability to catalyze the monooxidation of inert C-H bonds, costly NAD(P)H and complex electron transport systems required for P450BM3 catalysis limit their practical applications. This study pioneers the development of innovative artificial biocatalysts by strategically engineering the active site of P450BM3. Specifically, the substitution of the highly conserved threonine 268 with aspartic acid effectively induces peroxygenase activity, allowing for enhanced catalytic efficiency. Remarkably, the engineered P450BM3 mutants achieved degradation rates of 98.38–99.18 % for five chloroanilines (4-chloroaniline, 2-chloroaniline, 2,4-dichloroaniline, 3,4-dichloroaniline, and 3,5-dichloroaniline) in just 10–15 min, all without the need for NAD(P)H or dual-functional small molecules. Comprehensive degradation mechanism analysis via UPLC-MS corroborated the remarkable performance of these biocatalysts. This research not only demonstrates a novel approach for engineering P450 monooxygenases to exhibit peroxygenase activity but also significantly broadens their potential applications in synthetic chemistry and synthetic biology, paving the way for greener and more sustainable remediation technologies.
通讯机构:
[Zhao, CW ; Xia, DD] J;[Jiang, L ] C;[Wan, LY ] N;Nanchang Hangkong Univ, Sch Mat Sci & Engn, Nanchang 330063, Peoples R China.;Jiangxi Acad Sci, Inst Appl Chem, Nanchang 330096, Peoples R China.
摘要:
In this study, we have successfully incorporated a small molecular acceptor, Y-LC, with conjugated pi-extension as a secondary acceptor in the PM6:BTP-eC9-based organic photovoltaics. The performance of the device was significantly promoted from 18.45% in the binary system of PM6:BTP-eC9 to over 19% in the ternary system with a minimal Y-LC loading. This enhancement in performance can be attributed to the alloy-like structures of acceptors and the optimized active layer morphology, which leads to improved hole and electron mobilities, thereby suppressing charge recombination, and finally resulting in a higher photocurrent in the solar cells. Furthermore, a complementary absorption of Y-LC is observed with PM6 and BTP-eC9, which can broaden the absorption spectrum of the photoactive layer and enable more photons from sunlight to be absorbed. Additionally, Y-LC facilitates efficient charge transfer from the donor to the acceptor by forming cascade energy levels between PM6 and BTP-eC9. These advantages collectively contribute to the superior performance obtained in the ternary solar cells. This work also highlights that the adoption of a nonfullerene acceptor with suitable conjugated pi-extensions as a minor additive in ternary photovoltaics is a powerful approach for achieving the state-of-the-art organic solar cells.
作者机构:
[Zhu, Ze-Lin; Tan, Hong-Ji; Lee, Chun-Sing; Cao, Chen; Chen, Huan] City Univ Hong Kong, Ctr Superdiamond & Adv Films COSDAF, Hong Kong 999077, Peoples R China.;[Tan, Hong-Ji; Lee, Chun-Sing; Cao, Chen; Chen, Huan; Zhu, Ze-Lin] City Univ Hong Kong, Dept Chem, Hong Kong 999077, Peoples R China.;[Chen, Wen-Cheng; Jin, Jia-Ming; Tan, Ji-Hua] Guangdong Univ Technol, Sch Chem Engn & Light Ind, Guangzhou 510006, Peoples R China.;[Lin, Jiu-Dong] WISPO Adv Mat Suzhou Co Ltd, Bldg 12,200 Xingpu Rd, Suzhou 215000, Peoples R China.;[Yuan, Yi; Yuan, Y] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构:
[Zhu, ZL; Lee, CS ] C;[Yuan, Y ] U;City Univ Hong Kong, Ctr Superdiamond & Adv Films COSDAF, Hong Kong 999077, Peoples R China.;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
关键词:
acridone derivatives;aggregation-induced emission;conformation;hydrogen atom transfer;isotope effects
摘要:
A new aggregation-induced emission (AIE) luminogen is obtained by dimerizing acridin-9(10H)-one (Ac), an aggregation-caused quenching (ACQ) effect monomer via an N & horbar;N bond and forming 9H,9 ' H-[10,10 '-biacridine]-9,9 '-dione (DiAc) with D2d symmetry. The quenching of DiAc in solution is ascribed to the enhanced basicity promoting hydrogen bonding and then a hydrogen abstraction (HA) reaction and/or an unallowed transition in frontier orbitals with the same symmetry facilitating intersystem crossing. It is found that emissive Ac is one product of the non-emissive DiAc solution in the HA reaction activated by UV irradiation. By exploiting the AIE properties and the HA reaction of DiAc, photolithographic patterning is demonstrated with a paper wetted with DiAc solution.
摘要:
The formation and regulation mechanisms of pore structures in porous geopolymers (PGs) remain qualitatively unclear, posing significant challenges to their practical application and performance optimization. In this study, PGs were synthesized utilizing metakaolin as the primary raw material and hydrogen peroxide as the foaming agent. Three distinct surfactants—sodium dodecyl sulfate, hydroxypropyl methylcellulose, and cetyltrimethylammonium bromide—were incorporated to fabricate three unique categories of PGs. The mechanical properties that were evaluated to quantify the surfactant effect were total porosity, pore distribution, and pore size variations using techniques such as image analysis and mercury intrusion porosimetry. This analysis highlighted the significant influence of slurry viscosity on the evolution and modification of pore structure. The results illustrate that viscosity acts as a crucial determinant influencing pore deformation, coalescence, ultimate foaming height, and connectivity within PGs. In addition, this study investigates the correlation between pore structure and the macroscopic properties of PGs. The synthesized PG samples display a broad spectrum of compressive strengths (10.03–17.89 MPa), dry densities (0.87–1.09 g/cm 3 ), and porosities (47.71%–57.41%). These findings provide valuable insights into the design and application of PGs.
The formation and regulation mechanisms of pore structures in porous geopolymers (PGs) remain qualitatively unclear, posing significant challenges to their practical application and performance optimization. In this study, PGs were synthesized utilizing metakaolin as the primary raw material and hydrogen peroxide as the foaming agent. Three distinct surfactants—sodium dodecyl sulfate, hydroxypropyl methylcellulose, and cetyltrimethylammonium bromide—were incorporated to fabricate three unique categories of PGs. The mechanical properties that were evaluated to quantify the surfactant effect were total porosity, pore distribution, and pore size variations using techniques such as image analysis and mercury intrusion porosimetry. This analysis highlighted the significant influence of slurry viscosity on the evolution and modification of pore structure. The results illustrate that viscosity acts as a crucial determinant influencing pore deformation, coalescence, ultimate foaming height, and connectivity within PGs. In addition, this study investigates the correlation between pore structure and the macroscopic properties of PGs. The synthesized PG samples display a broad spectrum of compressive strengths (10.03–17.89 MPa), dry densities (0.87–1.09 g/cm 3 ), and porosities (47.71%–57.41%). These findings provide valuable insights into the design and application of PGs.
作者机构:
[Tao, Yang; Peng, Guowen] School of Resource Environment and Safety Engineering, University of South China Hengyang 421001 China 852376775@qq.com;[Tang, Manzhen; Xiao, Tiyang; Hou, Sanying; Fu, Qing; Xiong, Yiyang] School of Chemistry and Chemical Engineering, University of South China Hengyang 421001 China tysgying@163.com;[Miao, Bin] School of Mechanical and Aerospace Engineering, Nanyang Technological University Singapore 639798 Singapore
通讯机构:
[Xiao, Tiyang; Tao, Yang] S;School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China<&wdkj&>School of Resource Environment and Safety Engineering, University of South China, Hengyang 421001, China
摘要:
A high-performance Fe–N co-doped carbon-based catalyst was prepared to activate PMS by a one-step pyrolysis using ferbam, melamine and sucrose. The best catalyst Fe–N/C exhibited high catalytic activity against PMS at an ultra-low catalyst dosage (50 mg L −1 ), and the TC decomposition rate reached 92.3% within 30 min. The results demonstrated that graphite N, pyridine N, Fe 0 and Fe 3 C were the main active substances for catalyzing PMS. Free radical quenching analysis and EPR experiments further proved that the O 2 ˙ − served as the main active oxygen species. Finally, the environmental hazard of the intermediate product was studied by ECOSAR system.
A high-performance Fe–N co-doped carbon-based catalyst was prepared to activate PMS by a one-step pyrolysis using ferbam, melamine and sucrose. The best catalyst Fe–N/C exhibited high catalytic activity against PMS at an ultra-low catalyst dosage (50 mg L −1 ), and the TC decomposition rate reached 92.3% within 30 min. The results demonstrated that graphite N, pyridine N, Fe 0 and Fe 3 C were the main active substances for catalyzing PMS. Free radical quenching analysis and EPR experiments further proved that the O 2 ˙ − served as the main active oxygen species. Finally, the environmental hazard of the intermediate product was studied by ECOSAR system.
摘要:
Aptamers have recently become novel probes for biosensors because of their good biocompatibility, strong specificity, and high sensitivity. Biosensors based on peptides or nucleic acid aptamers are used in implantable and wearable devices owing to their ease of synthesis and economic efficiency. Simultaneously, amphoteric ionic peptides are being explored as antifouling layers for biosensors resistant to interference from extraneous proteins in serum. Thus, this paper reviews recently developed aptamer-based biosensors and introduces peptide- and nucleic acid-based biosensors, while focusing on the three primary classes of biosensors: electrochemical sensors, fluorescent or colorimetric biosensors, and electroluminescent sensors. Furthermore, we summarize their general construction strategies, describe specific electrochemical sensors that use peptides as an antipollution layer, and elucidate their advantages.
摘要:
Lightweight Al 2 O 3 –MgO refractory castables were prepared using microporous corundum–spinel aggregate, which was fabricated using the Kirkendall effect. The physical properties, microstructure, thermal conductivity, and slag resistance of the castables were analyzed using X-ray diffractometry (XRD), scanning electron microscopy (SEM), and thermodynamic calculations. A comparative analysis was carried out between these findings and the corresponding ones for dense aggregates of Al 2 O 3 –MgO castables. Compared with dense aggregates, the reaction between microporous aggregate and matrix results in a smaller pore size in lightweight aggregate castables. The less soluble spinel in the microporous aggregate contributes to the reduced solubility of lightweight castables in slag, thus enhancing their corrosion resistance. Porous aggregates could absorb more Fe 2+ /Mn 2+ ions from slag than dense aggregates, resulting in an increased viscosity of the slag. This, combined with the small pore size of the matrix, contributes to the superior penetration resistance of the lightweight aggregates castable compared with the dense aggregates castable. Consequently, lightweight aggregate castables exhibit superior corrosion and penetration resistance compared with dense aggregate castables. In contrast to dense aggregates castables, lightweight aggregates castables exhibit a 16.3% reduction in bulk density, an 8.2% decrease in thermal conductivity, and a notable enhancement in slag corrosion resistance.
摘要:
The development of sustainable and efficient synthetic methodologies for high-valued chemicals from renewable resources is one of the principal aims of chemical industries. Herein, we document the combination of photocatalytic PCET and SCS-enabled direct C-H benzylation of N-heteroarenes with benzaldehydes as the benzyl sources. A variety of benzylated N-heteroarenes was obtained in moderate to excellent yields at room temperature under metal-, oxidant-free and mild conditions in continuous-flow mode. Mechanistic studies indicated that this benzylation proceeded via PCET activation of benzaldehydes to yield ketyl radicals, the addition of the ketyl radicals to N-heteroarenes to form C-C(OH) bonds, the SCS cleavage to produce benzylic radical and HAT process to deliver the benzylated products.
期刊:
WATER AIR AND SOIL POLLUTION,2025年236(1):1-12 ISSN:0049-6979
通讯作者:
Xue, JH
作者机构:
[Wang, Xinqing; Huang, Boshi; Xue, Jinhua; Xiao, Xilin] Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hengyang, Hunan, Peoples R China.;[Lin, Dongying] Univ South China, Sch Nucl Sci & Technol, Hengyang 421001, Hunan, Peoples R China.;[Liu, Jingjing; Ren, Lanxing] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Xiao, Xilin] Hunan Univ, State Key Lab Chemo Biosensing & Chemometr, Changsha, Hunan, Peoples R China.
通讯机构:
[Xue, JH ] U;Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hengyang, Hunan, Peoples R China.
关键词:
Cadmium (II);FR;PAN;Fluorescence quenching
摘要:
The objective of this study was to establish a novel method of fluorescence for the determination of cadmium using fluorescein (FR) and 1-(2-Pyridinylazo)-2-Naohthalenol (PAN). In the pH 9.75 buffer solution of the ammonia-ammonium chloride, the energy transfer between FR and the PAN can occur, which can result in the quenching of the fluorescence. The addition of Cd (II) to this system enhances the degree of quenching. This phenomenon has led to the establishment of a novel method for the determination of cadmium, which has been optimized in terms of the required experimental conditions. In the optimal experimental conditions, the fluorescence intensity of the system decreased linearly in the range of 7.81 x 10-7 to 2.14 x 10-5 mol L-1. The linear regression equation used in this study was F = 123.63 + 170.65c (x 10-6 mol L-1) under the correlation coefficient of 0.9951, the detection limit of 2.34 x 10-7 mol L-1, and the relative standard deviation of 0.18%. The proposed method was simple, sensitive, fast, and economical. The method can be employed for the determination of cadmium in real samples (tap-water, pond water and Xiangjiang River) with the results demonstrating consistency with the graphite furnace atomic absorption method (t-test). This approach offers an innovative method for the quantification of Cd (II).
关键词:
Advanced oxidation process;TC degradation;Carbon nanotubes;Fe/Fe 3 C nanoparticles;Encapsulated structures
摘要:
In this study, nitrogen-doped nanotube-encapsulated iron nanoparticle catalysts (Fe/Fe3C@NCNTs) were prepared using a one-step pyrolysis strategy for the efficiently activating of peroxymonosulfate (PMS) to degrade tetracycline hydrochloride (TC). The embedded structure greatly minimized the leaching of metals and enhanced the catalyst stability. The prepared Fe/Fe3C@NCNT-800 (0.05 g/L) exhibited excellent PMS (0.5 g/L) catalytic activity for the rapid degradation of TC (30 mg/L) with degradation rate of 90.5 % within 5 min under the pH of 7 and 25 degrees C. Its performance was nearly unaffected by environmental factors (temperature, pH, inorganic anions and organic matter). Moreover, the Fe/Fe3C@NCNT-800/PMS system maintained a TC removal rate of 85.5 % after four cycles of degradation experiments, with a negligible amount of metal leaching. X-ray photoelectron spectroscopy, electron paramagnetic resonance spectroscopy and electrochemical measurements showed that iron nanoparticles and graphitic nitrogen promoted Fe2+/Fe3+ cycling and reactive oxygen species generation as catalytic centers. Among them, 1O2 and electron transfer were shown to be the main degradation pathways for degrading TC.
摘要:
An activatable photosensitizer with a reaction‐tunable donor/acceptor push‐pull electronic effect is designed and developed, which shows high sensitivity toward nitric oxide (NO) NO with the formation of triazole segment. Moreover, the turn‐on PDT behavior and endoplasmic reticulum (ER) targeting ability enable the developed photosensitizer good inhibition effect toward tumor cells both in vitro and in vivo, which presents high promise for precise tumor therapy in practical. Abstract Photodynamic therapy (PDT) is a powerful strategy for tumor therapy with noninvasiveness and desirable efficacy. However, the phototoxicity of photosensitizer after the post‐PDT is the major obstacle limiting the clinic applications. Herein, a nitric oxide (NO)‐activatable photosensitizer is reported with turn‐on PDT behavior and endoplasmic reticulum (ER) targeting ability for precise tumor therapy. Four o‐thiophenediamine derivatives with reaction‐tunable donor/acceptor push‐pull electronic effect are established, and the systematic structure and property relationship observation reveals the following features: 1) the reactivity against NO can be improved by enhancing the electron density and further facilitated upon photo‐irradiation. 2) the reactivity with NO enables the improved intramolecular charge transfer process with the evoking of photosensitizing effect. 3) only o‐thiophenediamine derivative with ER enrichment behavior exhibited cancer cell ablation effect compared to photosensitizers localized in lysosome and lipid droplet. Thus, the efficient inhibition of cancer cells both in vitro and in vivo is realized based on the photo‐controlled PDT strategy. This work provides more insights into developing promising activatable photosensitizers for advanced therapy based on tumor microenvironment trigger.
作者机构:
[Huang, Jun] University of South China, School of Chemistry and Chemical Engineering, Heng Yang, Heng Yang, CHINA;[Zhu, Lei] University of South China, School of Chemistry and Chemical Engineering, 421001, Hengyang, CHINA
摘要:
The presence of sterically rigid contiguous quaternary stereocenters in natural products imposes conformational constraints with significant effects on their biological activities. However, achieving the direct synthesis of multiple contiguous quaternary stereocenters in a single step remains a formidable challenge. Here, we present the totalsynthesis of the antibacterial metabolite lugdunomycin (1) inthirteenstepsvia a sequence of photochemical transformations. A photoenolization, keto-enol tautomerization, and spiroketalization sequence was developed to generate the spiroketal 4from actinaphthoran B (3). Subsequently, a photoinduced isobenzofuran Diels-Alder reaction between elmonin (4) and iso-maleimycin (5) was developed to construct the polycyclic benzaza[4,3,3]propellane framework bearing three contiguous quaternary stereocentersin the compact C-ring along with a distal hydroxyl group at C19. The mechanism of these photochemical reactions was investigated using synthetic and computational approaches.