CHEMISTRY OF MATERIALS
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2025
·
IF 7
Fangmei Fu,Congcong Chen,Yutong Lin,Jiawei Lin,Pan Wang,Xiaoqin Ji,Lingling Mao
Chiral hybrid metal halides are emerging as promising optoelectronic materials due to their tunable chirality and superior optoelectronic properties. However, the current synthesis predominantly relies on chiral organic cations to induce chirality, which constrains their structural diversity and design flexibility. Herein, we report a supramolecular assembly strategy based on the coassembly of 18-crown-6 (18C6) or its chiral methyl-modified derivatives (S/R-18C6) with chiral 4-substituted phenethylammonium groups. This coassembly strategy yields two types of Cu(I) halides, each incorporating a distinct inorganic polyhedral anion: the dimeric [Cu2I4]2– or the tetrameric [Cu4I6]2–. Structural analyses reveal that the stacking modes of the supermolecule influence inorganic anion architecture. Furthermore, the [Cu4I6]2– clusters exhibit broad yellow emission with near-unity PLQYs. The interaction between R/S-18C6 and chiral organic ammonium cations generates a highly asymmetric local chiral environment that induces distortion of the [Cu4I6]2– geometry (angular variance σ2 of up to 27.50 deg2), leading to remarkable circularly polarized luminescence (CPL) signal with a dissymmetry factor (glum) of up to +7.9 ± 0.4 × 10–3/–6.5 ± 0.1 × 10–3. A CPL-active white light-emitting diode (WLED) is fabricated using these materials, demonstrating high-quality white light with a significant CPL signal. This work establishes a supramolecular dual-chirality synergy strategy for the rational design of chiral metal halides, offering an effective strategy for the development of high-performance chiroptical materials.
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Acta Pharmaceutica Sinica B
·
2021
·
IF 11.614
Wenjuan Liu,Zhenqiang Li,Simeng Chu,Xiaoyao Ma,Xiaoying Wang,Min Jiang,Gang Bai
Hyperaldosteronism is a common disease that is closely related to endocrine hypertension and other cardiovascular diseases. Cytochrome P450 11B2 (CYP11B2), an important enzyme in aldosterone (ALD) synthesis, is a promising target for the treatment of hyperaldosteronism. However, selective inhibitors targeting CYP11B2 are still lacking due to the high similarity with CYP11B1. In this study, atractylenolide-I (AT-I) was found to significantly reduce the production of ALD but had no effect on cortisol synthesis, which is catalyzed by CYP11B1. Chemical biology studies revealed that due to the presence of Ala320, AT-I is selectively bound to the catalytic pocket of CYP11B2, and the C8/C9 double bond of AT-I can be epoxidized, which then undergoes nucleophilic addition with the sulfhydryl group of Cys450 in CYP11B2. The covalent binding of AT-I disrupts the interaction between heme and CYP11B2 and inactivates CYP11B2, leading to the suppression of ALD synthesis; AT-I shows a significant therapeutic effect for improving hyperaldosteronism.
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POLYMER DEGRADATION AND STABILITY
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2021
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IF 5.03
Pingping Tang,Tingting Zheng,Lirui Shen,Guoying Li
Collagen hydrogels with a three-dimensional network structure were prepared through self-assembly of collagen molecules, and incubated in laccase-catalyzed gallic acid solutions (L-GA) with different concentrations (0.5–10%, w/v, calculated from the L-GA mother solution). UV-visible spectroscopy and Fourier transform infrared spectrometry suggested that quinones and cross-links between the quinones and the collagen molecules had formed. With an increase in L-GA concentration from 0.5 to 5%, the degree of cross-linking increased from 8.78% to 19.13%; when the L-GA concentration exceeded 5%, the degree of cross-linking increased slightly. At L-GA concentrations ≤ 5%, the thermal denaturation temperature (from 67.4to 74.7°C), the storage modulus (from 90 to 251.42 Pa) and the ABTS• + free radical scavenging activity (from 4.89 to 98.92%) significantly increased, and a distinct decrease was observed in the degree of enzymatic degradation (from 81.48 to 49.34%). At L-GA concentrations >5%, only a slight improvement in these properties was observed. The gel strength of the modified collagen hydrogels reached a maximum value of 1346 g, which was more than twice that of the native collagen hydrogel (656 g) at 5%L-GA. Furthermore, afterthe concentration of L-GA exceeded 1%, the pore sizes observed by scanning electron microscopy began to diminish and showed denser network structures. These data indicated that the properties of collagen hydrogels can be substantially improved by modification with an appropriate concentration of L-GA.
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Device
·
2024
·
IF 0
Xue Ma,Bin Zhao,Pengfei Guo,Yalan Zhang,Jianheng Zhou,Lang Liu,Yu Zhang,Yuanyuan Zhou,Ning Wang
Preventing the formation of Sn-I defect pairs is of vital importance for the fabrication of stable and efficient Sn perovskite solar cells (PSCs). This has spurred intensive efforts, which leave a formidable challenge of simultaneously addressing the unfavored chemical activities of Sn 2+ and I − in Sn perovskites. Herein, we report a europium (Eu) redox-doping method that leverages the facile reactions between Eu 2+ , Sn 4+ , and I 0 in the acidic environment of perovskite solution and thus alleviates the Sn-I defect pair issue. Experimental and theoretical investigations suggest that Eu 2+ could enter Sn perovskite lattice, altering the geometric and electronic structures of [SnI 6 ] 4− octahedra. This could reduce the energy barrier for charge transfer along the inorganic framework. Sn-PSCs with Eu redox doping deliver power conversion efficiencies up to 13.66% and improved stabilities.
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JOURNAL OF ORGANIC CHEMISTRY
·
2024
·
IF 3.3
Lizhu Zhang,Wenqian Du,Jiawen Wu,Rongjie Yang,Fen Zhao,Baomin Fan,Zhonghua Xia
A gold-catalyzed sulfonylation of aryl/vinyl iodides to synthesize aryl sulfones facilitated by the ligand-enabled Au(I)/Au(III) redox catalysis was developed. In the reaction, aryl sodium sulfinates or sulphinic acids can react smoothly with aryl/vinyl iodides to directly construct various aryl sulfones. The strong synthetic capabilities of sulfone synthesis are demonstrated by its easily available and handled reagents, good functional group compatibility, and late-stage application of complicated biomolecules. Mechanistic studies suggest that the silver salt plays a crucial role in the transmetalation with the Au(I)/Au(III) intermediate, and the gold complex favors Au–S bond formation over Au–O bond formation.
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ACS ES&T Water
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2024
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IF 4.8
Zhennan Zhou,Haibo Li,Yikang Lin,Jiali Fan,Hua Tong,Jing Yang,Wei Liu,Gangfeng Ouyang
It is necessary and urgent to develop new materials that are sensitive to antibiotics and can detect them in wastewater. Here, we report a zwitterionic copper(I)-iodide hybrid cluster with strong luminescence and excellent stability. We demonstrate for the first time that this compound can be an efficient optical sensor for tetracyclines, a widely used type of antibiotic, in an aqueous system, with the limit of detection reaching as low as 521–851 ppb. Further, possible electron and energy transfer mechanisms are discussed. This study has opened up new applications for this type of material in the field of chemical sensing.
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iScience
·
2023
·Vol. 26
·期 4
·106461-106461
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IF 5.8
Shuaibo Zhai,Jiaqi Gong,Yifei Feng,Zhongbao Que,Weiwei Mao,Xuemin He,Yannan Xie,Xing’ao Li,Liang Chu
Memristors are promising information storage devices for commercial applications because of their long endurance and low power consumption. Particularly, perovskite memristors have revealed excellent resistive switching (RS) properties owing to the fast ion migration and solution fabrication process. Here, an n-i-p type double perovskite memristor with "ITO/SnO 2 /Cs 2 AgBiBr 6 /NiO x /Ag" architecture was developed and demonstrated to reveal three resistance states because of the p-n junction electric field coupled with ion migration. The devices exhibited reliable filamentary with an on/off ratio exceeding 50. The RS characteristics remained unchanged after 1000 s read and 300 switching cycles. The synaptic functions were examined through long-term depression and potentiation measurements. Significantly, the device still worked after one year to reveal long-term stability because of the all-inorganic layers. This work indicates a novel idea for designing a multistate memristor by utilizing the p-n junction unidirectional conductivity during the forward and reverse scanning.
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ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Min Wang,Xuerong Wang,Zixi He,Zhengdong Liu,Rong Chen,Kaili Wang,Jicai Wu,Jikun Han,Shulin Zhao,Yuhui Chen,Juqing Liu
Smart textiles with multifunction and highly stable performance are essential for their application in wearable electronics. Despite the advancement of various smart textiles through the decoration of conductive materials on textile surfaces, improving their stability and functionality remains a challenging topic. In this study, we developed an ionic textile (i-textile) with air permeability, water resistance, UV resistance, and sensing capabilities through in situ photopolymerization of ionogel onto the textile surface. The i-textile presents air permeability comparable to that of bare textile while possessing enhanced UV resistance. Remarkably, the i-textile maintains excellent electrical properties after washing 20 times or being subjected to 300 stretching cycles at 30% tension. When applied to human joint motion detection, the i-textile-based sensors can effectively distinguish joint motion based on their sensitivity and response speed. This research presents a novel method for developing smart textiles that further advances wearable electronics.
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Nanoscale
·
2024
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IF 5.8
Mengjia Cen,Jiawei Wang,Ming Cheng,Ziyan Lei,Ye Li,Zhenming Wang,Xueqian Zhao,Zixuan Wu,Huanian Zhang,Yan Jun Liu
Manipulating circular dichroism in chiral metasurfaces has been increasingly important for a wide range of polarization-sensitive photonic applications. However, simple methods for presenting chiral nanostructures with tunable and considerable chiroptical responses in the near-infrared-I regime remains underexplored. Herein, two sheets of suspended symmetric bilayer metagratings fabricated via single-step electron beam lithography are stacked into a moiré metasurface with its circular dichroism value reaching up to 20.9°. The chirality of the moiré metasurface can be fully tuned in terms of both its sign and magnitude by adjusting the in-plane angle between the two twisted sheets of metagratings. The multilayered design is accessible to the coupling of hybridized plasmons for governing the chiroptical properties in the near-infrared-I regime. The ratio between the resonance wavelength and the grating period is about 1.65, which is much lower compared to that in most existing moiré metasurfaces with strong chiroptical responses. Furthermore, the superchiral fields in the inter-sheet region are further exploited for label-free enantiodiscrimination with ultrahigh sensitivity of 10.17 nm fmol−1 mm2. The proposed moiré metasurfaces with strong near-infrared-I chirality hold great potential for supporting polarization engineering and biomolecular detection, paving a way for advanced applications in medical diagnosis, biomedical imaging, and display technologies.
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TALANTA
·
2025
·
IF 6.1
Xilin Chen,Yanli Li,Ling Chen,Junrong Tu,Jianbin Pan,Xiaoru Zeng,Yu Fu,Duanping Sun
Acute myocardial infarction (AMI) is the most common cause of death in individuals with cardiovascular disease. Cardiac troponin I (cTnI) is acknowledged as the most prominent biomarker for AMI. However, the key problem of practical applications is how to effectively improve the detection speed and sensitivity. In this study, we designed a novel electrochemiluminescence (ECL) aptasensor for the rapid and quantitative determination of cTnI. This sensor employs self-luminous europium-based metal-organic framework@CdS quantum dots (Eu-MOF@CdS QDs) as a signal probe. The Eu-MOF@CdS QDs can produce a robust cathodic ECL signal via a synergistic effect. Furthermore, a ferrocene-labeled aptamer was used as a quenching probe for quenching the ECL emission of the Eu-MOF@CdS QDs. In the presence of cTnI, the ECL intensity increased with increasing cTnI concentration after ferrocene-labeled aptamer specifically recognized AFB1 and was detached from the electrode interface. Under optimal conditions, the aptasensor demonstrated precise analytical capabilities for cTnI ranging from 1.0 pg/mL to 1.0 ng/mL with a notably low detection limit of 0.08 pg/mL within 60 min. The results show that the developed ECL sensing device demonstrates the potential applications and perspectives for the detection of cTnI in serum samples as well as in the field of biomedical analyses.
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Frontiers in Chemistry
·
2020
·
IF 3.693
Xu Yubing,Wang Xin,Pan Yuzhu,Li Yuwei,Emeka Elemike Elias,Li Qing,Zhang Xiaobing,Chen Jing,Zhao Zhiwei,Lei Wei
Organic-inorganic hybrid perovskite single crystals (PSCs) have been emerged as remarkable materials for some optoelectronic applications such as solid-state photodetectors, solar cells and light emitting diodes due to their excellent optoelectronic properties. To decrease the dark current, function layers based on spin-coating method are frequently requested for intrinsic PSCs to block the injected current by forming energy barrier. However, the amorphous function layers suffer from small carrier mobility and high traps density, which limit the speed of the photoelectric response of perovskite devices. This work supposes to grow thick MAPbBr3 and MAPbI3 mono-crystalline thin films on the surface of intrinsic MAPbBr2.5Cl0.5 PSCs substrate by a heteroepitaxial growth technique to act as electron-blocking layers. Meanwhile, C60 and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) layers are deposited on the opposite surface of substrate PSCs by spin-coating method to block injected holes. This Au-MAPbI3-MAPbBr3-MAPbBr2.5Cl0.5PSCs-C60-PCBM-Ag heterostructure can be used as excellent X-ray photodetector (XPD) due to its low dark current density of 6.97 × 10−11 A cm−2 at −0.5 V bias, high responsivity of 870 mA/W at −100 V bias and X-ray sensitivity as high as 59.7 μC mGy−1 cm−2 at −50 V bias.
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CHEMISTRY OF MATERIALS
·
2023
·
IF 8.6
Zong Chang,Liangjian Liu,Jingying Zhai,Chenchen Liu,Xiao Wang,Chengbo Liu,Xiaojiang Xie,Qinchao Sun
Molecular electronic coupling has been found to play a crucial role in the light-induced processes of natural and artificial systems. The light-induced acoustic process (photoacoustic) is also considered to be one of the most essential characters of the light-absorbing molecules. Herein, we report an interesting observation of the molecular electronic coupling-induced photoacoustic effect (MECPA) in which the PA intensity is dominated by the molecular electronic coupling, rather than the absorption intensity as usually concerned. The molecular electronic coupling effect results in a significant exciton absorption suppression from the monomer to pentamer. However, the corresponding PA efficiency was found to be approximately 2 orders of magnitude greater for the latter. A well-behaved linear correlation between the molecular exciton absorbance and PA efficiency was observed. The surprisingly significant MECPA effect was realized via novel NIR-II squaraine-benzothiopyrylium dyes. Excellent photophysical properties of the novel NIR-II dyes were achieved, such as a large absorption extinction coefficient and high photostability. In vivo duplex PA imaging was demonstrated for tumor tissue and macrophage cells and blood and lymphoid vessels. The MECPA effect would open a new window for the design of PA contrast agent systems for in vivo imaging.
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