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ACS Materials Letters · 2024 · IF 9.6

Isomeric Zero-Dimensional Hybrid Copper(I) Iodides as Highly Efficient Multicolor Phosphors

Jian Chen,Shining Geng,Xuanyu Zhang,Xin Pan,Congcong Chen,Ruiqian Li,Junqian Wen,Chen Sun,Rui Chen,Zewen Xiao,Lingling Mao

The design and construction of new phosphors with significantly different emission colors are key areas in solid-state lighting technologies. Hybrid copper(I) iodides are excellent candidates with multicolor luminescence due to their remarkable structural diversity, superior luminescence performance, and highly tunable optical characteristics. Here, we synthesize and characterize a series of new 0D isomeric copper iodides, namely, Cu4I4(3-trifluoromethylpyridine)4. The emission center [Cu4I4] cubane coordinates with a sterically hindered 3-trifluoromethylpyridine ligand to form four 0D isolated copper iodide clusters, which show ligand-configuration-dependent photoluminescence. The four polymorphs emit blue, green, yellow, and pure white-light, respectively, with high photoluminescence quantum yields (PLQYs) in the range of 80–95%. Time-resolved photoluminescence spectra of all compounds show long averaged decay lifetime up to 10 μs. Density functional theory calculations reveal the electronic structures and the emission characteristics at excited states, illustrating the structure–emission relations. Our results demonstrate that the ligand configurations and orientations have strong impact on the distortion of [Cu4I4] cubane at the excited state, leading to different energy transitions and emission colors. This work provides a new design strategy for multicolor luminescent phosphors and presents the first example of pure white-light emission in a copper(I) iodide system with a near-unity PLQY.

研究领域: 材料科学 · 固态照明 · 光学材料 · 发光材料
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

A straightforward strategy to modulate ROS generation of AIE photosensitizers for type-I PDT

Zhencheng Sun,Jiaxin Wang,Minghui Xiao,Kaiyu Wu,Cheng Wang,Hao Fu,Shuyi Lv,Linqi Shi,Chunlei Zhu

Type-I photodynamic therapy (PDT), valued for its reduced oxygen requirement, generates highly cytotoxic •OH radicals. However, conventional strategies for developing type-I photosensitizers (PSs) are complex and involve intricate organic synthesis. Herein, we present a novel strategy to alter the generation of reactive oxygen species (ROS) by simply manipulating the twisting degree of donor–acceptor (D−A) type aggregation-induced emission (AIE) PSs. Specifically, natural saturated fatty acids are employed to modulate the twisting state of AIE PSs, with higher doping ratios yielding more twisted structures and increased type-I ROS generation. In contrast, fatty acids with higher crystallinity promote planar structures and type-II ROS generation. Theoretical calculations suggest that AIE PSs with highly twisted structures lead to a prominent reduction in Δ E ST and effective separation of electron−hole pairs, thereby favoring efficient intersystem crossing and charge transfer. The PDT system primarily driven by type-I ROS exhibits efficient bactericidal activity against clinically drug-resistant bacteria, which remarkably accelerates the recovery of bacteria-infected wounds in mice. This study demonstrates the first example of modulating ROS generation type by manipulating the twisting degree of D−A type AIE PSs, eliminating the need for intricate molecular design and organic synthesis. The proposed strategy opens up new avenues for advancing PDT applications.

CAS / MDL: 109244-58-8
研究领域: 光动力治疗 · 材料科学 · 生物医学工程 · 化学 · 细菌学
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SENSORS AND ACTUATORS B-CHEMICAL · 2024 · IF 8

Highly specific imaging of pathological type I collagen in connective tissues by dual SERS peptide probes

Linge Nian,Wenhua Li,Minhui Dai,Chunxia Zhang,Lu Li,Guangrui Zhang,Jianxi Xiao

The precise detection of pathological type I collagen is critical for diagnosing and prognosticating various diseases such as fibrosis and tumors. Surface-enhanced Raman scattering (SERS) is emerging as a promising high-resolution imaging technique, yet the intricate process of covalently modifying antibodies often results in SERS probes with diminished selectivity. We herein for the first time report the development of dual SERS peptide probes, Ag@R1@PCTP (S-P) and Ag@R2@ICTP (S-I), which integrate collagen targeting peptides (CTPs), Raman reporters, and silver nanoparticles (Ag NPs) for specific imaging of pathological type I collagen in connective tissues. The S-P/S-I dual SERS peptide probes displayed distinct peaks at 2154 cm −1 and 2227 cm −1 in the Raman silent region with no overlap, showcasing their capability for multiplex imaging free from cross-interference. The SERS peptide probe S-P is specifically tuned to target pathological collagen, excluding intact collagen, while S-I effectively recognizes type I collagen in both its pathological and healthy states. The S-P/S-I probes have exhibited outstanding effectiveness in identifying pathological type I collagen across various connective tissues and have been successfully applied for imaging this collagen in a variety of cancer tissues. The innovative dual SERS peptide probes offer a highly specific and robust tool for imaging pathological type I collagen in tissues, presenting significant potential for the accurate diagnosis and treatment of a range of collagen-related diseases.

CAS / MDL: 7761-88-8
研究领域: 生物医学工程 · 分子生物学 · 成像科学 · 病理学 · 材料科学
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ACS Nano · 2025 · IF 16

Bioinspired Ultrastable Cu(I)-Bovine Serum Albumin Single-Atom Nanozymes Enable MRI-Trackable Synergistic Catalytic Therapy and Cuproptosis for Tumors

Hui Wang,Weitao Yang,Yan Xu,Weiwei Zeng,Dinghua Liu,Tianming Cui,Yanjing Yun,Chang Liu,Zhuoyao Wu,Bingbo Zhang

Monovalent copper (Cu(I)) drives cuproptosis and catalytic therapy, yet its rapid oxidation reduces the activity. We developed bioinspired Cu(I)-bovine serum albumin single-atom nanozymes (Cu(I)-BSA SAzymes) via mild biomineralization, achieving stability (>90 days) and dual enzyme-like activities (peroxidase (POD)/catalase (CAT)) to convert tumor H2O2 into cytotoxic reactive oxygen species (ROS) while alleviating hypoxia. These SAzymes deplete glutathione to amplify oxidative stress and release Cu(I), which aggregates dihydrolipoamide S-acetyltransferase (DLAT) to induce cuproptosis─distinct from apoptosis/ferroptosis. Mechanistically, transcriptomics analyses suggest that Cu(I)-BSA SAzymes exerted their effects by regulating the oxidative stress and energy metabolism in 4T1 cells. The tumor microenvironment further mediates SAzymes aggregation and in situ transformation into paramagnetic Cu(II), enabling self-amplified T1-weighted MRI contrast for real-time activation monitoring. In breast (4T1) and colon (CT26) tumors, Cu(I)-BSA SAzymes suppress growth by 68.8% and 80.3% ([Cu] = 4 mg kg–1). This study reports a stable Cu(I) platform for catalytic-plus-cuproptosis theranostics.

研究领域: 肿瘤学 · 纳米医学 · 生物材料 · 分子影像 · 氧化应激 · 细胞死亡机制 · 转化医学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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ADVANCED MATERIALS · 2025 · IF 26.8

Single Organic Cation Engineering Cu(I)-Based Ionic and Coordinate Type Halides as High-Efficiency Hydrogel Scintillator

Tianrui Li,Baoling Tang,Jiance Jin,Kai Han,Haoran Zhang,Hailian Zhao,Xuejie Zhang,Maxim Molokeev,Yuzhen Wang,Zhiguo Xia,Bingfu Lei

Cu(I)-based halide scintillators are promising candidates for X-ray detection due to excellent scintillation and low-cost solution processability. However, the rational design of Cu(I)-based halide scintillators remains challenging due to insufficient theoretical frameworks elucidating their structure-property correlations. In this work, two Cu(I)-based hybrid metal halides, Cu 2 I 4 -IC (Ionic compound) are designed and Cu 4 I 4 -CC (Coordination compound) via bonding mode control engineering. The Cu 2 I 4 -IC exhibits blue emission, and the Cu 4 I 4 -CC exhibits yellow emission, and the photoluminescence quantum yield (PLQY) of Cu 2 I 4 -IC and Cu 2 I 4 -IC are 91% and 100% respectively. The non-radiative transitions are reduced due to the high rigidity of Cu 4 I 4 , resulting in a light yield up to 67 500 photons MeV −1 and a detection limit as low as 47.3 nGy s −1 of Cu 4 I 4 -CC. Additionally, a high-performance scintillator hydrogel based on Cu 4 I 4 -CC with polyvinyl alcohol (PVA),H 2 O and dimethyl sulfoxide (DMSO) is innovatively developed. Owing to the high transmittance, the large-area scintillator hydrogel film (10 × 10 cm 2 ) achieves an X-ray imaging resolution of 14 lp mm −1 . Furthermore, the synergistic effects of hydrogen bonding and coordination bonding endow the hydrogel scintillator with excellent plasticity and flexible stretchability. The Cu 4 I 4 -CC@PVA hydrogel proves promising for X-ray imaging with excellent stability in harsh environments, matching state-of-the-art scintillators.

研究领域: 材料科学 · 核医学 · 生物医学工程 · 放射影像学 · 无机化学 · 高分子材料 · 功能材料
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Materials Today Chemistry · 2024 · IF 6.7

Ultra-broadband emission from Mg7Ga2GeO12:Ni2+,Cr3+ phosphor spanning the NIR I–III regions for spectroscopy applications

Yuan Tang,Pengbo Lyu,Desheng Yin,Zhaoqi Liu,Nian Pan,Kai Li,Ying Ye,Changfu Xu,Lizhong Sun

Ultra-broadband near-infrared (NIR) lighting sources covering NIR Ⅰ to III regions are pivotal components for NIR spectroscopy devices. However, achieving ultra-broadband and efficient emission covering the entire NIR Ⅰ to III regions remains a significant challenge. To address this, we selected Mg 7 Ga 2 GeO 12 as host material to realize ultra-broadband NIR emission. Density functional theory calculations on formation energies confirmed the feasibility of doping both Ni 2+ and Cr 3+ within Mg 7 Ga 2 GeO 12 . Band structure calculations reveal a significantly reduced band gap upon the doping of Ni 2+ . Following that, we synthesized Mg 7 Ga 2 GeO 12 :Ni 2+ through conventional solid-state-reaction method. This phosphor exhibits broadband NIR emission with a full-width-at-half-maximum of 377 nm in the range of NIR II ∼ III (1100–2100 nm). To further enhance the emission efficiency, we co-doped Mg 7 Ga 2 GeO 12 :Ni 2+ phosphor with Cr 3+ . This co-doping strategy not only dramatically enhances the Ni 2+ emission intensity, but also extends the lower limit of emission band to 600 nm. However, a spectral gap around 1150 nm remains between Cr 3+ and Ni 2+ emission centers. To bridge this spectral gap, we employed LiScSiO 4 :Cr 3+ phosphor alongside Mg 7 Ga 2 GeO 12 :Ni 2+ ,Cr 3+ phosphor to fabricate a phosphor converted LED (pc-LED) with ultra-broadband NIR emission covering entire NIR Ⅰ to III regions. By utilizing this pc-LED as the lighting source for NIR spectral detection, multiple organic functional group signals can be identified simultaneously in NIR II and III bands from 1000 to 2100 nm. The performance of such an NIR pc-LED not only confirms the application potential of Mg 7 Ga 2 GeO 12 :Ni 2+ ,Cr 3+ phosphor in non-destructive spectral analysis but also underscores the feasibility of combining two phosphors to achieve ultra-broadband NIR pc-LEDs, rendering them suitable to be lighting sources for portable spectrometers.

研究领域: 材料科学 · 光学 · 光谱学 · 光子学 · 化学
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ANALYTICA CHIMICA ACTA · 2024 · IF 5.7

A magnetic SERS-imprinted sensor for the determination of cardiac troponin I based on Proteolytic Peptide Technology

Shuqian Wang,Jinli Qin,Yin Liang,Youai Ye,Yamei Guo,Shushu Li,Xiao Yang,Yong Liang

ABSTRACT Acute myocardial infarction is a sudden and high-mortality disease that can be accurately diagnosed by measuring the level of cardiac troponin I in the blood. Currently, cTnI commonly used clinical detection methods usually have excellent sensitivity and are suitable for large-scale sample detection analysis. However, most of these methods are operated through multiple steps of fixation, incubation, reaction and separation, and most of them require professionals to operate complex instruments, which greatly limits their applicability in real-time rapid detection. Therefore, a method that requires low professional skills and can perform rapid detection is necessary. We presents an alternative strategy to quantify cTnI in clinical serum samples using a combination of SERS and magnetic molecularly imprinted polymers (MMIP). MMIPs was synthesized under Polyvinyl Pyrrolidone (PVP) conditions without vinyl modification using characteristic peptide as template, MAA and DMAm as functional monomers. The internal Raman probe 4-MBA was connected through Ag-SH bonds in MMIPs to solve the problem that the target object had no Raman characteristic peak. MMIPs with high magnetic and adsorptive properties showed characteristic absorption peaks at the Raman shift of 1582 cm -1 after specific capture of the target templates. The Raman signals of the 4-MBA were reduced due to shielding effects and the detection range of this method was 0.001-100 ng·mL -1 . The recoveries and relative standard deviations (RSDs) of the spiked experiments were 103.1%-106.3% and 3.54 %-7.38 %, respectively. In summary, this work had appropriate sensitivity and specificity, and there was no significant difference in detection results after ELISA verification. It provided a flexible and practical analysis method for detecting cTnI based on SERS technology. In addition, the imprinting materials of other disease markers can be prepared by changing the template molecules, which provides a new idea for the detection of other biomarkers.

研究领域: 分析化学 · 生物医学工程 · 心脏病学 · 纳米技术
✓ 已验证 产品关联 DOI PubMed 高影响因子
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TALANTA · 2020 · IF 5.339

Plasmon-enhanced quantum dots electrochemiluminescence aptasensor for selective and sensitive detection of cardiac troponin I

Shimeles Addisu Kitte,Terefe Tafese,Chen Xu,Muhammad Saqib,Haijuan Li,Yongdong Jin

The development of highly sensitive electrochemiluminescence (ECL) immunosensors by using functional nanoparticles as signal amplifiers is a solution towards sensitive determination of many low concentration disease biomarkers. Herein, a sensitive aptamer-based, sandwich-type surface plasmon enhanced electrochemiluminescence (SPEECL) immunosensor was demonstrated for the detection of cardiac troponin I (cTnI), by means of aptamer conjugated CdS QDs and AuNPs as ECL luminophores and plasmon sources, respectively, in which Tro4 aptamer was used as a capture probe for cTnI and Tro6 aptamer as a detecting probe. The signal of the developed SPEECL system showed ~ 5-fold increment as compared to that of without AuNPs. Using this ECL platform for the detection of cTnI, a linear range and the limit of detection (LOD) were found to be 1 fg/mL - 10 ng/mL and 0.75 fg/mL, respectively.

研究领域: 分析化学 · 生物化学 · 纳米技术 · 生物医学工程 · 心脏病学
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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 18 ·2309844 · IF 27.4

Physically and Chemically Stable Molybdenum-Based Composite Electrodes for p–i–n Perovskite Solar Cells

Rundong Fan,Wei Sun,Congmeng Li,Yihua Chen,Haipeng Xie,Yongli Gao,Yue Ma,Zongyang Peng,Zijian Huang,Ruiyang Yin,Fengtao Pei,Wentao Zhou,Yuetong Wu,Huifen Liu,Kailin Li,Tinglu Song,Dechun Zou,Huachao Zai,Hui Li,Qi Chen,Qian Wang,Huanping Zhou

Metal halide perovskite solar cells (PSCs) have garnered much attention in recent years. Despite the remarkable advancements in PSCs utilizing traditional metal electrodes, challenges such as stability concerns and elevated costs have necessitated the exploration of innovative electrode designs to facilitate industrial commercialization. Herein, a physically and chemically stable molybdenum (Mo) electrode is developed to fundamentally tackle the instability factors introduced by electrodes. The combined spatially resolved element analyses and theoretical study demonstrate the high diffusion barrier of Mo ions within the device. Structural and morphology characterization also reveals the negligible plastic deformation and halide-metal reaction during aging when Mo is in contact with perovskite (PVSK). The electrode/underlayer junction is further stabilized by a thin seed layer of titanium (Ti) to improve Mo film's uniformity and adhesion. Based on a corresponding p–i–n PSCs (ITO/PTAA/PVSK/C 60 /SnO 2 /ITO/Ti/Mo), the champion sample could deliver an efficiency of 22.25%, which is among the highest value for PSCs based on Mo electrodes. Meanwhile, the device shows negligible performance decay after 2000 h operation, and retains 91% of the initial value after 1300 h at 50–60 °C. In summary, the multilayer Mo electrode opens an effective avenue to all-round stable electrode design in high-performance PSCs.

研究领域: 材料科学 · 光伏技术 · 能源材料 · 薄膜技术 · 器件物理
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ANALYTICA CHIMICA ACTA · 2024 · IF 5.7

Win-win integration: A mitochondria targeted AIE photosensitizer for hypochlorite detection and type I & type II photodynamic therapy

Jiahao Ni,Lichao Yu,Yixuan Wang,Tong Yang,Yueqi Bai,Bowen Zheng,Manshan Liang,Xiaoxia Ye,Yun-Yun Quan,Feifei Lin,Zu-Sheng Huang

Background Photodynamic therapy (PDT) is a pioneering and effective anticancer modality with low adverse effects and high selectivity. Hypochlorous acid or hypochlorite (HClO/ClO − ) is a type of inflammatory cytokine. The abnormal increase of ClO − in tumor cells is related to tumor pathogenesis and may be a “friend” for the design and synthesis of responsive phototherapy agents. However, preparing responsive phototherapy agents for all-in-one noninvasive diagnosis and simultaneous in situ therapy in a complex tumor environment is highly desirable but still remains an enormously demanding task. Results An acceptor-π bridge-donor-π bridge-acceptor (A-π-D-π-A) type photosensitizer TPTPy was designed and synthesized based on the phenothiazine structure which was used as the donor moiety as well as a ClO − responsive group. TPTPy was a multifunctional mitochondria targeted aggregation-induced emission (AIE) photosensitizer which could quickly and sensitively respond to ClO − with fluorescence “turn on” performance (19-fold fluorescence enhancement) and enhanced type I reactive oxygen species (ROS) generation to effectively ablate hypoxic tumor cells. The detection limit of TPTPy to ClO − was calculated to be 185.38 nM. The well-tailored TPTPy anchoring to mitochondria and producing ROS in situ could disrupt mitochondria and promote cell apoptosis. TPTPy was able to image inflammatory cells and tumor cells through ClO − response. In vivo results revealed that TPTPy was successfully utilized for PDT in tumor bearing nude mice and exhibited excellent biological safety for major organs. Significance and novelty A win-win integration strategy was proposed to design a tumor intracellular ClO − responsive photosensitizer TPTPy capable of both type I and type II ROS production to achieve photodynamic therapy of tumor. This work sheds light on the win-win integration design by taking full advantage of the characteristics of tumor microenvironment to build up responsive photosensitizer for in situ PDT of tumor.

CAS / MDL: 307554-62-7 632-69-9
研究领域: 癌症研究 · 药学 · 生物医学工程 · 化学 · 生物学
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DALTON TRANSACTIONS · 2023 ·Vol. 52 ·期 23 ·8142-8154 · IF 4

Heteroleptic copper(I) complexes [Cu(dmp)(N^P)]BF4 for photoinduced atom-transfer radical addition reactions

You-Hui Zhao,Hai-Yan Li,David James Young,Xiangqian Cao,Da-Liang Zhu,Zhi-Gang Ren,Hong-Xi Li

Earth-abundant copper(I) coordination complexes of an imine-phosphine and a diimine have been developed as visible-light photocatalysts. Reaction of [Cu(MeCN)4]BF4 with hetero-bidentate phosphinopyrazole (phpz) ligand R1R2C3HN2PPh3 (R1 = R2 = H (1a); R1 = H, R2 = Me (1b); R1 = H, R2 = Ph (1c); R1 = R2 = Me (1d)) and 2,9-dimethyl-1,10-phenanthroline (dmp) gave four heteroleptic bis-chelate Cu(I) complexes [Cu(dmp)(R1R2C3HN2PPh3)]BF4 (R1 = R2 = H (2a); R1 = H, R2 = Me (2b); R1 = H, R2 = Ph (2c); R1 = R2 = Me (2d)) with distorted tetrahedral geometries. Complexes 2a–2d exhibited broad absorption in the visible spectrum and could facilitate photochemical intermolecular atom-transfer radical addition reactions of CBr4, or CCl3Br, CHI3 to styrenes in yields up to 91% and with a broad substrate scope. The absorption, emission, redox potential and photocatalytic activity were dependent on the substituents on the phpz ligand. Mechanistic studies supported an atom-transfer radical addition (ATRA) mechanism.

研究领域: 无机化学 · 光化学 · 催化
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ANALYTICA CHIMICA ACTA · 2021 · IF 6.558

Sandwich-type electrochemical aptasensor based on hollow mesoporous carbon spheres loaded with porous dendritic Pd@Pt nanoparticles as signal amplifier for ultrasensitive detection of cardiac troponin I

Zhenxing Wang,Hongli Zhao,Kaicha Chen,Hongyuan Li,Minbo Lan

Signal amplification is crucial to improve the sensitivity for the electrochemical detection of cardiac troponin I (cTnI), one of the ideal biomarkers for early acute myocardial infarction (AMI) diagnosis. Herein, we developed a novel signal amplification strategy to construct a sandwich-type electrochemical aptasensor for the detection of cTnI. Core-shell [email protected] dendritic bimetallic nanoparticles loaded on melamine modified hollow mesoporous carbon spheres ( [email protected] DNs/NH 2 -HMCS) was prepared as labels to conjugate with thiol-modification DNA aptamers probe for signal amplification. While introducing numerous amino groups, the melamine functionalized hollow mesoporous carbon spheres (NH 2 -HMCS) retained the edge-plane-like defective sites for the adhesion and electrocatalytic reduction of H 2 O 2 . With the unique characteristics of NH 2 -HMCS, it not only enhanced the dispersity and loading capacity of core-shell [email protected] dendritic bimetallic nanoparticles ( [email protected] DNs), but also improved the stability of bonding by the affinity interaction between [email protected] DNs and amino groups of melamine. Meanwhile, the synergistic catalysis effect between [email protected] DNs and NH 2 -HMCS significantly enhanced the electrocatalytic reduction of H 2 O 2 and further amplified the signal. Under optimal conditions, this recommended aptasensor for cTnI detection displayed a wide dynamic range from 0.1 pg/mL to 100.0 ng/mL and a low detection limit of 15.4 fg/mL (S/N = 3). The sensor also successfully realized the analysis of cTnI-spiked human serum samples, meaning potential applications in AMI diagnosis.

研究领域: 医学诊断 · 纳米材料科学 · 生物传感技术
✓ 已验证 DOI PubMed 高影响因子
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