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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Engineering oxygen vacancy of MoOx nanoenzyme by Mn doping for dual-route cascaded catalysis mediated high tumor eradication

Rui Zhang,Changlin Liu,Ruoxi Zhao,Yaqian Du,Dan Yang,He Ding,Guixin Yang,Shili Gai,Fei He,Piaoping Yang

There is an urgent need to develop photosensitive nanoenzymes with better phototherapeutic efficiency through simple processes. By exploiting semiconductor catalysis and defect chemistry principles, herein, a MnMoO x composite semiconductor nanoenzyme was developed to achieve a fully integrated theranostic nanoenzyme for highly efficient photo/chemo-enzyme-dynamic eradication of deep tumors. Relative to iron oxides, manganese oxides offer ideal catalytic performance under near-neutral conditions, which helps to broaden the suitable pH range of the MnMoO x nanoenzyme for antitumor therapy. Furthermore, with the assistance of glutathione depletion, Mn 4+ /Mo 6+ was successfully converted to Mn 2+ /Mo 5+ , inhibiting the scavenging of reactive oxygen species (ROS) and promoting cycling. Therefore, MnMoO x has favorable catalase (CAT)-like activity and oxidase (OXD)-like activity in the tumor microenvironment (TME) for promoting the “H 2 O 2 O 2 O 2 − ” and “H 2 O 2 OH” cascade reactions. The abundant oxygen vacancy defects also promote the surface plasmon resonance (SPR) effect in the second near-infrared (NIR-II) window of MnMoO x , which significantly enhanced its photothermal therapy (PTT) effect and catalytic activity. In detail, ROS production was significantly enhanced due to the adsorption of water and oxygen molecules by the rich oxygen vacancies of MnMoO x . MnMoO x also exhibited excellent multi-modal imaging activity (including computed tomography (CT), magnetic resonance imaging (MRI), and photoacoustic (PA)), which can be exploited to better guide the administration of medication.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

MXene-MoS2 carbon-fiber-based flexible electrochemical interface for multiple bioanalysis in biofluids

Jiaying Zhao,Congjuan He,Weixuan Wu,Huisi Yang,Lan Peng,Li Wen,Zhikun Hu,Changjun Hou,Danqun Huo

Flexible sensing technology has received widespread attention in the monitoring of human physiological indicators. Thus, it is of great significance to develop a universal flexible sensing interface for early diagnosis of multi-level biomarkers. Herein, we reported a multifunctional 3D carbon fiber paper (CFP)-MXene-MoS 2 (CMM) sensing interface, which provided a flexible electrochemical biosensing platform for the ultrasensitive detection of multiple bioanalysis in biofluids. Notably, the CMM electrochemical interface was comprised of staggered carbon fibers on which the organ-like MXene-MoS 2 heterostructure covered with MoS 2 nanosheet arrays was uniformly allocated, permitting local enrichment of biomolecules for enhanced biomolecular capture efficiency, laying a solid foundation for the ultrasensitive detection of multiple biomolecules. In proof-of-concept experiments, we validated that the flexible CMM interface could be applied for ultrasensitive analyzing of quite a few biomolecules like ascorbic acid (AA), uric acid (UA), dopamine (DA) and microRNA (miRNA), with charming sensitivity and reproducibility. It was worth mentioned that an ultra-high sensitivity of 3.16 aM was acquired towards detecting microRNA. Under optimal parameters, the designed electrochemical interface worked well in complex biofluids such as human serum and urine samples. Overall, this flexible and disposable CMM interface with ultrahigh sensitivity provided insights for a more portable, accessible and valuable approach for monitoring biomolecules in clinical diagnosis.

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MOLECULES · 2022 ·Vol. 27 ·期 9 ·3016 · IF 4.927

Construction of Enzyme-Responsive Micelles Based on Theranostic Zwitterionic Conjugated Bottlebrush Copolymers with Brush-on-Brush Architecture for Cell Imaging and Anticancer Drug Delivery

Fangjun Liu,Dun Wang,Jiaqi Wang,Liwei Ma,Cuiyun Yu,Hua Wei

Bottlebrush copolymers with different chemical structures and compositions as well as diverse architectures represent an important kind of material for various applications, such as biomedical devices. To our knowledge, zwitterionic conjugated bottlebrush copolymers integrating fluorescence imaging and tumor microenvironment-specific responsiveness for efficient intracellular drug release have been rarely reported, likely because of the lack of an efficient synthetic approach. For this purpose, in this study, we reported the successful preparation of well-defined theranostic zwitterionic bottlebrush copolymers with unique brush-on-brush architecture. Specifically, the bottlebrush copolymers were composed of a fluorescent backbone of polyfluorene derivate (PFONPN) possessing the fluorescence resonance energy transfer with doxorubicin (DOX), primary brushes of poly(2-hydroxyethyl methacrylate) (PHEMA), and secondary graft brushes of an enzyme-degradable polytyrosine (PTyr) block as well as a zwitterionic poly(oligo (ethylene glycol) monomethyl ether methacrylate-co-sulfobetaine methacrylate) (P(OEGMA-co-SBMA)) chain with super hydrophilicity and highly antifouling ability via elegant integration of Suzuki coupling, NCA ROP and ATRP techniques. Notably, the resulting bottlebrush copolymer, PFONPN9-g-(PHEMA15-g-(PTyr16-b-P(OEGMA6-co-SBMA6)2)) (P2) with a lower MW ratio of the hydrophobic side chains of PTyr and hydrophilic side chains of P(OEGMA-co-SBMA) could self-assemble into stabilized unimolecular micelles in an aqueous phase. The resulting unimolecular micelles showed a fluorescence quantum yield of 3.9% that is mainly affected by the pendant phenol groups of PTyr side chains and a drug-loading content (DLC) of approximately 15.4% and entrapment efficiency (EE) of 90.6% for DOX, higher than the other micelle analogs, because of the efficient supramolecular interactions of π–π stacking between the PTyr blocks and drug molecules, as well as the moderate hydrophilic chain length. The fluorescence of the PFONPN backbone enables fluorescence resonance energy transfer (FRET) with DOX and visualization of intracellular trafficking of the theranostic micelles. Most importantly, the drug-loaded micelles showed accelerated drug release in the presence of proteinase K because of the enzyme-triggered degradation of PTyr blocks and subsequent deshielding of P(OEGMA-co-SBMA) corona for micelle destruction. Taken together, we developed an efficient approach for the synthesis of enzyme-responsive theranostic zwitterionic conjugated bottlebrush copolymers with a brush-on-brush architecture, and the resulting theranostic micelles with high DLC and tumor microenvironment-specific responsiveness represent a novel nanoplatform for simultaneous cell image and drug delivery.Keywords:brush-on-brush;zwitterionic;enzyme-responsive;theranostic;FRET

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Bioactive Materials · 2022 · IF 16.874

Polymeric dual-modal imaging nanoprobe with two-photon aggregation-induced emission for fluorescence imaging and gadolinium-chelation for magnetic resonance imaging

Xueyang Xiao,Hao Cai,Qiaorong Huang,Bing Wang,Xiaoming Wang,Qiang Luo,Yinggang Li,Hu Zhang,Qiyong Gong,Xuelei Ma,Zhongwei Gu,Kui Luo

Nanoprobes that offer both fluorescence imaging (FI) and magnetic resonance imaging (MRI) can provide supplementary information and hold synergistic advantages. However, synthesis of such dual-modality imaging probes that simultaneously exhibit tunability of functional groups, high stability, great biocompatibility and desired dual-modality imaging results remains challenging. In this study, we used an amphiphilic block polymer from (ethylene glycol) methyl ether methacrylate (OEGMA) and N -(2-hydroxypropyl) methacrylamide (HPMA) derivatives as a carrier to conjugate a MR contrast agent, Gd-DOTA, and a two-photon fluorophore with an aggregation-induced emission (AIE) effect, TPBP, to construct a MR/two-photon fluorescence dual-modality contrast agent, Gd-DOTA-TPBP. Incorporation of gadolinium in the hydrophilic chain segment of the OEGMA-based carrier resulted in a high r 1 value for Gd-DOTA-TPBP, revealing a great MR imaging resolution. The contrast agent specifically accumulated in the tumor region, allowing a long enhancement duration for vascular and tumor contrast-enhanced MR imaging. Meanwhile, coupling TPBP with AIE properties to the hydrophobic chain segment of the carrier not only improved its water solubility and reduced its cytotoxicity, but also significantly enhanced its imaging performance in an aqueous phase. Gd-DOTA-TPBP was also demonstrated to act as an excellent fluorescence probe for two-photon-excited bioimaging with higher resolution and greater sensitivity than MRI. Since high-resolution, complementary MRI/FI dual-modal images were acquired at both cellular and tissue levels in tumor-bearing mice after application of Gd-DOTA-TPBP, it has great potential in the early phase of disease diagnosis.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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MICROCHIMICA ACTA · 2022 ·Vol. 189 ·期 2 ·1-10 · IF 6.408

Fabrication of rGO/MXene-Pd/rGO hierarchical framework as high-performance electrochemical sensing platform for luteolin detection

Huang Hui,Xie Shuqian,Deng Lu,Yuan Jie,Yue Ruirui,Xu Jingkun

A  nanocomposite of rGO/MXene-Pd/rGO with hierarchical structure based on Ti 3 C 2 T x MXene, Pd nanoparticles, and reduced graphene oxide (rGO) was synthesized by a green approach. Ti 3 C 2 T x MXene decorated with Pd nanoparticles (MXene-Pd) was prepared first. Then, graphene oxide (GO), MXene-Pd, and GO were coated on the surface of the glassy carbon electrode (GCE) in sequence. After each coating of the GO layer, the GO nanosheets were reduced to rGO electrochemically. The fabricated rGO/MXene-Pd/rGO hierarchical framework performs a pie structure with MXene-Pd as the stuffing and rGO nanosheets as the crust, which will be beneficial to the enhancement of its electrochemical sensing performance. As compared with other electrodes, the rGO/MXene-Pd/rGO/GCE exhibited higher electrocatalytic activity and better sensing performance for luteolin detection, with a wide linear range of 6.0 × 10 −10 to 8 × 10 −7  M and 1.0 × 10 −6 to 1.0 × 10 −5  M (oxidation peak potential E pa  = 0.34 V vs . SCE), a low detection limit of 2.0 × 10 −10  M, and a high sensitivity of 112.72 µA µM −1  cm −2 . Moreover, the fabricated sensor also showed high selectivity, reproducibility, and repeatability toward the detection of luteolin. The real sample analysis for luteolin in honeysuckle was successfully carried out by rGO/MXene-Pd/rGO and verified with high-performance liquid chromatography (HPLC) analysis techniques with acceptable results. All the above tests indicate the promising application prospect of the rGO/MXene-Pd/rGO framework for luteolin detection in honeysuckle and other herbs containing luteolin. Graphical abstract

✓ 已验证 产品关联 DOI PubMed 高影响因子
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2022 · IF 5.999

GMT8 aptamer conjugated PEGylated Ag@Au core-shell nanoparticles as a novel radiosensitizer for targeted radiotherapy of glioma

Dongdong Li,Jing Zhao,Jun Ma,Huiquan Yang,Xiaodong Zhang,Yuyu Cao,Peidang Liu

Radiotherapy is one of the main treatment modalities for glioma, but the therapeutic efficacy is often limited by the radioresistance of tumor cells. The radiosensitization effects of silver nanoparticles (AgNPs) and gold nanoparticles (AuNPs) on tumors have been confirmed by previous studies. To enhance the specific killing effect of irradiation on tumor cells, targeted modification of radiosensitizers is urgently needed. Herein, we developed polyethylene glycol (PEG)-coated [email protected] core-shell nanoparticles (PSGNPs) modified with GMT8 aptamer (GSGNPs) and evaluated their radiosensitization effects on glioma cells through in vivo and in vitro experiments. Transmission electron microscope image showed that the prepared PSGNPs had a spherical core-shell structure with an average size of 11 nm. The ultraviolet-visible absorption spectra and Fourier transform infrared spectra displayed that GMT8 was successfully conjugated to PSGNPs. The results of dark-field imaging revealed that the targeting ability of GSGNPs to U87 glioma cells was much better than that to normal human microvascular endothelial cells. Additionally, it was also found that the endocytic pathways of GSGNPs mainly involved clathrin-mediated endocytosis and macropinocytosis . The sensitization enhancement ratio of GSGNPs was calculated to be 1.62, which was higher than that of PSGNPs. In vivo imaging results showed that GSGNPs exhibited good tumor targeting and retention capabilities, and the fluorescence intensity ratio of Cy5-GSGNPs to Cy5-PSGNPs reached a peak at 4 h after injection. More importantly, the median survival time of mice bearing U87 glioma was significantly prolonged after intravenous administration of GSGNPs combined with radiotherapy. This work demonstrated that GSGNPs could be used as an effective nano-radiosensitizer for targeted radiotherapy of glioma.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2022 · IF 7.926

Removal of polycyclic aromatic hydrocarbons by g-C3N4 nanosheets under visible light irradiation and effect of typical co-existence substances in river water

Meng Qiao,Lujing Fu,Damia Barcelo

Polycyclic aromatic hydrocarbons (PAHs) ubiquitously exist in aqueous environment , posing considerable chronic and acute ecological risk to aquatic species. Non-metallic photocatalyst g-C 3 N 4 is a promising photocatalyst that can be used in river remediation under visible light irradiation. The removal of a typical PAH phenanthrene (PHE) by g-C 3 N 4 under visible light was detailed studied. The removal efficiency of PHE (initial concentration 5 mg/L) by g-C 3 N 4 -nano sheet (NS) (1 g/L) reached 100% within 10 min under visible light. Reactive oxygenated species, including •O 2 - , 1 O 2 , and •OH, were generated in the g-C 3 N 4 -NS/visible light system. •O 2 - and 1 O 2 were determined as the main active species , whereas photoelectric-hole and •OH were also involved in the reaction. The effects of co-existed substances were investigated, including humic acid (HA), Cl - , and NO 3 - . HA decreased the removal rate of PHE, probably due to its reaction with photo-generated holes. Cl - with lower concentration (0.2 – 10.0 mmol/L) decreased the removal rate of PHE, while with higher concentration (20 mmol/L) increased the removal rate of PHE, probably because of the interaction of Cl - with •OH. NO 3 - with the concentration of 10–100 μmol/L did not significantly affect the removal rate of PHE. This study will provide a possible in-situ route for the removal of typical PAHs in urban river environment.

CAS / MDL: 461-58-5 3317-61-1
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Synthesis of ZIF-67 derived honeycomb porous Co/NC catalyst for AO7 degradation via activation of peroxymonosulfate

Yuhan Long,Songrong Li,Peizhen Yang,Xi Chen,Wenhao Liu,Xuesong Zhan,Cheng Xue,Dongfang Liu,Wenli Huang

MOF-derived metal-carbon composite catalyst was an alternative high-efficient catalyst for activating peroxymonosulfate (PMS). In this study, a novel cobalt-carbon-nitrogen doped composite catalyst with honeycomb porous structure (Co-HPNC) was obtained through a simple strategy consisting of three steps: self-growth of ZIF-67 on the SiO 2 core, pyrolysis, and NaOH etching away SiO 2 core. The Co-HPNC exhibited an outstanding catalytic performance (98.1% in 10 min) to activate PMS for acid orange 7 (AO7) degradation. The observed reaction kinetic constant (0.4319 min −1 ) was 2.64 times superior to that of the unmodified Co/NC catalysis system (0.1636 min −1 ). In the meantime, the catalyst demonstrated a high PMS activation capacity over a wide pH range of 3–11 and strong adaptability to the high concentration of inorganic anions (Cl - , SO 4 2- , and CO 3 2– ). After being recycled three times, the removal efficiency could still reach 92.7% in 25 min. The quenching tests and EPR spectrum illustrated the existence of radical and non-radical pathways, in which singlet oxygen was dominant during the degradation process. It was hypothesized that Co(0)/Co(Ⅱ)/Co(Ⅲ), pyridinic-N and pyrrolic-N contributed to the generation of hydroxyl and sulfate radicals, while C=O functional group and graphitic-N were catalytic sites for singlet oxygen. Finally, the radical electrophilic attacking sites of AO7 were calculated by the density functional theory (DFT), and the degradation routes of AO7 were speculated by GC–MS. The toxicity test illustrated that the Co-HPNC/PMS system was an environmental-friendly technology for AO7 degradation. The prepared Co-HPNC with a unique honeycomb porous structure presents a novel synthesis route for MOF-derived catalyst applied in the PMS activation system for wastewater treatment.

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Foods · 2022 ·Vol. 11 ·期 2 ·165 · IF 5.561

Effects of Baicalein and Chrysin on the Structure and Functional Properties of β-Lactoglobulin

Ang Li,Lei Chen,Weijie Zhou,Junhui Pan,Deming Gong,Guowen Zhang

Two flavonoids with similar structures, baicalein (Bai) and chrysin (Chr), were selected to investigate the interactions with β-lactoglobulin (BLG) and the influences on the structure and functional properties of BLG by multispectral methods combined with molecular docking and dynamic (MD) simulation techniques. The results of fluorescence quenching suggested that both Bai and Chr interacted with BLG to form complexes with the binding constant of the magnitude of 105L·mol−1. The binding affinity between BLG and Bai was stronger than that of Chr due to more hydrogen bond formation in Bai–BLG binding. The existence of Bai or Chr induced a looser conformation of BLG, but Chr had a greater effect on the secondary structure of BLG. The surface hydrophobicity and free sulfhydryl group content of BLG lessened due to the presence of the two flavonoids. Molecular docking was performed at the binding site of Bai or Chr located in the surface of BLG, and hydrophobic interaction and hydrogen bond actuated the formation of the Bai/Chr–BLG complex. Molecular dynamics simulation verified that the combination of Chr and BLG decreased the stability of BLG, while Bai had little effect on it. Moreover, the foaming properties of BLG got better in the presence of the two flavonoids compounds and Bai improved its emulsification stability of the protein, but Chr had the opposite effect. This work provides a new idea for the development of novel dietary supplements using functional proteins as flavonoid delivery vectors.Keywords:baicalein;chrysin;β-lactoglobulin;functional property;spectrophotometry;molecular dynamics simulation

CAS / MDL: 7440-47-3 69-78-3
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF THE ENERGY INSTITUTE · 2022 · IF 6.47

Investigation on co-gasification of N-rich fiberboard and glucose: Nitrogen evolution and changes in char properties

Ming Zhao,Jun Sun,Muhammad Asif Akhtar,Shu Zhang,Juntao Wei,Deliang Xu,Xun Hu,Mortaza Gholizadeh,Hong Zhang

Waste wood-based panels (WBPs) with high nitrogen content is a typical kind of industrial biomass waste, and a large amount of NO x will be generated during its incineration treatment. Therefore, this work is aimed at studying the retention and conversion characteristics of nitrogen in gasification char of WBPs. For fixing more nitrogen in char, co-gasification experiments of fiberboard (FB, the main kind of WBPs) and glucose were carried out using a fixed bed reactor , and the subsequent analysis was conducted by element analyzer, XPS , SEM and BET. The results show that the addition of glucose could efficiently fix nitrogen in gasification char , the nitrogen retention ratios of FB-glucose char under N 2 and CO 2 atmosphere were 2.6–5.6 times and 1.4–2.0 times greater than that of individual FB char, respectively, due to the enhanced Maillard reaction. As the temperature increased, the portions of N-5 and N-6 decreased along with the formation of N-Q and N–O. Moreover, the addition of glucose led to the delay of the conversion from N-5 and N-6 to N-Q and N–O in char. BET results demonstrate that the surface area and total pore volume of co-gasified char were significantly lower than those of individual FB gasified char. The glucose had a negative effect on the pore structure development of co-gasified char. These results could offer strategies on reducing NO x emission in biomass thermal conversion and regulating nitrogen functional groups in biochar.

CAS / MDL: 50-99-7
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Journal of Materials Chemistry B · 2022 ·Vol. 10 ·期 5 ·748-756 · IF 7.571

Ion channel-targeting near-infrared photothermal switch with synergistic effect for specific cancer therapy

Shuangling Wang,Jie Lv,Yu Pang,Shuyang Hu,Yulong Lin,Meng Li

Despite significant achievement in chemotherapy, the off-target actions and low pharmaceutical selectivity of the therapeutic agents still limit their clinical efficacy. Herein, a multifunctional nanoplatform which integrates chemotherapy, chemodynamic therapy (CDT) and photoactivation of TRPV1 channels has been successfully established for specific cancer therapy. Polydopamine (PDA) coated hollow prussian blue nanocages (hPBNCs) are used as the photothermal switches and drug carriers for loading chemotherapeutic drug, doxorubicin (Dox). Conjugating with the TRPV1 antibodies enables the nanoplatform to bind specifically to TRPV1 channels on the plasma membrane of the TRPV1-positive cancer cells and then activate them by local heating upon NIR irradiation, leading to the over-influx of Ca2+. Critically, the laser irradiation can be carefully controlled to not only open the TRPV1 channels but also avoid burning of tumors by hyperthermia. Moreover, the exposed hPBNCs in the acidic tumor cells can decompose endogenous H2O2 into ˙OH by Fenton reaction to realize CDT, which further aggravates cancer cell apoptosis. Together with the chemotherapy caused by Dox, our nanoplatform displays an enhanced anticancer effect both in vitro and in vivo. Our work provides a powerful means for site-specific cancer synergetic therapy with high spatial and temporal resolution.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Sulfuric-acid-mediated synthesis strategy for multi-colour aggregation-induced emission fluorescent carbon dots: Application in anti-counterfeiting, information encryption, and rapid cytoplasmic imaging

Lijuan Yang,Shaochi Liu,Tian Quan,Yongqing Tao,Meng Tian,Luchun Wang,Junji Wang,Dandan Wang,Die Gao

Aggregation-induced emission fluorescent carbon dots (AIE-CDs) have applications in the fields of multi-colour anti-counterfeiting, information encryption, and imaging. In this study, four AIE-CDs (B-AIE-CDs, G-AIE-CDs, Y-AIE-CDs, and O-AIE-CDs) with blue, green, yellow, and orange fluorescence at high concentrations were fabricated using crystal violet as a precursor, solutions with different sulfuric acid concentrations as solvents under different temperatures and reaction times for the first time. The structural properties and fluorescence behaviour of the AIE-CDs were investigated. The results revealed that the sulfuric acid concentration had a significant effect on the fluorescence colour of the AIE-CDs because sulfuric acid can affect the degree of carbonisation, the type and content of nitrogen. Moreover, the reaction temperature and time affected the surface-defect state and the degree of carbonisation of the AIE-CDs, which affected the emission wavelength and quantum yield (QY) of the AIE-CDs. Furthermore, to exploit the unique characteristics (polychromatic aggregation fluorescence and acid-sensitive properties) of the obtained-AIE-CDs, anti-counterfeiting and information encryption methodologies (i.e., acid-stimuli-response producing multi-colour fluorescence) were preliminarily developed. Finally, B-AIE-CDs with a high QY of 43.5% were successfully used for rapid cytoplasmic imaging, demonstrating their applicability in biological fields.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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