LANGMUIR
·
2021
·
IF 3.882
Cong Xie,Yubin Zhao,Wenbin Shi,Ping Yang
The existing defects on the surface of CsPbX3 nanocrystals (NCs) resulted in the decrease of the photoluminescence quantum yields (PLQYs) of NCs. In this study, we developed a simple strategy, which can make the treated CsPbX3 NCs exhibit high PLQYs and better stability by CdX2 post-treatment at room temperature. The treated CsPbX3 NCs were characterized by X-ray diffraction (XRD) patterns and PL spectra. The shape, size, and crystal structure of the NCs remained unchanged after Cd ion treatment. The PLQYs of CsPbCl3 increased from 24 to 73% and the PLQYs of CsPbBr3 NCs increased from 85 to 92% after treatment. The significant enhancement of PLQYs is ascribed to the effective passivation of surface defects, in which Cd2+ and X– ions occupied the Pb–X vacancies existing on the surface of the NCs. In addition, this strategy was also applied to a mixed halide perovskite. The practical application of CsPbX3 NCs will be extended by this method.
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高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Yingcui Bu,Xiaojiao Zhu,Haoran Wang,Jie Zhang,Lianke Wang,Zhipeng Yu,Yupeng Tian,Hongping Zhou,Yi Xie
Considering the multiple biological barriers before the entry of photosensitizers (PSs) into cytoplasm, it is of paramount importance to track PSs to elucidate their behaviors and distributions to guide the photodynamic therapy (PDT). Also, the developed PSs suffer from strong oxygen dependency. However, reports on such ideal theranostic platforms are rare. Herein, we developed a theranostic platform (CMTP-2) based on the coumarin-based D-π-A system, which, for the first time, can reveal the holistic intracellular delivery pathway and near-infrared (NIR)-activated mitophagy to guide synergistic type-I PDT and photothermal therapy. The dynamic endo-lysosomal escape of CMTP-2 was monitored, as well as its changeable distributions in endosomes, lysosomes, and mitochondria, demonstrating the preferential accumulation in mitochondria at the end. Upon NIR-I irradiation, CMTP-2 generated toxic radicals and heat, triggering the execution of mitophagy and apoptosis. In vivo experiments on mice indicated that CMTP-2 under 808 nm irradiation realized complete cancer ablation, showing great potential for advancements in synergistic phototherapy.
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高影响因子
Solar RRL
·
2021
·Vol. 5
·期 9
·2100292
·
IF 8.582
Junzhuo Li,Zhaohui Ruan,Lei Zhu,Yudong Li,Xianzhu Xu,Yulin Yang,Yuan Yuan,Kaifeng Lin
Heteroatoms doping and morphology design have been considered as effective approaches to enhancing the photocatalytic activity of graphitic carbon nitride (g-C 3 N 4 ), whereas few of them have focused on the synergistic effect of codoping and the optical property of the porous structure during the catalytic process. Herein, a porous g-C 3 N 4 sphere codoped with K and I is designed and prepared to investigate the different roles played during the reaction. Compared with the pristine carbon nitride, the activity of the prepared catalyst increased by 7.9 times to 75.2 μmol h −1 . Experimental results with density function theory calculations indicate the different roles of two elements played during the photocatalysis process and optical simulations are given to prove the enhancement of the porous structure in light absorption ability. The pore structure improves the light absorption and mass transfer capabilities of the catalyst, while the codoping of metal and nonmetal develop the separation capabilities of the carriers and optimize the energy band structure respectively, which synthetically lead to an enhanced performance of the photocatalysis.
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CHEMICAL PHYSICS LETTERS
·
2021
·
IF 2.328
Ziyu Pan,Bin Liu,Bo Wang,Yingchao Liu,Tingyu Si,Wencai Yi,Yangqing Wu,Jinkai Li,Bingqiang Cao
Lead-free double-perovskite Cs 2 SnX 6 (X = Cl, Br, I) containing Sn 4+ is a more stable lead-free photovoltaic material than its homologue CsSnX 3 . However, its stability in air still affects its application. In this Letter, lead-free inorganic Cs 2 SnX 6 (X = Cl, Br, I) nanocrystals (NCs) were synthesized by a hot injection method and in-situ loaded into mesoporous SiO 2 . With the change of halogen content, the PL emission peak of pristine Cs 2 SnX 6 NCs were tuned from 430 nm to 780 nm covering the visible and near infrared spectrum region. Taking Cs 2 SnI 6 /SiO 2 NCs as an example, the optical property stability in solution is obviously improved, and it can be stored in air for over 2 h. Especially, the more stable NIR emission, non-toxicity and easy hydrolysis characteristics of Cs 2 SnX 6 /SiO 2 composite nanoparticles will have potential medical applications like photothermal and photodynamic therapies for cancers.
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高影响因子
Acta Biomaterialia
·
2024
·
IF 9.4
Xing Zhao,Xi Wu,Ranran Shang,Huachao Chen,Ninghua Tan
The Golgi apparatus (GA) is a vital target for anticancer therapy due to its sensitivity against reactive oxygen species (ROS)-induced oxidative stress that could lead to cell death. In this study, we designed a series of aggregation-induced emission (AIE)-based photosensitizers (TPAPyTZ, TPAPyTC, TPAPyTI, and TPAPyTM) carrying different ROS with selective GA-targeted ability. The in vitro study showed that TPAPyTZ and TPAPyTC displayed strong AIE characteristics, robust type-I/II ROS production capabilities, specific GA-targeted, high photostability, and high imaging quality. The cell-uptake of TPAPyTZ was found primarily through an energy-dependent caveolae/raft-mediated endocytosis pathway. Remarkably, TPAPyTZ induced GA-oxidative stress, leading to GA fragmentation, downregulation of GM130 expression, and activation of mitochondria caspase-related apoptosis during photodynamic therapy (PDT). In vivo experiments revealed that TPAPyTZ significantly inhibited tumor proliferation under lower-intensity white light irradiation with minimal side effects. Overall, our work presents a promising strategy for designing AIEgens for fluorescence imaging-guided PDT. Additionally, it enriched the collection of GA-targeted leads for the development of cancer theranostics capable of visualizing dynamic changes in the GA during cancer cell apoptosis, which could potentially enable early diagnosis applications in the future. Statement of significance AIE luminogens (AIEgens) are potent phototheranostic agents that can exhibit strong fluorescence emission and enhance ROS production in the aggregate states. In this study, through the precise design of photosensitizers with four different electron-acceptors, we constructed a series of potent AIEgens (TPAPyTZ, TPAPyTC, TPAPyTM, and TPAPyTI) with strong fluorescence intensity and ROS generation capacity. Among them, TPAPyTZ with an extended π-conjugation displayed the strongest ROS generation ability and anti-tumor activity, resulting in an 88% reduction in tumor weight. Our studies revealed that the enhanced activity of TPAPyTZ may be due to its unique Golgi apparatus (GA)-targeted ability, which causes GA oxidative stress followed by effective cancer cell apoptosis. This unique GA-targeted feature of TPAPyTZ remains rare in the reported AIEgens, which mainly target organelles such as lysosome, mitochondria, and cell membrane. The successful design of a GA-targeted and potent AIEgen could enrich the collection of GA-targeted luminogens, providing a lead theranostic for the further development of fluorescence imaging-guided PDT, and serving as a tool to explore the potential mechanism and discover new GA-specific drug targets.
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DOI
PubMed
高影响因子
LANGMUIR
·
2021
·
IF 3.882
Sai-Nan Guo,Hao Wu,Dan Wang,Jie-Xin Wang
Lead halide perovskite quantum dots (QDs) are known as prospective optoelectronic device materials because of their excellent luminescence, extraordinary photoelectric performance, and specific octahedron framework. Herein, we report a cost-effective approach for synthesizing highly stable CH3NH3PbBr3 QDs in low-polarity binary solvents without nitrogen protection. The CH3NH3PbBr3 QDs are tunable from 1.2 to 4.2 nm by adjusting the proportion of oleic acid and oleylamine as capping ligands. The photoluminescence quantum yield of CH3NH3PbBr3 QDs can reach 87.4%. The fluorescence can maintain over 80% of its earliest emission intensity under the atmosphere after 5 days, which is much better than that (∼10%) of QDs with ligand-assisted reprecipitation. The possible reaction mechanism of preparing CH3NH3PbBr3 QDs was also addressed. Notably, such a strategy can be applied extensively in the preparation of other lead halide perovskite QDs. Furthermore, the as-prepared thick PMMA-coated CH3NH3PbBr3 QDs were further conjoined with a red luminescence powder on a blue InGaN chip to obtain a powerful efficiency (45.4 lm W–1) warm white light-emitting diode.
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Green Synthesis and Catalysis
·
2024
·
IF 8.2
Shaixiao Tian,Xinying Ge,Qipeng Yan,Min Li,Qun Huang,Xinhua Zhang,Ming Ma,Bo Chen,Jian-bo Wang
We report for the first time the combination of directed evolution focused on enhancing and reversing the stereoselectivity of an enzyme with Cu(I)-mediated click chemistry (CuAAC), providing an asymmetric click approach for versatile chiral triazoles products. In this study, the halohydrin dehalogenase HheG was used as the enzyme which was evolved to induce a stereoselective ring-opening reaction of cyclic epoxides in the presence of NaN 3 with the formation of chiral azido products. Two mutants of opposite stereopreference were generated, which convert cyclohexene oxide as well as cycloheptene oxide to (1 S , 2 S )-2-azidocyclohexanol, (1 R , 2 R )-2-azidocyclohexanol, (1 S , 2 S )-2-azidocycloheptanol and (1 R , 2 R )-2-azidocycloheptanol with essentially high stereoselectivity. The chiral products were then subjected to CuAAC in reactions with structurally different alkynes. Since HheG was found to be compatible with Cu(I), the process was also performed successfully in a unique 2-step one-pot process leading to various chiral triazoles. In order to understand the enhancement and reversal of the evolved enantioselectivity, QM and MD computations were performed. This approach harnesses the modifiability and high stereoselectivity of the evolved biocatalysts in combination with click chemistry. It holds great potential for diverse fields, particularly in the area of pharmaceuticals.
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Small
·
2024
·
IF 13
Jing Gao,Yuan Gao,Jinghua Hao,Xiaolin Sun,Fuhua Zhao,Yuan Zhang,Wenyan Si,Jianfei Wu
All-solid-state lithium sulfide-based batteries (ASSLSBs) have drawn much attention due to their intrinsic safety and excellent performance in overcoming the polysulfide shuttle effect. However, the sluggish kinetics of Li 2 S cathode severely impede commercial utilization. Here, a Cu + , I − co-doping strategy is employed to activate the kinetics of Li 2 S to construct high-performance ASSLSBs. The electronic conductivity and Li-ion diffusion coefficient of the co-doped Li 2 S are increased by five and two orders of magnitude, respectively. Cu + as a redox medium greatly improves the reaction kinetics, which is supported by ex situ X-ray photoelectron spectroscopy. Density functional theory calculation (DFT) shows that Cu + , I − co-doping reduces the Li-ions diffusion energy barrier. The co-doped Li 2 S exhibits a remarkable improvement in capacity (1165.23 mAh g −1 (6.65 times that of pristine Li 2 S) at 0.02 C and 592.75 mAh g −1 at 2 C), and excellent cycling stability (84.58% capacity retention after 6200 cycles at 2 C) at room temperature. Moreover, an ASSLSB, fabricated with a lithium-free (Si─C) anode, obtains a high specific capacity of 1082.7 mAh g −1 at 0.05 C and 97% capacity retention after 400 cycles at 0.5 C. This work provides a broad prospect for the development of ASSLSBs with practical energy density exceeding that of traditional lithium-ion batteries.
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INORGANICA CHIMICA ACTA
·
2021
·
IF 2.545
Tian-Cheng Wu,Qiao-Long Hu,Ting-Hong Huang,Yi-Shun Cui,Dan Zheng,Changyan Ji,Cheng Luo
A series of copper(I) - diimine complexes, [Cu(bdpp)(bpy)]BF 4 ( 1 ), [Cu(bdpp) (pen)]BF 4 ( 2 ), [Cu(bdpp)(damp)]BF 4 ( 3 ), [Cu(bdpp)(pen)]BF 4 ( 4 ) (bdpp = 4,6-bis-(biphenyl phosphino) phenoxazine, bpy = 2,2′-bipyridine, phen = 1,10-Phenanthroline, dmp = 2,9-dimethyl-1,10-phenanthroline, bphen = 4,7-diphenyl-1,10-phenanthroline), have been synthesized and characterized by IR, 1 H NMR, 31 P NMR, XRD and X-ray crystal structure analysis. Structural analysis reveals that each Cu + in 1 – 4 is four-coordinated by two N atoms and two P atoms and adopts a distorted tetrahedral geometry. DFT calculations show that the HOMOs in 1 – 4 are mainly comprised of bdpp and copper d–orbitals, while the LUMOs are mainly dominated by diimine ligands. Calculation of atomic charges indicates that the charges of the central Cu atoms in 1 – 4 are less than + 1, and the diimine ligands may be the key to the metal charge transfer to the coordinated atom. In 1 – 4 , the maximum phosphorescent lifetimes and quantum yields are up to 349 μs and 22%, respectively. Moreover, complex 3 is used for fabricating the LED device, showing a decent performance with the maximum EQE of 11%.
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高影响因子
CERAMICS INTERNATIONAL
·
2020
·
IF 3.83
Fei He,Wenjie Li,Lijuan Yang,Zhen Zhu,Liang Zhou,Xin Zhang,Xiaodong He
Unidirectional alumina aerogels (AAs) were prepared by simultaneously using boehmite hydrosols and alumina nano-powder as solid solutes at different freezing temperatures. In order to understand the porous structural characteristics under different freezing parameters, the real-time frozen parameters were recorded at the designated positions under different freezing temperatures. Fourier transform infrared (FT-IR) spectra, X-ray diffraction (XRD), mercury intrusion porosimetry (MIP) and scanning electron microscopy (SEM) were used to investigate the functional groups, phase composites, microstructures and porous characteristics. The regularities and influence factors of unidirectional porous structures of AAs were detailedly explored under different frozen parameters. The results show that the AAs are characterized with unidirectional porous structures at the direction of ice-crystal growth. The cooling rate and ice front rate ( v inf ) increase and the structure wavelengths ( λ s) decrease with the decrease of the freezing temperature. The relationship between λ and v inf approximately satisfies a power law, which perhaps is related to the uniform dilute solution containing nanoparticle .
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Dandan Li,Wenrong Zhao,Gang Li,Yan Xu,Liang Xu,Bo Tang
Graphical Two novel star-shaped fluorophores named PDI−S and PDI−Se are constructed by S/Se-fused perylene diimides (PDIs) connected with bicarbazole core. Particularly, PDI−S presents excellent two-photon absorption cross-action (δ TPA ) of 3775 GM excited with 800 nm light, which is the highest value based on PDIs motif in the NIR−I region (700–900 nm). Two-photon absorption (TPA) has attracted growing attention over recent years owing to the wide range of applications in organic nonlinear optical (NLO) materials. The quantitative sensitivity of a two-photon molecular entity is determined by its TPA cross-section (δ TPA ). Perylene diimides (PDIs) are excellent n-type organic semiconductor materials demonstrating distinguished thermal, optical, and chemical stability. Nonetheless, PDIs-based scaffolds exhibit poor δ TPA in the NIR−I region (700–900 nm) due to the lack of suitable molecular design. Here, two novel star-shaped PDIs fluorophores, namely PDI−S and PDI−Se, were constructed by four periphery S/Se-fused PDIs connected with bicarbazole core. PDI−S manifested excellent δ TPA of 3775 GM, which are among the highest values reported for PDIs excited in the NIR−I region.
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PubMed
高影响因子
APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Lin Yuan,Yufeng Zhou,Ze Wang,Enrou Mei,Xiaojuan Liang,Weidong Xiang
Colloidal lead halide perovskite nanocrystals (NCs) have recently emerged as versatile photonic sources. However, their performance stability has been far from the requirements, and this type of material is toxic to the environment after degradation. In this paper, a hot injection strategy was used to prepare a CsPbX 3 perovskite NC solution, wherein the photoluminescence quantum yield (PLQY) of CsPbBrI 2 reached 78% and that of CsPbBr 3 was 63%. Then, CsPbX 3 NCs are successfully adsorbed on natural layered mineral pyrophyllite for improving heat, light, and water stability. Monodispersed CsPbX 3 NCs are evenly distributed on the surface of the pyrophyllite sheet in a high-density manner, which possibly originates from the electrostatic attraction effect of abundant anions on the surface of pyrophyllite to CsPbX 3 NCs. In a series of CsPbX 3 @pyrophyllite nanocomposites prepared, the PLQYs of green-emitting CsPbBr 3 and red-emitting CsPbBrI 2 were 47% and 29%, respectively. The materials were employed to fabricate white light-emitting diodes (WLEDs) with a wide color gamut of 117%. Importantly, because of the swelling and cation-adsorbent properties of pyrophyllite, the dissolution of lead in water was greatly reduced, which plays a certain role in ecological protection.
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危险品化学品经营许可证（带存储）