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LANGMUIR · 2021 · IF 3.882

Cost-Effective Strategy for the Synthesis of Air-Stable CH3NH3PbX3 (X = Cl, Br, and I) Quantum Dots with Bright Emission

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.

研究领域: 材料科学 · 光学工程 · 化学
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Acta Biomaterialia · 2024 · IF 9.4

A structure-guided strategy to design Golgi apparatus-targeted type-I/II aggregation-induced emission photosensitizers for efficient photodynamic therapy

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.

研究领域: 癌症研究 · 药学 · 生物医学工程 · 材料科学 · 细胞生物学
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Journal of Materials Chemistry A · 2023 ·Vol. 11 ·期 20 ·10766-10775 · IF 11.9

Direct hydrogenation of CO2 to ethanol at ambient conditions using Cu(I)-MOF in a dielectric barrier discharge plasma reactor

Nan Zou,Jie Chen,Ting Qiu,Ying Zheng

Direct hydrogenation of CO2 to ethanol is a highly economical carbon reduction strategy. However, the CO2 hydrogenation process traditionally requires high temperatures, typically higher than 300 °C, to activate CO2 molecules, which is unfavorable to the formation of ethanol. In contrast, we applied the novel non-thermal plasma to activate CO2 at ambient conditions and a Cu(I)-MOF catalyst to selectively synthesize ethanol for the selective transformation of CO2 into ethanol. The best catalyst, Cu(I)-HKUST-17.5, achieved 41.2% CO2 conversion and up to 62.9% ethanol selectivity under ambient conditions. The control experiments indicated that the Cu(I) sites are key to realizing C–C coupling and ethanol synthesis. An unreported synergistic catalytic mechanism between non thermal plasma and the Cu(I) and Cu(II) sites on the catalyst is proposed based on the DRIFTS analysis. Overall, our work confirms the feasibility of utilizing non thermal plasma assisted catalysis for the selective conversion of CO2 to ethanol under mild conditions.

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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

Assessment of solid–liquid equilibrium behavior and thermodynamic analysis of natural plant extracts artemisinin (Form I) in twelve mono-solvents

Pengshuai Zhang,Haiyan Luo,Lan Cui,Jixiu Deng,Shiyu Xie,Danfeng Liu,Shuqi Wang,Xiaoying Si,Zichao Wang,Yameng Wan,En Zhang,Xing Li,Lu Zhang

Solid-liquid equilibrium solubility of artemisinin (ART) Form I in twelve mono-solvents namely N, N-dimethylformamide (DMF), oxolane (THF), n -propanol (NPA), 4-methylpentan-2-one (MIBK), ethyl formate (EF), butyl acetate (BAC), 2-ethoxyethanol (EGEE), 1,4-Dioxane, 2-methoxyethanol (EGME), 2-propoxyethanol (EGPE), propyl acetate (NPAC) and 2-butoxyethanol (EGBE) from 283.15 K to 323.15 K were determined by a laser dynamic method under 0.1 MPa. The minimum solubility of ART (Form I) was found in NPA at 283.15 K (0.004541), the maximum mole fraction solubility of ART (Form I) was observed as 0.2523 in DMF at 323.15 K. At the temperature of 298.15 K, the experimental mole fraction solubility order of ART Form I in the tested solvents was DMF (0.1559) > 1,4-Dioxane (0.09117) > THF (0.08301) > MIBK (0.05054) > EF (0.04902) > NPAC (0.03860) > BAC (0.03658) > EGME (0.02031) > EGEE (0.01859) > EGPE (0.01817) > EGBE (0.01689) > NPA (0.007185). The solubility behavior was computationally correlated by Margules model, Wilson model, NRTL model, NRTL-SAC model, Buchowski-Ksiazczak λh model and UNIQUAC model, the total RMSD was no>0.025 in the selected models. With the help of Hansen solubility parameters (HSPs) analysis, molecular similarities of ART (Form I) in twelve mono-solvents were investigated. Besides, Hirschfeld surface analysis (HSs) was considered to evaluate the intermolecular interaction of artemisinin. Moreover, thermodynamic properties including Δ mix H , Δ mix G , Δ mix S , lnγ 1 , l n γ 1 ∞ lnγ1∞ of ART (Form I) in the selected solvents were estimated. All the negative Δ mix G and positive Δ mix S values indicated that the mixing process were spontaneous and entropy-increasing.

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JOURNAL OF COORDINATION CHEMISTRY · 2022 · IF 1.869

Synthesis, characterization and discussion of two copper(I) complexes with different luminescent properties under the influence of multiple weak forces

Chengjie Gao,Zhenzhou Sun,Ning Zhu,Hongliang Han,Zhongfeng Li,Chaoyue Gu,Yuping Yang,Xiulan Xin,Qiming Qiu,Wei Yang,Guo Wang,Qionghua Jin

Two new complexes, [Cu(dmp)(2-bdppmapy)](CF3SO3)·CH2Cl2 (1) and [Cu(imidazo[4,5-f])(2-bdppmapy)](SCN) (2) (2-bdppmapy = N,N-bis[(diphenylphosphino)methyl]-2-pyridinamine, dmp = 2,9-dimethyl-(1,10)phenanthroline and imidazo[4,5-f] = 1H-imidazo[4,5f][1,10]phenanthroline), have been synthesized in mixed solvents of CH3OH and CH2Cl2 (1:1, V/V). On the basis of studying the structure and photophysical properties of the Cu(I) complexes, the effects of different N ligands and counter anions on the luminescence properties of the Cu(I) complexes were characterized by single-crystal X-ray diffraction, fluorescence spectra and terahertz time-domain spectroscopy (THz-TDS). The research shows that 1 exhibits excellent photoluminescence quantum yields. It is ascribed to the unique stacked structure. In addition, the relationship between the multiple weak forces, structure, and photophysical properties of the complexes was investigated.

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RSC Advances · 2022 ·Vol. 12 ·期 55 ·36012-36017 · IF 4.036

Colorimetric/photothermal dual-mode sensing detection of ascorbic acid based on a Ag[I] ion/3,3′,5,5′-tetramethylbenzidine (TMB) system

Ya Di,Jiyao Zheng,Yunwang Zhao,Zikai Yang,Changshun Xie,Jiahan Yu,Yue Zheng,Liming Gao

In this work, a novel strategy of colorimetric and photothermal dual-mode sensing determination of ascorbic acid (AA) based on a Ag+/3,3′,5,5′-tetramethylbenzidine (TMB) system was developed. In this sensing system, Ag+ could oxidize TMB with a distinct color change from colorless to blue color, strong absorbance at 652 nm and a photothermal effect under 808 nm laser irradiation due to the formation of oxidized TMB (oxTMB). When AA was present, oxTMB was reduced accompanied by a change from blue to colorless, and a decrease in absorption peak intensity and the photothermal effect. AA concentration showed a negative linear correlation with the value of both the absorbance intensity at 652 nm and temperature in the range of 0.2–10 μM (A = −0.03C + 0.343 (R2, 0.9887; LOD, 50 nM); ΔT = −0.57C + 8.453 (R2, 0.997; LOD, 7.8 nM)). Based on this, a sensing approach for detection of AA was proposed with dual-mode and without the complicated synthesis of nanomaterials. The photothermal effect and colorimetric signal provided a dual-mode detection strategy for AA, overcoming the limitations of any single mode. This colorimetric and photothermal dual-mode detection has great potential in the detection of AA in clinical pharmaceuticals and the construction of portable and highly sensitive sensors.

CAS / MDL: 7761-88-8 54827-17-7
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Journal of Materials Chemistry C · 2023 ·Vol. 12 ·期 4 ·1386-1395 · IF 6.4

Solution-processed copper(I) iodide via co-doping for enhanced hole selective contacts in p-type crystalline silicon solar cells

Wang Fu,Wuqi Liu,Yaju Wei,Dan Liu,Songyu Li,Di Zhao,Xiaoping Wu,Lingbo Xu,Ping Lin,Can Cui,Xuegong Yu,Peng Wang

In studies addressing contact recombination, carrier-selective contacts (CSCs) have played a key role in crystalline silicon (c-Si) solar cells resulting in a higher photoelectrical conversion efficiency (PCE). Recently, wide-bandgap metal compound materials with extreme work functions or suitable energy band alignment have drawn considerable interest for CSC materials. Among them, cuprous iodide (CuI) is a very promising hole-selective layer, however, very little research has been conducted for c-Si solar cells. In this work, we have demonstrated that solution-processed CuI films act as effective full-area hole-selective contact layers for p-Si solar cells. Moreover, iodine (I2) doping suppresses the generation of I− vacancies (VI), and enhances the film conductivity due to an increase in copper vacancies (VCu). Aluminum ion (Al3+) doping further promotes the generation of more VCu and increases the work function of the CuI film. The proposed I2 and Al3+ co-doping strategy for CuI films significantly improves the passivating contact performance of the Al3+–I2:CuI/p-Si heterojunction, contributing to the significantly improved PCE from 15.12% to 18.28%, which is the highest for solution-processed copper-based hole transport layers for c-Si solar cells to date. The results demonstrate the great potential of the CuI hole-selective layer applied for highly efficient c-Si solar cells.

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ACS Nano · 2023 · IF 17.1

Interfacial Engineering of In2Se3/h-BN/CsPb(Br/I)3 Heterostructure Photodetector and Its Application in Automatic Obstacle Avoidance System

Yingying Niu,Xin Zhou,Wei Gao,Maixia Fu,Yule Duan,Jiandong Yao,Bing Wang,Mengmeng Yang,Zhaoqiang Zheng,Jingbo Li

Driven by the rapid development of autonomous vehicles, ultrasensitive photodetectors with high signal-to-noise ratio and ultraweak light detection capability are urgently needed. Due to its intriguing attributes, the emerging van der Waals material, indium selenide (In2Se3), has attracted extensive attention as an ultrasensitive photoactive material. However, the lack of an effective photoconductive gain mechanism in individual In2Se3 inhibits its further application. Herein, we propose a heterostructure photodetector consisting of an In2Se3 photoactive channel, a hexagonal boron nitride (h-BN) passivation layer, and a CsPb(Br/I)3 quantum dot gain layer. This device manifests a signal-to-noise ratio of 2 × 106 with responsivity of 2994 A/W and detectivity of 4.3 × 1014 Jones. Especially, it enables the detection of weak light as low as 0.03 μW/cm2. These performance characteristics are ascribed to the interfacial engineering. In2Se3 and CsPb(Br/I)3 with type-II band alignment promote the separation of photocarriers, while h-BN passivates the impurities on CsPb(Br/I)3 and promises a high-quality carrier transport interface. Furthermore, this device is successfully integrated into an automatic obstacle avoidance system, demonstrating promising application prospects in autonomous vehicles.

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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Manganese and oxygen dual-doping MoS2 boosts reduction and adsorption activity toward efficient recovery of gold(I) from thiosulfate solutions

Yumeng Liang,Weiquan Zhan,Yuan Yuan,Noe Zamora-Romero,Feifei Jia,Bingqiao Yang,Zamoniddin Nasrddinov,José Luis Arauz-Lara,Shaoxian Song

The necessity for application of molybdenum disulfide (MoS 2 ) in photocatalytic reduction field required speedy improvement with high reduction and adsorption performance. Here, manganese (Mn) and oxygen (O) dual-doping strategy were taken for demonstrating that enhancing photocatalytic reduction could achieve simultaneous modulation of the reduction and adsorption parameters by optimizing the electronic configuration and hydrophilicity ability in MoS 2 . Benefiting from the Mn and O dual-doping collective effect, the developed Mn,O-MoS 2 exhibited outstanding photocatalytic reduction and recovery performances of gold(I) from thiosulfate leaching solutions with reduction capacity of 1386.98 mg/g and the corresponding recovery of 92.50%. Besides, Mn and O atoms dual doping in MoS 2 accelerated the recovery rate, which was 3 folds higher compared with that of MoS 2 . Experimental and first-principle approaches suggested that the reduction and adsorption ability of MoS 2 were strengthened through tuning the electronic structure and surface property with Mn and O dopants : (1) Mn atoms notably enhanced the conductivity and optimized the electronic structure for facilitating the reduction performance; (2) The incorporated O atoms greatly promoted the adsorption of [Au(S 2 O 3 ) 2 ] 3- by improving the affinity of water molecules and Mn,O-MoS 2 . The work provides a promising strategy to manipulate two-dimensional materials for various applications about catalysts and adsorbent.

CAS / MDL: 7783-18-8
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Catalysis Science & Technology · 2022 ·Vol. 12 ·期 21 ·6416-6426 · IF 6.177

Mild and highly selective hydrogenation of cyclohexyl acetate to cyclohexanol over Cu(I) coordinated amino-functionalized poly(ionic liquid)s

Binxiong Guang,Wei Zhang,Yiwei Zhang,Yahui Xiao,Yong Liu

A novel, efficient and economical process of cyclohexanol (CHOL) production based on cyclohexene esterification–hydrogenation has become a research hotspot in recent years. Wherein, hydrogenation of cyclohexyl acetate (CHA) derived from the esterification of cyclohexene with acetic acid is a crucial step. Combining the advantages of metal complexes and heterogeneous catalysts, the robust Cu(I) coordinated amino-functionalized poly(ionic liquid)s (PILs-Cu(I)) were, in this research, synthesized for use in the mild and highly selective hydrogenation of CHA to CHOL. The results of FT-IR, UV-vis, BET, XPS and SEM-EDS confirmed that the Cu(I) was dominant in the PILs-Cu(I), and was homogeneously and stably coordinated on the amino-functionalized poly(ionic liquid)s. Benefiting from that, the PILs-Cu(I) was endowed with an unprecedented performance in the mild and highly selective hydrogenation of CHA to CHOL. Specifically, 95.6% CHA conversion with 96.6% selectivity of CHOL, and 97.0% selectivity of ethanol was obtained under extremely mild conditions of 80 °C and 2 MPa H2. Furthermore, no significant activity loss was observed over the PILs-Cu(I) after recycling for at least five times, delivering excellent stability and reusability.

CAS / MDL: 75-05-8
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Improved photocatalytic activity of Bi2MoO6 by modifying the halogen ions (Cl−, Br−, or I−) for photoreduction of N2 into NH3

Dekun Shi,Zhaojun Shi,Lixin Zhang,Yaan Cao

A series of halogen ions (Cl − , Br − , or I − ) modified Bi 2 MoO 6 (Bi 2 MoO 6 –Cl, Bi 2 MoO 6 –Br, or Bi 2 MoO 6 –I) are synthesized via a one-step solvothermal method . It is determined that the halogen ions (Cl − , Br − , or I − ) are modified on the surface of Bi 2 MoO 6 as the -Bi-Cl, -Bi-Br, or -Bi-I species (the connected Bi 3+ is coordinated with three lattice O2- ions in Bi 2 MoO 6 ). The -Bi-Cl, -Bi-Br, or -Bi-I species on the Bi 2 MoO 6 surface can act as highly active sites to polarize and activate the N 2 and H 2 O molecules adsorbed on the surface of catalysts. Moreover, due to the surface-modified -Bi-Cl, -Bi-Br, or -Bi-I species, the visible light absorption is improved, the separation of photogenerated charge carriers is promoted, as well the band structure is better matched with the redox potential of photoreduction of N 2 . As a result, the photocatalytic activity of Bi 2 MoO 6 –Cl, Bi 2 MoO 6 –Br, or Bi 2 MoO 6 –I is improved for photoreduction of N 2 into NH 3 compared with Bi 2 MoO 6 . Overall, this work provides new insights into the doping states of halogen ions, the surface-active sites, the band structure, the photocatalytic activity, and the mechanism for photoreduction of N 2 into NH 3 for Bi 2 MoO 6 with modification of halogen ions (Cl − , Br − , or I − ).

CAS / MDL: 64-17-5 10035-06-0
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CERAMICS INTERNATIONAL · 2022 · IF 5.532

All-inorganic halide perovskite (CsPbX3, X=Cl, Br, I) quantum dots synthesized via fast anion hot injection by using trimethylhalosilanes

Zhangwen Long,Shuai Yang,Jiacheng Pi,Dacheng Zhou,Qi Wang,Yong Yang,Hao Wu,Jianbei Qiu

All-inorganic metal halides perovskites , such as CsPbX 3 quantum dots (QDs), are high-performance photoelectric materials ; they have attracted considerable attention for applications such as LEDs and laser and solar cells. Herein, we report an anion hot injection (HI) method to prepare CsPbX 3 (X = Cl, Br, I, Cl/Br, and Br/I) QDs using trimethylhalosilane (TMXS) as a halogen ion donor. By adjusting the ratio of different TMXSs (trimethylchlorosilane, trimethylbromosilane, and trimethyliodosilane), the synthesized samples can achieve tunable emission in the range of 416–710 nm, narrow emission line widths of 13–33 nm, and luminescence lifetimes of 32–223 ns. These QDs also have better stability in external environment compared with those obtained using traditional HI method.

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