Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 16
·2969-2978
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IF 5.958
Jie-hao Li,Jie Ren,Ying Liu,Hui-ying Mu,Rui-hong Liu,Jun Zhao,Lan-ju Chen,Fa-tang Li
In this paper, a novel ionic liquid-assisted solvothermal method to prepare Cl-doped bismuth oxycarbonate (Bi2O2CO3) is presented. The ionic liquid of [Hnmp]Cl not only enhances the solvothermal process to help the formation of Bi2O2CO3, but also provides chloride element as a dopant. XRD and XPS show that all three samples are Bi2O2CO3 with high purity. XPS, solid EPR, and TEM results prove that Cl is doped into the Bi2O2CO3 lattice and oxygen vacancies are generated. DRS results show that after Cl doping, the absorption of visible light by Bi2O2CO3 is enhanced. Surface photovoltage (SPV) and transient photocurrent tests show that as the doping amount of Cl increases, the separation efficiency of photogenerated electron–hole pairs over Bi2O2CO3 improves. The photocatalytic activity of Bi2O2CO3 is evaluated by the degradation of rhodamine B, which is increased after Cl doping. This work would broaden the application of ionic liquids in the solvothermal process and deepen the understanding of anionic ion doping in Bi2O2CO3.
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ACS Catalysis
·
2021
·
IF 13.084
Yiwen Yang,Haifeng Qi,Huixiang Li,Zhanwei Xu,Xiumei Liu,Shuyin Yu,Zongchao Conrad Zhang
Efficient hydrolysis of β-1,4-glycosidic bonds of cellulose is a pivotal step in biorefineries of cellulosic biomass. In this work, we discovered that paired PdCl2–CuCl exhibited excellent synergetic catalytic activity over the single PdCl2 or CuCl in the hydrolysis of β-1,4-glycosidic bonds in 1-butyl-3-methylimidazolium chloride ([BMim]Cl) and further investigated the catalytic species in this system. The catalytic activity increased and reached a plateau at a CuCl/PdCl2 ratio of 1 with increasing molar ratio of CuCl/PdCl2 while keeping the Pd concentration constant. A combination of experimental evidence based on in situ far-infrared absorption, X-ray absorption, X-ray photoelectron, and electron paramagnetic resonance spectroscopies and DFT calculations demonstrate the coupling reaction between [PdIICl4]2– and [CuICl3]2– via the Cl bridge to form the heterometallic complex anion [Cl2PdII–Cl–CuICl2]2–. The heterometallic species is stable during the reaction and maintains its catalytic performance in the presence of various oxygenate additives. Using paired PdCl2–CuCl as a catalyst, the activation energy of hydrolytic cleavage of β-1,4-glycosidic bonds of cellobiose is determined as low as 95.8 kJ/mol. PdCl2–CuCl/[BMim]Cl combined with CrCl3 can be reused five times in cellobiose conversion to 5-hydroxymethylfurfural (5-HMF) without an apparent decrease of catalytic activity. The performance of this catalytic system is further verified for efficient cellulose conversion. More than 60% product yield is obtained at 100 °C from the cellulose, affording monosaccharides for efficient production of high value-added chemicals, such as 5-HMF, when CrCl3 is present to catalyze the conversion of glucose to 5-HMF.
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OPTICAL MATERIALS
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2019
·
IF 2.687
Jidong Deng,Jiao Xun,Rongxing He
All-inorganic cesium lead halide perovskite nanocrystals (NCs) are promising photoelectric materials for their high photoluminescence quantum yield (PLQY), narrow emission width and tunable optical band gap. Traditionally, the hot injection (HI) method has been utilized to prepare perovskite NCs. However, the HI method requires high temperature, protection under inert gas and other harsh synthetic conditions, which severely hinders large-scale production of these NCs. Herein, we directly synthesized CsPbBr 3 perovskite NCs by a modified LARP (ligand-assisted re-precipitation) approach, and then conducted a specific anion exchange reaction with inexpensive, readily available, non-toxic, and non-polluting KX (X = Cl, I) salts aqueous solution to obtain various compositions of CsPbX 3 perovskite NCs at room temperature (RT). The obtained RT-NCs have high PLQY and outstanding stability, and their photoluminescence can be precisely regulated across the whole visible region (419–670 nm). The use of inorganic salts for the ion exchange provides an efficient method for the design of various halogenated perovskite NCs and their large-scale synthesis at RT.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2019
·Vol. 30
·期 5
·4446-4454
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IF 2.195
Wang Kai-Li,Li Yan,Sun Tao,Mao Fang,Wu Ji-Kui,Xue Bin
Co-doping is a promising approach to change the electronic structure and increase the photocatalytic ability of graphitic carbon nitride (g-C 3 N 4 ). Here, we reported a facile and green fabrication of Na, Cl co-doped g-C 3 N 4 photocatalysts. In the fabrication, sodium and chlorine were incorporated into g-C 3 N 4 synchronously. The bandgap of Na, Cl co-doped g-C 3 N 4 decreased compared with pure g-C 3 N 4 and the position of the valence band moved in the direction of enhanced oxidizing power. The co-doped photocatalysts exhibited the improved visible-light absorption and the reduced recombination rate of photogenerated electrons and holes. As a result, photocatalytic activity of Na, Cl co-doped g-C 3 N 4 was remarkably improved for the photodegradation of rhodamine B and tetracycline hydrochloride under visible light irradiation. The photocatalysis mechanism of Na, Cl co-doped g-C 3 N 4 was also discussed according to the results of active species trapping experiments.
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NANOTECHNOLOGY
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2018
·Vol. 30
·期 7
·075704
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IF 3.404
Weiwei Chen,Xiaosheng Tang,Zhigang Zang,Yue Shi,Zhaoqi Yang,Juan Du
Doping of Mn2+ into semiconductor nanocrystals has been demonstrated to endow them with novel electronic, optical and magnetic functionalities. In this paper, Mn-doped CsPbX3 (X = Br, Cl) quantum dots (QDs) were synthesized at room temperature via a facile strategy by introducing dimethyl sulfoxide (DMSO)-MnBr2/PbX2 composite as a precursor. The excitonic emission spectra of the as-obtained Mn-doped CsPbX3 QDs can be tuned from 517 nm to 418 nm by adjusting the ratio of PbBr2/PbCl2 precisely, and the luminescence mechanism of the doped QDs is discussed in detail. Moreover, the highest photoluminescence quantum yield of the Mn2+ emission achieves 36.7%, which is comparable with QDs prepared by the conventional hot-injection method. Depending on the ratios of PbPb2/PbCl2, the energy transfer rate from the band-edge to Mn2+ excited state is in the range of 0.006–20.42 × 107 s−1. Furthermore, white light-emitting diodes (LEDs) were successfully fabricated by combining the as-prepared Mn-doped CsPbX3 QDs with commercial UV GaN chips, and the high luminous efficiency of the as-prepared white LEDs was developed to 55.9 lm W−1. This work strongly supports the fact that Mn-doped CsPbX3 QDs are promising materials for application in lighting and displaying fields.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2013
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IF 3.172
Guangfang Li,Fan Qin,Runming Wang,Shengqiang Xiao,Hongzhe Sun,Rong Chen
A facile microwave irradiation method has been successfully developed for the controllable fabrication of BiOX (X = Cl, Br, I) nanostructures in mannitol solution. The morphology and size of BiOX nanostructures could be readily tailored by adjusting the amount of halide, reaction precursor, and mannitol concentration. Mannitol molecule acts as both a capping agent and a cohesive agent in the formation of BiOX nanostructures. A possible two-stage formation mechanism was discussed based on the morphology evolution of BiOI nanostructures obtained in mannitol solution with different concentrations. The as-synthesized BiOX nanostructures exhibit much higher photocatalytic activities than that of commercial TiO 2 . In particular, flower-like BiOX hierarchical nanostructures display the best photocatalytic performance, which is mainly ascribed to their unique hierarchical structure, high BET surface area, and large band gap. Moreover, BiOX nanostructures also demonstrate superior Cr(VI) removal capacity. The Cr(VI) adsorption behavior was also analyzed by the Langmuir and Freundlich adsorption isotherms.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
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2024
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IF 3
Zou Yanyan,Pau Dennis,Yi Linlin,Li Yaoqiang,Li Kaiyuan
13X zeolite–calcium oxide (CaO) composite capture agent application in the pyrolysis recovery of polyvinyl chloride (PVC)-based waste cables was investigated in this research to elucidate the agent’s efficiency in capturing chlorine (Cl) and carbon (C) during pyrolysis. The 13X zeolite–CaO mixture is subjected to separate pyrolysis of the PVC-based cable outer sheath in experimental furnaces of simulated solar-powered and thermogravimetry. Subsequently, a range of spectroscopic techniques are employed to quantitatively analyze the gaseous and solid products resulting from the pyrolysis process. Through X-ray fluorescence, total carbon, and other analyses, the research outcomes demonstrated that the capture agent exhibits superior Cl and C capture performance compared to using a single agent for plastic pyrolysis. The yield of Cl element in the solid residue has increased significantly by 130–140% under the presence of optimized composite capture agent. By determining the dynamic changes of gaseous and solid products during the cable outer sheath pyrolysis, the influence of the capture agent on the redistribution and transformation mechanisms of Cl and C elements was identified, and it was found that contaminating volatiles were well immobilized in the solid residue. This research provides a new solution for efficient Cl and C capture in the pyrolysis recovery of waste cables and determines the fixation and transformation mechanisms of Cl and C elements by the composite capture agent, indicating a potential for feasible and sustainable resource utilization of waste cables.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Yongfeng Liu,Yupeng Ying,Qingyu Xie,Zhaoju Gao,Xiuwen Shao,Min Zhou,Wei Pei,Xiaosheng Tang,Yusong Tu
Mixed-halide CsPb(Br/Cl)3 perovskite quantum dots (PeQDs) have attracted extensive attention in light-emitting diodes (LEDs), but their low photoluminescent efficiency and especially poor stability impede their practical applications. Here, we employ bifunctional didodecyldimethylammonium thiocyanide (DDASCN) with a pseudohalogen SCN– and branched DDA+ to obtain blue-emitting CsPbBr2Cl PeQDs. DDASCN significantly boosts the photoluminescence quantum yield to 92% by inhibiting nonradiative recombination. Importantly, DDASCN PeQDs show excellent stabilities against air, UV light, heat, and polar solvents. These improved performances were explained by density functional theory calculation, which shows that SCN– fills the Cl– vacancy by simultaneously binding with undercoordinated Pb2+ and Cs+, while DDA+ connects undercoordinated Br– and lies parallel to the PeQD core, leading to efficient passivation and a strong binding capacity. Finally, we achieved high-performance white LEDs by integrating our PeQDs, resulting in a color-rendering index of 92.9, a color gamut of 119.61%, and chromaticity coordinates of (0.33, 0.33). This provides an effective method to obtain efficient and stable CsPb(Br/Cl)3 PeQDs for practical applications.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Wanzheng Ren,Jian Pan,Zhuoqun Li,Min Huang,Lilan Huang,Liqiang Gu,Hailin Cong
The substrate membrane plays a crucial role in determining the performance of composite nanofiltration membranes prepared by interfacial polymerization (IP). In this study, persistent hydrophilic modification of polyvinylidene fluoride-co-chlorotrifluoroethylene (PVDF-CTFE) was achieved by incorporating N-methylglucamine (N-MG) without altering the membrane's morphology or pore size. Moreover, thin-film nanofibrous composite (TFNC) nanofiltration membranes were prepared using the surfactant assembly regulated interfacial polymerization (SARIP) method with the modified PVDF-CTFE@N-MG nanofibrous membrane as the substrate. The effect of N-MG addition on the substrate membrane's hydrophilicity and the structure and performance of the polyamide (PA) separation layer was investigated. The results showed that the addition of N-MG significantly improved the hydrophilicity of the PVDF-CTFE nanofibrous membrane. The TFNC-5 membrane, prepared with the modified PVDF-CTFE@N-MG nanofibrous membrane as the substrate, exhibited permeability exceeding 13.5 L m −2 h −1 ·bar −1 for various dye solutions at 3 bar pressure, with rejection rates above 98 %. It also demonstrated excellent selective separation performance (separation factor for NaCl/Orange G reaching 97.38) and long-term operational stability. This work provides a method for the preparation of low-pressure, high-flux nanofiltration membranes, which is applicable to seawater desalination and dye wastewater treatment .
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ACS Applied Materials & Interfaces
·
2016
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IF 7.145
Lisi Xie,Yan Tan,Zhiyong Wang,Hong Liu,Na Zhang,Chao Zou,Xin Liu,Gang Liu,Jian Lu,Hairong Zheng
RNA interference (RNAi) therapy is a promising treatment for various diseases. However, its application is still restricted by the lack of efficient and safe delivery systems. A novel siRNA delivery vehicle based on ε-caprolactone-modified polyethylenimine (PEI-CL) is presented here. The PEI-CL macromolecules with different grafting degrees were synthesized via a simple ring-opening reaction. This macromolecule strongly protects the siRNA from degradation in serum and promotes the cellular uptake and endosomal escape detected via chemical exchange saturation transfer magnetic resonance analysis and fluorescence imaging. The in vivo measurement was performed with HCT-116 colon tumor xenograft that stably expressed luciferase. The data showed that the PEI-CL/siRNA nanocomplexes elicited strong RNAi response. More interestingly, enhanced gene transfection efficiency was achieved by simultaneous cotransfection with siRNA and DNA plasmid via this novel nanosystem. Overall, our study suggests the PEI-CL macromolecule with great promise for siRNA delivery.
研究领域:
药学
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生物技术
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纳米技术
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分子生物学
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-9
·
IF 17.694
Feng Xuezhen,Zheng Renji,Gao Caiyan,Wei Wenfei,Peng Jiangguli,Wang Ranhao,Yang Songhe,Zou Wensong,Wu Xiaoyong,Ji Yongfei,Chen Hong
Ultrathin two-dimensional (2D) metal oxyhalides exhibit outstanding photocatalytic properties with unique electronic and interfacial structures. Compared with monometallic oxyhalides, bimetallic oxyhalides are less explored. In this work, we have developed a novel top-down wet-chemistry desalination approach to remove the alkali-halide salt layer within the complicated precursor bulk structural matrix Pb 0.6 Bi 1.4 Cs 0.6 O 2 Cl 2 , and successfully fabricate a new 2D ultrathin bimetallic oxyhalide Pb 0.6 Bi 1.4 O 2 Cl 1.4 . The unlocked larger surface area, rich bimetallic active sites, and faster carrier dynamics within Pb 0.6 Bi 1.4 O 2 Cl 1.4 layers significantly enhance the photocatalytic efficiency for atmospheric CO 2 reduction. It outperforms the corresponding parental matrix phase and other state-of-the-art bismuth-based monometallic oxyhalides photocatalysts. This work reports a top-down desalination strategy to engineering ultrathin bimetallic 2D material for photocatalytic atmospheric CO 2 reduction, which sheds light on further constructing other ultrathin 2D catalysts for environmental and energy applications from similar complicate structure matrixes.
研究领域:
材料科学
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环境科学
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化学
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能源科学
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CRYSTENGCOMM
·
2023
·Vol. 26
·期 4
·557-565
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IF 3.1
Jiaqiang Ding,Bingyu Xiao,Jinqiu Wu,Dongliang Chen,Dongling Huang,Zuochun Xiong
Poly(ε-caprolactone-co-trimethylene carbonate) (PCLTMC) is a biodegradable copolymer, which is widely used for medicine and tissue repair systems, and its morphology, degradation and mechanical properties have been extensively investigated. However, its crystallization behavior with different copolymerization ratios has not been studied systematically, which is of great significance for the study of property regulation and an understanding of the crystallization behavior of random copolymers. In this paper, the relationship between the crystallization temperature Tc, melting point temperature Tm and crystallinity Xc of copolymers with different molar ratios was determined by differential scanning calorimetry (DSC) using a non-isothermal crystallization method. The results show that the melting point and crystallinity of the copolymer decrease with an increase in TMC composition. The equilibrium melting point of the copolymers was predicted by an isothermal crystallization method, using the Hoffman–Weeks extrapolation method and crystallization rate growth fitting method both based on Lauritzen–Hoffman theory. It is proved that Lauritzen–Hoffman theory is of great significance for guiding the kinetic behavior of PCLTMC crystallization.
研究领域:
材料科学
·
生物医学工程
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