Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 16
·2969-2978
·
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
·
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
·
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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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yunlong Xia,Mengliang Gao,Ge Pu,Xingqiang Lu,Jie Gao,Jiale Wu,Qianhui Yang
The generation of high-quality syngas combined with high-purity hydrogen is an essential challenge in the chemical looping steam methane reforming (CL-SMR) process, in which the design of oxygen carriers (OCs) is crucial. In this study, La 2 FeBO 6 (B Cr, Ni，Co) and La 2 Fe 2-x Co x O 6 (x = 0.2, 0.4, 0.6, 0.8, 1.0) double perovskites have been investigated as OCs in the CL-SMR process. Various analytical techniques (BET, XPS, XRD, H 2 -TPR, Raman.) have been deployed to characterize the OCs' specific surface area, crystal structure, and surface oxygen species. The fixed-bed experiments revealed that the Cr-modified perovskite had the lowest reactivity, which was attributed to the creation of LaCrO 3 limiting the oxygen release rate of the OC. Meanwhile, Ni doping exhibited the maximum methane conversion (99.15 %), but it resulted in more carbon deposition due to methane cracking, and its carbon deposition was four times than that of Co doping. Whereas, the Co doped double perovskite OCs showed excellent overall performance, in which La 2 Fe 1.8 Co 0.2 O 6 (L 2 F 1.8 Co 0.2 ) exhibited the optimum CO selectivity (90.72 %), H 2 selectivity (96.91 %), and H 2 purity (96.84 %), as well as the lowest carbon deposition. Moreover, the L 2 F 1.8 Co 0.2 also exhibited outstanding stability in 10 cycles, and it could be a prospective material for CL-SMR, enabling the simultaneous generation of high-quality syngas and high-purity hydrogen.
研究领域:
化学工程
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材料科学
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能源工程
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ACS Applied Materials & Interfaces
·
2016
·
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
·
生物技术
·
纳米技术
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分子生物学
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高影响因子
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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高影响因子
ACS Applied Nano Materials
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2024
·
IF 5.3
Yu Yao,Qianhong Shen,Qifeng Chen,Yanyan He,Libei Jiang,Jie Liu,Yue Li,Xudan Cao,Hui Yang
A silver phosphate (Ag3PO4)/silver (Ag)/silver halide (AgX, X = Cl, Br, or I) ternary composite photocatalysts were prepared by loading Ag nanoparticles on Ag3PO4 tetrapods followed with in situ halogenation. The interface charge transfer behavior in the Ag3PO4/Ag/AgX nanocomposite was studied, and the photocatalytic performance was also evaluated. The results show that the Ag3PO4/Ag/AgI photocatalyst exhibits higher photocatalytic activity than the other two photocatalysts due to the more matched band structure between AgI and Ag3PO4. An internal electric field (IEF) from Ag3PO4 to AgI is formed at the heterogeneous interface, so the photogenerated electrons at the conduction band of AgI can rapidly transfer to the valence band of Ag3PO4 and recombine with photogenerated holes, which is consistent with the S-scheme charge transfer mechanism. Meanwhile, the photogenerated electrons left at the conduction band of Ag3PO4 can transfer to Ag nanoparticles due to the Schottky junction and react with oxygen to produce •O2–, which is proved to be the main active species in the photocatalytic procedure. This tandem junction modulated between the S-scheme heterojunction and Schottky junction promotes the efficient separation of photogenerated carriers, thus significantly increasing the average PL lifetime of electrons by 2.95 times. Therefore, the Ag3PO4/Ag/AgI photocatalyst exhibits excellent photocatalytic activity for the degradation of methylene blue and norfloxacin. The seven consecutive cyclic tests prove the good stability of the photocatalyst, thus showing the application potential in the field of sewage treatment.
研究领域:
环境科学
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材料科学
·
化学
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 11
·111502
·
IF 3.1
Thanh Hai Pham,Viorel Chihaia,Phung K. Le,Do Ngoc Son
The influences of -NH2 and -Cl groups on the copper corrosion inhibition in 0.5 M H2SO4 solution by benzotriazole were studied using experimental methods and density functional theory calculations. Mass loss tests, potentiodynamic polarization, and surface morphology analyses revealed notable differences: while unmodified benzotriazole showed an inhibition efficiency of 76.6%, the -Cl derivative increased this to 87.6%, whereas the -NH2 derivative dropped it to 61.0% at the concentration of 5 × 10−4 M. Density functional theory calculations indicated these differences are not due to electronic properties or inhibitor-copper interaction energies but rather to the inhibitor's influence on the oxygen reduction reaction, especially O2 and H2O adsorption. The -NH2 group formed strong hydrogen bonds with O2 and H2O, reducing oxygen reduction inhibition, while the -Cl group repelled O2, resulting in enhanced inhibition. Free energy analysis of the oxygen reduction reaction supported these findings. These new insights into benzotriazole derivatives' copper corrosion inhibition mechanisms offer valuable guidance for developing next-generation corrosion inhibitors.
研究领域:
材料科学
·
化学
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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
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生物医学工程
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2025
·
IF 2.1
Ruxue Yao,Yang Ge,Jiangtao Song,Fei Yuan,Yafei Guo,Tianlong Deng
The Qaidam Basin has potassium- and calcium-rich oil field brine resources at high temperatures. Since the phase diagram is a powerful tool to guide the separation and purification of inorganic chemical engineering for the development of potassium resources in oil field brine, the quaternary oil field brine system (Na+, K+, Ca2+//Cl– -H2O) and its two subsystems ((Na+, Ca2+//Cl– -H2O) and (K+, Ca2+, //Cl– -H2O)) at 338.15 K were reported for the first time by the isothermal dissolution equilibrium method. The compositions of the equilibrium solid phases were analyzed and identified by combined chemical analyzing and X-ray diffraction. The quaternary system has four crystallized regions corresponding to NaCl, KCl, KCl·CaCl2, and CaCl2·2H2O at 338.15 K, and the incongruent double salt KCl·CaCl2 occurred at 338.15 K. The study facilitates the enrichment of thermodynamic data and exploits brine-based potassium resources.
研究领域:
化学工程
·
无机化学
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