APPLIED CATALYSIS A-GENERAL
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2023
·
IF 5.5
Liyan Zhang,Yinze Yang,Leilei Zhou,Fengyu Zhao,Haiyang Cheng
The synthesis of 1,6–hexamethylenediamine via the reductive amination of 1,6–hexanediol is a fascinating green process and a challenging topic. We developed a kind of Ru/PRL(x)–Al 2 O 3 catalyst for the reductive amination of 1,6–hexanediol, the active Ru species was highly dispersed and anchored by the CN x species formed from 1,10-phenanthroline (PRL). The Ru particle dispersion, electronic interaction, and acid–basic property as well as the catalytic mechanism and the rate determining step were discussed in detail. The new and more acid–base pairs formed, and the electron deficient Ru species and smaller nanoparticles are responsible for the improved catalytic performances of Ru/PRL–Al 2 O 3 catalyst. The yield of 1,6–hexamethylenediamine could reach to 54%, which is the best results reported up to now. The present catalytic process is of great potential for industrial application as it is a green process compared to the traditional method for 1,6–hexamethylenediamine production.
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Science Bulletin
·
2023
·
IF 18.9
Weikang Wang,Yan Bai,Pin Yang,Shuai Yuan,Feiyang Li,Weiwei Zhao,Beibei Jin,Xuan Zhang,Shujuan Liu,Daqiang Yuan,Qiang Zhao
Chemical transformation strategy is capable of fabricating nanomaterials with well-defined structures and fascinating performance via controllable crystallization kinetics in the phase transformation. V 2 CT x MXene has been used as precursors to fabricate vanadium porphyrin metal–organic frameworks (V-PMOFs) via the coordination of deprotonated carboxylic acid ligands. However, the rational and in-depth exploration of synthesis mechanism with the aim of enriching the variety of MXene (i.e., Ti 3 C 2 T x ) and organic ligands (i.e., catechol-based) to design new MOFs is rarely reported. Herein, we have first developed a metal ion assistant transformation strategy to synthesize three-dimensional catechol-based TiCu-HHTP (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) MOFs with a non-interpenetrating SrSi 2 ( srs ) framework using two-dimensional Ti 3 C 2 T x as precursors. The unique synergetic transformation mechanism involves the electron transfer from Ti 3 C 2 T x to electrostatically adsorbed Cu 2+ ion for redox reaction , the subsequent Ti–C bond rupture for Ti 4+ ion release , and the continuous chelation coordination between Ti 4+ /Cu 2+ and HHTP. Ti 3 C 2 T x precursors and auxiliary metal ion could be rationally substituted by V 2 CT x and M n + (e.g., Ni 2+ , Co 2+ , Mn 2+ , and Zn 2+ ), respectively. This strategy lays the foundation for the design and synthesis of innovative and multifarious MOFs derived from MXene or other unconventional metal precursors .
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Analytical Methods
·
2018
·Vol. 10
·期 26
·3188-3196
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IF 2.073
Li-Jun Xia,Xiao-Feng Guo,Yan Ji,Liu Chen,Hong Wang
Herein, a highly reactive long-wavelength fluorescent labeling reagent, 1,7-dimethyl-3,5-distyryl-8-phenyl-(4-oxy-acetic acid N-hydroxysuccinimidyl ester) difluoroboradiaza-s-indacene (DMDSPAB-OSu), was designed and synthesized for amino compounds. Using DMDSPAB-OSu as a pre-column derivatization reagent, an HPLC-fluorescence detection method was developed for the determination of trace amounts of aliphatic amines in samples. Prior to analysis, amines were derivatized with DMDSPAB-OSu at room temperature in 0.2 mol L−1 pH 8.8 borate buffer for only 5 min, and the baseline separation of 11 aliphatic amines was achieved within 25 min. Limits of detection between 0.8 to 1.2 nM were obtained at 630 nm with an excitation wavelength of 610 nm. Furthermore, the proposed DMDSPAB-OSu-based HPLC method was applied to the analysis of lake water and human urine with satisfying recoveries ranging from 93.0–109.7%.
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Nanoscale
·
2017
·Vol. 10
·期 3
·1532-1539
·
IF 7.367
Xiaolong Wu,Liling Ma,Shan Sun,Kai Jiang,Ling Zhang,Yuhui Wang,Haibo Zeng,Hengwei Lin
In this work, a versatile platform for the highly efficient preparation of graphene quantum dots (GQDs) with diverse properties was developed. First of all, an excess amount of oxidants and an additional high temperature step of the Hummers’ method for the synthesis of graphene oxide (GO) was applied to obtain nanosized graphene oxide (NGO). Then, high quality GQDs (quantum yields up to 18.2%) with different photoluminescence emission wavelengths, adjustable hydrophilicity–hydrophobicity, and selective cell organelle imaging capacity can be facilely achieved through a one-pot hydrothermal reaction between the NGO and ammonia, fatty primary amines, or amino-substituted organelle targetable compounds, respectively. The superior features of the as-developed method are extremely high conversion ratio (ca. 60 wt% from graphite to the functional GQDs) and great expandability. Such a high conversion ratio is deemed to be due to effectively decreasing aggregation of the NGO (in comparison with GO) during the post-treatment process. This work provides a robust strategy for the highly efficient preparation of GQDs with diverse properties and functions, and is believed to be beneficial for boosting their applications in the future.
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高影响因子
LANGMUIR
·
2016
·
IF 3.993
Wen Xu,Tao Wang
Cu(II) complex ink consisting of copper formate (Cuf) and a primary alkylamine could yield highly conductive copper films at low heating temperatures without a reducing atmosphere. A synergetic effect of the blended alkylamines on the formation of conductive films was observed. It was found that blending two types of amines with different alkyl chain lengths as ligands could improve the conductivity of copper films, compared with using one of these amines alone. The decomposition mechanism of the Cuf–amine complex and the role of amines with different alkyl chain lengths were investigated. It was found that the decrease in the decomposition temperature and the formation of copper films were attributed to the activating effect and capping effect of the amine, and these two effects were dependent on the alkyl chain length. The relative intensity of the dual effects determined the decomposition rate of the complex and the nucleation and growth of particles. The use of blended amines with different alkyl chain lengths as ligands could balance the two effects and lead to appropriate nucleation and growth rates, so that densely packed copper films with low resistivity could be obtained at low heating temperature in a short time. The Cuf–butylamine–octylamine (Cuf–butyl–octyl) ink with 1:1 molar ratio of the amines showed the best performance. The understanding of the synergetic effect could provide guidance to the design of copper complex inks to control the morphology of the films.
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Journal of Materials Chemistry C
·
2017
·Vol. 5
·期 12
·3035-3041
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IF 5.256
Kaisi Liu,Bin Yao,Yongfeng Li,Zhanhui Ding,Hao Sun,Yuhong Jiang,Gang Wang,Daocheng Pan
Herein, we successfully prepared dithiocarbamate-based Cu2ZnSnS4 (CZTS) precursor solutions using various amino groups such as methylamine, ethylamine, propylamine, butylamine, amylamine, hexylamine, octylamine, and ethanolamine. These solutions exhibited a distinguishing wetting behavior, viscosity, and stability and could be used to fabricate CZTS thin films by a simple spin-coating and annealing process. We compared the thermogravimetric analysis of the precursor solutions and the XRD patterns of the as-prepared CZTS films and clear differences between the samples were observed. Furthermore, we fabricated high-quality CZTS films using the ethanoldithiocarbamate-based CZTS precursor solution, and the Cu2ZnSn(S,Se)4 solar cell with the best power conversion efficiency (7.66%) under 1.5 AM illumination was achieved.
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Journal of Energy Chemistry
·
2024
·
IF 14
Gomaa Mohamed Gomaa Khalaf,Xinzhao Zhao,Mingyu Li,Chunxia Li,Salman Ali,Tianjun Ma,Hsien-Yi Hsu,Jianbin Zhang,Haisheng Song
Lead sulfide quantum dots (PbS QDs) hold unique characteristics, including bandgap tunability, solution-processability etc., which make them highly applicable in tandem solar cells (TSCs). In all QD TSCs, its efficiency lags much behind to their single junction counterparts due to the deficient interconnection layer (ICL) and defective subcells. To improve TSCs performance, we developed three kinds of ICL structures based on 1.34 and 0.96 eV PbS QDs subcells. The control, 1,2-ethanedithiol capped PbS QDs (PbS-EDT)/Au/tin dioxide (SnO 2 )/zinc oxide (ZnO), utilized SnO 2 layer to obtain high surface compactness. However, its energy level mismatch causes incomplete recombination. Bypassing it, the second ICL (PbS-EDT/Au/ZnO) removed SnO 2 and boosted the power conversion efficiency (PCE) from 5.75% to 8.69%. In the third ICL (PbS-EDT/poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA)/Au/ZnO), a thin layer of PTAA can effectively fill fissures on the surface of PbS-EDT and also protect the front cells from solvent penetration. This TSC obtained a PCE of 9.49% with an open circuit voltage of 0.91 V, a short circuit current density of 15.47 mA/cm 2 , and a fill factor of 67.7%. To the best of our knowledge, this was the highest PCE achieved by all PbS QD TSCs reported to date. These TSCs maintained stable performance for a long working time under ambient conditions.
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OPTICAL MATERIALS
·
2025
·
IF 4.2
Yu Lu,Zhixu Wu,Pengfei Xiang,Taiming Ji,Rongxin Tang,Yuhao Wang,Yong Xia
Lead sulfide (PbS) colloidal quantum dots (CQDs) are widely used for infrared detection and imaging. Currently, the most popular device structures for PbS CQDs photodetectors (PDs) are p-i-n type. Among them, the PbS CQDs films treated with 1,2-ethanedithiol (EDT) are extensively utilized as hole transport layers. However, the energy band alignment based on the PbS-EDT layer has a great impact on the device performance and has not been thoroughly investigated. To systematically explore the effect of the bandgap of PbS-EDT layer on device performance, this work is firstly based on the PbS-EDT layer simulated through SCAPS-1D software. When the PbS-EDT layer bandgap is 1.4 eV, the device can build a suitable gradient energy band structure and the dark current density (J dark ) reaches the lowest. Based on the simulation results, the corresponding PbS CQDs PDs were fabricated, which showed excellent performance with the J dark of 265 nA/cm 2 at a bias voltage of −0.5V, the responsivity and specific detectivity reached 0.65 A/W and 5.73 × 10 12 Jones, respectively. A single-element scanning infrared imaging system demonstrates the excellent imaging capability of the device. The energy band alignment strategy based on the PbS-EDT layer is expected to promote infrared optoelectronic applications in this field.
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Science China-Chemistry
·
2024
·
IF 10.4
Zhang Luzhi,Huang Hongfei,Sun Lijie,Ma Xiaopeng,Tan Hui,You Zhengwei
Sequence regulation provides an effective approach to controlling the properties of polymer materials. However, this approach remains an open question in the field of dynamic polymers, which emerge as more and more important new generation materials. Herein, we systematically investigate the effect of sequence control of dynamic covalent units in tuning the properties of materials. Different sequence-controlled poly(oxime-urethanes) are designed. The dynamic oxime-urethane groups are relatively dispersed (SCP-1) or concentrated (SCP-2) distributed in their molecular chains. The sequence control strategy provides an efficient way to decouple the mechanical and self-healing performance of polymers, which is one of the most pressing challenges in the field. The relatively dispersed oxime-urethane groups in SCP-1 not only facilitate the reorganization of the dynamic covalent bonds but also increase the probability of the reformation of hydrogen bonds. The reversible dissociation/reassociation of dynamic bonds is conducive to dissipating energy to enhance mechanical performance and promote self-healing properties. As a result, SCP-1 exhibits much faster self-healing than SCP-2, and its tensile strength is nearly twice that of SCP-2. In addition, energy dissipation capacity and degradation behavior also show significant sequence dependence. Overall, this work reveals a new molecular structure-property relationship and provides a powerful strategy to construct high-performance polymers.
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Bioactive Materials
·
2025
·
IF 20.3
Tianyi Zhang,Yuhui Wu,Ye Tian,Youxiang Wang,Peng Zhang,Qiannuan Shi,Qun Fang,Jianzhang Pan,Qiao Jin,Jian Ji
Antimicrobial peptides (AMPs)-mimicking antimicrobial polymers show great potential as therapeutic alternatives to antibiotics in the looming “post-antibiotic era”. However, the discovery of new AMP-mimicking antimicrobial polymers is challenging due to the vast chemical space of side-chain combinations. The advancement of AI-guided high-throughput screening enables more efficient, precise, and intelligent material design. Herein, we integrate combinatorial chemistry, machine learning, and automated high-throughput synthesis and characterization platforms to establish a new paradigm for the design of antimicrobial polymers with excellent biocompatibility. Starting with a library of 13,728 combinations, a seed dataset of 400 structures is generated, followed by four Design-Build-Test-Learn iterations using a new machine learning model. 7 top-performing candidates are screened with a minimum inhibitory concentration (MIC) ≤ 8 μg/mL and an inhibitory concentration causing 20 % cell death (IC 20 ) ≥ 64 μg/mL. The highest-performing polymer (MIC 2 μg/mL, IC 20 256 μg/mL) shows similar in vivo therapeutic efficacy with ceftazidime. Overall, the integration of AI-guided high-throughput screening and combinatorial chemistry accelerates the discovery of new antimicrobial polymers, which provides a scalable strategy for developing novel antimicrobial agents.
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JOURNAL OF SUPERCRITICAL FLUIDS
·
2025
·
IF 4.4
Jinglong Li,Meiyu Zhen,Yutao Feng,Ziyi Lu,Chang Wang,Xiaoqing Xiong
Alkyl-chain anthraquinone dyes have promising performance but face application constraints due to hydrophobicity and pollution in conventional water-based dyeing. This study developed an eco-friendly synthesis and dyeing approach. Six dyes (AQ-5 to AQ-7, CAQ-5 to CAQ-7) were synthesized in supercritical carbon dioxide (scCO₂) via reactions of 1-chloroanthraquinone/1,5-dichloroanthraquinone with n -alkylamines. They showed good light absorption and thermal stability (5% weight loss at 245–298°C, suitable for scCO₂ dyeing). Meanwhile, scCO₂ dyeing regularity was revealed through the synergistic regulation of multiple parameters. Optimal scCO₂ dyeing conditions for polyester were determined: 16 MPa, 130°C, 90 min for AQ-5–AQ-7; the optimal dyeing conditions for CAQ-5–CAQ-7 were determined and these were included in the range of 120-135 °C, 16 MPa, 70-100 min. Dyed fabrics had uniform fixation with excellent washing, dry, and wet rubbing over than grade 4, and good light fastness. This work establishes a green scCO₂ system, overcoming traditional limitations, and provides a theoretical basis for eco-friendly dyes/technologies.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Zijing Hao,Jiaqing Zhao,Jinhong Li,Jianbo Gao
Compressive strength is vital for porous cordierite ceramics widely used in thermal storage, thermal insulation, refractory materials, and catalyst supports, but conventional reinforcement methods often come at the cost of sacrificing porosity. This work aimed to produce high-strength porous cordierite ceramics from emulsions stabilized by submicron-sized, plate-like cordierite particles. The strong adsorption of pentylamine-modified particles at the oil-water interface and the formation of an attractive particle network throughout the continuous phase stabilized the emulsions to withstand room-temperature drying without structural distortion. The high-aspect-ratio particle morphology facilitated their preferred orientation during emulsification and sintering processes, thereby imparting remarkable mechanical properties to the ceramic bodies. By adjusting sintering temperature and pentylamine concentration, compressive strengths ranging from 32.6 to 67.4 MPa were obtained from porous cordierites with a porosity of 54.8 %–69.0 %. Such high strength values were attributed to the strong pore walls endowed by high interfacial coverage and the dense struts formed by stacked plate-like particles in the continuous phase.
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