Catalysis Science & Technology
·
2022
·Vol. 12
·期 22
·6687-6703
·
IF 6.177
Furong Cao,Yun Wang,Xing Wang,Wenjuan Zhang,Gregory A. Solan,Rui Wang,Yanping Ma,Xiang Hao,Wen-Hua Sun
Five types of N-(2-(diphenylphosphino)ethyl)-2-R-5,6,7,8-tetrahydroquinolin-8-amines (R = H L1, Me L2, iPr L3, Cl L4, Ph L5) along with one example of an N-isopropyl-5,6,7,8-tetrahydroquinolin-8-amine (L6) have been prepared and employed as neutral ligand supports for zinc(II) chloride complexes, LZnCl2 (Zn1–Zn6). All zinc compounds were characterized by multinuclear NMR spectroscopy (1H/13C/31P) and elemental analysis, while the structures of Zn2 and Zn5 were further studied by single crystal X-ray diffraction: distorted tetrahedral geometries with the diphenylphosphine moieties non-coordinated were a feature. Pre-treatment of Zn1–Zn5 with two equivalents of either LiCH2SiMe3 or LiN(SiMe3)2 led to catalysts displaying good to exceptionally high activity for the ring opening polymerization (ROP) of ε-caprolactone (ε-CL) at 50 °C. For example, Zn4/2LiCH2SiMe3 displayed a TOF of 2.1 × 104 h−1 with 71% conversion seen within 10 minutes with the ε-CL : Zn molar ratio at 5000 : 1; the resulting polycaprolactone (PCL) comprised predominately cyclic structures along with lower levels of trimethylsilylmethyl-capped linear PCL. By comparison, Zn1–Zn5 on treatment with two equivalents of LiN(SiMe3)2 at the same high monomer to zinc ratio, led to catalysts exhibiting an order of magnitude higher activity. Zn1/2LiN(SiMe3)2 in the presence of BnOH exhibited a remarkable TOF of 1.35 × 105 h−1 with 90% monomer conversion within two minutes. In these cases, a distinct selectivity towards linear polymers capped with CH3O end-groups (derived from the quenching solvent) was observed with cyclic polyesters only observable with larger amounts of ε-CL. As a general observation, the 2-R substituent on the chelating ligand showed noticeable effects on the efficiency and on the molecular weight of the PCLs, with 2-Cl-containing Zn4 in combination with LiCH2SiMe3 and BnOH affording the highest molecular weight PCL of the study (9.57 × 104 g mol−1). Based on the microstructural properties of the PCL, distinct mechanisms (viz., coordination–insertion and ring expansion) have been proposed to account for the mode of propagation mediated by Zn/2LiCH2SiMe3 and Zn/2LiN(SiMe3)2. In addition, a zinc silylamido L1−HZn[N(SiMe3)2] (Zn7) species has been tentatively assigned (obtained via deprotonation of L1 with Zn[N(SiMe3)2]2), that proved inactive for the ROP of ε-CL but displayed good activity for ROP of rac-LA.
研究领域:
有机化学
·
高分子化学
·
材料科学
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiaomin Song,Qi Huang,Bo Jin,Rufang Peng
To improve the encapsulation of GO to CL-20, PEI was utilized as a linker bridge to self-assemble into composite CL-20/PEI/GO in this study. The self-assembly was in-depth characterized, including Zeta potential, SEM, DLS, XPS, Raman spectra, HPLC and power-XRD. The possible self-assembled mechanism was also proposed, which indicates the electrostatic interaction introduced by PEI should be responsible for the self-assembly. The performance of a self-assembled composite was characterized by BAM and DSC analysis. And the results indicate the enhanced interaction promotes GO more efficiently encapsulate CL-20 and improve the safety of the energetic material. Therefore, this work demonstrates a novel and facile method to solve the deprived interaction and corresponding weak desensitization between desensitizer and energetic material.
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Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 23
·5113-5123
·
IF 6.569
Runtian Kang,Hang Chen,Ruijie Ji,Haoyang Wang,Takatoshi Seto,Yuhua Wang
It is of great significance for white light-emitting diodes (wLEDs) to explore new, efficient and stable inorganic phosphors excited by wideband near-ultraviolet (n-UV) light. A new type of efficient emission-tunable Ce3+/Mn2+ doped Ca2YHf2Al3O12 (CYHAO) garnet phosphor which can be excited by n-UV light is studied in this work. Due to the effective energy transfer (ET) from Ce3+ to Mn2+ in CYHAO, CYHAO:0.09Ce3+,xMn2+ phosphors have a wide excitation band in the 370–470 nm region with a peak at 410 nm. Under excitation at 410 nm, all the samples show tunable color emission and match with the near UV chip. Through the decay time, it is determined that the energy transfer efficiency is as high as 88.83%. The calculated activation energy is about 0.217 eV, indicating the relatively good thermal stability. The cathodoluminescence (CL) properties show that the phosphor has a high saturation current and saturation voltage. A single component white LED is fabricated by using the CYHAO:0.09Ce3+,0.3Mn2+ phosphor and a 400 nm n-UV chip. It is worth noting that the detailed study of the energy transfer mechanism, thermal quenching mechanism and CL mechanism has reference value for the development of new co-doped phosphors.
研究领域:
材料科学
·
光学工程
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JOURNAL OF SOLUTION CHEMISTRY
·
2026
·
IF 1.3
Xu Saiyuan,Guo Yujun,Wu Yibin,Chen Bin,Xu Yingjie
This study aims to develop and characterize a novel mixed system composed of sodium phenoxide (NaOPh) and a deep eutectic solvent (DES) formed from 1-ethyl-3-methylimidazole chloride ([Emim]Cl) and ethylene glycol (EG), in order to address the phase separation issue commonly encountered in aqueous phenoxide solutions during CO₂ absorption—caused by the generation of phenol. The physicochemical properties, CO 2 absorption performance and absorption mechanism of the NaOPh/DES mixed system were investigated. The results indicate that the density, viscosity, and CO 2 absorption capacity of the studied NaOPh/DES mixed systems increase with NaOPh content. The NaOPh1.0/DES system exhibits the best absorption performance of these systems, with a CO 2 absorption capacity of 2.10 mol‧kg −1 at 313.15 K and 0.1 MPa. DFT calculations reveal that the Na + from NaOPh, the O–H group from EG, and the Cl − from [Emim] Cl can form a stable four-membered ring. This weakens the electrostatic interaction between Na + and [PhO] − , promoting the dissociation of the NaOPh and facilitating the chemical reaction between the “free” [PhO]⁻ and CO 2 to form carbonates. This mechanism is confirmed by FT-IR and 13 C NMR spectra. Using [Emim]Cl–EG DES as a solvent to dissolve NaOPh leverages the reactivity of [PhO] − with CO 2 for efficient absorption, while effectively avoiding phase separation. This expands the application of phenoxide-based systems in CO₂ capture.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Hongyang Zhao,Sihan Fan,Yulong Xiang,Junfeng Li,Yue Li,Xuelu Wang,Xinjuan Liu,Likun Pan
Asymmetric Ni-N-Cl sites are built by NH 4 Cl vaporization. • Ni-N-Cl overcomes the kinetic challenges and delivers excellent CO 2 reduction performance. • XAFS, DFT and CW-ODMR reveal the asymmetric coordination mechanism. • Cl coordination creates electron-rich Ni centers with shifted d-band. • Ni-N-Cl achieves 86.2% CO Faradaic efficiency and enables durable Zn-CO 2 batteries for 53 h operation. Electrocatalytic CO 2 reduction reaction to value-added chemicals represents a promising pathway for sustainable carbon utilization. However, the symmetric coordination environment of conventional M-N 4 single atom sites restricts electronic structure regulation and limits their intrinsic activity. Herein, we develop an asymmetric Ni-N-Cl coordination structure synthesized via high-temperature NH 4 Cl vaporization assisted strategy. This Cl-mediated asymmetric coordination induces a distinct charge redistribution, generates an electron enriched Ni center and an upward shift of the d-band center closer to the Fermi level. These intrinsic modulations significantly facilitate CO 2 activation and proton transfer to the *COOH, thereby lowering the reaction energy barrier. Consequently, the Ni-N-Cl catalyst achieves a CO Faradaic efficiency of 99.67% at -0.7 V vs. RHE in H cell and 17 h long term stability at -100 mA cm -2 in flow cell. Furthermore, this catalyst delivers a peak power density of 1.62 mW cm -2 and a durability of 53 h. This study provides a general methodology for the rational design of asymmetric single atom catalysts through orbital engineering for high-efficiency energy storage technologies. Download: Download high-res image (199KB) Download: Download full-size image
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GREEN CHEMISTRY
·
2026
·
IF 10.6
Yang Li,Guoen Zhang,Chuanshun Feng,Feng Lin,Huan Ye,Wenqi Wei,Qicheng Zhang,Wenchao Peng,Xiaobin Fan
Electrocatalytic conversion of polyethylene terephthalate (PET) plastic waste into formate coupled with hydrogen generation represents a sustainable pathway for plastic upcycling. Herein, a nickel sulfide catalyst (Mo,Cl-Ni3S2) is developed for efficient and stable ethylene glycol (PET monomer) oxidation reaction (EGOR) through a Mo and Cl co-doping strategy. The optimized catalyst Mo,Cl-Ni3S2 possesses a high formate Faradaic efficiency of 94.0% at 1.55 V vs. RHE. Moreover, it maintains 83.3% of its initial activity after 95 hours continuous operation at an industrial current density of 300 mA/cm2. Experiment and theoretical simulations demonstrate Mo and Cl co-doping optimizes the electronic structure of Ni3S2 by upshifting the Ni d-band center and facilitates the in situ structure reconstruction during EGOR. Finally, an integrated acidification-precipitation-recrystallization strategy is proposed to separate and recover terephthalic acid (TPA) and potassium formate. This method offers a holistic approach for upcycling PET waste into value-added chemicals and hydrogen.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Kai Zhang,Peifeng Wang,Zhuohui Sun,Hongwei Zhang,Rui Chang,Youlong Xu
Poor electronic conductivity, low potential plateau, rapid capacity decay, and poor rate capability are critical challenges hindering the development of layered transition metal oxides such as P2-Na0.7MnO2. To address these issues, a high-entropy design combined with Cl substitution has been implemented, resulting in the material P2-Na0.7Li0.02K0.02Mg0.02Fe0.05Cu0.05Ni0.25Ti0.02Nb0.02Mn0.59O1.93Cl0.07. Hall effect tests reveal a transition from hole-dominated to electron-dominated conduction, significantly improving the Na+ transport kinetics, enhancing electronic conductivity, and facilitating the release of a high specific capacity and specific energy. Notably, the bulk carrier concentration increases from 1.63 × 1011 to 2.63 × 1012 cm–3, the surface carrier concentration rises from 2.47 × 1010 to 2.16 × 1011 cm–2, and the mobility improves from 322.7 to 455.9 cm2 (V s)−1. Consequently, the electronic conductivity undergoes a remarkable 20-fold increase from 8.44 × 10–6 to 1.915 × 10–4 S cm–1. The material delivers a reversible capacity of 196.80 mAh g–1 and a specific energy of 587.07 Wh kg–1 at a current rate of 0.05 C.
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DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Lei Cao,Tongtong Zhu,Minghui Zan,Yulu Liu,Xiaoman Xing,Qing Qian,Qian Mei,Wen-Fei Dong,Li Li
Tea polyphenols (TP), which is accounting for 15–30% of the dry weight of green tea and are widely used in the food industry as antioxidants , preservatives, color preservatives, and flavoring agents . To determine the concentration of TP, a fluorescent method based on nitrogen and chlorine co-doped carbon dots (R-CDs) was investigated. The R-CDs we prepared showed red emission with an absolute quantum yield (QY) of approximately 16.67 ± 0.85%. The limit of detection (LOD) was calculated to be approximately 68 ± 0.94 ng/mL, with an R 2 of 0.999 over the TP range of 1–20 μg/mL. Compared to the ferrous tartrate standard curve method, the concentration of TP in green tea, which was purchased from the market, detected using our method showed an error within 5%, indicating good potential applications in the food industry. Cell imaging experiments suggested that the R-CDs exhibit excellent lysosomal targeting as the Pearson’s correlation coefficient (PCC) in colocalization analysis was found to be 0.91. Further experiments showed that owing to their excitation-independent emission and high QY, the R-CDs could be applied to not only for detecting TP content but also for targeting lysosomes as substitute for commercial dyes.
研究领域:
食品科学
·
细胞生物学
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2020
·Vol. 2020
·期 7
·626-630
·
IF 2.529
Min Li,Guan-Cheng Xu,Wen-Bo Xin,Yin-Qiang Zhang
Graphical The new organic-inorganic hybrid compound (CH 3 NH 3 ) 4 [InCl 6 ]Cl has been successfully synthesized by reaction of methylammonium with indium(III) chloride tetrahydrate. It undergoes a first-order phase transition accompanied with an obvious step-like dielectric switching. A new organic-inorganic phase transition material (CH 3 NH 3 ) 4 [InCl 6 ]Cl ( 1 ), has been successfully synthesized and characterized. The compound undergoes a reversible first-order phase transition at Curie temperature Tc=284 K, accompanied with a wide hysteresis of 12 K, which investigated by differential scanning calorimetry (DSC). The temperature dependence of the dielectric permittivity discloses an obvious step-like dielectric anomaly. Single crystal X-ray diffraction reveals that the order-disorder transition of the [InCl 6 ] 3– anion and the methylammonium cation were the main factor drove the phase transition from high temperature phase with the space group P 2/ m to low temperature phase with the space group P 2/ n . This finding indicates that In-based organic–inorganic hybrids compounds can be used to build phase transition materials, which broaden the way for exploring dielectric switching materials.
研究领域:
材料科学
·
晶体学
·
物理化学
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高影响因子
Defence Technology
·
2026
·
IF 6.4
Yanpeng Lyu,Fan Liao,Ligang Zhang,Handong Shi,Guoqiang He,Xintong Han,Jiaoyang Liu,Chuanhao Xu,Chongwei An
High energy and low sensitivity are generally mutually exclusive in energetic materials, and precise regulation of the microstructure is an effective strategy to balance these properties. In this study, CL-20/DAAF composite microspheres with various microstructures—including core-shell, hollow, porous, and irregular hollow structures—were fabricated using a tubular continuous-flow device combined with the principles of phase separation and recrystallization. The influence of the binder on the morphology and properties was also investigated. The results demonstrated that, compared with raw CL-20, the composite microspheres exhibited significantly reduced sensitivity and improved mechanical properties. Specifically, the impact energy increased from 1.75 J to 7.50 J, and the friction sensitivity threshold increased from 108 N to 168 N. The average compressive stress and compressive strain of the PBX charges were enhanced by 22.89%–108.19% and 25.75%–50.28%, respectively, with the 2.5% NC + 2.5% F 2602 composite binder delivering the optimal mechanical performance. In ignition experiments, hollow microspheres showed the highest combustion efficiency, while core-shell microspheres released energy more steadily, achieving a maximum combustion duration of 2175 ms. Theoretical calculations indicated that this composite binder system possesses a higher theoretical detonation velocity. The study confirms that adjusting the microstructure can effectively enhance the combustion and mechanical properties of composite microspheres, thereby balancing high energy with low sensitivity. The tubular continuous-flow self-assembly technology, integrated with phase separation and recrystallization principles, provides a feasible pathway for the controllable construction of composite microsphere architectures and offers a reference for the design and fabrication of other energetic composite microspheres.
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产品关联
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高影响因子
CORROSION SCIENCE
·
2023
·
IF 8.3
Shupei Liu,Xinfang Zhang,Jinsong Rao,Liang Yu,Wei Lu,Huan Zhou,Shibo Chen,Yuxin Zhang,Xiaoying Liu
Ni-Co Layered Double Hydroxide (LDH) shows great application potential in the field of anti-corrosion. However, the poor carrying capacity limits the performance of anticorrosion performance. In this study, Ni-Co hydrotalcite was grown on the surface of DE, and Ni-Co/DE@SP microcapsule with corrosion inhibitor loading up to 14.7% was successfully prepared. The adsorption capacity of Ni-Co/DE@SP for Cl − in 600 mmol/L NaCl solution was 6.72 mmol/g. It is worth noting that the impedance modulus of the prepared composite coating (EP/Ni-Co/DE@SP) is two orders of magnitude higher than that of the pure resin coating, and the wear resistance was improved by 33%.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Le Ma,Xiansheng Li,Xuehan Chen,Jingyu Li,Pengfei Liu,Changting Wei,Qingshan Ma,Leimeng Xu,Wenhua Zhang,Jizhong Song
Mixed halide CsPb(Br/Cl) 3 quantum dots (QDs) exhibit fine tunable blue light and narrow photoluminescence (PL) full-width at half-maximum (FWHM), which has attracted significant attention as a promising candidate to realize a new generation of blue light technology. However, the introduction of Cl − makes it very easy to be eroded by water in the environment, which will lead to deep-level defects and degrade the luminescence and stability of QDs. Here, we propose to introduce tetra- n -octylammonium oxalate (TOAOxa) to improve the water-resistance stability and exciton recombination of CsPb(Br/Cl) 3 QDs and QD-based light-emitting diodes (QLEDs). The oxalate ion (Oxa 2− ) of TOAOxa could form strong interaction with undercoordinated Pb 2+ on CsPb(Br/Cl) 3 QD surface, which was confirmed by FTIR and XPS analysis. Oxa 2− passivated QDs (Oxa-QDs) exhibited improved photoluminescence quantum yield (PLQY) and enhanced water-resistance stability compared to pristine QDs. For example, after soaking in water–acetone co-solvent for 1 h, Oxa-QDs can maintain the initial cubic morphology and 43.9% of initial PL intensity, while the morphology and luminescence of pristine QDs are almost damaged. Based on the above concept, the Oxa-QD-based QLED presented a maximum external quantum efficiency (EQE) of 4.0%, and operational lifetime (T 50 ) of 84 s, which was a 5-fold enhancement in EQE, and 7-fold enhancement in stability compared to pristine QLED, respectively. Besides, the Oxa-QD-based QLED exhibits better stability in high-humidity air. To sum up, the Oxa 2− passivation strategy has significantly improved the efficiency and water-resistant stability of QDs and devices and would rapidly promote the development of blue-emitting QDs.
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危险品化学品经营许可证（带存储）