Chemistry-An Asian Journal
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2024
·Vol. 19
·期 24
·e202400798
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IF 3.5
Haiyun Zhou,Pingping Li,Tingting Zhong,Yunzhen Teng,Siqi Li,Xiaofeng Luo,Xinning Wang,Min Yang,Guowei Deng
Mn doping has been used to improve the physical chemistry of lead halide perovskite nanocrystals such as CsPbX 3 , where X is a halogen ion. In this paper, a two-phase method for Mn-doped CsPbX 3 nanosheets (where X=Br, Cl), namely water-hexane system, is reported. Compared to conventional catalyst arrays, the band gap of CsPbBr 3 nanocrystalline is easily tuned, the carrier diffusion distance is remote, the band edge position of the band structure is favorable for a wide range of electrocatalytic redox reactions, and the catalytic active site is maximally exposed, providing a larger electrolyte contact area. The porous hierarchical structure also accelerates the release of hydrogen bubbles. The results showed that the optimized Mn : CsPbBr 3 catalyst exhibited excellent electrolytic performance of aquatic hydrogen in alkaline electrolyte (1 mol/L KOH). The overpotentials of the oxygen evolution reaction (OER) at the current densities of 10 and 100 mA cm −2 are only 114.4 and 505.4 mV, respectively, with a Tafel slope of 43 mV dec −1 . At a current density of 10 mA cm −2 , the excess potential required for the hydrogen evolution reaction (HER) is 158.6 mV and it exhibits excellent electrochemical stability. The Mn : CsPbBr 3 nanocrystalline consists of two electrodes for hydrolysis of water, requiring only a voltage of 1.45 V. This provides implications for the optimization of electrocatalysts in alkaline electrolytes with the aim of developing next generation 2D electrocatalysts for overall water splitting.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Lufang He,Zhuo Liu,Yuchi Zhang,Le Han,Yan Xu
Nitrite is commonly found in the natural environment and in everyday human activities. However, excessive nitrite consumption can potentially harm human health. Consequently, it is crucial to develop a reliable and sensitive method for nitrite detection. In this work, trichloroacetic acid functionalized Cl-Fe-MIL-88B metal-organic framework is obtained through nucleophilic reaction between animated Fe-MIL-88B and trichloroacetic acid, which is then annealed with melamine in an N 2 atmosphere to produce the Fe/Cl/N triply-doped bamboo-like carbon nanotubes (CNTs) wrapped with Fe 3 C nanoparticles. Owing to the effective doping of Fe/Cl/N elements, the charge distribution and chemical activity of the bamboo-like structure are tailored, greatly improving the conductivity and facilitating electron transfer of the composite for potential electrocatalytic reaction. The Fe 3 C nanoparticles wrapped inside the CNTs contribute to expose more active sites and provide effective surface area. Accordingly, the Fe/Cl/N doped bamboo-like structure modified glassy carbon electrode shows excellent electrochemical nitrite sensing properties with a high sensitivity of 1060 µA cm −2 mM −1 , a low detection limit of 0.61 µM in a wide linear concentration range of 5–5000 μM, as well as good anti-interference and long-term stability. Also, the electrochemical sensor has a satisfactory recovery rate for detecting nitrite ions in spiked milk samples. This work proposes a simple precursor chlorination and pyrolysis strategy to obtain metal-filled bamboo-like structure with high electrical conductivity and electrocatalytic properties, endowing great potential in food safety and environment monitoring.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 24
·期 8
·1898-1904
·
IF 5.317
Shaofan Fang,Guangshe Li,Yantong Lu,Liping Li
Graphical Lifting the curse : We reported on a novel route by using solid metal halides as halide sources that achieve an anion exchange with CsPbX 3 without any pretreatment. Introducing small amounts of oleic acid or oleylamine speed up the exchange reaction rate, although showing different promotion mechanisms (see figure). Cesium lead halide perovskite (CsPbX 3 ) nanocrystals (NCs) exhibit an excellent photoelectric performance, which is directly governed by fine-tuning of the composition and preparation of materials with a special phase structure and morphology. However, it is still facing challenges to achieve highly stable and luminescent CsPbX 3 NCs at room temperature. Herein, we report on a novel exchange reaction, in which metal halides MX 2 (M=Zn, Mg, Cu, or Ca; X=Cl, Br, or I) solids act as anion source to directly prepare CsPbX 3 NCs at room temperature without any pretreatment. Introducing small amount of oleic acid or oleylamine speed up the exchange reaction through different promotion mechanisms. Oleic acid coordinates to the surface of the NCs, which increases the reaction activity, and oleylamine greatly enhances the dissolution of ZnCl 2 . XRD and TEM tests demonstrate that the cubic phase structure and the morphology of the parent CsPbX 3 were well preserved. Moreover, the band-gap energies and photoluminescence (PL) spectra were readily tunable over the entire visible spectral region of λ =406–685 nm. Our findings could open up the possibilities of using metal halide solids as new anion sources to prepare high-quality CsPbX 3 NCs at room temperature.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 29
·42075-42087
·
IF 0
Zhang Qian,Lan Xin-yue,Huang Zhi,Liu Yan-ying,Hong Jun-ming
Highly active catalysts with salt and acid/alkali resistance are desired in peroxymonosulfate (PMS) activation processes and marine environment applications. F- and Cl-doped graphene (F-GN and Cl-GN) were prepared via electronegative and atom radius adjustment for tetracycline hydrochloride (TCH) pollution removal to satisfy these requirements. The introduction of special F and Cl functionalities into graphene exhibits superior electron transfer properties for PMS activation, considering the experimental and density functional theory (DFT) calculation results. The TCH degradation efficiency reached up to 80% under various pH and salt disturbance conditions with F-GN and Cl-GN. Cl-GN exhibited an activity superior to F-GN due to the higher electron polarization effect of C atoms adjacent to Cl atoms. The presence of more positive charged C sites in Cl-GN (around Cl doping) is more favorable for PMS attachment and sequence radical generation than F-GN. In addition, the main active species functionalized during reaction included ·OH and SO 4 − ·, and the stability of F-GN and Cl-GN was confirmed to be over 60% by recycle test. Final research results provide an effective strategy for designing and preparing PMS activators resistant to salt, acid, and alkali, thereby expanding their application potential.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Hui Wang,Hongtu Zhao,Wenbo Wu,Shifan Xu,Na Wang,Ting Wang,Xin Huang,Lina Zhou,Ying Bao,Hongxun Hao
The solubility performance of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane has been investigated by the combination of experimental measurement, solvent parameter analysis, and molecular simulation methods. The solubility in 10 pure solvents at 293.15 K to 343.15 K was determined. It was found that the solubility in nine solvents increased with temperature, except for isoamyl propionate. However, it has the largest solubility in isoamyl propionate (4.36 × 10 −2 ∼ 5.39 × 10 −2 ). Additionally, a correlation analysis was performed using four equations, which showed that the NRTL equation provided the best fit (overall average relative deviation = 3.74 %, overall coefficient of determination = 0.991). Moreover, the solvent effect was analyzed by Hansen solubility parameters, predicting good solubility in solvents with R a(V) ≤ 12.47 MPa 0.5 or Δ δ t ≤ 7.77 MPa 0.5 , indicating weak polarity of solvent and weak solvent–solvent intermolecular hydrogen bonds enhance dissolution. Furthermore, molecular electrostatic potential surface and radial distribution function analyses provided that weak hydrogen bonding C-H···O promotes dissolution.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
·
IF 4
Chenyang Liu,Shuxiang Jiao,Yuhua Liu,Tao Wu,Leilei Xie,Lijuan Zhang,Yun Zhang,Wenming Wang,Hongfei Wang
Three isomeric nitrosylruthenium complexes [RuCl(Qn)(Pro)(NO)] ( 1 – 3) were prepared, where Qn is 8-hydroxyquinoline and Pro is D-proline. The complexes 1 – 3 were characterized by 1 H-NMR, 13 C-NMR, ESI-MS, and their crystal structure were further determined with X-ray diffraction techniques. In complexes 1 and 3 , the O atom of D-proline coordinated trans to NO, while the O atom of 8-quinolinol coordinated trans to NO in complexes 2 , and the complexes 1 and 3 are the Ru-centered enantiomers. The photo induced NO release of the complexes were explored using time-resolved infrared spectroscopy (FT-IR) and electron paramagnetic resonance spectroscopy (EPR) in solution and the released NO was successfully imaged in living cells using a NO selective fluorescent probe. Furthermore, the cytotoxicity of the isomeric complexes against HeLa, HepG2 and A549 cells were evaluated. Among them, the selectivity for HeLa cells is significant (SI ≥ 5) with IC 50 values in the range of 1.15–1.94 μM. Moreover, the three complexes spontaneously bind to human serum albumin (HSA) through hydrogen bonding and van der Waals forces, the binding constants K b of 1 – 3 are 1.528 × 10 4 , 2.390 × 10 4 and 2.694 × 10 4 M −1 at 298 K, respectively. Molecular docking analyses reveals that 1 – 3 bind within subdomain IB of the protein, which suggest that HSA could be a delivery vehicel for these complexes. This study provides insight into the potential biological and pharmaceutical applications for these isomeric nitrosylruthenium complexes.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
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2025
·
IF 3.1
Ma SongYuChen,Li YinHui,Di Yang,Liu Tao,Wang DeQi,Shi WenJing,Ling ZhiGang,Li FengSheng,Liu Jie
To enhance the safety performance and thermal stability of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexazepane (CL-20), a core–shell composite was synthesized via in situ polymerization of aniline on polyethyleneimine (PEI)-modified CL-20. PEI modification introduced –NH 2 groups onto CL-20 surface, providing active sites for aniline polymerization and inhibiting its self-polymerization, thus forming dense polyaniline (PANI) shells with uniform thickness (about 2.8 mass%) while maintaining the high-energy crystal structure of CL-20. Compared to pure CL-20, CL-20-P@PANI showed a 15.8 °C increase in phase transition temperature (185.5 °C) and a 4 °C rise in thermal decomposition temperature (247.21 °C), attributed to the thermal barrier effect of PANI shells. The results of the mechanical sensitivity test indicate that the dense polyaniline shell layer effectively dissipates external forces, leading to a 51.43% reduction in impact sensitivity and a 20% decrease in friction sensitivity. This study provides a novel modification approach for high-energy materials by combining PEI-mediated interface engineering with in situ polymerization, ensuring both safety and energy characteristics. Graphic abstract
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
·
IF 4.1
Duanyang Wu,Shengnan Zhang,Jing Xu,Wei Cheng
Carbamazepine (CBZ) is a ubiquitous persistent micropollutant in water. This study evaluated the degradation of CBZ by UV/Chlorine process. The influencing factors, such as chlorine dosage, solution pH, and water matrix constituents (Cl − , HCO 3 – and NOM) on CBZ removal were systematically investigated. The reactive HO•, Cl• and ClO• species were mainly responsible for the degradation of CBZ, and their contributions determined by probes (Benzoic acid, Nitrobenzene and 1,4-Dimethoxybenzene) varied with pH. Theoretical quantum calculations involving a total of 79 transition states suggested that HO• attack CBZ by hydrogen atom transfer (HAT) and radical adduct formation (RAF) mechanisms, while Cl• and ClO• proceed mainly through HAT and RAF mechanism, respectively. The reaction rates between CBZ and free radicals were calculated by evaluating the energy barriers and transition states. Furthermore, the proposed formation pathways and reaction mechanisms of main hydroxylated products and chlorine substituted products were unequivocally authenticated by transition states calculations. Overall, this study combined experimental and computational approaches to provide an in-depth degradation mechanism of CBZ in UV/Chlorine process.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2024
·
IF 2
Jie Li,Huan Zhou,Jie Yang,Cunbing Xu,Sifan Wang,Yifan Li,Jiangbo Chen
The solid–liquid phase equilibria of the Li+, Na+, Ca2+//Cl––H2O quaternary system at 298.15 and 323.15 K are studied via the isothermal solubility phase equilibrium method. The solubility data and liquid properties of density and pH are obtained. The phase diagrams of the quaternary systems, including the water free diagram, the water diagram, and the dry salt diagram, are plotted to show the phase regions, water content, and salting-in effect. NaCl occupies the largest phase region at both 298.15 and 323.15 K. One double salt LiCl·CaCl2·5H2O occurs at 298.15 K and builds up two invariant points; one incommensurate invariant point saturated by (NaCl, LiCl·H2O, LiCl·CaCl2·5H2O) and one commensurate invariant point saturated by (NaCl, CaCl2·4H2O, LiCl·CaCl2·5H2O), but at 323.15 K, no double salt forms. The salting-in effect that happened in ternary systems still occurs in the quaternary Li+, Na+, Ca2+// Cl––H2O system at both temperatures. NaCl saturated concentration increases with LiCl and CaCl2 contents and results in a very high total salt content at commensurate invariant points, e.g., they are 56.92 and 60.62% at 298.15 and 323.15 K, respectively.
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Defence Technology
·
2025
·
IF 5.9
Hao Wang,Chenming Li,Enjie Zhang,Yapeng Ou,Xiaoxia Ma
Hexanitrohexaazaisowurtzitane (CL-20) is a high-energy explosive widely used in composite explosives and propellants, but its application is severely limited by thermally induced ε-to-γ polymorphic transition and high solubility in nitrate ester solvents. The transition reduces energy density and increasing sensitivity, and the solubility causes dissolution-recrystallization defects (e.g., voids, compositional inhomogeneities) during long-term storage. To address these issues while preserving its high energetic performance, this study developed a polydopamine@polyvinylidene fluoride (PDA@PVDF) dual-coating strategy, fabricating CL-20 composite particles with a core-shell structure. In-situ X-ray diffraction (XRD) results confirmed that the ε-to-γ phase transition temperature of CL-20 increased from 110 °C (pristine CL-20) to 140 °C. Meanwhile, the CL-20@PDA@9%PVDF sample exhibited the lowest solubility and the best solvent resistance, and the solubility of CL-20 in nitrate ester solvents was drastically reduced from 0.229 g/100 g to 0.026 g/100 g, an 88.6% decrease, effectively enhancing its structural and solvent resistance stability. For energetic performance, when mixed with aluminum powder at a 7:3 mass ratio, the CL-20@PDA@9%PVDF/Al composite achieved a combustion heat of 8275 J/g, 8.7% higher than that of the unmodified Al/CL-20 system (7611 J/g). Combustion pressure tests showed that although the modified system exhibited slightly lower initial peak pressure and pressure rise rate due to dilute CL-20 content from inert coatings, it presented a unique "delayed enhancement" effect, with pressure gradually surpassing and ultimately exceeding that of the unmodified system in the middle and late combustion stages, enabling more sustained high-pressure output. This work realizes the synergistic optimization of CL-20’s polymorphic/solvent stability and energetic performance, providing a feasible and scalable approach for the practical application of CL-20 in advanced energetic systems.
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FOOD CHEMISTRY
·
2020
·
IF 6.306
Yaoping Hu,Zhijin Gao,Junfei Luo
Facile detection of malachite green (MG), a toxic dye, in aquaculture is urgently demanded for environment and food safety. Herein, we design a novel fluorescent probe, namely red emissive Se,N,Cl-doped carbon dots (CDs), to accurately determinate MG. CDs are prepared by hydrothermal treatment of selenourea and o-phenylenediamine in HCl solution. This material exhibits excitation-independent dual emissions at 625 and 679 nm, with a high quantum yield of 23.6%. A selective and sensitive fluorescent sensor toward MG is established based on inner filter effect, because both the excitation and emission light of CDs can be strongly absorbed by MG. The fluorescence quenching of CDs is linear to the MG concentration over the range of 0.07–2.50 μM with a low detection limit of 21 nM. Trace-level analysis of MG in fish tissue is successfully explored, demonstrating the great potential of the proposed sensor for MG monitoring in aquatic products.
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高影响因子
POWDER TECHNOLOGY
·
2025
·
IF 4.6
Wenqing Li,Shimin Zhang,Songchao Shi,Xin Ruan,Qian Yang,Baoyun Ye,Chongwei An,Jingyu Wang
The proportion of oxidizer in the formulation of composite solid propellants (CSPs) is often more than 50 %. It is very important to explore the preparation of new high-energy oxidizers to improve the energy performance of CSPs. Porous CL-20/FOX-7@AP composite microspheres were prepared by combining high-energy density CL-20 and high safety FOX-7 with traditional oxidant AP through microchannel recrystallization technology coupled with solvent evaporation induced self-assembly technology. The experimental results show that the morphology of porous CL-20/FOX-7@AP composite microspheres is regular, and AP is uniformly attached to the surface of porous CL-20/FOX-7 composite microspheres. Compared with CL-20/FOX-7 composite microspheres, the oxygen balance of CL-20/FOX-7@AP increased from −14.12 % to −8.47 %, and the minimum impact excitation energy of CL-20/FOX-7@AP-1 and CL-20/FOX-7@AP-2 increased by 2.25 J and 3.25 J, respectively. When CL-20/FOX-7@AP-1 and CL-20/FOX-7@ AP-2 were used as new oxidants to replace 10 % AP in CSPs formula, the burning rate increased by 21.52 % and 27.85 % respectively, and the pressurization rate increased by 69.79 % and 75.44 % respectively. CL-20/FOX-7@AP composite microspheres with a porous synergistic core-shell structure are expected to be used as novel high-energy oxidants in CSPs to improve the energy density and energy release efficiency of CSPs.
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