ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Xiaoming Xu,Zhiwei Wang,Guoyan Hua,Sunxinyi Wang,Yuxuan Chen,Zepeng Zhang,Fuqiang Liu,Pengrui Jin,Huanting Wang
Nanofiltration (NF) technology is crucial in alleviating global water scarcity through desalination. Overcoming the permselectivity trade-off to improve both the permeance and rejection of polyamide (PA) nanofiltration (NF) membranes beyond the log–log upper bound remains a significant scientific challenge. Herein, we explored advanced ion-transport barriers by constructing a chitin-assisted PA NF membrane, incorporating a biomass-derived carboxylated chitin nanofiber (CO-ChNF) interlayer that simultaneously modulates the pore architecture and surface charge of the PA layer. CO-ChNFs, sustainably extracted from squid cartilage and featuring rich carboxyl and amino functionalities, effectively suppressed the diffusion kinetics of amine monomers during interfacial polymerization. The engineered CO-ChNF/PA membranes demonstrated a sharper pore size distribution and an enhanced charge density, providing an ideal platform to systematically investigate the mechanisms behind ion sieving at PA microinterfaces by exploring ion dehydration energy and electrostatic repulsion energy. Leveraging the enhanced transport barriers, the optimal CO-ChNF/PA membrane achieved impressive performances with a permeance of up to 31.4 L m–2 h–1 bar–1 and a superior Cl–/SO42– selectivity of 91.3, surpassing most commercial and reported NF membranes. This work sheds light on the regulatory mechanism of the chitin-assisted interfacial polymerization reaction and introduces an innovative approach for efficient Cl–/SO42– sieving.
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PubMed
高影响因子
FirePhysChem
·
2023
·
IF 0
Weijun He,Yaning Li,Peng Bao,Yuanlin Fan,Mingshuai Xue,Boliang Wang
To reduce the mechanical sensitivity of CL-20, this study is based on the surface modification of CL-20, and explores the effects of two preparation processes, the water solution-suspension method and the phase separation method, on the coating process of CL-20. Based on the structural characteristics of surfactants, a formulation was devised, using 2-cyanoethyltriethoxysilane (SCA2) as the surfactant and microcrystalline wax as the desensitizer. The samples underwent comprehensive characterization employing SEM, XPS, DSC, XRD, friction sensitivity testing, and impact sensitivity testing to evaluate both their structural composition and inherent properties. The results showed that the composite particles prepared using the phase separation method displayed a compact coating layer on CL-20 surfaces. Specifically, the composite particle CL-20@SCA2/Wax-P, which contained the surfactant, exhibited a thin and dense film on its surface. The proportion of -NO 2 groups on the surface of the composite particles experienced a reduction of 13.12% compared with CL-20. The crystal form of CL-20 remained unchanged in four composite particles. The decomposition peak temperatures and activation energy of all four composite particles were decreased, resulting in reduced thermal stability. The critical friction sensitivity load for composite particles produced via the aqueous suspension method is 252N, whereas for those prepared using the phase separation method, it elevates to 360N. The characteristic drop height (H 50 ) of composite particles prepared by the phase separation method increased significantly, 34cm for CL-20/W-P composite particles and 55cm for CL-20@SCA2/W-P composite particles, compared with the raw CL-20. These results suggest that the utilization of SCA2 effectively modified the surface of CL-20, and the composite particles prepared using the phase separation method demonstrated a considerable reduction in mechanical sensitivity.
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FirePhysChem
·
2025
·
IF 3.6
Chunyan Li,Shenjuan Shao,Jiao Chen,Chongwei An,Baoyun Ye
The development of miniaturized, flexible MEMS pyrotechnic devices necessitates advanced fabrication techniques. Herein, a strategy is reported that leverages the integration of ink-jet printing and dynamic cross-linking. The strategy successfully fabricates CL-20/PVA (polyvinyl alcohol)@PANI (polyaniline) energetic films with robust interfacial adhesion across heterogeneous structures. The PVA@PANI dynamic bonding system, designed through a molecular engineering strategy, provides dual interfacial enhancement characteristics. The 3D network structure formed by dynamic covalent cross-linking of borate ester bonds significantly enhances the flexibility of the system, as demonstrated by a 62.26% improvement in elastic recovery and a 55.26% increase in the plasticity index. Additionally, multiple hydrogen bonding interactions between hydroxyl groups and the substrate substantially improve interfacial adhesion, achieving a 4B rating on both glass and aluminum substrates. SEM characterization reveals a uniform and dense microstructure with homogeneously distributed crystals throughout the composite film. Performance testing confirms that CL-20 in the composite retains its ε-crystal form and exhibits a high detonation velocity of 7884 m·s⁻¹. Furthermore, the synergistic incorporation of PANI reduces the electrostatic sensitivity by 10.86% compared to the CL-20/PVA baseline. The interfacial dynamic enhancement technology developed in this work represents a key advancement in the integrated structure–function design of microscale energetic devices, underscoring its strong potential for MEMS applications such as flexible micro-initiators and miniature solid propellants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yuanli Li,Chunqiang Zhuang,Shi Qiu,Junfeng Gao,Quan Zhou,Zaicheng Sun,Zhenhui Kang,Xiaodong Han
Metal halide perovskites with broad optical absorption and long carrier lifetime are considered as ideal photocatalysts. However, their poor stability in water greatly impedes their application in photocatalytic H 2 evolution because they lose their crystalline structure in water. Herein, we proclaim a new class of photocatalysts: all-inorganic Cs-Cu-Cl perovskite quantum dots (QDs). It exhibits a high photocatalytic hydrogen production rate of ∼ 3.1 mmol/g/h without any cocatalyst under AM 1.5-G solar irradiation (100 mW/cm 2 ). Especially, it remains the high activity for up to 330 h without apparent deterioration of the hydrogen production rate. Density functional theory (DFT) calculations reveal that the Cu site works as the electron and proton absorption sites as the H 2 production active center. To our best knowledge, there is no report of metal halide perovskites as water-stable photocatalysts. This work opens an innovative way for guiding the exploration of metal halide perovskites photocatalysts for stable photocatalytic H 2 evolution.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jianmin Wang,Shanshan Zheng,Haijin Li,Ruoyu Huang,Yuan Zhu,Hao Zhang,Jinyang Qian,Yongtao Li,Xiaofang Liu,Xiaolong Deng
The oxygen evolution reaction (OER) is a vital half-reaction involved in water splitting applications. However, the slow kinetics of its four-electron transfer process have become a bottleneck for performance improvement. Surface engineering has emerged as a pivotal strategy to surmount the inherent kinetic limitations of OER. Herein, this work proposed a simple Cl − -promoted electrochemical surface reconstruction strategy. The as-obtained Ni 3 S 2 -PBA-NaCl-5000s exhibited excellent OER performance, with a low overpotential of 260 mV at 10 mA cm −2 and a small Tafel slope of 38.2 mV dec −1 in alkaline media. The addition of Cl − in the electrolyte not only accelerated the surface activation process but also modulated the structure of the in-situ generated NiFe oxide hydroxides/hydroxyls (NiFeOOH). Compared to the pure KOH condition, the obtained NiFeOOH exhibited a larger surface area, yielded a higher concentration of OH − environment on the surface, which facilitated the OER kinetics rate. Moreover, lattice oxygen is triggered, thus enabling the reaction via a faster lattice oxygen-mediated mechanism (LOM) pathway, which presents lower thermodynamic barriers. This work may offer a fresh perspective on clarifying the OER activity enhancement mechanism by the influence of Cl − in the electrolyte on the electrochemical surface reconstruction process.
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ACS Catalysis
·
2026
·
IF 13.6
Ningchao Zhu,Chunlan Chen,Zhongyao Zhang,Xiaohu Ge,Yueqiang Cao,Xiangzhou Liao,Xinggui Zhou,De Chen,Weikang Yuan,Xuezhi Duan
Selective dehydrochlorination of HCFC-244bb is a key step toward the synthesis of next-generation HFO-1234yf refrigerants, yet achieving high selectivity is hindered by competitive C−F bond activation. Herein, we report a series of Ni- and Cr-based catalysts with systematically tuned surface Lewis acidity. Mechanistically informed spectroscopic characterization and electronic structure analysis demonstrate that ligand electronegativity and metal oxidation state regulate the metal−ligand bonding continuum from predominantly covalent to increasingly ionic character. Catalytic testing reveals a pronounced trade-off between activity and selectivity, with NiO achieving an HFO-1234yf selectivity of 91.36%. Density functional theory calculations and frontier molecular orbital analyses identify the conduction band minimum (CBM) energy as a decisive electronic descriptor for selectivity. An S-shaped correlation between CBM energy and selectivity thereby emerges, providing a predictive framework for the rational design of high-performance dehydrohalogenation catalysts through band-structure engineering.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Mengjun Xiao,Yu Gui,Andraž Mavrič,Yao Nie,Wendong Zhang,Peng Chen,Pengpeng Wang,Yi Wang
The chlorine evolution reaction (CER) is essential for industrial chlorine production. However, achieving high CER selectivity remains a challenge due to the high cost and narrow potential gap between the CER and the competing oxygen evolution reaction (OER) in conventional noble oxide catalysts. In this work, Hemin is adopted as a model molecular catalyst for CER owing to its porphyrin macrocycle and the axial Cl ligand, achieving an overpotential of ∼190 mV at 10 mA cm–2 with ∼100% chlorine selectivity and excellent stability over 100 h in corrosive acidic brine. Spectroscopic and electrochemical analyses reveal that the axial Cl–Fe interaction stabilizes the rigid configuration geometry of the Hemin molecule, while the π-conjugated macrocycle and the Fe-centered electronic effect jointly modulate the electronic state of Fe. This combination effectively suppresses electrochemical demetalation and preserves structural integrity for enhancing selectivity and durability. It is hoped that this work can propose fundamental insight into the rational design of efficient molecular electrocatalysts for promoted chlorine evolution.
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PubMed
高影响因子
Crystals
·
2026
·Vol. 16
·期 6
·368
·
IF 2.9
Xiaolu Mao,Changsheng Yin,Yang Cao,Xiaodong Shen,Wenbo Xin
Carbon nanotubes (CNT) are among the strongest candidates for electromagnetic interference (EMI) shielding materials because of their excellent performance. However, when assembled into macroscale materials, their conductivity is usually limited to 104S/m, restricting further application as shielding materials. Here, we prepared a carbon nanotube composite film (Au/Cl-CNT) with high conductivity and excellent EMI properties. Characterizations confirm that Au exists in the form of uniform Au plates and particles anchored on the CNT surface, while Cl is doped into the CNT framework as halogen dopants. The optimized Au/Cl-CNT film delivers an ultra-high electrical conductivity of 3.39 × 105S/m, which is approximately 23 times higher than that of the pristine CNT film. The excellent electrical properties of the Au/Cl-CNT films endow them with excellent EMI shielding effectiveness (SE). Au/Cl-CNT films with a thickness of ~10.5 μm achieve an EMI SE of up to 67 dB across both the X-band and Ku-band. The superior EMI SE mainly results from the combined effect of various mechanisms, namely reflection inside and outside the material, as well as absorption inside the material. This work clarifies the synergistic enhancement mechanism of Au and Cl on CNT conductivity and EMI shielding, offering new insights into halogen-modified shielding materials.
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Journal of Materials Chemistry C
·
2026
·
IF 5.1
Cong Niu,Qingsong Zhang,Yulian Zhang,Qianqian Huang,Jinbao Chen,Xin Wang
Lead halide perovskite single crystals have demonstrated significant potential for X-ray and gamma-ray detection. While these high-energy photons generate charge carriers within the crystal, they also induce irradiation damage, a phenomenon that has not been extensively studied in these materials. In this work, we investigate the structural and charge transport properties of MAPbBr 2.5 Cl 0.5 perovskite single crystals under 50 kV X-ray irradiation. Transmission electron microscopy reveals that irradiation induces lattice defects. Furthermore, analyses via the space-charge-limited current and time-of-flight methods confirm that these defects increase trap density and reduce charge carrier mobility. The degradation of charge transport properties is also found to be strongly dependent on both the crystal orientation and the direction of the incident radiation. This study provides critical insights into the irradiation damage mechanisms in lead halide perovskite single crystals.
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PETROLEUM CHEMISTRY
·
2026
·Vol. 66
·期 1
·49-56
·
IF 1.1
Yu Hongyin,Zhao Rongxiang,Li Xiuping,Hou Liangpei
A deep eutectic solvents (DES) was synthesized by stirring mixture of 1-butyl-pyridinehydrochloride ([C 4 pyr]Cl) and oxalic acid (C 2 H 2 O 4 ) at 100°C. The [C 4 pyr]Cl/C 2 H 2 O 4 DES was characterized by FT-IR and 1 H NMR spectroscopy. This DES is capable of extracting thiophene-type sulfides due to the similar polarity of 1-butyl-pyridine and DBT. The –COOH groups within the [C 4 pyr]Cl/C 2 H 2 O 4 DES are readily oxidized to ‒COOOH by H 2 O 2 , which susequently catalyzes the thiophene oxidation into sulfone in the model oil. The higher polarity of sulfone compared to that of thiophone enhances their solubility in the solvent. When the V(DES)/V(model oil) = 0.2, T = 50°C, and O/S = 6, the DBT removal rate reached 98.6% within 80 min. The catalytic activity of [C 4 pyr]Cl/C 2 H 2 O 4 exhibited only a slight decrease after nine regeneration cycles. The apparent activation energy for DBT removal using [C 4 pyr]Cl/C 2 H 2 O 4 was 33.3 kJ/mol. Experimental results indicate that the low apparent activation energy contributes to the high desulfurization efficiency.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yali Wang,Hongbao Ren,Ruizhi Cui,Bo Zhang,Qiuye Yang,Wu Li
A glycerol-water coordination method was developed to prepare high-pure KCl from K(Cl, Br) solid solutions. • Glycerol inhibits Br − from entering the KCl lattice. 30 wt% mixed solvent shows better separation performance. • KCl with 99.994% purity and 97.30% yield was obtained, while bromide was concentrated in the liquid phase. High-purity KCl is essential for semiconductors and laser crystals, yet even trace bromine severely compromises its performance. During the preparation of KCl via underground brine crystallization, Br − readily enters the KCl lattice to replace Cl − , forming crystals with a single-salt structure rather than a simple mixture. This makes it difficult to use conventional separation methods to produce high-purity KCl. To address this issue, this study proposes a separation strategy that involves intervening in the recrystallization process by regulating coordination interactions within the solvent system, thereby yielding ultra-pure potassium chloride. Systematic studies involving phase equilibrium experiments, solid-liquid phase characterization and molecular simulations indicate that as the number of hydroxyl groups in the alcohol molecule increases, the solvent's separation capacity increases accordingly, with glycerol exhibiting the best performance. As the simplest trihydric alcohol, glycerol's three hydroxyl groups create distinct solvation environments for Cl − and Br − , thereby inhibiting Br − from occupying the KCl lattice during the concentration and crystallization processes. Furthermore, the introduction of 30 wt% mass water inhibits intermolecular hydrogen bonding and self-aggregation of glycerol, releasing free coordination sites and significantly increasing the solubility of KCl in the system (from 1.7 wt% to 9.63 wt%), thereby further optimizing separation efficiency. The separation process, designed based on the phase diagram of the KCl − KBr − Gly(30 wt%) − H₂O system at 298.15 K, enables the efficient recovery of high-purity KCl (purity up to 99.9940%, recovery rate of 97.30%) and the simultaneous enrichment of bromine resources in the liquid phase (bromine content increased from 3.36 wt% to 44.30 wt%).
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Small
·
2026
·
IF 11.8
Yujie Song,Ya Guo,Ruibing Lv,Nan Wu,Xiaoqing Zhou,Shilong Hao,Hongzhen Li,Qi Zhang
Hierarchical homostructured core-shell architectures (HHCS) integrate the advantages of maintaining high energy density and enhancing interfacial stability. However, their rational design and controllable construction remain significantly challenging. Herein, we propose a self-limiting surface pseudomorphic replacement strategy mediated by localized solvation regulation, enabling the precise construction of HHCS of ε-2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (ε-CL-20). Specifically, a γ-butyrolactone (γ-BL)/H 2 O mixed solvent system induces a selective surface dissolution—recrystallization process on ε-CL-20 crystals, forming a stable CL-20∙γ-BL solvate (S γ-BL ) layer. This layer undergoes interfacially induced nucleation on the crystal surface and exhibits self-limiting growth while preserving the morphology of the parent crystal, thereby enabling a morphology-preserving pseudomorphic replacement process. Upon thermal treatment, solvent removal and solid-state rearrangement facilitate the conversion of the outer solvate shell into the CL-20 phase, yielding a homogeneous shell with hierarchical nanoporous features. The resulting HHCS of CL-20 exhibits a remarkable enhancement in safety performance: its impact sensitivity value increases from 2.5 to 12 J, while the packing density decreases by only 4.85%. Importantly, the core-shell structure consists solely of ε-CL-20, with no heterogeneous materials. This work presents an interfacial-engineering strategy that provides new theoretical and methodological insights for the safety-oriented design and structural regulation of high-energy molecular crystals.
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