ENERGY & FUELS
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2025
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IF 5.3
Jing Guo,Rui Liu,Chunhui Shen,Shanjun Gao
The N-spirocyclic ammonium with exceptional alkaline stability is employed to fabricate anion exchange membranes (AEMs) suitable for long-lasting fuel cell applications. In this paper, two types of N-spirocyclic ammonium, namely 3-(2-(piperidine-4-yl)ethyl)-6-azaspiro[5.5]undecan-6-ium (ASU) and 3,6-diazaspiro[5.5]undecan-6-ium (DSU), are incorporated into an acrylonitrile-styrene copolymer (SAN) to enhance the alkaline stability of AEMs. The introduction of N-spirocyclic ammonium results in AEMs exhibiting excellent alkaline tolerance, particularly the SAN resin membranes incorporating the ASU group (SAN-ASU-OH), which retain 95.0% of their initial conductivity after undergoing a 720-h alkaline treatment at 80 °C, and 1H NMR shows that almost no β-elimination occurred in the SAN-ASU-OH membranes. The utilization of SAN resin as the primary structural component provides a reasonable tensile strength (8.51 MPa) for SAN-ASU-OH, enhances the ion conductivity of AEMs significantly, and ensures a certain water uptake (WU) at the same time to ensure a low swelling ratio (SR). For instance, hydroxide conductivity of the membranes reached 67.7 mS cm–1 at 80 °C for the SAN-ASU-OH membrane while WU reached 81.65% and SR was limited to only 18.42% at 80 °C. The results indicate that the membranes based on SAN resins incorporating N-spirocyclic ammonium are expected to be promising candidates for future fuel cell applications.
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Journal of Physical Chemistry C
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2011
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IF 4.524
Lijuan Shi,Na Li,Liqiang Zheng
The aggregation behavior of long-chain N-aryl imidazolium ionic liquids (ILs), 1-(2,4,6-trimethylphenyl)-3-alkylimidazolium bromide [Cnpim]Br (n = 10, 12, 14), was investigated in a room temperature IL, 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim][BF4]) by surface tension measurements. Freeze-fracture transmission electron microscopy (FF-TEM) and dynamic light scattering (DLS) measurements further verified that micelles are formed. A relatively lower critical micelle concentration (CMC) and smaller micelle size were observed compared with that of N-alkylimidazolium ILs [Cnmim]Br. The main reason for this phenomenon is that the electrostatic repulsion between the head groups of [Cnpim]Br is weakened due to the incorporation of the 2,4,6-trimethylphenyl group. The thermodynamic parameters of micelle formation of [Cnpim]Br in [bmim][BF4] were estimated from the CMC values and their temperature dependence. The micelle formation process is enthalpy-driven in the investigated temperature range, similar to the case in water. The novel N-aryl imidazolium ILs present strong fluorescence properties in [bmim][BF4], indicating their potential application in the field of photochemistry.
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Molecular Catalysis
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2024
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IF 3.9
Zheng Zhang,Yuqing Chi,Mengya Guo,Li Wang,Xiangwen Zhang,Guozhu Li
Selective hydrogenation is still challenging due to the trade-off between activity and selectivity of the catalyst. Hollow carbon shell confining cobalt nanoparticles is a competitive candidate catalyst, of which the structure and composition should be finely tailored for selective hydrogenation. In this work, Co in ZIF-67 is partially replaced by Zn and coated by polydopamine followed by pyrolysis to realize synergistic Zn regulation and N doping of shell-shaped carbon-cobalt catalyst. By changing Co/Zn ratio, the state of cobalt particles and the structure and composition of the N-doped carbon shell are effectively tuned. When Co/Zn ratio was 1:1, the as-prepared catalyst exhibited the best performance for selective nitro hydrogenation. H 2 is dissociated on cobalt nanoparticles to generate active H radicals, which can be exchanged with H atoms of isopropanol as the solvent for facilitating hydrogenation. Selective adsorption of nitro group occurs on the N-doped carbon shell and the confined cobalt nanoparticles. The catalyst possesses good stability, which still maintained the original performance after 5 cycles.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Songhao Yu,Guifen Tian,Liduan Li,Fei Wang,Kefeng Wang,Junyu Lei,Haijun Hao,Qinghong Xu
TpFO-PA, a novel spherical hollow mesoporous polyamide, was firstly synthesized by the reaction among 1,3,5-tris(4-aminophenyl)benzene (TAPB), furylamine and oxalyl chloride in using silica-gel nanoparticle as hard template, and the composite Cu(I)@TpFO-PA with high catalytic activities in C-N coupling reactions between (hetero)aryl bromide and (hetero)aryl amines under mild conditions was prepared basing on presence of N in the framework. A maximum activity of the catalyst with yield of C-N coupling product were about 311.9 g (product) /mol Cu(I) ·h and 95 % respectively, and the activity could be maintained at least 5 times after the catalyst was reused. The composite Cu(I)@TpFO-PA is a few heterogeneous catalysts reported in catalyzing coupling reaction between aromatic amines and brominated aromatic compounds.
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Journal of Energy Storage
·
2025
·
IF 9.8
Yangyang Wang,Wenzheng Zhu,Guanyu Wang,Caiyun Chen,Wei Xu,Yanjiao Li,Lizhuang Chen,Yingying Chen,Hongxun Yang
Carbon-based materials have excellent conductivity, low cost, and environmental friendliness, making them the primary choice for negative electrode in sodium ion batteries (SIBs). Among them, hard-carbon and soft-carbon as amorphous carbon are considered to have potential as negative electrode for SIBs. However, soft-carbon exhibits a slow charging speed and poor low-temperature performance and hard-carbon behaves a low initial coulombic efficiency, resulting in a key obstacle to their extensive applications in SIBs. Herein, a new N/O co-doping soft-hard carbon nanofiber (PCNF) composite was prepared by electrospinning with heat treatment method, petroleum coke (PC) as soft-carbon and oxygen source and polyacrylonitrile (PAN) as hard-carbon and nitrogen source. The optimal PCNF-800 carbonization at 800 °C delivers an enhancement capacity of 296.1 mAh g −1 at 25 mA g −1 after 100 cycles with the capacity retention of 88.2 %. The excellent electrochemical property is ascribed to the co-doping of N/O in the carbon resulting in the large number of defects which could enhance Na + adsorption and transport, the appropriate interlayer spacing, the porous nanofiber mircostructure, and the synergistic effect between soft and hard carbon. Meanwhile, this study provides a possible new idea for the high-value utilization of petroleum coke.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yukang Fan,Fangbao Fu,Dongjie Yang,Weifeng Liu,Xueqing Qiu
Constructing heteroatom-doped porous carbons with distinct charge storage properties is significant for high-energy–density supercapacitors, yet it remains a formidable challenge. Herein, we employed a thiocyanogen-modulated alkali activation strategy to synthesize N and S co-doped lignin hierarchical porous carbon (NSLHPC). In this process, thiocyanogen serves as a surface modulation mediator to substitute oxygen with nitrogen and sulfur species, while the combination of KOH activation and MgO template generates numerous nanopores within the carbon structure. The three-dimensional interconnected nanosheet architecture facilitates rapid ion transfer and enhances accessibility to active sites. Density functional theory (DFT) calculations demonstrate that introducing N and S heteroatoms through oxygen substitution reduces the adsorption energy barrier of Zn 2+ . Consequently, the optimized NSLHPC exhibits a remarkable specific capacitance of 438F/g at 0.5 A/g in 6 M KOH, delivering an energy density of 10.4 Wh/kg in the symmetric supercapacitor and an impressive energy density of 104.9 Wh/kg in the zinc-ion hybrid capacitor. The NSLHPC cathode also shows an excellent lifespan with capacitance retention of 99.0 % and Columbic efficiency of 100 % over 10,000 cycles. This study presents innovative strategies for engineering high-performance porous carbon electrode materials by emphasizing pore structure modulation and N, S co-doping as crucial approaches.
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PubMed
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Materials
·
2024
·
IF 3.1
Jing Zhan,Liangchen Mao,Rongshui Qin,Jing Qian,Xiaowei Mu
Biomass has been widely used due to its environmental friendliness, sustainability, and low toxicity. In this study, aminophosphorylated cellulose (PNC), a biomass flame retardant containing phosphorus and nitrogen, was synthesized by esterification from cellulose and introduced into polyurethane to prepare flame-retardant rigid polyurethane foam. The combustion properties of the PU and PU/PNC composites were studied using the limiting oxygen index (LOI), UL-94, and cone calorimeter (CCT) methods. The thermal degradation behavior of the PU and PU/PNC composites was analyzed by thermogravimetric analysis (TGA) and thermogravimetric infrared spectroscopy (TG-IR). The char layer after combustion was characterized using SEM, Raman, and XPS. The experimental results showed that the introduction of PNC significantly improved the flame-retardant effect and safety of PU/PNC composites. Adding 15 wt% PNC to PU resulted in a vertical burning grade of V-0 and a limiting oxygen index of 23.5%. Compared to the pure sample, the residual char content of PU/PNC15 in a nitrogen atmosphere increased by 181%, and the total heat release (THR) decreased by 56.3%. A Raman analysis of the char layer after CCT combustion revealed that the ID/IG ratio of PU/PNC15 decreased from 4.11 to 3.61, indicating that the flame retardant could increase the stability of the char layer. The TG-IR results showed that PNC diluted the concentration of O 2 and combustible gases by releasing inert gases such as CO 2 . These findings suggest that the developed PU/PNC composites have significant potential for real-world applications, particularly in industries requiring enhanced fire safety, such as construction, transportation, and electronics. The use of PNC provides an eco-friendly alternative to traditional flame retardants. This research paves the way for the development of safer, more sustainable, and environmentally friendly fire-resistant materials for a wide range of applications.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yueer Ma,Zhao Zhang,Wei Chen,Qianlin Zhang,Shuai Chang,Mei Pan,Xingqiang Lv,Hui Chang
A novel synthetic strategy is proposed to create high zero-valent platinum (Pt) components, sub-nanometer Pt clusters, and three-dimensional (3D) Pt/ nitrogen-doped MXene (N-Ti 3 C 2 T x ) catalyst through electrostatic self-assembly combined with non-in-situ doping pyrolysis. Compared with the primary Pt/Ti 3 C 2 T x , the N-doped Pt/N-Ti 3 C 2 T x , which has a 3D wrinkled porous structure, increases the residence time of methylcyclohexane (MCH) on the catalyst surface during gas–solid reactions and improves the mass transfer efficiency of MCH. In addition, the N-doped Pt/N-Ti 3 C 2 T x , which optimizes the electronic coordination environment, produces sub-nanometer Pt clusters, in which Pt mainly exists as Pt (0) (80.78 %) and avoids the presence of low catalytic activity Pt (IV). The Pt 0.5% /N-MXene catalyst exhibits significant catalytic performance in the dehydrogenation of MCH in a fixed-bed reactor, with a hydrogen evolution rate of 636.30 mmol·g Pt -1 ·min - 1 , which significantly surpasses 176.60 mmol·g Pt -1 ·min - 1 for N-undoped Pt 1% /MXene and 78.13 mmol·g Pt -1 ·min - 1 for commercial Pt 1% /TiO 2 . Density functional theory calculations, Pt/N-Ti 3 C 2 T x exhibits lower Pt electronic states and has a d -band center closer to the Fermi level than Pt/Ti 3 C 2 T x . This configuration leads to the stronger MCH adsorption on the Pt sites of Pt/N-Ti 3 C 2 T x , promoting faster H 2 generation and release, thereby achieving a higher catalytic activity.
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Nanomaterials
·
2024
·Vol. 14
·期 21
·1690
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IF 4.4
Shihao Cui,Dejian Xu,Zhiyuan Wang,Libo Wang,Yikun Zhao,Wei Deng,Qingshan Zhao,Mingbo Wu
Palladium (Pd) catalysts play a crucial role in facilitating Suzuki cross-coupling reactions for the synthesis of valuable organic compounds. However, conventional heterogeneous Pd catalysts often encounter challenges such as leaching and deactivation during reactions, leading to reduced catalytic efficiency. In this study, we employed an innovative intercalation templating strategy to prepare two-dimensional carbon nanosheets with high nitrogen doping derived from petroleum asphalt, which were utilized as a versatile support for immobilizing Pd nanoparticles (Pd/N-CNS) in efficient Suzuki cross-coupling reactions. The results indicate that the anchoring effect of high-pyridinic N species on the two-dimensional carbon nanosheets enhances interactions between Pd and the support, effectively improving both the dispersibility and stability of the Pd nanoparticles. Notably, the Pd/N-CNS catalyst achieved an overall turnover frequency (TOF) of 2390 h−1for the Suzuki cross-coupling reaction under mild conditions, representing approximately a nine-fold increase in activity compared to commercial Pd/C catalysts. Furthermore, this catalyst maintained an overall TOF of 2294 h−1even after five reaction cycles, demonstrating excellent stability. Theoretical calculations corroborate these observed enhancements in catalytic performance by attributing them to improved electron transfer from Pd to the support facilitated by abundant pyridinic N species. This work provides valuable insights into feasible strategies for developing efficient catalysts aimed at sustainable production of biaromatic compounds.
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EUROPEAN POLYMER JOURNAL
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2024
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IF 5.8
Xiaoya Li,Shirong Sun,Qian Zhang,Weidong Wu,Yingchun Liu,Liheng Chen,Xueqing Qiu
This work explores the potential of porphyrin-grafted lignin nanoparticles (TCPP- g -AL-NPs) as a novel, effective, and biocompatible photosensitizer for antibacterial applications. Lignin acted as a sustainable framework, enhancing water-compatibility and single oxygen ( 1 O 2 ) generation of porphyrin. The mechanism study revealed the successful formation of a p-n heterojunction between lignin and porphyrin, which promoted the charge separation and the photocatalytic process of O 2 to 1 O 2 . In vitro antibacterial assessments demonstrated the efficacy of TCPP- g -AL-NPs in eradicating both Gram-negative ( E. coli ) and Gram-positive ( S. aureus ) bacteria under blue LED light irradiation. The observed lower antibacterial effectiveness against E. coli compared to S. aureus could be attributed to the thicker cell membrane of Gram-negative bacteria. Additionally, TCPP- g -AL-NPs exhibited no cytotoxicity towards mouse fibroblast cells (L929). This study presents a straightforward and promising approach for developing lignin-based photosensitizers for photodynamic therapy.
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
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2025
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IF 4.9
Yuzhen Kang,Dongyu Wu,Tiantian Zhang,Yue Zhang,Yan Zhong,Shiqi Chen,Xiaoyu Wang,Xuyu Chai
In this study, we investigated the feasibility of using poly(N-acryloyl 6-aminocaproic acid) (PA6ACA) as a pH-responsive polymer for oral enteric drug delivery. PA6ACA, characterized by its acylamino group, carboxyl group, and flexible 5-carbon chain, demonstrates pH sensitivity due to the presence of ionizable carboxyl groups and hydrogen bonding interactions between the carboxyl and amino moieties. Our research focused primarily on the preparation, characterization, and evaluation of enteric drugs delivered via PA6ACA. We evaluated the morphology, structure, thermal properties, and crystallinity of PA6ACA. Cytotoxicity experiments conducted in Caco-2 cells and the oral administration studies in mice provided preliminary safety evidence for PA6ACA. Three model drugs (budesonide, sulfasalazine, and diclofenac sodium) were employed to fabricate drug-polymer coprecipitates, and PA6ACA exhibited high loading capacities for these drugs. Furthermore, the drug release profiles revealed that the drug-loaded polymers were resistant to acid at pH 1.0 and nearly completely dissolved within the next 8 h at pH 6.8. The kinetic model fitting results indicated that the release of drugs from the coprecipitates were more consistent with the Higuchi model, suggesting minimal polymer swelling in the media and a primary drug release mechanism via diffusion. Based on these findings, we conclude that PA6ACA holds promise for the development of innovative and efficient intestine-specific drug delivery systems.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Xinlei Jia,Donghui Guo,Zelong Wang,Ning Zhou,Runze Jin,Baosheng Xu
Regulating the composition and microstructure of nanomaterials is a major challenge in the development of high-performance materials for electromagnetic wave (EMW) absorption. This paper introduces a new lightweight EMW-absorbing material Co@N/C with a yolk–shell structure and compositions of ferromagnetic metal and carbon materials. The minimum reflection loss (RL min ) of the as-designed Co@N/C nanospheres with a filler loading of 25 wt% reaches −67.68 dB and the effective absorption bandwidth of a 1.9 mm thickness is 5.3 GHz. The exceptional absorption performance of the EMW absorption is primarily achieved through the synergistic effect between the Co–carbonaceous material and the yolk–shell structure, which optimizes the impedance matching. The polarization loss, conductivity loss, magnetic loss, and multiple scattering mainly contribute to the excellent EMW-absorption ability of the materials. The proposed method for regulating the structure and morphology of Co@N/C can efficiently construct high-performance EMW absorbers.
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