Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Jun Li,Sen Li,Renting Li,Suying Chu,Zhanhua Ma,Lanyi Sun
During the alcoholysis of polyvinyl acetate to produce polyvinyl alcohol, large volumes of wastewater containing methanol (MeOH) and methyl acetate (MA) are generated. Due to the azeotropic nature of the MeOH-MA mixture under atmospheric pressure, their separation via conventional distillation is highly challenging. Extractive distillation presents a promising alternative; however, traditional entrainers often suffer from high volatility, toxicity, and significant energy requirements. Deep eutectic solvents (DESs), characterized by low vapor pressure, biodegradability, and ease of regeneration, have emerged as green alternatives. This study aims to identify efficient DESs for separating the MeOH/MA azeotrope. Guided by conductor-like screening model for segment activity coefficient (COSMO-SAC) model predictions, three choline chloride (ChCl)-based DESs—DES1 (ChCl:urea), DES2 (ChCl:ethylene glycol), and DES3 (ChCl:glycerol)—were selected and evaluated through vapor-liquid equilibrium (VLE) experiments at 101.3 kPa. The addition of 20 mol% DESs significantly enhanced the relative volatility of MA with respect to MeOH. The VLE data were well correlated using the non-random two-liquid (NRTL) model. To elucidate the separation mechanism, molecular dynamics simulations were performed to identify stable DES-MeOH/MA cluster configurations. Electrostatic potential (ESP) analysis, electron density difference mapping, van der Waals surface penetration, Hirshfeld surface (HS) analysis, the independent gradient model based on Hirshfeld partition (IGMH), and electron localization function (ELF) analyses revealed that hydrogen bonding plays a dominant role in selectivity. Finally, a quantitative structure-activity relationship (QS-AR) based toxicity assessment confirmed that all three DESs exhibit substantially lower toxicity than conventional extractants. These findings underscore the potential of DESs as green entrainers for the efficient and sustainable separation of the MeOH/MA azeotropic system.
研究领域:
环境化学
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分离科学
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绿色化工
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分子模拟
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物理化学
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可持续工程
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工业废水处理
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产品关联
DOI
高影响因子
Toxics
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2024
·Vol. 12
·期 7
·524
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IF 3.9
Yuanzhen Li,Yinming Fan,Yanhong Wang,Yinian Zhu,Zongqiang Zhu,Shengpeng Mo,Xiaobin Zhou,Yanping Zhang
VOCs can be used instead of ammonia as a reducing agent to remove NO, achieving the effect of removing VOCs and NO simultaneously. Due to the high energy consumption and low photocatalytic efficiency required for conventional thermocatalytic purification, photothermal coupled catalytic purification can integrate the advantages of photocatalysis and thermocatalysis in order to achieve the effect of pollutants being treated efficiently with a low energy consumption. In this study, samples loaded with Co and Mn catalysts were prepared using the hydrothermal method on Fe-MOF with various morphologies. The catalytic performance of each catalyst was analyzed by studying the effects of their physicochemical properties through various characterizations, including XRD, SEM, BET, XPS, H2-TPR, TEM and O2-TPD. The characterization results demonstrated that the specific surface area, pore volume, high valence Co and Mn atoms, surface adsorbed oxygen and the abundance of oxygen lattice defects in the catalysts were the most critical factors affecting the performance of the catalysts. Based on the results of the performance tests, the catalysts prepared with an octahedral-shaped Fe-MOF loaded with Co and Mn showed a better performance than those loaded with Co and Mn on a rod-shaped Fe-MOF. The conversions of acetone and NO reached 50% and 64%, respectively, at 240 °C. The results showed that the catalysts were capable of removing acetone and NO at the same time. Compared with the pure Fe-MOF without Co and Mn, the loaded catalysts showed a significantly higher ability to remove acetone and NO simultaneously under the combination of various factors. The key reaction steps for the catalytic conversion of acetone and NO on the catalyst surface were investigated according to the Mars–van Krevelen (MvK) mechanism, and a possible mechanism was proposed. This study presents a new idea for the simultaneous removal of acetone and NOxby photothermal coupling.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2024
·
IF 4.7
Meng Liu,Caixia Miao,Zhijie Wu
The direct synthesis of methyl acetate (MA) from methanol is an appealing and green approach, but an efficient catalyst is urgently needed. Herein, Cu-Ni bimetallic clusters, with a diameter of ∼1.2 nm, have been successfully encapsulated within BEA zeolite by an in-situ two-step encapsulation method (Cu-Ni@Beta), which significantly favors the dispersion of metals compared to the ion-exchanging (Cu/Ni@Beta) and wet impregnation approach (Cu-Ni/Beta). The as-synthesized Cu-Ni@Beta catalyst shows a MA formation rate of 1.46 mmol s −1 g (Cu+Ni) −1 , which is much higher than Cu/Ni@Beta of 0.02 mmol s −1 g (Cu+Ni) −1 and Cu-Ni/Beta of 0.12 mmol s −1 g (Cu+Ni) −1 . Characterization studies reveal that zeolite constraints could not only provide the spatial confinement for metal clusters but also induce an electronic interaction between confined Cu and Ni species in Cu-Ni@Beta. This interaction can increase and stabilize Cu + sites as well as Lewis acid sites, which are crucial for improving catalytic performance. In-situ FTIR experiments indicate that the formation of formaldehyde (CH 2 O*) is the critical step for methanol to MA, and the CH 2 O* further couples with methoxy (CH 3 O*) to form acetate species (CH 3 CHO*), which subsequently couples with CH 3 O* to produce MA.
研究领域:
催化化学
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材料科学
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绿色化学
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产品关联
DOI
高影响因子
LANGMUIR
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2024
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IF 3.7
Yunju Wang,Xintong Zhang,Yichun Liu,Shunchao Ma,Li Qi,Hongyu Wang
Intercalation of anions unlocks graphite as a positive material in energy storage devices, and the performance could be affected by solvents in solutions. In this context, it is vital to investigate the role of solvents in anion intercalation. Herein, a hierarchical intercalation phenomenon, in which different graphite intercalation compounds are generated in the same solution, is studied in lithium tetrafluoroborate (LiBF4) solutions of carboxylate ester solvents γ-butyrolactone (GBL) and methyl acetate (MA). The evolution modes of the graphite cathode structure during electrochemical intercalation and deintercalation are discussed via in situ X-ray diffraction (XRD) measurements. Based on this, the relationship between GICs and potentials, together with concentrations, is compared in detail. Furthermore, various graphite materials with different surface properties are applied to adjust the anions’ solvation status inside graphite sheets.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
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2024
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IF 5.7
Zhen Wei,Yanxin Li,Shuyue Guo,Rui Han,Xiliang Luo
The accurate and reliable quantification of the levels of disease markers in human sweat is of significance for health monitoring through wearable sensing technology, but the sensors performed in real sweat always suffer from biofouling that cause performance degradation or even malfunction. We herein developed a wearable antifouling electrochemical sensor based on a novel multifunctional hydrogel for the detection of targets in sweat. The integration of polyethylene glycol (PEG) into the sulfobetaine methacrylate (SBMA) hydrogel results in a robust network structure characterized by abundant hydrophilic groups on its surface, significantly enhancing the PEG-SBMA hydrogel's antifouling and mechanical properties. The wearable sweat sensor is specifically designed for ascorbic acid (AA) detection. The incorporation of a silver nanoparticles-molybdenum disulfide (AgNPs-MoS 2 ) composite material into the hydrogel significantly enhances its catalytic properties towards AA. Electrochemical analysis confirms that the sensor reliably detects AA in real sweat with minimal interference from other components and bacteria, demonstrating its practical application potential. Furthermore, this multifunctional hydrogel's mechanical robustness and strong adhesion to various substrates ensure its practical applicability in wearable devices. This technology provides a foundation for accurate health monitoring in wearable sensors, enabling advanced, non-invasive diagnostic tools for personalized healthcare.
研究领域:
生物医学工程
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材料科学
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健康监测技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Chengzhou Tao,Tianle Zheng,Pengfei Jia,Wuze Gong,Guma Yila,Lina Wang,Tianxi Liu
Hindered by the high diffusion energy barrier of Li+ in graphite anode layers, the low-temperature application of traditional Li-ion batteries is limited. Lithium metal without intercalation and with excellent specific capacity is expected to support battery operation at low temperatures. However, due to the low conductivity, high freezing point, and strong solvation energy of traditional carbonate electrolytes, the application of lithium–metal batteries at low temperatures remains challenged. In this paper, an all-ester-based ternary solvent electrolyte based on fluorinated carbonate and methyl acetate is developed to improve the cyclic efficiency of the Li-metal anode at subzero temperatures. Methyl acetate, with low viscosity and low freezing point, endows Li+ with efficient transfer in the bulk phase at low temperatures. Fluorinated cosolvent regulates the solvation structure, thereby facilitating Li+ desolvation while forming a LiF-rich solid electrolyte interphase. The electrolyte exhibits good compatibility with the Li-metal anode, as confirmed by the significantly reduced kinetic barrier of Li+ diffusion at the interface. The theoretical calculations suggest that anions occupy the dominant positions within the inner solvation sheath. The in situ/ex situ characterizations provide straightforward evidence of a dendrite-free Li-metal electrode during cycling. As a result, the symmetric Li||Li cell is able to cycle stably for thousands of hours at current densities of 0.5 mA cm–2 and 1 mAh cm–2. When paired with a LiFePO4 cathode, the battery at 0.2 C (1 C = 170 mA g–1) has a capacity retention of 95.4% after 200 cycles at −15 °C and 92.6% after 100 cycles at −20 °C, respectively.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
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IF 9
Zhenggang Wang,Jing Yin,Yuanhang Jin,Feifan Yang,Haipeng Zhu,Siyuan Huang,Boqun Cao,Gongping Liu,Wanqin Jin
Pervaporation membrane process is promising for separation of organic-organic azeotropic systems, while a trade-off relationship restricts the performance of widely-studied polymeric membranes. In this work, we proposed a MOF ligand engineering strategy to boost the molecular-sieving property of mixed-matrix membrane (MMM) by synergistically manipulating the channel size, affinity and interfacial morphology. Specially, we designed UiO-66-(NH 2 ) 2 /polyvinyl alcohol (PVA) mixed-matrix membranes to separate methanol (MeOH)/methyl acetate (MeOAc) azeotropic mixture via pervaporation process. By comparing the incorporation of UiO-66-(NH 2 ) 2 , UiO-66 and p-phenylenediamine (PPD), the MOF pore size and chemistry were systematically investigated on the influence of microstructures and separation performance of the MMMs. The results demonstrated that the rationally introduced para-position –NH 2 groups on the terephthalic acid (BDC) ligands not only finely reduce the MOF pore size of UiO-66 filler, but also improve the interfacial compatibility via hydrogen bonding between UiO-66 and PVA chain, as well as enhance the MeOH affinity in the MMM. The optimized 7.5 wt% UiO-66-(NH 2 ) 2 /PVA MMM exhibited a total flux of 1554.6 g/m 2 h and a separation factor of 70.9 in 20 wt% MeOH/MeOAc azeotropic mixture at 30 °C, which is superior to the state-of-the-art membranes. The ligand engineering strategy offers a route for regulating the morphology and molecular transport property of mixed-matrix membranes.
研究领域:
化学工程
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材料科学
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膜分离技术
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物理化学
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纳米技术
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产品关联
DOI
高影响因子
POLYMER DEGRADATION AND STABILITY
·
2024
·
IF 6.3
Peng Zhao,Xiaojing Cui,Chizhou Wang,Xiaojie Shao,Hongyan Li,Ning Zhang,Xianglin Hou,Tiansheng Deng
Enormous challenges have been encountered in the degradation and recycling of unsaturated polyester resin (UPR) in water, primarily due to its water resistance. Herein, a novel, efficient and green catalytic system of methanesulfonic acid (MSA)/sodium laurylsulfonate (SLS) was proposed to aqueously degrade UPR under mild conditions (200°C). This method is considerably milder compared to other reported works based on aqueous hydrolysis (230°C-380°C). What's more, amphiphilic SLS as a phase transfer reagent enhanced the concentration of catalyst at the H 2 O-UPR interface, which facilitated the mass transfer between organic motifs with inorganic reagents and thus accelerated the reaction. The NMR and FT-IR characterizations indicated the ester bonds were cleaved via hydrolysis with H 2 O catalyzed by MSA, and high value-added products, i.e., copolymer of styrene and maleic anhydride (SMA) and phthalic acid (PA), were reclaimed by a simple separation process, with the yield of 86.77% and 84.37%, respectively. Furthermore, a viable mechanism for degradation was proposed through the degradation performance of the model compounds. This study provides a practical approach for the chemical degradation and conversion of other resins containing ester bonds.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CELLULOSE
·
2024
·
IF 4.9
Mo Minfu,Lin Yaling,Lin Junkang,Ma Xiaojuan,Hong Yubin,Chen Lihui,Wang Dong,Huang Liulian
In this work, an antimicrobial cellulose acetate composite nanofiltration membrane was successfully prepared via in-situ hybridization by anchoring silver nanoparticles (AgNPs) onto the surface of the cellulose acetate nanofiltration membranes for water treatment. DETA monomer was used as a reducing agent to reduce Ag + in AgNO 3 to AgNPs, while the primary amine group of Diethylenetriamine (DETA) monomer can react with 1,3,5-Trimesoyl chloride (TMC) to form a polyamides layer. As a result, the cellulose acetate nanofiltration membranes modified by AgNPs exhibited smoother surfaces and improved hydrophilicity, which resulted in enhanced permeability and resistance to fouling. The flux of the membrane increased from 12 to 37.7 L/m 2 h, and the FRR values of the membrane increased from 98.4 to 100% respectively in 3.5 cycles. Owing to robust electrostatic interaction between AgNPs and carboxyl groups of the cellulose acetate support, the membranes showed stable separation performance. Over extended operational periods, the membrane retained 37.7 L/m 2 h of flux and 92% of Na 2 SO 4 retention rate. Benefiting from the broad-spectrum antibacterial properties of silver, the membranes showed an excellent bactericidal rate of E. coli and S. aureus (> 99%). This work provided a new method for preparing cellulose acetate nanofiltration membranes with excellent antibacterial and separation performance. It also paved a new avenue to water treatment.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Luhang Xu,Yuang Fu,Yuhao Li,Guodong Zhou,Xinhui Lu
The migration of mobile ionic halide vacancies is usually considered detrimental to the performance and stability of perovskite optoelectronic devices. Taking advantage of this intrinsic feature, we fabricated a CsPbI3 perovskite quantum dot (PQD)-based write-once-read-many-times (WORM) memory device with a simple sandwich structure that demonstrates intrinsic ternary states with a high ON/OFF ratio of 103:102:1 and a long retention time of 104 s. Through electrochemical impedance spectroscopy, we proved that the resistive switching is achieved by the migration of mobile iodine vacancies (VIs) under an electric field to form conductive filaments (CFs). Using in situ conductive atomic force microscopy, we further revealed that the multilevel property arises from the different activation energies for VIs to migrate at grain boundaries and grain interiors, resulting in two distinct pathways for CFs to grow. Our work highlights the potential of CsPbI3 PQD-based WORM devices, showcasing intrinsic multilevel properties achieved in a simple device structure by rationally controlling the drift of ionic defects.
研究领域:
材料科学
·
电子工程
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Huiyuan Bai,Zhibin Huang,Yuhang Xu,Yijie Wang,Lei Zhang
All-inorganic blue-emissive CsPbBr3 perovskite nanoplatelets (NPLs) are promising for optoelectronic applications due to excellent optical properties, but their applicability is seriously restricted by a low photoluminescence efficiency and poor stability. Here, we develop a postsynthetic surface-mediated engineering strategy to prepare high-quality blue CsPbBr3 NPLs at room temperature by using strongly bound polystyrene sulfonic acid (PSS). PSS efficiently passivates the surface trap sites of NPLs via strong coordination bonds, thereby achieving high-efficiency exciton recombination and enhancing photostability. The optimized PSS-NPLs reveal intense blue emission with a central wavelength of ∼466 nm and a high photoluminescence quantum yield of ∼83.2%, indicating a substantial improvement from ∼48.3% of pristine NPLs. Simultaneously, the PSS-treated NPLs exhibit significantly enhanced stability in comparison with pristine NPLs during UV exposure and thermal treatment. Finally, we achieve efficient blue NPL-LEDs (peaked at ∼468 nm) using a PSS-NPL-polymer composite film, corresponding to CIE color coordinates of (0.124, 0.067), which closely approach to the Rec. 2020 blue standard. Hence, our work offers a facile strategy for fabricating high-performance perovskite NPLs and promotes their potential applications in blue-emitting optoelectronic devices.
研究领域:
材料科学
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光学工程
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电子器件
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Weikang Mei,Guobao Xu,Hongyu Wang
Li4Ti5O12 (LTO)/LiNi0.5Mn1.5O4 (LNMO) batteries have appealing features, such as suitable energy density and high safety. A proper binder of the LNMO cathode and electrolyte can improve the performance of batteries. Herein, we first combined the polyacrylic acid (PAA) binder with an ester-based electrolyte due to their homologous structure. This system has better performance than other binders of LNMO cathode, like poly(vinylidene fluoride) (PVDF), styrene–butadiene rubber (SBR), and polytetrafluoroethylene (PTFE). In the methyl acetate (MA) electrolyte, the LTO/LNMO battery with the PAA binder exhibited the highest discharge capacity (137 mAh g–1 at 0.5 C) and the best rate performance (112 mAh g–1 at 5 C). In addition, MA boosted the low-temperature performance of this battery, which can work at −40 °C with a remarkable reversible capacity of 90 mAh g–1 and a discharge capacity of 140 mAh g–1.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）