Materials Science and Engineering B-Advanced Functional Solid-State Materials
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2024
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IF 3.9
Congzhi Hu,Yuye Li,Tingting Du,Youyong Pang,Yongping Liu,Botian Liu,Ling Li,Huidan Lu,Bin Huang
In this paper, a new supramolecular Z-scheme heterojunction photocatalyst, designated as Ag/Ag 3 PO 4 /Perylene diimide organic molecules after secondary acid-base self-assembly (PDI-2), was synthesized through precipitation and photoreduction techniques. Ag/Ag 3 PO 4 /60 %PDI-2 (APP-6) exhibited the best photocatalytic activity due to the synergistic effect of Z-scheme heterojunction and surface plasmon resonance (SPR) effect of Ag nanoparticles (Ag NPs). Under visible light (λ > 420 nm), the degradation efficiency of APP-6 for Rhodamine B (RhB) and Bisphenol A (BPA) was 99.7 % and 90.7 %, respectively. Additionally, PDI-2 was transformed into smaller nanoclusters, which increased the specific surface area of the photocatalyst, and reduced the charge transport distance. Moreover, APP-6 exhibited the smallest electrochemical impedance, the largest photocurrent, the smallest fluorescence lifetime. Free radical trapping experiments showed that •O 2 − was the main reactive group and a possible photocatalytic mechanism was proposed by combining the Ultraviolet–visible diffuse reflectance spectrophotometer (UV–vis DRS) and the Mott-Schottky plots.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xiaojiang Li,Xingqiao Zhang,Chengwei Zuo,Han Zhang,Zhenfu Jia
Cleaner recovery of petroleum hydrocarbons is a key process for waste oil and gas resources, especially oily waste solid. However, the direct recovery of petroleum hydrocarbons is difficult with deep eutectic solvents (DES) without other additives (such as water). In this work, ionic liquid-based DESs (ILs-DESs) with a controllable polarity were prepared for the sustainable recovery of petroleum hydrocarbons. Here, CO2-responsive ionic liquids were prepared by the neutralization reaction of 1,8-diazabicyclo[5.4.0]undec-7-ene and iminazole (Im), pyrazol (Py), or triazole (Tri). Then, the ILs-DESs were separately prepared by using ionic liquids as proton acceptors and straight-chain alcohols (carbon number = 4, 6, 8, 10, and 12) as proton donors. The polarity transformation of the ILs-DESs was regulated only by the introduction and removal of CO2, which was caused by the reversible transformation from ILs-DESs with a lower polarity to alkyl carbonate and carbamate with higher polarity upon CO2. Because of the polarity changes, the simulated oil (such as n-dodecane or diesel oil) was mixed with ILs-DESs, and the samples were directly separated by introducing CO2. Finally, a sustainable process for treating oil sands and oily sludge by using ILs-DESs was developed, where the ILs-DESs were also reused more than twice. This implies that a sustainable approach for petroleum hydrocarbon recovery was realized by using DESs.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 1.6
Ping Xie,Tianhao Zhong,Tao Li,Yiwu Lu,Yingmin Yu,Qingshan Zhao,Zhongtao Li
There is an urgent need to develop green catalytic transesterification technology to reduce liquid waste and instrument corrosion. Ionic liquids with controlled activity, easy recovery, and corrosion resistance have great potential as catalysts for transesterification reactions. In this paper, a series of ionic liquids were prepared using imidazole and ammonium compounds as cations, and sulphuric acid, p -toluenesulfonate, and bistrifluoromethanesulfonate anions as anions. In comparison, the ionic liquid made from imidazole with H 2 SO 4 (IMIHS) was found to be the best catalyst for the esterification reaction with high speed, high activity, low corrosion, and high stability, and its catalytic performance was superior to that of sulphuric acid. The optimum reaction conditions were as follows: the molar ratio of ethanol to acetic acid was 1:1, the catalyst amount was 5 wt.%, the reaction temperature was 80°C, and the reaction time was 120 min. The maximum yield of ethyl acetate was 66.2% under the optimum reaction conditions. The catalytic activity was not declined obviously by reusing six times. The activation energy of the reaction is 48.748 kJ/mol.
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ACS Applied Polymer Materials
·
2025
·
IF 4.7
Jun Hu,Ling Lin,Chao Shi,Lu Cai,Haiyan Mao,Xiaosai Hu,Yuanyu Ge,Ziyin Li
Metal–organic frameworks (MOFs) are often used as proton conductor fillers to enhance the proton conductivity of hybrid membranes. It is interesting but still challenging to discuss the influence of the molecular morphology and distribution of proton carriers within MOFs on their proton exchange membranes (PEMs) and their overall performance. In this work, two types of imidazole-loaded proton conductors were synthesized based on MIL-101(Cr), with one containing free imidazole molecules and the other containing imidazole molecules coordinating with Cr-metal sites. Furthermore, series composite membranes (CPM/IM-x and CPM@IM-x, x = 1, 2, 3) were fabricated using imidazole-loaded proton conductor as filler and a cross-linked poly(vinyl alcohol) (CL-PVA) that contains both hydrophilic and hydrophobic structures as matrix. The CPM/IM membranes with coordinated imidazole molecules exhibit significantly enhanced water affinity, stability, and ion exchange capacity. This is mainly due to the coordinated imidazole improving the two-phase dispersion, promoting imidazole deprotonation, and facilitating low-energy-barrier proton transport, while the CPM@IM membranes with the free imidazole molecules exhibit relatively lower proton conductivity but higher activation energy (Ea). Surprisingly, the proton conductivity of the CPM/IM-2 membrane can reach up to 2.7 × 10–2 S cm–1 at 85 °C and 90% RH, but with the lowest Ea of 20.9 kJ/mol. This remarkable performance indicates more efficient H+ transportation. Moreover, the single-cell power density of CPM/IM-2 is up to 89.7 mW cm–2, proving it exhibits high potential application prospects as a proton exchange membrane for hydrogen-based fuel cells.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Hui Niu,Huan Lin,Huiting Zhang,Longfeng Hu,Gangqiang Yu,Shuhong Wu,Jinlin Long,Quan-Fu An
Photocatalytic hydrogen evolution presents a sustainable method for clean energy generation, yet its efficiency remains limited by insufficient charge separation and transfer. Herein, we report a novel strategy to enhance photocatalytic efficiency by integrating both bulk and surface electric fields within self-assembled supramolecular photocatalyst. We synthesized perylene 3,4-dicarboxylic acid (PDA) with a large dipole moment and polar carboxyl groups, which self-assembles into ultrathin 2D nanosheets in water. The accumulation of dipole moments induces a bulk electric field, enabling ultrafast exciton dissociation into free charges. Concurrently, the exposed carboxyl groups generate a surface electric field, facilitating efficient charge extraction and transfer on the surface for proton reduction. The synergistic interplay between bulk and surface electric fields results in an impressive photocatalytic hydrogen production rate of 3.2 mmol g⁻¹ h⁻¹ , significantly surpassing that of the other perylene-based nanosheets relying solely on either bulk or surface electric fields. This study offers valuable insights into the distinct roles of bulk and surface electric fields in photocatalytic processes, and introduces a new design paradigm for photocatalysts to enhance solar-to-hydrogen conversion efficiency.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jinyang Peng,Xinran Zhao,Yuxi Huang,Cuijiao Zhao,Jun Yang,Minjie Shi
Capacitive deionization (CDI) employing pseudocapacitive electrodes is emerging as a promising electrochemical technology for contaminant removal and water purification. While organic materials hold significant potential as pseudocapacitive electrodes, their applications in CDI devices are hindered by inadequate redox availability and sluggish adsorption kinetics. Addressing these limitations, an innovative electron-delocalized organic molecule, designated as NDDQ is developed, which incorporates a π-conjugated benzimidazole-linked framework with extensive electron delocalization and a reduced HOMO-LUMO gap. This molecular architecture enables a high 81.8% utilization efficiency of its available C═O and C═N active sites, augmenting NH 4 + electrosorption capacity, as validated by in situ analyses and theoretical calculations. When implemented into a CDI device, the NDDQ electrode delivers a high NH 4 + adsorption capacity of 232 mg g −1 and an impressive rate of 7.66 mg g −1 min −1 , outperforming all existing CDI technologies (typically <150 mg g −1 ) while maintaining regeneration stability over 100 cycles. The CDI-based electrochemical system can rapidly reduce NH 4 + concentration from an initial 500 to 7.8 mg L −1 within a mere 90-min operation period, achieving a consistent volumetric treatment capacity in the range of 6.126–8.052 L m −2 h −1 , which offers an efficient, rapid, and sustainable solution for water treatment applications.
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Advanced Healthcare Materials
·
2024
·
IF 10
Jinhao Yan,Haoqi Wang,Xueqin Zhao,Longxiang Tao,Xuefu Wang,Jun Yin
Malignant tumor has become one of the hellish killers threatening the health of people around the world, its diagnosis and treatment has become the concerns of public. However, the optimal therapeutic dose, undesired side-effect, and long-term immune activation were key and bottleneck problems in tumor treatment. Herein, different batches of supramolecular therapeutic platforms, including vesicles, spherical nanoparticles, and cylindrical nanorods, with precise ratios of dye to drug (1:2) and multiple stimulus responsiveness were constructed by host-guest complexation between cyanine-camptothecin conjugates (IR780-CPT2) and β-cyclodextrin (β-CD) pendent hydrophilic copolymers. The reduction responsiveness, near-infrared photothermal conversion and singlet oxygen ( 1 O 2 ) generation performances endowed these platforms excellent cancer cells killing effect in both of in vitro cellular experiments and in vivo mice models. More importantly, without affecting the weight of mice, the maturation of dendritic cells, proliferation of T cells, up-regulation of high mobility group protein B1, and reduction of immunosuppressive regulatory T cells were detected after employing a synergistic chemo-photo therapy, demonstrating the body's immune effect was successfully activated. Thus, during the treatment of primary tumor, the distal tumor was also inhibited. We believe this work could provide a distinctive way to fabricate supramolecular theranostic platforms with different morphologies and improve antitumor and antimetastasis capabilities.
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ACS Applied Polymer Materials
·
2025
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IF 4.7
Jingqi Yang,Ying Lu,Jun Geng,Shuping Xue,Yixuan Zhang,Jingyi Teng,Maochun Zhu,Xue Bai,Shuxia Liu
The design and preparation of proton exchange membranes (PEMs) with wide working temperature ranges play a crucial role in expanding their application, but most of the reported PEMs are difficult to meet the demand for operating at subzero temperatures. Herein, a series of composite membranes have been successfully fabricated by functionalizing a sulfonated poly(ether ether ketone) (SPEEK) membrane with phosphotungstic acid-ionic liquid (HPW-IL) and mesoporous graphite phase carbon nitride (mpg-C3N4). Notably, the optimal composite membrane SPEEK/HPW-IL/mpg-C3N4-1.0 exhibits attractive antifreeze property (<−75 °C) and great proton conductivity ranging from −40 °C (7.2 × 10–4 S cm–1, ambient humidity) to 85 °C (2.2 × 10–1 S cm–1, 95% RH) attributing to the formation of continuous proton transport channels induced by the double acid–base pairs (one is HPW and IL, the other is SPEEK and mpg-C3N4) and abundant hydrogen-bonding interactions among various components. Meanwhile, its antiswelling property has been greatly improved compared to the SPEEK membrane, thanks to the incorporation of mpg-C3N4. Given its excellent proton conductivity, a full-cell performance test was performed, achieving a maximum output power density of up to 230.3 mW cm–2, an open-circuit voltage of up to 0.85 V, and a long-term stability for 25 h at 80 °C, 100% RH. This work provides broad vision into the design of PEMs with remarkable performances that can be used in a wide temperature range.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 9
·1-10
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IF 5.3
Zhai Xiurong,Li Qian,Cao Yang,Han Mengjie,Sun Hailian,Du Lelin,Yang Xiyun,Wei Yuxin,Yu Congcong
An electrochemical platform for signal amplification probing chloride ions (Cl − ) is constructed by the composite integrating core–shell structured nitrogen-doped porous carbon@Ag-based metal–organic frameworks (NC@Ag-MOF) with polypyrrole (PPy). It is based on the signal of solid-state AgCl derived from Ag-MOF, since both NC and PPy have good electrical conductivity and promote the electron transport capacity of solid-state AgCl. NC@Ag-MOF was firstly synthesized with NC as the scaffold and then, PPy was anchored on NC@Ag-MOF by chemical polymerization. The composite NC@Ag-MOF-PPy was utilized to modify the electrode, which exhibited a higher peak current and lower peak potential during Ag oxidation compared with those of Ag-MOF and NC@Ag-MOF-modified electrodes. More importantly, in the coexistence of chloride (Cl − ) ions in solution, the NC@Ag-MOF-PPy-modified electrode displayed a fairly stable and sharp peak of solid-state AgCl with the peak potentials gradually approaching zero, which might effectively overcome the background interference caused by electroactive substances. The oxidation peak currents of solid-state AgCl increased linearly with the concentration of Cl − ions in a broad range of 0.15 µM–40 mM and 40–250 mM, with detection limits of 0.10 µM and 40 mM, respectively. The practical applicability for Cl − ions determination was demonstrated using human serum and urine samples. The results suggest that NC@Ag-MOF-PPy composite could be a promising candidate for the construction of the electrochemical sensor.
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RSC Advances
·
2025
·Vol. 15
·期 11
·8719-8728
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IF 4.6
Piao Luo,Kai Zhang,Nanjie Wu,Lanlan Wei,Shigui Peng,Qiao Fan,Tingting Luo,Yucheng Yin,Xiang Zhang,Yufei Liu,Min He,Jie Yu,Shuhao Qin
Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a promising conductive polymer material, but its acidic nature leads to device deterioration and poor long-term durability. It is usual practice to neutralise PEDOT:PSS solutions with bases, resulting in a decrease of conductivity. The causes of the decline in conductivity remain disputed and uncertain. In this study, three bases (sodium hydroxide, ammonium hydroxide, and imidazole) were employed to treat PEDOT:PSS to investigate their effects on doping level, composition, and structure. The results show that bases may dedope PEDOT:PSS by removing the proton doping from the PEDOT chain. Meanwhile, insulating PSS is removed, and the aggregated structure is optimised to ensure that conductivity is not significantly reduced. The PEDOT:PSS treated with the weak base imidazole showed the least loss of conductivity due to only a modest decrease in doping level and the greatest loss of insulating PSS. Aluminium electrolytic capacitors made using imidazole pH-adjusted solutions have a capacitance ratio of up to 98.28% and an equivalent series resistance of 26 mΩ. These findings provide a valuable reference for developing high electrical characteristics and neutral PEDOT:PSS materials.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2024
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IF 5.9
Xiaoxiao Zhao,Yifan Liu,Yuancai Lv,Minghua Liu
Lignin is a sustainable biomass resource with abundant hydroxyl groups that holds great promise for use as a feedstock for polyurethane foam production. Therefore, the flexible polyurethane foams (FPUFs) were prepared using the oxidized alkali lignin (OAL) as the matrix to enhance its compatibility. The OAL was obtained under the following conditions of 60 °C, 80 min treatment, a ratio of hydrogen peroxide to lignin of 1.2:1, and a ratio of iron hydroxide to lignin of 0.01. It was demonstrated that incorporating OAL enhanced the density, compressive strength, sound-absorbing performance and degradability of foam composites. The compressive strength was also improved by more than five times than that of blank foam under the optimal conditions, reaching 0.11 MPa. The thermogravimetric analysis (TGA) revealed that the foam composite containing 30 % modified lignin content exhibited the highest thermal stability. The results of solvent resistance testing demonstrated the durability of the foam composites in both water and solvents. Lignin-modified polyurethane foam exhibited an acoustic absorption coefficient above 0.2 across a wide frequency range, with the highest value reaching 0.84, meeting the conventional requirements for sound absorption materials (α > 0.2). The results suggested that this environmentally friendly preparation method was feasible for producing high-performance polyurethane foams, which was appropriate for the production of sound absorption boards for industry, transportation by train and automobile.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Dongyu Wang,Yujuan Pu,JuFeng Li,Yong Zhai,Qingwei Wang,Ligang Wang,Yunchuan Yang,Jisheng Geng,Quanwei Song,Jun Wang,Yongfa Zhu
Conventional free radical advanced oxidation processes are prone to inefficient mineralization and generation of toxic by-products due to the depletion of free radicals by non-target pollutants, and thus it is crucial to remove difficult-to-degrade organic pollutants efficiently and selectively in complex water bodies. Herein, we constructed a photochemical direct charge transfer elective oxidation/mineralization system based on peryleneimide supramolecular photocatalysts and variable-valent metal ions (PDI/M n+x ) to selectively oxidize and mineralize phenolic organic pollutants, achieving an 8–13-fold increase in the mineralization rate. Experimental and theoretical calculations elucidated the possible selectivity mechanism: the oxidation potentials of active species (photogenerated charge) and phenolic organic pollutants (PCs) in the system govern the oxidation kinetics and mineralization efficiency, and a typical negative correlation exists. Additionally, by leveraging the dyeing properties of PDI photocatalysts to load them onto white nonwoven fabrics, efficient degradation of organic pollutants in water under natural light conditions can be achieved. The system exhibits a mineralization capacity 2.3–4.7 times higher than that of the homogeneous Fenton system, along with lower treatment costs and comparable removal rates. This study provides a cost-effective solution for the purification of difficult-to-degrade organic pollutants in complex water bodies through non-radical pathways.
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危险品化学品经营许可证（带存储）