JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Rongsheng Ning,Heliang Pang,Zhongsen Yan,Zhenyu Lu,Qiankun Wang,Zengling Wu,Wenxin Dai,Lingshan Liu,Zhongsheng Li,Gongduan Fan,Xianzhi Fu
The development of high efficient photocatalysts for antibiotics contamination in water remains a severe challenge. In this study, a novel step-scheme (S-scheme) photocatalytic heterojunction nanocomposites were fabricated from integrating AgCl nanoparticles on the MIL-100(Fe) octahedron surface through facile multi-stage stirring strategy. The S-scheme heterojunction structure in AgCl/MIL-100(Fe) (AM) nanocomposite provided a more rational utilization of electrons (e - ) and holes (h + ), accelerated the carrier transport at the junction interface, and enhanced the overall photocatalytic performance of nanomaterials . The visible-light-driven photocatalysts were used to degrade sulfamethazine (SMZ) which attained a high removal efficiency (99.9%). The reaction mechanisms of SMZ degradation in the AM photocatalytic system were explored by electron spin resonance (ESR) and active species capture experiments, which superoxide radical (•O 2 - ), hydroxyl radical (•OH), and h + performed as major roles. More importantly, the SMZ degradation pathway and toxicity assessment were proposed. There were four main pathways of SMZ degradation, including the processes of oxidation , hydroxylation, denitrification, and desulfonation. The toxicity of the final products in each pathway was lower than that of the parent according to the toxicity evaluation results. Therefore, this work might provide new insights into the environmentally-friendly photocatalytic processes of S-scheme AM nanocomposites for the efficient degradation of antibiotics pollutants.
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Polymers
·
2022
·Vol. 14
·期 4
·699
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IF 4.967
Linlin Wang,Jie Zhou,Lei Li,Shengyu Feng
Supramolecular elastomers integrated with high mechanical toughness and excellent self-healing ability offer attractive applications in various fields such as biomedical materials and wearable electronics. However, the multistep preparation process for creating functional polymer precursors and the expensive stock materials required are two factors that limit the widespread use of supramolecular elastomers. Herein, for the first time, poly(β-hydroxyl amine)s generated by amine-epoxy polymerization were used in the development of supramolecular polymer materials. Based on the novel silicon-containing poly(β-hydroxyl amine)s synthesized by the polymerization between 1,3-bis(3-glycidyloxypropyl)tetramethyldisiloxane and 3-amino-1,2-propanediol, dually cross-linked supramolecular elastomers with both hydrogen bonding and metal coordination were achieved, displaying adjustable mechanical properties with the tensile strength varying from 0.70 MPa to 2.52 MPa, respectively. Thanks to the dynamic nature of the supramolecular interactions, these elastomers exhibited favorable hot-pressing reprocessability and excellent self-healing performance, with the healing efficiency reaching up to 98% at 60 °C for 48 h. Potential applications for photoluminescent materials and flexible electronic devices were demonstrated. We believe that its simplicity of synthesis, adjustable mechanical properties, and robust self-healing capacities bode well for future applications of this new supramolecular elastomer.Keywords:dual-cross-linked elastomer;supramolecular elastomer;poly(β-hydroxyl amine);self-healing
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Sitao Wang,Zhijie Liu,Bolun Pang,Yuting Gao,Santu Luo,Qiaosong Li,Hailan Chen,Michael G Kong
Antibiotics are widely used to treat or prevent infectious diseases in human and veterinary medicine. Excessive residues in the aquatic environment lead to increasingly prominent antibiotic pollution; therefore, it is urgent to develop sustainable strategies for rapidly degrading antibiotics. In this study, a highly synergetic effect for norfloxacin (NOR) remediation is achieved by coupling underwater bubble plasma formation with a Fe (III)–S (IV) system due to the efficient utilization of reactive species in chain reactions. The degradation rate using synergetic approach can reach 76.4% within 50 min discharge, and further increases significantly to 94.4% after 5 h post-discharge. The effects of pulsed peak voltage and Fe (III)/S (IV) dosage on NOR removal are characterized. The existence of hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) are proved by electron spin resonance spectrometer (ESR) during degradation. Furthermore, radical scavenger experiments demonstrate that • OH and SO 4 •− play a crucial role in degradation. Underwater bubble plasma provides the oxic and acidic liquid environment for the Fe (III)–S (IV) system to accelerate the self-perpetuating chain reactions. These reactions not only introduce SO 4 •− and generate more • OH during plasma-on, but also induce their regeneration and further prolong the degradation process during plasma-off through plasma-generated effects. Finally, the degradation intermediates of NOR are identified, and a possible degradation pathway is proposed. The possible contribution weight of each approach on the degradation rate is speculated. These new findings offer promising applications for developing a technology with real potential for the treatment of organic compounds in industrial wastewater treatment.
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ORGANIC PROCESS RESEARCH & DEVELOPMENT
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2022
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IF 3.858
Jianjiong Li,Shanshan Yu,Yingang Wang,Peiyuan Yao,Qiaqing Wu,Dunming Zhu
(S)-2-Aminobutane, d-alanine, and d-homoalanine are important intermediates for the production of various active pharmaceutical ingredients and food additives. The preparation of these small chiral amine or amino acids with high water solubility still demands searching for efficient methods. In this work, we identified an ω-transaminase (ω-TA) from Sinirhodobacter hungdaonensis (ShdTA) that catalyzed the kinetic resolution of racemic 2-aminobutane at a concentration of 800 mM using pyruvate as the amino acceptor, leading to the simultaneous isolation of enantiopure (S)-2-aminobutane and d-alanine in 46% and 90% yield, respectively. In addition, (S)-2-aminobutane (98% ee) and d-homoalanine (99% ee) were isolated in 45% and 93% yield, respectively, in the kinetic resolution of racemic 2-aminobutane at a concentration of 400 mM coupled with deamination of l-threonine by threonine deaminase. We thus developed a biocatalytic process for the practical synthesis of these valuable small chiral amine and d-amino acids.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Shasha Wei,Li Liu,Xuan Huang,Yichuan Zhang,Fusheng Liu,Liang Deng,Emiliano Bilotti,Guangming Chen
Organic thermoelectric (TE) composites and flexible devices have gained a rapid development in recent decade. Herein, a flexible and foldable film of poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)/single-walled carbon nanotube (PEDOT:PSS/SWCNT) composite is fabricated by post-treatment with an ionic liquid (IL), and an S-shape TE generator (TEG) is designed to harvest heat from human body via a vertical temperature gradient. After being post-treated with IL of bis(trifluoromethane)sulfonimide lithium salt (LiTFSI), the PEDOT:PSS/SWNCT composite displays an improved electrical conductivity from 1063 ± 80 to 1562 ± 170 S cm–1, with an almost constant Seebeck coefficient of ∼21.9 μV K–1 with a 30 wt % content of SWCNT. The TE properties exhibit excellent stability against repeated bending or folding cycles. Furthermore, an S-shape architecture is designed for TEG assembling, which enables effective utilization of a vertical temperature gradient between the human body and surroundings. The present study proposes a universal strategy for harvesting heat using a wearable TEG via a vertical temperature gradient, which represents great prospects for application in self-powered wearable electronics.
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COMPOSITES SCIENCE AND TECHNOLOGY
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2021
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IF 8.528
Shuai Yang,Yang He,Jinsong Leng
Multi-stimuli selective actuation of shape memory polymers (SMPs) with multi memory capabilities have attracted great attention in recent years, due to diverse active deformation application scenarios. Current multi-SMPs with low T t , however, are faced with inherent barriers, such as low fixation and inaccurate control, because the shape retainability, controllability, and responsiveness of SMPs are highly determined by transition temperature (T t ). Herein, quadruple-shape memory poly(aryl ether ketone) (PAEK) with tunable high T t and selective response characteristics were successfully fabricated for the first time, which especially harnessed ultra-high programmability and controllability. More significantly, the quadruple shape memory PAEK-based smart architectures such as “fingers” and “flower” were demonstrated to exhibit the controllable multi-stages actions. Utilizing a “man” as an example, we put forward different programming routes up to ten to make it perform complex pre-set deformation actions. The quadruple shape memory PAEK of high T t possessed great utilizing potential in fields of soft robots , actuators, and deformable devices.
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Catalysis Science & Technology
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2021
·Vol. 12
·期 4
·1144-1158
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IF 6.119
Junke Li,Mei Li,Zhiliang Jin
An S-scheme surface heterojunction between Co3S4 and Mo2S3 was constructed successfully via a stepwise hydrothermal method. A rhombic dodecahedral cobalt-based metal–organic zeolite imidazole framework (ZIF-67) is used as the cobalt source and template to participate in the reaction process. ZIF-67 with a dodecahedral structure is first reshaped into cobalt sulfide with a hollow polyhedral structure via a one-step sulfidation reaction. And then, Mo and S species were introduced on the surface of Co3S4 to fabricate Co3S4@Mo2S3 with a hierarchical core–shell structure and S-scheme heterojunction. In comparison, the H2 evolution activity of Co3S4@Mo2S3 is about 7 and 3 times higher than those of pure Mo2S3 and Co3S4. Density functional theory (DFT) calculations were used to construct the molecular model of Co3S4 and Mo2S3, and the sample's energy band structure was also analyzed. Based on the analysis of a series of characterization results, a H2 evolution mechanism of Co3S4@Mo2S3 with a S-scheme surface heterojunction was proposed. The formation of the S-scheme surface heterojunction between Co3S4 and Mo2S3 results in a more developed channel to transfer photogenerated electrons and allows the system to retain a more effective redox potential. Besides, the Mo2S3 nanosheet's criss-cross growth on the Co3S4 surface is beneficial to the improvement of the cycle stability of the Co3S4@Mo2S3 composite. This work uses a ZIF-67 polyhedron as the template to provide a new strategy for preparing a hierarchical S-scheme surface heterojunction photocatalyst based on MOFs.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Jiafeng Qian,Chenyi Wang,Xiaojing Zhang,Jianxiong Hu,Xiaoyan Zhao,Jian Li,Qiang Ren
Quaternary ammonium-functionalized anion exchange membranes (AEMs) have important potential application value in water electrolysis. In order to further improve the ionic conductivity and stability of AEMs, a series of crosslinked AEMs based on poly (aryl ether sulfone)s (Co-PAES-QA-x-m, “x” represents the functionalized polymer segment, “m” represents the crosslinking ratio) are prepared by introducing dense quaternary ammonium cations on the side chains via Menshutkin reaction. Their polymer structures are characterized by hydrogen nuclear magnetic resonance (1H NMR) and Fourier transform infrared spectroscopy FT-IR, and the microscopic phase separation structure of the obtained membranes is observed by atomic force microscope AFM. The ion exchange capacity (IEC) of Co-PAES-QA-x-m (x = 25%, m = 40%–100%) is between 2.03–2.48 mmol g −1 , and their water uptake (WU), swelling ratio (SR) and ionic conductivity are in the range of 26.9–56.7%, 6.3–12.9% and 53.43–119.43 mS cm −1 at 80 °C, respectively. The test of chemical stability show that the ionic conductivity retention ratio of these AEMs reaches 84.7% after soaking in 2 mol L −1 NaOH solution for 480 h at 80 °C. The water electrolyzer assembled with representative Co-PAES-QA-25-60 reaches 1646.7 mA cm −2 in 2 mol L −1 NaOH solution at 2.0 V and 80 °C, and the durability test shows that its voltage only rises by 5% after 480 h at the current density of 500 mA cm −2 . This work is expected to provide an effective modification method for high-performance AEMs which are used in water electrolyzer.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 19
·6551-6558
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IF 4
Wenjuan Dong,Lu Wang,Rongrong Zhang,Chaochao Wen,Ren Su,Xiaojuan Gong,Wenting Liang
Carbon dots are popular luminescent materials because of their excellent fluorescence properties, but the low quantum yield limits their application. Heteroatom doping is a more convenient and popular approach to increase the quantum yield of carbon dots. Here, novel N,S,P heteroatom co-doped carbon dots (N,S,P-CDs) were synthesized by a simple one-step hydrothermal method using m-phenylenediamine, L-cysteine and phosphoric acid as raw materials. The as-prepared N,S,P-CDs showed excellent photoluminescence properties with a fluorescence quantum yield of up to 41%, which greatly encourages their application in fluorescence sensing. The N,S,P-CDs exhibited good fluorescence stability under salt solution, xenon lamp irradiation and ultraviolet lamp irradiation except for a high sensitivity to extreme acidity. The fluorescence intensity of the N,S,P-CDs can be decreased by as much as 85% when the pH of the solution changes from 2.50 to 4.75, that is, a small fluctuation in pH can cause an intense response of the fluorescence of the N,S,P-CDs. Therefore, an excellent fluorescence sensing platform for accurately monitoring the pH of extreme acidity has been constructed. In addition, the N,S,P-CDs can be applied for quantitative detection of folic acid based on the strong quenching effect of folic acid on the fluorescence of the N,S,P-CDs. Good linearity was obtained in the concentration range of 4.85–82.45 μM, with a detection limit of 0.148 μM. The constructed sensing platform was used for the determination of folic acid in actual samples of orange juice, oatmeal and tablets with satisfactory results.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Cheng Cheng,Jian Wang,Zhihao Zhao,Changchun Chen,Sheng Cui,Yifeng Wang,Lin Pan,Yaru Ni,Chunhua Lu
Semiconductor catalyst with high photocatalytic activity can be exploited via heterojunction. In this study, a new S-scheme SrTiO 3 /porous ZnO composite was rationally devised, successfully prepared by utilizing a two-step pyrolysis of SrTiO 3 /ZIF-8, and analyzed by various characterization technologies including XRD, SEM, TEM, BET, XPS, PL, UV–vis DRS, and photoelectrochemical and DFT theoretical calculations. A porous structure, tight contact, and a heterojunction formed between SrTiO 3 and porous ZnO (ZnOT) can be observed by SEM and TEM images. BET testing indicates that the SrTiO 3 /porous ZnO composite (S3ZT) shows the highest specific surface area (30.37 m 2 /g). The band gap values (E g ) of SrTiO 3 and ZnOT are around 3.17 and 2.95 eV, which agree with those obtained from DFT calculations. Compared to other samples, the SrTiO 3 /porous ZnO composite (S3ZT) shows higher light absorption and lower transfer resistance as demonstrated by UV–vis DRS and EIS results. S3ZT presents a superior photocatalytic efficiency of 48.8% in degrading 5 mg/L methyl orange (MO) irradiated by 1 h UV–vis light, which are 7- and 1.5-fold higher than pristine SrTiO 3 and ZnOT, respectively. Moreover, based on Mott-Schottky theory, active species trapping experiments, XPS determination, and DFT calculations (energy band gap and work function), it was shown to be reasonable to utilize the S-scheme charge migration process for an explanation regarding the better photocatalytic activity of SrTiO 3 /porous ZnO composite. Overall, this work will provide an effective protocol for devising and preparing semiconductor photocatalysts with S-scheme heterojunction by utilizing the superior characteristics of MOFs.
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Journal of Cleaner Production
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2021
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IF 9.297
Yuan-Yuan Yu,Zhong-Qiu Liu,Guo-Qiang Zhang,Yu-Jing Liu,An-Guo Ying
The selective valorization of lignite into monocyclic aromatic compounds (MCACs) is extremely challenging due to its chemical inertness and geometrical complexity. The catalytic efficiency of lignite valorization into MCACs over solid acids is significantly reduced by the presence of H 2 O resulting in the leaching and deactivation of acid sites. Moreover, the precise fabrication of poly(ionic liquid)s (PILs) containing Brønsted-Lewis acidic sites, well-defined mesoporous channels, and hydrophobicity remains a considerable challenge. Herein, a novel hydrophobic mesoporous PILs with strong Brønsted-Lewis acid sites was successfully constructed by a synergistic regulation-induced copolymerization strategy for the first time. More exotically, the resultant multifunctional PILs was found to be ultra-efficient catalyst for the selective valorization of Yiwu lignite (YL) into MCACs with 23.5 wt.% yield, which is the highest yield reported for lignite catalytic valorization by precious metal-free catalysts under mild conditions. The co-catalysis mechanisms of YL valorization into MCACs over the multifunctional PILs are confirmed by characterization methods and the synergistic catalysis mechanisms are as follows: (1) hydrophobic micro-environment: the hydrophobic micro-environment created by hydrophobic block is favorable for preventing the leaching and deactivation of Brønsted-Lewis acid sites; (2) mesoporous confinement: the well-defined mesoporous channels strengthen the adsorption amount of H 2 and increases the concentration of substrates; (3) synergistic catalytic active hydrogen transfer of Brønsted-Lewis acid sites: Brønsted-Lewis acid sites synergistically promote H 2 heterolysis to the mobile H + and immobile H − , and then the resulting mobile H + transfers to oxygen atom in lignite to produce MCACs via C–O bond cleavage . This work not only sheds some light on developing the multifunctional solid acid catalysts , but also demonstrates an efficient catalyzing method to produce lignite-based MCACs by co-catalysis of Brønsted-Lewis acidic sites, mesoporous confinement, and hydrophobic micro-environment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xiaoyang Yue,Lei Cheng,Jiajie Fan,Quanjun Xiang
Heterojunction construction is a universal and effective approach to achieve high-efficiency photocatalysts. Towards these well-designed heterojunctions, modulation on steering dynamic charge transfer holds great promise in further performance stimulation. Herein, 2D/2D BiVO 4 /CsPbBr 3 S-scheme heterojunctions, of which CsPbBr 3 nanosheets (NSs) are in-situ face-to-face grown onto BiVO 4 NSs, are designed as cornerstones for further carrier managements. Briefly, with controllable heterostructure regulation, an intimate heterointerface between BiVO 4 and CsPbBr 3 NSs with similar size can be obtained accompanied with a maximally intensified interfacial interaction, largely boosting charge transfer across the interfacial conjunction. Moreover, by further tailoring the intrinsic O vacancy ( V O • • ) of BiVO 4 , the gradient Fermi level shift towards its valence band is finely tuned, yielding an enlarged Fermi level gap and an enhanced internal electric field (IEF) over BiVO 4 /CsPbBr 3 heterojunctions. Such an intensified IEF provides a powerful driving force for directional charge migration, resulting in high charge separation and utilization efficiency. Hence, the optimized BiVO 4 /CsPbBr 3 S-scheme heterojunction features desirable accelerated dynamic carrier mobility, delivering comparably high CO 2 -to-CO conversion with a turnover number (TON) near 230 without any co-catalyst or sacrificial agent. The accelerated S-scheme charge transfer mechanism is revealed in detail by X-ray photoelectron spectroscopy (XPS), theoretical calculations, photo-irradiated Kelvin probe force microscopy and in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS).
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