Small
·
2024
·Vol. 20
·期 33
·2401167
·
IF 13
Ying Lin,Changjiang Wang,Jinxiang Wu,Jian Tang,Guangmao Ye,Xiaobing Zhao,Hua Li,Yi He
Covalent organic frameworks (COFs) are promising iodine adsorbents. For improved performances, it is critical and essential to fundamentally understand the underlying mechanism. Here, using the operando dark-field optical microscopy (DFM) imaging technique, the observation of an extraordinary structure shrinkage of 2D triphenylbenzene (TPB)-dimethoxyterephthaldehyde (DMTP)-COF upon the adsorption of I 2 vapor at the single-particle resolution is reported. Combining single-particle DFM imaging with other experimental and theoretical methods, it is revealed that the shrinkage mechanism of the TPB-DMTP-COF is attributed to the I 2 sorption-induced synchronous skeleton-pore interactions. The redox reaction of I 2 and TPB-DMTP-COF yields some cationic skeletons and I 3 − species, which triggers the multi-directional halogen-bonding interactions of I 2 and I 3 − as well as strong cation-π interactions between neutral and cationic skeletons, accompanying the synchronous in-plane skeleton shrinking in the xy plane and compact out-of-plane layer packing in the z- direction. This understanding of the synchronous action between the skeleton and pore breaks the perspective on the structure robustness of 2D COFs with excellent stability during the I 2 uptake, which offers pivotal guidance for the rational design and creation of advanced microporous adsorbents.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2024
·
IF 4.3
Qian Wu,Guo Feng,Feng Jiang,Xiaojun Zhang,Yanqiao Xu,Jianmin Liu,Jian Liang,Xinbin Lao,Zhiqi Guo
This paper reports a facile treatment to enhance the capacity of petal-like MgAl 2 O 4 for Congo red (CR) adsorption. The influence of dehydroxylation treatment on the adsorption performance of petal-like MgAl 2 O 4 is investigated. FT-IR, XPS, TG, XRD and FE-SEM are employed to analyze the differences between samples without and with dehydroxylation. Mechanism on the adsorption capacity improvement of CR by MgAl 2 O 4 after dehydroxylation is investigated systematically. Results show that the adsorption process conforms well to the pseudo-second-order kinetic model and Langmuir isotherm model. The adsorption mechanism study shows that the adsorption of CR on petal-like MgAl 2 O 4 is mainly due to chemisorption including Lewis acid-base interaction and electrostatic attraction. It is observed that the maximum adsorption capacity of petal-like MgAl 2 O 4 after dehydroxylation reaches 3264.54 mg/g, much higher than sample without dehydroxylation (591.72 mg/g). Most Lewis acid sites of petal-like MgAl 2 O 4 (Mg 2+ and Al 3+ ) without dehydroxylation process are occupied by hydroxyl groups. It is not conductive to combine with –NH 2 and –SO 3 2- in CR molecular, resulting in the deterioration of adsorption performance. The activity of Mg 2+ and Al 3+ in MgAl 2 O 4 can be recovered greatly after the removal of hydroxyl groups, and it is favorable to the adsorption between MgAl 2 O 4 and CR.
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CARBOHYDRATE POLYMERS
·
2024
·
IF 10.7
Xiuqin Fang,Chang Wang,Hong-Hui Shu,Sheng-Li Han,Cheng-Mei Liu
Bisphenol A (BPA), a prominent endocrine-disrupting compound, has garnered considerable attention due to its urgent need for rapid removal from water. Herein, we first used a novel reactive phosphine oxide containing tertiary amines as crosslinker to prepare water-insoluble crosslinked β-cyclodextrin (β-CD) adsorbent via radical-mediated thiol–ene polymerization. Owing to the synergistic hydrogen-bond (H-bond) interactions of functional groups (tertiary amine and P O groups) toward BPA, the resulted adsorbents showed fast adsorption kinetics to BPA with an adsorption equilibrium time of 5 min. After six adsorption–desorption cycles, the removal efficiency of BPA was 92.5 %, indicating its excellent reusability. Due to the presence of the C S bonds, the β-CD -derived bio-adsorbents offered binding sites for Cu 2+ ions, resulting in a maximum adsorption capacity of 113.89 mg g −1 .
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ULTRASONICS SONOCHEMISTRY
·
2024
·
IF 8.7
Yuheng Li,Chao Zhang,Shuyi Li,Zhenzhou Zhu,Xuehua Wang,Giancarlo Cravotto
The industrial preparation of kudzu starch (KS) significantly reduces the remaining of flavonoids like puerarin (PU) in the product, weakening its biological activity and making pre-treatments on kudzu crucial. Ultrasonic technique, widely used for modifying biomolecules, can enhance nutrient interactions like those between starch and polyphenols in foods. Thus, a puerarin-kudzu starch (PKS) complex was prepared with the introduction of ultrasonic pretreatment. The results indicated that sonication increased the binding of PU to KS from 0.399 ± 0.01 to 0.609 ± 0.05 mg/g. Particle size analysis and SEM revealed that the particles of the ultrasonic puerarin-kudzu starch complex (UPKS) were larger than those of the untreated complexes. XRD, UV–vis, and FT-IR spectroscopic analyses indicated that hydrogen bonding primarily governs the interaction between PU and KS. Additionally, incorporating PU decreased the starch structure’s orderliness, while ultrasonic treatment altered the helical configuration of straight-chain starch, leading to the formation of a new, ordered structure through the creation of new hydrogen bonds. Additionally, gels formed from UPKS exhibited higher viscosity, elasticity, and shear stress, suggesting that ultrasound significantly altered the intermolecular interactions between PKS. In conclusion, the use of ultrasound under optimal conditions has demonstrated its effectiveness in preparing PKS complexes, highlighting its significant potential to produce high value-added kudzu-based products.
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POLYMER
·
2024
·
IF 4.1
Qingtao Niu,Aihua He,Chongdian Si,Guodong Liu,Mingxuan Xiao,Guifan Chen,Manman Jin
Four TiCl 4 /MgCl 2 Ziegler-Natta catalysts (Cat-1∼Cat-4) with titanium contents in the range of 0.038–0.578 wt% were synthesized by the chemical rout and used for isoprene polymerizations. Four catalysts had similar possessed rod-like morphologies and their surface areas gradually increased as Ti contents increased. Cat-1 with the lowest Ti content (0.038 wt%) had the highest catalytic activity (28039.6 g∙P/(g∙Ti∙h)). To our knowledge, this was the highest activity achieved for isoprene polymerization using the heterogeneous TiCl 4 /MgCl 2 Ziegler-Natta catalyst. With the increasing Ti content, the catalyst activity gradually decreased in the order of Cat-1 < Cat-2 < Cat-3 < Cat-4, whereas the trans -1,4 stereoselectivity increased. Cat-4 with the highest Ti content (0.578 wt %) gave highest trans -1,4 units (97.7 mol%). The polymers were mainly composed of fraction C, D and G. C and D had high trans -1,4 structure while G fraction had low trans -1,4 structure. The plausible stereospecific transformation models of MgCl 2 -supported Ziegler-Natta catalyst with different Ti contents were discussed.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Baorui Liu,Hongqing Cheng,Fangchao Cheng,Dongying Hu
Bifacial dye-sensitized solar cells (DSSCs) have the potential to address the challenge of low photoelectric conversion efficiency (PCE) in various applications. However, achieving a harmonious alignment between the counter electrode (CE) structure and its crucial properties remains a significant challenge. Herein, a lignin-induced orientation strategy was developed for poly (3,4-ethylenedioxythiophene) (PEDOT) using lignosulfonate (SL) as both a surfactant and initiator during the electrochemical deposition process. This approach enabled the successful construction of high-performance CEs for DSSCs. The resulting SL/PEDOT CEs exhibited a low disordered orientation distribution and high redox capacity, achieving a high backside light absorption of 10.7 % and a high conductivity of 104 S/m. Additionally, SL/PEDOT CEs featured excellent corrosion resistance, high electro-catalytic activity, and long service life, maintaining over 90 % of their initial efficiency after 500h. Notably, the incorporation of SL into pristine PEDOT increased the number of electron transport sites, leading to an increase in short-circuit current densities from 21.49 to 29.04 mA/cm 2 . Under one-sided and double-sided irradiation, DSSCs modified with SL/PEDOT CEs achieved higher PCE values of 9.49 % and 16.13 %, respectively, which exceeded those of numerous previously reported DSSCs. Benefiting from the matching effect between molecular/microstructure regulation and performance optimization resulting from SL-induced the orientation of PEDOT molecules, this work offers a new paradigm for the development of high-efficiency bifacial DSSCs.
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Arabian Journal of Chemistry
·
2024
·
IF 5.3
Jie Lian,Wenyu Gong,Jianing Guo,Mingxing Wu
Construction of mesoporous structure and improving the conductivity of carbon counter electrode are feasible paths to enhance the catalytic activity in dye-sensitized solar cells (DSCs) toward the I 3 - /I - redox couple regenerating (IRR). Herein, mesoporous carbon fiber (PCf) has been first synthesized and the DSCs using PCf counter electrode results in a power conversion efficiency (PCE) of 7.12%, significantly surpassing the PCE of 6.01% generated by the DSCs with carbon fiber (Cf) counter electrode without mesoporous structure. Additionally, doping with heteroatoms B or N can further enhance the catalytic performance of PCf. Consequently, B or N doped Cf (BPCf or NPCf) counter electrode-based DSCs achieve high PCE values of 8.43% and 7.96%, respectively, demonstrating PCE improvements of 40.3% and 32.4%. This enhancement in catalytic activity for IRR in DSCs can be first attributed to the increased specific surface area of Cf which can provide more catalytic activated sites. Meanwhile, the enhanced conductivity of PCf by heteroatoms B or N doping is also an important factor for the improved catalytic activity. This work is expected to provide potential path to enhanced the catalytic activity of carbon counter electrode in DSCs toward IRR.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Wang Yao,Zhikai Liu,Letao Guo,Shirong Song,Mei Yang,Guangwen Chen
A robust microreactor with a sudden expansion structure was employed to facilitate controllable mixing with a mixing time ranging from 5.3 to 225.8 ms for water-acetonitrile mixing. Using this well-established mixing setup, a comprehensive investigation was conducted to analyze the inherent effects of various experimental variables on the size of PEG-PLGA NPs during nanoprecipitation. A consistent observation was that the size of PEG-PLGA NPs decreased as the mixing time decreased, ultimately reaching a limited size that no longer changed with the mixing time. This trend led to the classification of the nanoparticle formation process into slow and fast mixing stages. In the fast mixing stage, polymer concentration had minimal impact on particle size, while the anti-solvent to solvent flow rate ratio, solvent pair, and salt concentration influenced particle size by altering the solution environment. Lastly, the smallest attainable particle sizes of PEG-PLGA NPs under various experimental variables were revealed.
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SOLID STATE SCIENCES
·
2025
·
IF 3.3
Zhiwei Jiao,Aolong Sun,Xufang Zhang,Mulan Mu,Haoran Dong
Black phosphorus (BP) has attracted much attention for its excellent electrical and optical properties and its potential in field-effect transistors (FETs). In this work, BP doped with oxygen group elements (sulfur, selenium, and tellurium) was successfully synthesized using the chemical vapor transport method (CVT), and their optoelectronic properties were studied systematically. It is confirmed by X-ray diffraction (XRD) that BP crystals doped with the oxygen group elements exhibited high crystalline quality and yield. Changes in the absorption spectra and surface morphology indicated that doped BP demonstrated significantly enhanced environmental stability compared to undoped BP under prolonged air exposure. Among the doped samples, tellurium (Te)-doped BP showed the highest stability, with a degradation rate of only 9.91 % after 10 days. FETs based on doped BP were successfully fabricated, and their electrical performances were thoroughly evaluated. We found that the hole mobility of BP was dramatically improved by doping, and the selenium (Se)-doped BP possessed the highest hole mobility of 1684.24 cm 2 /V·s.
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Journal of the American Chemical Society
·
2024
·
IF 14.4
Qingjin Fu,Wei Zhang,Xidie Liu,Yinna Liu,Zhengyang Lei,Mengtian Zhang,Haotian Qu,Xiao Xiao,Xiongwei Zhong,Zhexuan Liu,Peiwu Qin,Jun Yang,Guangmin Zhou
On-body batteries with hydrogel electrolytes are a pivotal enabling technology to drive bioelectronics for healthcare and sports, yet they are prone to failure due to dynamic interfacial interference, accompanied by e-waste production. Here, dynamic imine chemistry is proposed to design on-electrode paintable biogel electrolytes that feature temperature-controlled reversible phase transition (gelling within 1.5 min) and ultrafast self-healing capability (6 s), establishing a dynamically self-adaptive interface on cyclically deforming electrodes for shielding on-body Zn-ion batteries from interfacial interference. Consequently, the deformed Zn anode shows an exceptional cycling stability of 400 h regardless of the bending radius, and the as-assembled Zn–I2 battery delivers sufficient durability to endure 5000 deformation cycles, together extending to 1300 h and 15 000 deformation cycles via dynamically restarting the interfacial electric field, respectively. Also, the features of recyclability, biodegradation, and biocompatibility make the proposed on-body Zn–I2 batteries appealing in terms of sustainability and biosafety, enabling their successful power supply of heart rate monitors in sports. This work demonstrates the promise of dynamic biogel chemistry for green and biorelated energy-storage systems.
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Journal of Materials Chemistry C
·
2024
·
IF 5.7
Xinru Zhang,Ning Li,Xiaojing Cui,Yu Li,Zhaosu Wang,Kai Zhuo,Hulin Zhang
Most traffic accidents are caused by driver fatigue, so achieving effective monitoring of fatigue status is particularly important. However, current detection methods mainly rely on complex biosensors that lack independence from power supply and adaptive adhesion, and have a risk of ingestion, especially for infants. Here, we propose an edible thermogalvanic hydrogel with I−/I3− as a redox pair for self-powered physiological monitoring by coupling thermogalvanic and piezoresistive effects. The gelatin/glycerol (Gel/GL) hydrogel exhibits excellent thermo-reversible gelling and temperature-responsive adhesion that can ensure on-demand reliable adhesion to skin for capturing physiological signals under hot compress and facilitate easy removal under cold compress due to the decomplexation and re-entanglement of gelatin chains. Moreover, a low-cost passive patch based on this self-adaptable thermogalvanic gel has been invented to simultaneously monitor breathing, blinking, yawning, and pulse at the canthus, philtrum and radial artery of the human body by acquiring thermoelectric signals correlated with physiological action, achieving a self-powered accurate surveillance of fatigue status, which can provide timely reminders based on fatigue levels. This work is beneficial for improving driving safety and exhibits the potential of the designed hydrogel for application in intelligent transportation.
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Electrocatalysis
·
2024
·Vol. 15
·期 4
·344-352
·
IF 2.7
Zhang Xihuan,Jaouhari Abdelhadi El,Li Chunyue,Adnane Maimoune,Liu Wanying,Mellalou Abderrahman,Ghamouss Fouad,Lin Yuanhua
The oxygen evolution reaction (OER) holds pivotal importance in sustainable energy conversion, as it forms the critical half-reaction in various electrochemical processes, including water splitting for hydrogen production and rechargeable metal-air batteries. Here, a CoFe 2 O 4 @Co 3 O 4 nano-composite was synthesized using a facile hydrothermal process and deposited onto the surface of nickel foam through electrophoresis. Characterization using XRD, Raman spectroscopy, and XPS confirmed the successful synthesis of the composite, exhibiting characteristic peaks of both Co 3 O 4 and CoFe 2 O 4 . The nano-composite exhibited a more amorphous phase than pure oxides, benefiting electrocatalytic activity. Scanning and transmission electron microscopy highlighted the composite’s morphological characteristics, showcasing a Co 3 O 4 island distribution on the CoFe 2 O 4 surface. Electrochemical evaluations revealed the superior oxygen evolution reaction (OER) performance of CoFe 2 O 4 @Co 3 O 4 , with low overpotentials, faster kinetics, and enhanced stability compared to pure oxides and the benchmark RuO 2 catalyst. A comprehensive analysis was carried out to investigate the dynamic behavior during electrocatalytic oxygen evolution reaction. This study unveils the intricate charge and electron transfer mechanisms between cobalt and iron atoms, providing insights into their collaborative role throughout the OER process. Graphical Abstract
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