INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Yuxia Liu,Shiting Wang,Zhifeng Dai,Yubing Xiong
The cycloaddition reaction of CO2 and epoxides to form cyclic carbonates is a promising strategy to alleviate the climate change caused by CO2 in view of its high atomic economic efficiency and solvent-free and mild conditions. Inspired by the mechanism of cycloaddition reactions catalyzed by Lewis acid/Lewis base binary systems, we explored a series of heterogeneous catalysts functionalized by cobalt porphyrin cross-linked phosphonium salt poly(ionic liquid)s. Specifically, poly(4-vinylbenzyl chloride) (PVBnCl) was used as the polymer backbone. Then, PVBnCl was cross-linked by 5,10,15,20-tetra(4-pyridyl) porphyrin (TPyP) and quaternized by triphenylphosphine (PPh3). After complexing with CoCl2 and anion exchange, the as-prepared polymers CoTPyP-c-PVBnPPh3X were characterized using FTIR, SEM, TEM, XPS, TGA, ICP, and solid-state 13C NMR measurements. The results demonstrated that CoTPyP-c-PVBnPPh3X were efficient catalysts for the cycloaddition of CO2 and epoxides under mild conditions. Almost quantitative conversion of epoxides could be achieved at 80 °C and 1 atm CO2, and CoTPyP-c-PVBnPPh3X could be easily separated and reused for four cycles only with a little decrease in the catalysis activity. The synergistic catalysis of the Lewis acid metal center and nucleophilic halogen ion addressed the excellent performance of CoTPyP-c-PVBnPPh3X. Therefore, our findings provided a new solution for the development of efficient heterogeneous catalysts with multi-centers for CO2 conversion.
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APPLIED SURFACE SCIENCE
·
2021
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IF 6.707
Ziyu Qin,Xiaoxiao Song,Junyong Wang,Xiang Li,Congyi Wu,Xiaoxia Wang,Xueqiong Yin,Dawen Zeng
For the important applications of gas identification related to specific diseases in healthcare, flexible gas sensors have attracted more attention. Among them, two-dimensional transition metal dichalcogenides (2D TMDs) have been known as good promising flexible gas-sensitive materials. While how to tightly attach 2D materials on flexible substrates is still challenging. Here, we propose an enhanced room-temperature flexible paper-substrate sensors based on 2D tungsten disulfide (WS 2 ) with S defects, which are facilely synthesized by chemical exfoliation and vacuum filtration method. Structure characterization shows that most of the as-prepared 2D WS 2 are within 3 layers. Spectroscopic characterization proves the existence of S defects on the surface of 2D WS 2 produced by chemical exfoliation. The room-temperature (25 °C) NH 3 gas sensitivity results show that the response intensity of 2D WS 2 with rich S defects is nearly three times higher than the highly crystalline 2D WS 2 . The results of the flexible gas sensitivity indicate the fast response and high stability of our devices in breathing detection and bending experiments. Furthermore, the devices can effectively distinguish bending stress changes and gas-sensitive response signals at the same time, realizing multifunctional sensing detection. Our work will be a reference for fabricating flexible sensors based on 2D materials.
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iScience
·
2025
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IF 4.1
Zhiwei Meng,Zirui Peng,Yupeng Yan,Qin Zhang,Yang Li
Photocatalytic technology is currently one of the most effective methods for removing tetracycline (TC) from the environment; however, the underlying photocatalytic mechanism remains unclear. In this study, zinc oxide quantum dots (ZnO-QDs)/hollow-sphere g-C 3 N 4 (CNHS) S-scheme heterojunction photocatalysts were synthesized for the photocatalytic degradation of tetracycline. Experimental results showed that the 7% ZnO-QDs/CNHS photocatalyst exhibited excellent TC degradation efficiency, with a removal rate of 80.2% within 15 min. Through free radical conversion pathway analysis, singlet oxygen ( 1 O 2 ) was identified as the primary active species responsible for tetracycline degradation. Further calculations indicated that the combination of holes (h + ) and superoxide radicals (O 2 − ) produces 1 O 2 , accounting for 83.28% of the total contribution. These findings provide theoretical support for 1 O 2 as the primary active species in pollutant degradation.
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高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 42
·22584-22591
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IF 14.511
Xiaoying Song,Min Wang,Sheng Wang,Zhu Cheng,Ting Zhang,Ting Zhu,Hucheng Song,Linwei Yu,Jun Xu,Kunji Chen
Solid-sate lithium-ion batteries (LIBs), especially lithium–sulfur (Li–S) batteries, are one of the most promising candidates for developing high energy density and high safety energy storage devices. However, current solid-state Li–S batteries can only work well at a relatively high operating temperature (>50 °C) due to the poor Li-ion transfer kinetics at electrodes/electrolyte and their interfaces which make these batteries lose most of their capacity and power as the temperature falls below room temperature. Here, we report an extra-wide operating temperature solid-state Li–S battery that can efficiently harvest omnidirectional solar energy and convert it into heat via a hierarchical copper–silicon nanowire photothermal current collector. Such a current collector enables broad solar spectrum absorption (>93%) with a wide incident angle (0 degree to 70 degree) and efficient conversion of light-to-heat, improving charge storage and transmission at electrodes/electrolyte and their interfaces even at low operating temperatures. As a result, the battery demonstrates low impedance (∼102 Ω cm2), a high discharge capacity of ∼900 mA h g−1 at room temperature, ∼960 mA h g−1 at 60 °C and a discharge capacity of ∼260 mA h g−1 at −60 °C. Such a design provides an effective solution for all-solid-state LIBs operating at a low temperature.
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Polymer Chemistry
·
2016
·Vol. 7
·期 18
·3172-3178
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IF 5.687
Zikun Wang,Youhua Tao,Zhen Wang,Jingling Yan
Four N-vinyl-1,2,3-triazole monomers were prepared in high yields from 2-aminoethanol and α-diazo-β-oxoamides via modified Wolff's cyclocondensation reactions. Then a series of poly(N-vinyl-1,2,3-triazole)s were synthesized through conventional free radical polymerization of these monomers. The chemical structures of these monomers and polymers were confirmed by proton and carbon nuclear magnetic resonance (1H and 13C NMR). The properties of poly(N-vinyl-1,2,3-triazole)s were systematically characterized by a variety of analytical techniques including thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), gel permeation chromatography (GPC), and solubility testing. The results indicated that these polymers exhibited higher glass transition temperatures (196–212 °C) than most of the commodity vinyl polymers such as polystyrene (100 °C) and poly(methyl methacrylate) (110 °C). Moreover, these polymers can be further functionalized through hydrolysis of amide groups. These results revealed that this methodology has great potential for constructing 1,2,3-triazole-containing monomers and polymers.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Renhui Ling,Mingxing Li,Xin Li,Laihuan Pei,Xiaoyan Luo,Congmin Wang
MOFs have high adsorption performance of ammonia (NH 3 ) because of its porosity and abundant coordination sites, especially MOFs containing carboxylic acid ligands have emerged as effect NH 3 adsorbents. But, it’s troublous for reversible ammonia adsorption for the strong metal-NH 3 coordination or the collapse of adsorbents. [MEDTA] 2- is a very stable and classic carboxylic acid-containing complex, but there was no relevant report. Therefore, this work carried out the design and synthesis of PVIm-R8-MEDTA based on the use of the coordination structure of [MEDTA] 2- and the stability of PILs’ skeleton. The characterization indicated the [MEDTA] 2- could be introduced into PILs successfully for the hydrogen bonding interactions with the imidazolium cation, and the obtained PVIm-R8-MEDTA presented enhanced NH 3 capacity (10.4–14.7 mmol/g) than their precursor PVIm-R8-Br (7.8 mmol/g). The mechanism of NH 3 adsorption was proposed by DFT calculation, spectroscopic method, and the calorimetric test, it indicated the NH 3 was fixed by imdazolium cation through hydrogen bonding and inserted into two of the carboxylate and metal bonds of [MEDTA] 2- . Because of the multi-meshing coordination of [EDTA] 4- and metal ions, the disconnected carboxylate ions could easily coordinate with metal ions again and repair the chelating structure of [MEDTA] 2- , which caused the ammonia easily be desorbed. In the process of gas adsorption, there was no bonding breakage of the skeleton of PILs, which helped the PVIm-R8-MEDTA be recovered under moisture and NH 3 atmosphere. Thanks for the designability of PILs, such as the cationic structure, structure and size of cross-linking agent, the choice of complex anion and so on, it provides a new design idea and theoretical basis for efficient and reversible ammonia adsorption materials.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Wei Huang,Haojie Chen,Hefan Zhang,Xueying Wang,Chunlan Xu,Jiahao Liu,Lan Zhang,Changyu Lu
The design of green and low-cost S-scheme heterojunctions with strong interface interactions is key to their photocatalytic performance and practical application. Here, novel S-scheme heterojunctions of self-grown CuO/sediment (CUS) were successfully fabricated using a calcination method with sediment derived from nature. Various methods were employed to evaluate the micromorphology, crystal structure, chemical composition, and optical characteristics of the photocatalysts. Supported by ultra-violet photoelectron spectroscopy (UPS) analyses, an S-scheme charge migration path was revealed in the CUS during the photocatalytic reaction. The CUS3:7 S-scheme heterojunction exhibited optimal photocatalytic activity at 4.08 times and 1.57 times higher than those of pure CuO and SM-300, respectively, and excellent photocatalytic activity was detected in the peroxymonosulfate (PMS) system. Notably, metal and nonmetal ions in sediment themselves and 1 O 2 generated in PMS system are resistant to anionic and cationic interferences in water decontamination. In addition, the photocatalytic mechanism, possible intermediates, and degradation pathways were elucidated using theoretical calculations and experimental results. Moreover, mung bean sprout cultivation experiments confirmed the non-toxicity of the developed heterojunction and degraded tetracycline solution. These findings offer new insights to aid in synthesizing photocatalysts for wastewater treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Keting Feng,Kangqi Wu,Kai Li,Weijun Wang,Shihui Gao,Jun Fan,Tao Sun,Enzhou Liu
Localized surface plasmon resonance (LSPR) effect plays a crucial role in the field of solar energy utilization. In this work, we successfully prepared a Cu 2-x Se/ZnSe S-scheme heterojunction with a broad-spectrum response using the hot-injection and low-temperature water bath method. Importantly, we demonstrated that the photothermal effect induced by the LSPR of nonstoichiometric Cu 2-x Se can significantly improve the slow kinetics of water splitting, resulting in an apparent activation energy reduction from 50.1 to 28.7 kJ·mol −1 . This improvement is responsible for achieving the highest photocatalytic H 2 evolution rate of 63.6 mmol·g −1 ·h −1 over 2.7 % Cu 2-x Se/ZnSe under the wavelength ranged from 200 to 2500 nm, which is 3.4 and 5.6 times higher than that of ZnSe and Cu 2-x Se, respectively. Furthermore, the composite exhibits a remarkable H 2 production rate of 0.108 mmol·g −1 ·h −1 under near-infrared spectroscopy (800<λ<2500 nm), while ZnSe shows limited capability in H 2 releasing. Additionally, Cu 2-x Se/ZnSe demonstrates distinct photocurrent response when λ > 800 nm. The enhanced performance in H 2 evolution can be attributed to the synergistic effect of LSPR-induced light absorption and S-scheme heterojunction, which not only expands the light absorption range to the near-infrared region but also facilitates hot electron injection, charge carrier separation and transfer, leading to a faster surface reaction kinetics. This study provides an effective approach for designing a broad-spectrum light responsive non-precious metal-based photothermal-assisted photocatalytic system.
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高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuyan Wang,Hongxia Zhang,Wei Gao,Ming Zhong,Bitao Su,Ziqiang Lei
In this work, two series of plasmonic S-type heterojunction photocatalysts containing Bi, TiO 2 , and biochar (Bi/TiO 2 @C) have been developed through a biomass-assisted hydrothermal-calcination strategy, utilizing grapefruit peel as a reducing agent and C resource. The calcination temperature and the mass ratio of biomass were optimized to obtain the optimal nanocomposite, which shows excellent adsorptive and visible-light photocatalytic performance in the removal of diverse antibiotic and dye pollutants, including tetracycline, oxytetracycline, ciprofloxacin, sulfamethoxazole, sulfisoxazole, malachite green, and rhodamine B. The remarkable performance can be attributed to the enhanced absorption of light absorption resulting from the localized surface plasmon resonance effect of the semimetal Bi, and the formation of heterogeneous interface between Bi and TiO 2 , which accelerates the transfer of photogenerated charge. Furthermore, trapping tests and electron spin resonance (ESR) analysis reveal that ∙O 2 - and h + are the primary active species involved in the removal of tetracycline. A plausible charge transfer mechanism has been proposed.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Shenghang Peng,Rong Li,Jing Li,Jian-Ping Zou,Alex Aziz,Xuxing Chen
Effective removal of ethylene (C 2 H 4 ) during fruit and vegetables storage and transport remains a critical challenge for post-harvest preservation. Although S-scheme heterojunctions can improve charge separation and redox capacity for ethylene degradation, their efficiency is still restricted by limited carrier transfer and sluggish oxygen activation. Here, we rationally designed a novel 2D/2D SnNb 2 O 6 /Bi 2 MoO 6 monolayer S-scheme heterojunction integrated with Pt co-catalyst to address these limitations. Density Functional Theory (DFT) calculations revealed the S-scheme charge transfer pathway, which was experimentally realized via electrostatic self-assembly followed by annealing-induced atomic interface bonding. Photodeposited Pt nanoparticles further promoted O 2 activation at reduction sites. The optimized Pt-50-SNOBMO achieved an outstanding visible-light-driven degradation rate (139.2 × 10 −3 min −1 ), 248.6 and 143.5 times higher than pristine SnNb 2 O 6 and Bi 2 MoO 6 , representing the best performance reported to date for ethylene removal. Extensive spectroscopic and microscopic analyses confirmed the robust interface interactions and S-scheme mechanism. This study provides new insights into heterojunction engineering and offers a promising strategy for advanced photocatalytic preservation technologies.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 51
·2208676
·
IF 19.924
Bo Pang,Zuquan Jin,Yunsheng Zhang,Zhiyong Liu,Wei She,Penggang Wang,Yong Yu,Xiaoying Zhang,Chuansheng Xiong,Ning Li,Guowen Sun,Peng Zhao,Guojian Liu,Xiaoyun Song,Song Gao
Cement-based sensors (CBSs) have demonstrated potential in structural health monitoring (SHM) despite rare applications due to their poor flexibility and sensing accuracy/protection with robustness. Herein, a promising strategy is reported to design a waterborne epoxy resin (WEP)-modified cement-based composite coating sensorcapable of simultaneous stable SHM and durable protection. The interpenetrating network (IPN) formed by WEP within cement paste is bionic to the toughness and crack resistance of biological muscle tissue and balances the ion permeation performance and polarization of hydration products. The polymerization-redispersion progress and mechanism of calcium silicate hydrate (C-S-H) gel modified with [3-(2-aminoethylamino)-propyl]trimethoxysilane silsesquioxane (C-POSS) are characterized and revealed. The results show that the muscle-like IPN increases the cement-based coatings’ maximum deflection angle to 30° and improves the monitoring accuracy of compressive, tensile, and fatigue microchanges of concrete structures to more than 95%. The POSS···Ca 2+ ···C-S-H interaction in C-POSS partially transferred the intra-adhesive hydrogen bonds surrounding the nanoconducer into electrostatic bridging ones to maintain an excellent electromechanical conductive dispersion.
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Carbon Energy
·
2025
·
IF 24.2
Mengmeng Ma,Runkang Lin,Kaige Huang,Shizhong Yue,Maohong Fan,Zhijie Wang,Shengchun Qu
Functionalization has emerged as a pivotal endeavor to tailor the surface properties of photocatalysts. We propose a facile amine functionalization strategy to establish a Cu−In−Zn−S (CIZS)/NiS x hybrid with covalent bonds using individual ethylenediamine (EDA) molecules. Our approach witnesses a remarkable photocatalytic hydrogen evolution (PHE) competence of 65.93 mmol g −1 h −1 driven by visible light, the highest value yielded by CIZS to date. X-ray absorption spectra of CIZS and density functional theory (DFT) calculations confirm the crucial amine N→Cu coordination after amine functionalization. The new emerging coordination via lone-pair electron donation profitably accesses the regulation of the coordination environment, electronic structures, and carrier behavior. Moreover, individual EDA molecule with two-terminal −NH 2 group serves as a molecular bridge to hybrid CIZS and NiS x cocatalyst via N→Cu and N→Ni coordination, favorably promoting efficient charge transport. This study provides advances in practical functionalizing photocatalysts.
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