ChemSusChem
·
2020
·Vol. 13
·期 7
·1906-1914
·
IF 7.962
Yuqi Ke,Jingzhu Zhang,Yuanbang Xie,Qiwei Yang,Qilong Ren,Huabin Xing
Graphical Flex those ABSs : Aqueous biphasic systems (ABSs) based on poly(ionic liquid)s (PILs) were designed and used for the extraction of bioactive compounds. Extraordinary partition coefficients were achieved by customizing the structure of the PILs. The performance of the PIL-based ABSs was tuned by changing the molecular weight and anionic character of the PIL. Ionic liquid (IL)-based aqueous biphasic systems (ABSs) provide a sustainable and efficient alternative to conventional liquid–liquid extraction techniques and can be used for the extraction, recovery, and purification of diverse solutes. However, the construction of a high-performance ABS that has both excellent phase separation ability and extraction performance remains challenging. This study concerns the preparation of a family of novel ABSs based on poly(ionic liquid)s (PILs) with customized structure and controllable molecular weight for the extraction of bioactive compounds. Several tailor-made PILs consisting of a hydrophobic backbone, hydrophilic imidazolium pendant groups and strong hydrogen bonding basic counteranions are prepared by reversible addition fragmentation chain-transfer polymerization. The PILs have a perfect balance of hydrophobicity/hydrophilicity and functionality, affording outstanding phase separation, which was better than with either the IL monomer poly(1-butyl-3-vinylimidazolium bromide ([BVIm]Br) or the normal free-radical polymer P[BVIm]Br*. More importantly, PIL-based ABSs exhibited unprecedented high partition coefficients for six bioactive compounds including tryptophan, phenylalanine, and caffeine, as well as high extraction yields. The performance of the PIL-based ABSs could also be tuned by changing the molecular weight and anionic character of the PILs. This work shows that tailor-made PIL-based ABSs are a promising platform for bioactive compound extraction and provides significant clues for the design of new ABSs for various applications.
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Longkai Pan,Li Yao,Hui Mei,Hongxia Liu,Zhipeng Jin,Shixiang Zhou,Minggang Zhang,Gangqiang Zhu,Laifei Cheng,Litong Zhang
In this study, a novel 3D Bi 2 S 3 /P-ZnO S-scheme gyroid metamaterial was prepared by 3D printing and the hydrothermal method. The unique gyroid macrostructure and nanoarray microstructure offer a large volume of active sites for the photothermal catalytic reaction, thus improving the overall utilization rate of light. ZnO obtained by sintering the precursor produces oxygen vacancies, primarily due to P doping. This enables it to have a photothermal effect. After loading Bi 2 S 3 , the photothermal effect of P-ZnO and Bi 2 S 3 is coupled, further increasing the surface temperature of composite structure and speeding up the reaction rate. P-ZnO and Bi 2 S 3 formed a S-scheme heterojunction, promoting the separation and transfer of photogenerated carriers. Under simulated sunlight, the CO and CH 4 yield of Bi 2 S 3 /P-ZnO S-scheme gyroid metamaterials are 8.87 and 1.49 μmol h −1 . These are 3.45 times and 4.65 times of P-ZnO gyroid structure, respectively. Through SEM, TEM, XPS, ESR and in-situ FTIR characterizations, the transfer paths of photogenerated carriers between heterojunctions were revealed, and the reaction paths of photothermal catalytic CO 2 reduction were explored. The co-design of 3D structure and material allows for a novel concept for further improving photothermal catalytic performance.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Jianhua Yu,Xiancai Pang,Qunchao Yin,Di Chen,Hongzhou Dong,Qian Zhang,Jing Sui,Lina Sui,Lifeng Dong
Constructing self-supporting porous electrode material with abundant electrochemical active sites can effectively improve the energy storage capacity of supercapacitors . Herein, a novel electrode material (NCS@Co-ZIF/NF) is developed by depositing zeolitic imidazolate frameworks (Co-ZIF) on nickel foams (NF), which is adopted as a precursor (Co-ZIF/NF) to electrodeposit nickel-cobalt sulfides (NCS). The nanosheet arrays with cross-porous structures provide NCS@Co-ZIF/NF with excellent electrochemical characteristics, including a high specific capacity of 144.4 mAh g −1 at the current density of 1 mA cm −2 , 60.5% capacity retention at 50 mA cm −2 , and superb long-term cycle stability. Furthermore, NCS@Co-ZIF/NF//AC hybrid supercapacitor is fabricated by using NCS@Co-ZIF/NF as positive electrodes and activated carbon (AC) as negative electrodes , which exhibits a high energy density of 33.9 Wh kg −1 at a power density of 145 W kg −1 .
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高影响因子
Materials Today Chemistry
·
2024
·
IF 6.7
Xiaoyu Zhou,Chuanliang Wu,Zelin Zhao,Yusheng Wang,Yuanyuan Yang,Jingxing Guo,Jia Wang,Xiaolong He,Yinyu Xiang,Ning Han,Junsheng Li
Despite the bright future of aluminum-sulfur (Al–S) batteries due to the ultrahigh energy-to-price ratios, the development of this new energy storage system is plagued by the shutting of polysulfides and sluggish kinetics during redox conversions. Herein, ferrocene as efficient polysulfide mediators and electrocatalysts is covalently grafted onto glass fiber (GF) membranes, which serves as separators in Al–S batteries. Attributed to the strong chemisorption and catalytic effect of metallocene toward polysulfide conversions, Al–S cells assembled with the grafted separators deliver an ultrahigh initial capacity of 1347.9 mAh g −1 (at 200 mA g −1 ) and desirable rate performance (328.1 mAh g −1 at 500 mA g −1 ). As validated by theoretical calculations, effective polysulfide binding is achieved through beneficial cation-π interactions between Al 3+ in polysulfides and the negatively charged cyclopentadienyl ligands in ferrocene, providing novel insights into the exploration of metal-sulfur chemistries for stable energy storage.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Shusen You,Songqi Ma,Jinyue Dai,Zhen Jia,Xiaoqing Liu,Jin Zhu
Hexahydro-s-triazine (HT) derivatives are acid-sensitive compounds. 4,4′,4″-(1,3,5-Hexahydro-s-triazine-1,3,5-triyl) tris(N-(2-aminoethyl) benzamide) (HT-A) bearing three amino groups was synthesized as a curing agent to prepare the acid-degradable epoxy resin. The chemical structures of HT-A and its precursor were confirmed by 1H NMR and 13C NMR. The synthesized HT-A, as well as the commercialized 4,4′-diaminodiphenylmethane (DDM) (for use as the control) were used to cure diglycidyl ether of bisphenol A (DGEBA), respectively. The property examinations performed by dynamic mechanical analysis (DMA), differential scanning calorimeter (DSC), thermogravimetric analysis (TGA), and tensile test demonstrated that the HT-A-cured epoxy presented high thermal and mechanical properties which were comparable with those of the DDM cured one. Meanwhile, degradation investigation indicated that the HT-A-cured epoxy could be controllably degraded with strong acid stimuli. Thus, HT-A has a great potential to produce recyclable thermosets with satisfactory properties.
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高影响因子
SOLAR ENERGY
·
2019
·
IF 4.674
Yefeng Wang,Jing Hui Zeng,Guangtao Zhao
Developing cost-effective solid-state electrolyte is a urgent issue and a common request for (photo) electrochemical cells. In this work, a series of organic ionic conductors based on the S -substituted benzothiophenium salts have been synthesized via a simple and low-cost method. Research on the thermal behavior, optical absorption and ionic conductivity shows that S -methylbenzothiophenium tetrafluoroborate ([MBT]BF 4 ) among them have the good thermal stability, high ionic conductivity and no absorption in the visible region. And the solid-state electrolyte using [MBT]BF 4 as the matrix exhibits the good interfacial compatibility with photoanode. Applying this solid-state electrolyte into the quantum-dot sensitized solar cell (QDSSCs), the device achieves an open circuit voltage of 0.71 V, a short circuit current density of 20.73 mW cm −2 , and a power conversion efficiency of 5.49% which is higher than those previously reported for the solid-state QDSSCs.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Hongbing Song,Yongjie Wang,Yule Liu,Lei Chen,Bingxiao Feng,Xin Jin,Yu Zhou,Tingting Huang,Meng Xiao,Fangmin Huang,Hengjun Gai
Three ionic liquid (IL) monomers consisting of one, two, and four benzene rings were designed with 2-phenylimidazole and polymerized with α,α′-dichloro-p-xylene (DCX) and formaldehyde dimethyl acetal (FDA) to form a series of novel poly(ionic liquid)s (PILs). In this process, the designed ILs were employed as active ionic sites, and DCX and FDA were selected as cross-linkers. Self-condensation of the cross-linker provided a large specific surface area for the hypercross-linked organic framework, while co-condensation between the cross-linker and IL introduced active sites to the framework. The obtained porous hypercross-linked PILs not only promoted CO2 capture and the selective absorption of CO2/N2 but also showed good activity for the cycloaddition of epoxide with CO2. HP-[BZPhIm]Cl-DCX-1 with a large surface area (763 m2·g–1) showed a CO2 uptake capacity of 1.47 mmol·g–1 and offered a 98.9% yield of the CO2 cycloaddition product with epichlorohydrin at 80 °C for 24 h under 0.1 MPa CO2 pressure. The designed PILs provide an important reaction for CO2 utilization.
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高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
·
2019
·Vol. 37
·期 4
·428-436
·
IF 2.804
Huang Yuzhang,Chen Ping,Wei Bo,Hu Rongrong,Tang Ben Zhong
Hyperbranched polymer with highly branched three-dimensional topological structure, a large number of end groups, and multifaceted functionalities have gained much attention, while polymers with aggregation-induced emission (AIE) properties become a group of popular luminescent materials recently. The design and synthesis of AIE-active hyperbranched polymers, which combine the advantages of these two types of materials, are attractive but challenging. In this work, four hyperbranched poly(tetrahydropyrimidine)s were synthesized from the metal-free room temperature multicomponent tandem polymerization of diester group-activated internal alkyne, polyfunctional aromatic amines, and formaldehyde in methanol under the catalysis of acetic acid. Through different monomer combination and controlling the monomer loading order, hyperbranched polymers with various topological structures as well as sequences of different functional groups in the polymer backbone were obtained with high molecular weights (up to 3.0 × 10 4 g/mol) in high yields (up to 98%). The hyperbranched poly(tetrahydropyrimidine) emitted faintly in solution, while its luminescence was notably enhanced in the aggregated state, suggesting its typical aggregation-induced emission property. It is anticipated that the multicomponent polymerization may provide a synthetic platform for the construction of hyperbranched polyheterocycles with diverse structures and functionalities.
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高影响因子
ACS Omega
·
2024
·
IF 3.7
Kexin Zhang,Rui Wang,Xin Zhong,Fubin Jiang
Rapid recombination of photogenerated electrons and holes affects the performance of a semiconductor device and limits the efficiency of photocatalytic water splitting for hydrogen production. The use of an S-scheme nanoscale heterojunction catalyst for the separation of photogenerated charge carriers is a feasible approach to achieve high-efficiency photocatalytic hydrogen evolution. Therefore, we synthesized a three-dimensional S-scheme nanoscale heterojunction catalyst (LaNi0.6Fe0.4O3/g-C3N4) and investigated its activity in photocatalytic water splitting. An analysis of the band structure (XPS, UPS, and Mott–Schottky) indicated effective interfacial charge transfer in an S-scheme nanoscale heterojunction composed of two n-type semiconductors. X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) spectroscopy confirmed that the light-induced charge transfer followed the S-scheme mechanism. Based on the capture test (EPR) of •OH free radicals, it can be seen that the enhanced activity is attributed to the S-scheme carrier migration mechanism in heterojunction, which promotes the rapid adsorption of H+ by the abundant amino sites in g-C3N4, thus effectively generating H2. The 2D/2D LaNi0.6Fe0.4O3/g-C3N4 heterojunction has a good interface and produces a built-in electric field, improving the separation of e– and h+ while increasing the oxygen vacancy. The synergistic effect of the heterostructure and oxygen vacancy makes the photocatalyst significantly better than LaNi0.6Fe0.4O3 and g-C3N4 in visible light. The hydrogen evolution rate of the composite catalyst (LaNi0.6Fe0.4O3/g-C3N4-70 wt %) was 34.50 mmol·h–1·g–1, which was 40.6 times and 9.2 times higher than that of the catalysts (LaNiO3 and g-C3N4), respectively. After 25 h of cyclic testing, the catalyst (LaNi0.6Fe0.4O3/g-C3N4-70 wt %) composite material still exhibited excellent hydrogen evolution performance and photostability. It was confirmed that the synergistic effect between abundant active sites, enriched oxygen vacancies, and 2D/2D heterojunctions improved the photoinduced carrier separation and the light absorption efficiency of visible light. This study opens up new possibilities for the logical design of efficient photodecomposition using 2D/2D heterojunctions combined with oxygen vacancies.
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高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Lei Feng,Ze-Min Zhu,Ying Yang,Zongbin He,Jiafeng Zou,Man-Bo Li,Yan Zhao,Zhikun Wu
Metal nanoclusters are rising stars in material science , and one advantage is their atomically precise tunability. It is well known that metal doping can efficiently modify the properties of metal nanoclusters. In particular, without altering the parent nanocluster framework, doping a single heterometal atom can tailor the properties of metal nanoclusters and aid investigations of the structure–property relationship of metal nanoclusters. To our knowledge, the simultaneous synthesis of a single heterometaldoped nanocluster and its parent nanocluster is challenging and has not been previously reported; however, this is highly desirable because it can prevent the influence of trace impurities and allow comparison between doped and undoped nanoclusters. The single Cd-doped gold nanocluster Au 22 Cd 1 (S-Adm) 16 (S-Adm = 1-adamantanethiolate) has been previously synthesized and structurally elucidated. However, the structure of the parent nanocluster, Au 23 (S-Adm) 16 , remains unknown, inspiring this investigation. In this study, we synthesized Au 23 (S-Adm) 16 and its single-doped Au 22 Cd 1 (S-Adm) 16 nanocluster in one pot for the first time, and we resolved their structures using single-crystal X-ray crystallography. The structure of Au 22 Cd 1 (S-Adm) 16 is similar to that of Au 23 (S-Adm) 16 except that a kernel Au atom in Au 23 (S-Adm) 16 is replaced with a Cd atom. This Cd replacement causes the kernel Au―Au bond length to increase owing to the loosening of the original closely packed structure. In contrast to prior reports, Au 23 (S-Adm) 16 is surprisingly more stable than Au 22 Cd 1 (S-Adm) 16 , as determined via ultraviolet visible-near infrared (UV-Vis-NIR) spectroscopy at 80 °C. This stability was attributed to the decrease in the kernel Au―Au bond length. Although the maximum absorption of Au 22 Cd 1 (S-Adm) 16 slightly red-shifted from 605 to 608 nm after Cd doping, the molar extinction coefficient of Au 23 (S-Adm) 16 at 605 nm was approximately twice that of Au 22 Cd 1 (S-Adm) 16 at 608 nm. Thus, the increase in kernel Au―Au bond length may decrease the photoexcitation electron transfer efficiency owing to lengthening of the photoexcitation electron transfer pathway. As further support for this opinion, although the two nanoclusters showed similar emission profiles and maxima (750 nm for Au 23 (S-Adm) 16 and 760 nm for Au 22 Cd 1 (S-Adm) 16 ), they exhibited obvious emission intensity differences. Specifically, the quantum yield of Au 23 (S-Adm) 16 (approximately 3.160 × 10 −5 ) was found to be 1.13 times that of Au 22 Cd 1 (S-Adm) 16 (approximately 2.793 × 10 −5 ). Thus, the stability and absorption and emission intensities correlate with the kernel Au―Au bond length. This study shows that two metal nanoclusters with slight structural differences can exhibit different properties in terms of optical and thermal stability, providing a good reference for studying their structure–property relationships. Download: Download high-res image (68KB) Download: Download full-size image
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高影响因子
Solar RRL
·
2021
·Vol. 5
·期 7
·2100210
·
IF 8.582
Lifen Su,Yuying Ning,Ziqiang Ma,Yuhao Zhang,Chuanlei Liu,Youli Zhang,Lei Miao,Jianhua Zhou,Bin Wu,Jiasheng Qian
Solar vapor generation is a sustainable and cost-effective approach to addressing the issue of water shortage. However, the challenges of solar steam generation still exist for achieving a high evaporation efficiency combined with long-term stability in the wastewater containing heavy metal ions and wide degrees of acidity and alkalinity (pH = 1–14). Herein, polypyrrole (PPy) loading on the N,S-doped graphene oxide (N,S-GO) foam is used for high-efficiency solar evaporation of treating wastewater. With the advantages of excellent broadband solar absorption ( >97%), extremely low emissivity (0.70), and outstanding hydrophilicity, the N,S-GO/PPy foam achieves a high evaporation efficiency of 90.5% under 1 sun illumination. More notably, the N,S-GO/PPy foam has strong adsorption of heavy metal ions (Fe 3+ , Cu 2+ , and Cr 6+ ) for treating wastewater synchronously evaporates at higher efficiencies of 94.7–98.4%. Interestingly, the high-toxicity Cr 6+ can be reduced to low-toxicity Cr 3+ effectively by the synergistic effect of N,S-GO and PPy. In addition, the N,S-GO foam shows a better long-term resistance of acidity and alkalinity for 45 days. A new insight is offered into high-efficiency solar evaporation for treating wastewater and water purification.
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高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2022
·Vol. 46
·期 14
·19480-19492
·
IF 4.672
Jiuqing Liu,Fanli Zeng,Meng Liu,Junying He,Qihou Li,Feifei Song,Zikun Hong,Ya Chen,Lishun Bai,Chen Cheng,Zehao Chen
Summary As one of the most promising energy storage systems, the application of lithium sulfur battery is hindered by low ionic conductivity, poor thermal stability, and a serious shuttle effect of polysulfide species of commercial polyolefin separators. Herein, a kind of novel porous polyetherimide (PEI) based separator (IAPEI-4) with excellent heat resistance and electrochemical properties was prepared. Briefly, by grafting amino group (–NH 2 ) onto the surface of SiO 2 , highly dispersed amino-functionalized SiO 2 (A-SiO 2 ) were synthesized as fillers to blend PEI matrix. Based on physical characterizations of the representative IAPEI-4 separator, abundant micropores and mesopores exist in the separator, and A-SiO 2 nanoparticles are uniformly distributed in the PEI matrix. The ameliorated Li + transport channels and the uniform distribution of A-SiO 2 nanoparticles endow IAPEI-4 separator with higher ionic conductivity (1.60 mS cm −1 ) and Li + transfer number (0.63). Besides, the IAPEI-4 separator exhibits good electrochemical stability and excellent thermal stability (no shrinkage at 200°C). The Li-S cells with the IAPEI separator also show greatly enhanced electrochemical performances. After 100 cycles, its specific discharge capacity can reach 695.4 mAh g −1 at 0.2 C and its capacity retention rate is 84.8%. This simple and effective separator modification method can provide a general strategy to achieve high-performance Li-S batteries.
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高影响因子
危险品化学品经营许可证（带存储）