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学者姓名：徐超
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Abstract ：
Photocatalytic oxidative coupling of amines is considered a mild, efficient, and sustainable strategy for the synthesis of imines. As a versatile organic semiconductor, conjugated microporous polymers (CMPs) are attractive in photocatalysis areas due to the diversity of their polymeric monomers. Herein, we report that in addition to the design of monomers, size-confined polymerization is also a feasible strategy to modulate the structure and photocatalysis properties of CMPs. We adopted dibromopyrazine as polymeric units to prepare pyrazine-involved hollow spherical CMPs (H-PyB) using a template method and successfully performed sizeconfined polymerization of hollow samples by resizing the templates. Interestingly, the small confinement space induced the formation of CMPs with better conjugate extensibility, resulting in enhanced conductivity, narrowed bandgaps, improved photoelectric performance, etc. As a result, small-sized H-PyB CMPs had superior activity for the photocatalytic oxidation of amines. Particularly, the smallest H-PyB CMPs that we designed in the present work exhibited excellent performance for the photocatalytic coupling oxidation of amines. When using benzylamine as a model substrate, the yield of the corresponding imine reached similar to 113 mmol center dot g(- 1)center dot h(-1), accompanied by almost 100 % selectivity. Furthermore, the as-designed confined samples exhibited stable photocatalytic activity as well as good applicability for oxidative coupling of different amines. This work not merely reports a kind of CMP photocatalysts with excellent performance for the imine coupling oxidation but also proposes an alternative strategy for constructing high-performance organic photocatalysts by size-confined synthesis.
Keyword ：
Amine Amine Conjugated microporous polymers Conjugated microporous polymers Photocatalytic oxidation Photocatalytic oxidation Size-confined synthesis Size-confined synthesis Visible light Visible light
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| GB/T 7714 | You, Shaojie , Ding, Zhengxin , Yuan, Rusheng et al. Confined synthesis of conjugated microporous polymers for selective photocatalytic oxidation of amines [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 664 : 63-73 . |
| MLA | You, Shaojie et al. "Confined synthesis of conjugated microporous polymers for selective photocatalytic oxidation of amines" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 664 (2024) : 63-73 . |
| APA | You, Shaojie , Ding, Zhengxin , Yuan, Rusheng , Long, Jinlin , Xu, Chao . Confined synthesis of conjugated microporous polymers for selective photocatalytic oxidation of amines . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 664 , 63-73 . |
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Prussian blue analogues (PBAs) have been widely studied as cathodes for potassium-ion batteries (PIBs) due to their three-dimensional framework structure and easily adjustable composition. However, the phase transition behavior and [Fe(CN)(6)](4-) anionic defects severely deteriorate electrochemical performances. Herein, we propose a defect-free potassium iron manganese hexacyanoferrate (K1.47Fe0.5Mn0.5[Fe(CN)(6)]1.26H(2)O, KFMHCF-1/2) as the cathode material for PIBs. The Fe-Mn binary synergistic and defect-free effects can inhibit the cell volume change and octahedral slip during the K-ion insertion/extraction process, so that the phase transformation behavior (monoclinic <-> cubic) is effectively inhibited, achieving a zero-strain solid solution mechanism employing Fe and Mn as dual active-sites. Thus, KFMHCF-1/2 contributes the highest initial capacity of 155.3 mAhg(-1) with an energy density of 599.5 Whkg(-1) at 10 mAg(-1) among the reported PBA cathodes, superior rate capability, and cyclic stability over 450 cycles. The assembled K-ion full battery using K deposited on graphite (K@G) as anode also delivers high reversible specific capacity of 131.1 mAhg(-1) at 20 mAg(-1) and ultralong lifespans over 1000 cycles at 50 mAg(-1) with the lowest capacity decay rate of 0.044% per cycle. This work will promote the rapid application of high-energy-density PIBs.
Keyword ：
ammonia synthesis ammonia synthesis flow-throughelectrode flow-throughelectrode lamellar electrified membrane lamellar electrified membrane MXene MXene nitrate reduction nitrate reduction sustainable operation sustainable operation
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| GB/T 7714 | Yang, Xin , Wei, Guanbao , Cao, Jihui et al. Mxene-Cu Electrified Membranes with Confined Lamellar Channels for the Flow-through Electrochemical Reduction of Nitrate to Ammonia [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (8) : 3378-3389 . |
| MLA | Yang, Xin et al. "Mxene-Cu Electrified Membranes with Confined Lamellar Channels for the Flow-through Electrochemical Reduction of Nitrate to Ammonia" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 12 . 8 (2024) : 3378-3389 . |
| APA | Yang, Xin , Wei, Guanbao , Cao, Jihui , Ding, Zhengxin , Yuan, Rusheng , Long, Jinlin et al. Mxene-Cu Electrified Membranes with Confined Lamellar Channels for the Flow-through Electrochemical Reduction of Nitrate to Ammonia . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (8) , 3378-3389 . |
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Ethers are among the most important chemicals in organic synthesis, the pharmaceutical industry, agrochemical production, and material science. C–O bond formation via substitution is one of the most widely used strategies for ether formation. However, known methods usually employ transition-metal and bases to facilitate the process. In this work, we describe the base- and transition-metal-free ether formation via alcohol and phenol-participated substitution. The protocol allows access to a large number of ethers with enyne functional moieties, and features mild reaction conditions, high efficiency, and good regio- and stereoselectivities. The reaction could be readily scaled up, and the products could be used in a range of further transformations. © 2023 Fudan University
Keyword ：
Alcohol Alcohol Base free Base free Ether synthesis Ether synthesis Transition-metal free Transition-metal free Yne-allylic substitution Yne-allylic substitution
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| GB/T 7714 | Xu, C. , Luo, Y. , Niu, S. et al. Transition-metal and base-free ether synthesis via alcohol-participated yne-allylic substitution [J]. | Green Synthesis and Catalysis , 2024 . |
| MLA | Xu, C. et al. "Transition-metal and base-free ether synthesis via alcohol-participated yne-allylic substitution" . | Green Synthesis and Catalysis (2024) . |
| APA | Xu, C. , Luo, Y. , Niu, S. , Gong, F. , Lan, S. , Luo, B. et al. Transition-metal and base-free ether synthesis via alcohol-participated yne-allylic substitution . | Green Synthesis and Catalysis , 2024 . |
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Flexible devices have shown great application potential in portable and miniaturized devices. However, work on flexible electrodes for capacitive deionization (CDI) has not been well developed due to the issues of desalination property, processability, and availability under actual bending conditions. Herein, we constructed a kind of flexible lamellar MXene membrane by assembling Ti3C2Tx sheets with both crumpled and perforated structures and studied their desalination performance in conventional planar and bent configurations. The crumpled and perforated features in Ti3C2Tx (C-P-TC) nanosheets could optimize the in-plane and out-of-plane diffusion channels of the stacked samples, respectively, effectively improving the accessibility of membranes. As a result, the desalination performance of such C-P-TC electrodes was superior to that of those assembled from crumpled or perforated sheets alone. Significantly, this flexible C-P-TC electrode still showed excellent performance at real bend deformation, which possessed not only almost the same CDI capacity as the traditional planar configuration but also good cycling stability. This work not merely proposes an alternative strategy to improve the CDI performance of lamellar MXene electrodes by regulating the nanostructures of channels but also confirms their effective deionization ability under real bent state, greatly facilitating the potential use of flexible electrodes in miniaturized CDI devices. © 2024
Keyword ：
Desalination Desalination Electrodes Electrodes Perforated plates Perforated plates
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| GB/T 7714 | Shang, Jing , Wang, Luhua , Cao, Jihui et al. Bendable, lamellar MXene membrane electrodes with diverse diffusion pathways for potential application in miniaturized capacitive deionization devices [J]. | Desalination , 2024 , 583 . |
| MLA | Shang, Jing et al. "Bendable, lamellar MXene membrane electrodes with diverse diffusion pathways for potential application in miniaturized capacitive deionization devices" . | Desalination 583 (2024) . |
| APA | Shang, Jing , Wang, Luhua , Cao, Jihui , Han, Shitong , Xu, Chao . Bendable, lamellar MXene membrane electrodes with diverse diffusion pathways for potential application in miniaturized capacitive deionization devices . | Desalination , 2024 , 583 . |
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Conjugated microporous polymers (CMPs) have been considered a type of promising visible-light-driven, organic photocatalysts. However, apart from designing high-performance CMPs from a molecular perspective, little attention is paid to improving the photocatalytic properties of these polymers through macrostructural regulation. Herein, we prepared a kind of hollow spherical CMPs involving carbazole monomers and studied their performance on the selective photocatalytic oxidation of benzyl alcohol under visible light irradiation. The results demonstrate that the introduction of a hollow spherical structure improves the physicochemical properties of the as-designed CMPs, including the specific surface areas, optoelectronic characteristics, as well as photocatalytic performance, etc. In particular, the hollow CMPs can more effectively oxidize benzyl alcohol compared to pristine ones under blue light illumination, and produce >1 mmol of benzaldehyde in 4.5 h with a yield of up to 9 mmol.g(-1).h(-1), which is almost 5 times higher than that of the pristine ones. Furthermore, such hollow architecture has a similar enhanced effect on the oxidation of some other aromatic alcohols. This work shows that the deliberate construction of specific macrostructures can better arouse the photocatalytic activity of the as-designed CMPs, which will contribute to the further use of these organic polymer semiconductors in photocatalysis areas. (c) 2023 Elsevier Inc. All rights reserved.
Keyword ：
Benzyl alcohol Benzyl alcohol Conjugated microporous polymers Conjugated microporous polymers Hollow spheres Hollow spheres Photocatalysis Photocatalysis Visible-light response Visible-light response
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| GB/T 7714 | Wei, Guanbao , Wang, Luhua , Ding, Zhengxin et al. Carbazole-involved conjugated microporous polymer hollow spheres for selective photocatalytic oxidation of benzyl alcohol under visible-light irradiation [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 642 : 648-657 . |
| MLA | Wei, Guanbao et al. "Carbazole-involved conjugated microporous polymer hollow spheres for selective photocatalytic oxidation of benzyl alcohol under visible-light irradiation" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 642 (2023) : 648-657 . |
| APA | Wei, Guanbao , Wang, Luhua , Ding, Zhengxin , Yuan, Rusheng , Long, Jinlin , Xu, Chao . Carbazole-involved conjugated microporous polymer hollow spheres for selective photocatalytic oxidation of benzyl alcohol under visible-light irradiation . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 642 , 648-657 . |
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Quaternary compound Cu2ZnSnX4 (X = S, Se) is of great interest to many researchers for photovoltaic appli-cations in recent years. In the present study, the first-principles calculations are performed to investigate the influence of cation substitution on the different physical properties of Cu2ZnSnS4 (CZTS) and Cu2ZnSnSe4 (CZTSe). The difference in stability between two Kesterite and Stannite structures is examined for each com-pound. The results show that the pristine Kesterite structure will be transformed into the Stannite structure when the Zn atoms are replaced by the Mg or Cd atoms. Our results are consistent well with the available literature. The mechanical stability of six compounds are proved and they are ductile materials. The allowed direct elec-tronic transition is found for all compounds at the Gamma point. The band gap variation is analyzed in detail. The band gaps calculated from hybrid functional PBE0 of the studied compounds can agree well with the experimental data. The suitable band gap values of 1.12 and 1.28 eV are obtained for Cu2MgSnSe4 (CMTSe) and Cu2CdSnS4 (CCTS) in single-junction solar cells, whereas the band gaps of Cu2MgSnS4 (CMTS, 1.70 eV) and Cu2CdSnSe4 (CCTSe, 0.77 eV) are too large or small. The band gap energy difference between two tetragonal structures is shown to be negligible for CMTS, CMTSe, CCTS, and CCTSe. Furthermore, the optical properties are compared, and CMTSe and CCTS show strong light absorption capacity from 300 to 800 nm. Our study indicates that both CMTSe and CCTS are the promising materials for solar cell applications.
Keyword ：
Cation substitution Cation substitution Cu2ZnSnX4 Cu2ZnSnX4 Electronic structure Electronic structure Optical properties Optical properties
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| GB/T 7714 | Liu, Diwen , Zhang, Qiqi , Xu, Chao et al. The structural, mechanical, and optoelectronic properties of Cu2-II-Sn-VI4 (II = Mg, Zn, Cd; VI = S, Se): A DFT study [J]. | MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING , 2023 , 154 . |
| MLA | Liu, Diwen et al. "The structural, mechanical, and optoelectronic properties of Cu2-II-Sn-VI4 (II = Mg, Zn, Cd; VI = S, Se): A DFT study" . | MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING 154 (2023) . |
| APA | Liu, Diwen , Zhang, Qiqi , Xu, Chao , Sa, Rongjian . The structural, mechanical, and optoelectronic properties of Cu2-II-Sn-VI4 (II = Mg, Zn, Cd; VI = S, Se): A DFT study . | MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING , 2023 , 154 . |
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Using solar photocatalytic CO2 reduction to produce high-value-added products is a promising solution to environmental problems caused by greenhouse gases. Metal phthalocyanine COFs possess a suitable band structure and strong light absorption ability, making them a promising candidate for photocatalytic CO2 reduction. However, the relationship between the electronic structure of these materials and photocatalytic properties, as well as the mechanism of photocatalytic CO2 reduction, is still unclear. Herein, the electronic structure of three MPc-TFPN-COFs (M = Ni, Co, Fe) and the reaction process of CO2 reduction to CO, HCOOH, HCHO and CH3OH were studied using DFT calculations. The calculated results demonstrate that these COFs have a good photo response to visible light and are new potential photocatalytic materials. Three COFs show different reaction mechanisms and selectivity in generating CO2 reduction products. NiPc-TFPN-COFs obtain CO through the reaction pathway of CO2 -> COOH -> CO, and the energy barrier of the rate-determining step is 2.82 eV. NiPc-TFPN-COFs and FePc-TFPN-COFs generate HCHO through CO2 -> COOH -> CO -> CHO -> HCHO, and the energy barrier of the rate step is 2.82 eV and 2.37 eV, respectively. Higher energies are required to produce HCOOH and CH3OH. This work is helping in understanding the mechanism of photocatalytic reduction of CO2 in metallophthalocyanine COFs. We elucidate the photocatalytic mechanism of CO2 reduction in metallophthalocyanine covalent organic frameworks through density functional theory calculations.
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| GB/T 7714 | Zhang, Qiqi , Chen, Meiyan , Zhang, Yanjie et al. Iron/cobalt/nickel regulation for efficient photocatalytic carbon dioxide reduction over phthalocyanine covalent organic frameworks [J]. | NANOSCALE , 2023 , 15 (39) : 16030-16038 . |
| MLA | Zhang, Qiqi et al. "Iron/cobalt/nickel regulation for efficient photocatalytic carbon dioxide reduction over phthalocyanine covalent organic frameworks" . | NANOSCALE 15 . 39 (2023) : 16030-16038 . |
| APA | Zhang, Qiqi , Chen, Meiyan , Zhang, Yanjie , Ye, Yuansong , Liu, Diwen , Xu, Chao et al. Iron/cobalt/nickel regulation for efficient photocatalytic carbon dioxide reduction over phthalocyanine covalent organic frameworks . | NANOSCALE , 2023 , 15 (39) , 16030-16038 . |
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Nanofiltration membrane-based molecular separation has become an indispensable technology for fine sieving processes. However, the difficulty in regulating the separation performance restricts the applicability of these nanofiltration membranes in different separation systems. Herein, we will show that the separation performance of Ti3C2Tx-MXene lamellar nanofiltration membranes on certain dye molecules can be modulated by employing external electrostatic fields. Specifically, for cationic dyes, the negative voltage applied to Ti3C2Tx lamellar nanofiltration membranes can improve their sieving abilities on dyes but reduce their water flux at the same time. On the contrary, a positive electric field will cause a decline in the retention capacities but improve the water flux of the membranes. Interestingly, when using anionic dye molecules as solute models, the filtration performance of the Ti3C2Tx membranes exhibits completely opposite variations to that of filtering cationic dyes, whether the applied electric field is negative or positive. The regulation mechanisms for the filtration performance of Ti3C2Tx membranes have been discussed, which are probably ascribed to the changes in the electrostatic interactions between dyes and Ti3C2Tx induced by the external electric field. Our findings indicate that the filtration performance of MXene lamellar membranes on both cationic and anionic dyes can be modulated by applying an external electric field, opening up enormous opportunities to use such electrified nanofiltration membranes in the field of membrane-based molecular separations.
Keyword ：
dye molecules dye molecules electrostatic modulation electrostatic modulation external electric field external electric field MXene MXene nanofiltration nanofiltration
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| GB/T 7714 | Li, Jing , Xu, Chao , Long, Jinlin et al. Lamellar MXene Nanofiltration Membranes for Electrostatic Modulation of Molecular Permeation: Implications for Fine Separation [J]. | ACS APPLIED NANO MATERIALS , 2022 , 5 (5) : 7373-7381 . |
| MLA | Li, Jing et al. "Lamellar MXene Nanofiltration Membranes for Electrostatic Modulation of Molecular Permeation: Implications for Fine Separation" . | ACS APPLIED NANO MATERIALS 5 . 5 (2022) : 7373-7381 . |
| APA | Li, Jing , Xu, Chao , Long, Jinlin , Ding, Zhengxin , Yuan, Rusheng , Li, Zhaohui . Lamellar MXene Nanofiltration Membranes for Electrostatic Modulation of Molecular Permeation: Implications for Fine Separation . | ACS APPLIED NANO MATERIALS , 2022 , 5 (5) , 7373-7381 . |
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Graphene-based membranes have been considered as promising separation membranes for water treatments due to their unique two-dimensional confined channels. However, subject to the preparation technology, the effective construction of graphene-based filtration membranes with suitable separation ability on heavy metal ions still face considerable challenges. Herein, we have successfully constructed a kind of graphene-based (reduced graphene oxide, rGO) nanofiltration membranes by adopting a plasma-assisted in-situ photocatalytic reduction method. Graphene oxide-Ag (GO-Ag) composite sheets are prepared firstly and then assembled into membranes by vacuum filtration. With the use of Ag nanoparticles as plasmonic photocatalyst, GO-Ag films can be in-situ reduced, leading to the formation of rGO-based composite membranes. Thanks to the mild in-situ reduction process, the filtration ability on heavy metal ions (Cr(VI), Cr3+, Cu2+ and Pb2+) caused by lamellar structure is well retained in the as-formed rGO-Ag membranes. Especially, when treating the typical toxic Cr(VI) solution, the retention capacity, water flux and stability of rGO-Ag membranes are all improved compared with that of the original GO-Ag ones. In addition, the effectively rejection of Cr(VI) from mixed solutions containing both Cr(VI) and Cr(III) also suggests the good applicability of such rGO-Ag membranes in a complex wastewater system.
Keyword ：
Graphene Graphene Heavy metal ion Heavy metal ion In-situ reduction In-situ reduction Nanofiltrati on membranes Nanofiltrati on membranes Plasmon Plasmon
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| GB/T 7714 | Han, Shitong , Li, Wenyue , Xi, Hailing et al. Plasma-assisted in-situ preparation of graphene-Ag nanofiltration membranes for efficient removal of heavy metal ions [J]. | JOURNAL OF HAZARDOUS MATERIALS , 2022 , 423 . |
| MLA | Han, Shitong et al. "Plasma-assisted in-situ preparation of graphene-Ag nanofiltration membranes for efficient removal of heavy metal ions" . | JOURNAL OF HAZARDOUS MATERIALS 423 (2022) . |
| APA | Han, Shitong , Li, Wenyue , Xi, Hailing , Yuan, Rusheng , Long, Jinlin , Xu, Chao . Plasma-assisted in-situ preparation of graphene-Ag nanofiltration membranes for efficient removal of heavy metal ions . | JOURNAL OF HAZARDOUS MATERIALS , 2022 , 423 . |
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Freestanding electrodes without the influences of additives have been considered as a kind of ideal electrode structure in the field of capacitive deionization (CDI). However, subjected to conductivity, available surface areas, hydrophilicity and etc., effectively construction of freestanding CDI electrodes with high water desalination performance still face great challenges. Herein, we will demonstrate a unique N-doped graphene freestanding porous membrane electrode with excellent water desalination performance. The preparation process mainly includes the assembly of core-shell composites with incomplete graphene oxide shells into bulk membranes using compression molding method and the heat-treatment under NH3 atmosphere. These reserved spherical shells with loopholes and N-doping make up the freestanding membrane electrodes with network porous architecture. The interconnected sphere shells efficiently improve the availability of surface and pores in the monolithic assembly, while the doping of nitrogen element further enhances the accessibility of graphene-based surface by the electrolyte. As a result, such graphene carbonaceous freestanding electrodes exhibit excellent water desalination performance with a high CDI capacity of about 21.8 mg/g in NaCI solution. Moreover, such freestanding membrane electrodes also possess good desalination abilities towards some other salts such as KCI, CaCl2 and MgCl2, suggesting their potential applications in complex brine solution. (C) 2021 Elsevier Ltd. All rights reserved.
Keyword ：
Capacitive deionization Capacitive deionization Freestanding porous membranes Freestanding porous membranes Graphene Graphene Interconnected pores Interconnected pores N-doping N-doping
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| GB/T 7714 | Zhang, Gujia , Li, Wenyue , Chen, Zhixin et al. Freestanding N-doped graphene membrane electrode with interconnected porous architecture for efficient capacitive deionization [J]. | CARBON , 2022 , 187 : 86-96 . |
| MLA | Zhang, Gujia et al. "Freestanding N-doped graphene membrane electrode with interconnected porous architecture for efficient capacitive deionization" . | CARBON 187 (2022) : 86-96 . |
| APA | Zhang, Gujia , Li, Wenyue , Chen, Zhixin , Long, Jinlin , Xu, Chao . Freestanding N-doped graphene membrane electrode with interconnected porous architecture for efficient capacitive deionization . | CARBON , 2022 , 187 , 86-96 . |
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