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学者姓名：陈雄
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Abstract ：
Covalent organic polymer (COP) thin film-based memristors have generated intensive research interest, but the studies are still in their infancy. Herein, by controlling the content of hydroxyl groups in the aldehyde monomer, Py-COP thin films with different electronic push-pull effects were fabricated bearing distinct memory performances, where the films were prepared by the solid-liquid interface method on the ITO substrates and further fabricated as memory devices with ITO/Py-COPs/Ag architectures. The Py-COP-1-based memory device only exhibited binary memory behavior with an ON/OFF ratio of 1:101.87. In contrast, the device based on Py-COP-2 demonstrated ternary memory behavior with an ON/OFF ratio of 1:100.6:103.1 and a ternary yield of 55%. The ternary memory mechanism of the ITO/Py-COP-2/Ag memory device is most likely due to the combination of the trapping of charge carriers and conductive filaments. Interestingly, the Py-COPs-based devices can successfully emulate the synaptic potentiation/depression behavior, clarifying the programmability of these devices in neuromorphic systems. These results suggest that the electronic properties of COPs can be precisely tuned at the molecular level, which provides a promising route for designing multi-level memory devices. © 2024
Keyword ：
Covalent organic polymers Covalent organic polymers Memristor Memristor Multi-level memory Multi-level memory Push-pull effects Push-pull effects
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| GB/T 7714 | Zhou, P. , Yu, H. , Chee, M.Y. et al. Electron push-pull effects induced performance promotion in covalent organic polymer thin films-based memristor for neuromorphic application [J]. | Chinese Chemical Letters , 2024 , 35 (5) . |
| MLA | Zhou, P. et al. "Electron push-pull effects induced performance promotion in covalent organic polymer thin films-based memristor for neuromorphic application" . | Chinese Chemical Letters 35 . 5 (2024) . |
| APA | Zhou, P. , Yu, H. , Chee, M.Y. , Zeng, T. , Jin, T. , Wu, S. et al. Electron push-pull effects induced performance promotion in covalent organic polymer thin films-based memristor for neuromorphic application . | Chinese Chemical Letters , 2024 , 35 (5) . |
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The burgeoning field of conjugated microporous polymers (CMPs) has generated widespread interest due to their potential as photocatalysts for hydrogen production from water. Nevertheless, their photocatalytic performance is sometimes hindered by inadequate charge separation and transfer, coupled with rapid charge recombination. Herein, a strategy to enhance photocatalytic performance via the customization of pi-bridges through the modulation of heteroatoms in a series of donor-pi-acceptor (D-pi-A) CMPs is proposed. This affords optimized energy levels and improved charge separation and transfer, thus boosting photocatalytic efficiency. Among various heteroatom substitutions, S-doped CMP (10 mg) demonstrates the highest photocatalytic hydrogen evolution rate of 203 mu mol h(-1) (AQY(450nm) = 7.4%) under visible light irradiation. Subsequent experimental analysis reveals its superior photocatalytic performance can be largely related to its minimized exciton binding energy, facilitated charge transfer efficiency, and impeded charge recombination among these heteroatom-doped D-pi-A CMPs. This research paves the way for the rational design and modification of organic semiconductors for advanced solar-driven photocatalysis by promoting charge separation and transfer.
Keyword ：
conjugated microporous polymers conjugated microporous polymers D-pi-A D-pi-A hydrogen evolution hydrogen evolution photocatalysis photocatalysis
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| GB/T 7714 | Li, Chunlei , Xu, Hetao , Xiong, Hao et al. Π-Bridge Modulations in D-π-A Conjugated Microporous Polymers to Facilitate Charge Separation and Transfer Kinetics for Efficient Photocatalysis [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 . |
| MLA | Li, Chunlei et al. "Π-Bridge Modulations in D-π-A Conjugated Microporous Polymers to Facilitate Charge Separation and Transfer Kinetics for Efficient Photocatalysis" . | ADVANCED FUNCTIONAL MATERIALS (2024) . |
| APA | Li, Chunlei , Xu, Hetao , Xiong, Hao , Xia, Shuling , Peng, Xu , Xu, Fei et al. Π-Bridge Modulations in D-π-A Conjugated Microporous Polymers to Facilitate Charge Separation and Transfer Kinetics for Efficient Photocatalysis . | ADVANCED FUNCTIONAL MATERIALS , 2024 . |
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The integration of electron donor (D) and acceptor (A) units into covalent organic frameworks (COFs) has received increasing interest due to its potential for efficient photocatalytic hydrogen (H2) evolution from water. Nevertheless, the advancement of D–A COFs is still constrained by the limited investigations on acceptor engineering, which enables the highly effective charge transfer pathways in COFs to deliver photoexcited electrons in a preferential orientation to enhance photocatalytic performance. Herein, two systems with D–A and D–A–A configurations based on the acceptor molecular engineering strategy are proposed to construct three distinct COFs. Specifically, TAPPy-DBTDP-COF merging one pyrene-based donor and two benzothiadiazole acceptors realized an average H2 evolution rate of 12.7 mmol h−1 g−1 under visible light, among the highest ever reported for typical D–A-type COF systems. The combination of experimental and theoretical analysis signifies the crucial role of the dual-acceptor arrangement in promoting exciton dissociation and carrier migration. These findings underscore the significant potential of D–A–A structural design, which is conducive to the efficient separation of photoexcited electrons and holes resulting in superior photocatalytic activities. © 2024 Wiley-VCH GmbH.
Keyword ：
covalent organic frameworks covalent organic frameworks donor-acceptor COFs donor-acceptor COFs H2 evolution H2 evolution photocatalysis photocatalysis
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| GB/T 7714 | Liu, N. , Xie, S. , Huang, Y. et al. Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution [J]. | Advanced Energy Materials , 2024 . |
| MLA | Liu, N. et al. "Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution" . | Advanced Energy Materials (2024) . |
| APA | Liu, N. , Xie, S. , Huang, Y. , Lu, J. , Shi, H. , Xu, S. et al. Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution . | Advanced Energy Materials , 2024 . |
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Memristors are essential components of neuromorphic systems that mimic the synaptic plasticity observed in biological neurons. In this study, a novel approach employing one-dimensional covalent organic framework (1D COF) films was explored to enhance the performance of memristors. The unique structural and electronic properties of two 1D COF films (COF-4,4 '-methylenedianiline (MDA) and COF-4,4 '-oxydianiline (ODA)) offer advantages for multilevel resistive switching, which is a key feature in neuromorphic computing applications. By further introducing a TiO2 layer on the COF-ODA film, a built-in electric field between the COF-TiO2 interfaces could be generated, demonstrating the feasibility of utilizing COFs as a platform for constructing memristors with tunable resistive states. The 1D nanochannels of these COF structures contributed to the efficient modulation of electrical conductance, enabling precise control over synaptic weights in neuromorphic circuits. This study also investigated the potential of these COF-based memristors to achieve energy-efficient and high-density memory devices. The unique structural and electronic properties of two one-dimensional (1D) covalent organic frameworks (COFs), namely COF-MDA and COF-ODA, were rationally designed to assess their capabilities in multilevel memory devices. This study further explored the potential of these COF-based memristors in realizing energy-efficient and high-density memory devices, and also showcased their potential for neuromorphic applications for the first time. image
Keyword ：
Image recognition Image recognition Memristors Memristors Multilevel memory device Multilevel memory device Neuromorphic computing Neuromorphic computing One-dimensional covalent organic framework One-dimensional covalent organic framework
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| GB/T 7714 | Zhou, Pan-Ke , Li, Yiping , Zeng, Tao et al. One-Dimensional Covalent Organic Framework-Based Multilevel Memristors for Neuromorphic Computing [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (20) . |
| MLA | Zhou, Pan-Ke et al. "One-Dimensional Covalent Organic Framework-Based Multilevel Memristors for Neuromorphic Computing" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 20 (2024) . |
| APA | Zhou, Pan-Ke , Li, Yiping , Zeng, Tao , Chee, Mun Yin , Huang, Yuxing , Yu, Ziyue et al. One-Dimensional Covalent Organic Framework-Based Multilevel Memristors for Neuromorphic Computing . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (20) . |
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The artificial photosynthesis of H2O2 from water and oxygen using semiconductor photocatalysts is attracting increasing levels of attention owing to its green, environmentally friendly, and energy-saving characteristics. Although covalent organic frameworks (COFs) are promising materials for promoting photocatalytic H2O2 production owing to their structural and functional diversity, they typically suffer from low charge-generation and -transfer efficiencies as well as rapid charge recombination, which restricts their use as catalysts for photocatalytic H2O2 production. Herein, we report a strategy for anchoring vinyl moieties to a COF skeleton to facilitate charge separation and migration, thereby promoting photocatalytic H2O2 generation. This vinyl-group-bearing COF photocatalyst exhibits a H2O2 -production rate of 84.5 mu mol h(-1) (per 10 mg), which is ten-times higher than that of the analog devoid of vinyl functionality and superior to most reported COF photocatalysts. Both experimental and theoretical studies provide deep insight into the origin of the improved photocatalytic performance. These findings are expected to facilitate the rational design and modification of organic semiconductors for use in photocatalytic applications.
Keyword ：
Charge separation Charge separation Covalent organic frameworks Covalent organic frameworks H2O2 production H2O2 production Photocatalysts Photocatalysts Vinyl groups Vinyl groups
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| GB/T 7714 | Yu, Hong , Zhang, Fengtao , Chen, Qian et al. Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
| MLA | Yu, Hong et al. "Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024) . |
| APA | Yu, Hong , Zhang, Fengtao , Chen, Qian , Zhou, Pan-Ke , Xing, Wandong , Wang, Sibo et al. Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
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Photocatalytic synthesis of H2O2 is an advantageous and ecologically sustainable alternative to the conventional anthraquinone process. However, achieving high conversion efficiency without sacrificial agents remains a challenge. In this study, two covalent organic frameworks (COF-O and COF-C) were prepared with identical skeletal structures but with their pore walls anchored to different alkyl chains. They were used to investigate the effect of the chemical microenvironment of pores on photocatalytic H2O2 production. Experimental results reveal a change of hydrophilicity in COF-O, leading to suppressed charge recombination, diminished charge transfer resistance, and accelerated interfacial electron transfer. An apparent quantum yield as high as 10.3 % (lambda=420 nm) can be achieved with H2O and O-2 through oxygen reduction reaction. This is among the highest ever reported for polymer photocatalysts. This study may provide a novel avenue for optimizing photocatalytic activity and selectivity in H2O2 generation.
Keyword ：
Hydrazone-lined covalent organic frameworks Hydrazone-lined covalent organic frameworks Microenvironment modulation Microenvironment modulation Photocatalytic H2O2 production Photocatalytic H2O2 production Selectivity Selectivity
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| GB/T 7714 | Xie, Zhipeng , Chen, Xiong , Wang, Wenbin et al. Variation of Chemical Microenvironment of Pores in Hydrazone-Linked Covalent Organic Frameworks for Photosynthesis of H2O2 [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (39) . |
| MLA | Xie, Zhipeng et al. "Variation of Chemical Microenvironment of Pores in Hydrazone-Linked Covalent Organic Frameworks for Photosynthesis of H2O2" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 39 (2024) . |
| APA | Xie, Zhipeng , Chen, Xiong , Wang, Wenbin , Ke, Xiating , Zhang, Xirui , Wang, Sibo et al. Variation of Chemical Microenvironment of Pores in Hydrazone-Linked Covalent Organic Frameworks for Photosynthesis of H2O2 . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (39) . |
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Despite the pivotal role of molecular oxygen (O-2) activation in artificial photosynthesis, the activation efficiency is often restricted by sluggish exciton dissociation and charge transfer kinetics within polymer photocatalysts. Herein, we propose two tetrathiafulvalene (TTF)-based imine-linked covalent organic frameworks (COFs) with tailored donor-acceptor (D-A) structures, TTF-PDI-COF and TTF-TFPP-COF, to promote O-2 activation. Because of enhanced electron push-pull interactions that facilitated charge separation and transfer behavior, TTF-PDI-COF exhibited superior photocatalytic activity in electron-induced O-2 activation reactions over TTF-TFPP-COF under visible light irradiation, including the photosynthesis of (E)-3-amino-2-thiocyano-alpha,beta-unsaturated compounds and H2O2. These findings highlight the significant potential of the rational design of COFs with D-A configurations as suitable candidates for advanced photocatalytic applications.
Keyword ：
Covalent organic frameworks Covalent organic frameworks Donor-acceptor polymers Donor-acceptor polymers H2O2 production H2O2 production Molecular oxygen activation Molecular oxygen activation Photocatalysis Photocatalysis
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| GB/T 7714 | Xu, Hetao , Xia, Shuling , Li, Chunlei et al. Programming Tetrathiafulvalene-Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
| MLA | Xu, Hetao et al. "Programming Tetrathiafulvalene-Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 29 (2024) . |
| APA | Xu, Hetao , Xia, Shuling , Li, Chunlei , Li, Yang , Xing, Wandong , Jiang, Yi et al. Programming Tetrathiafulvalene-Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
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Conjugated polymers (CPs) represent a promising platform for photocatalytic CO2 fixation owing to their suitable band structures that meet the requirements of the reduction potential of CO2 to value-added fuels. However, the photocatalytic performance of CPs is rather restrained by the low charge transfer efficiency. Herein, we rationally designed three CPs with a more delocalized electronic transmission channel and planar molecular structure, which are regarded to evidently reduce the exciton binding energy (E-b) and accelerate the internal charge transfer process. Besides, the assembly of suitable electron-output "tentacles" and cocatalysts on the surface of CPs could effectively facilitate interfacial electron delivery. Accordingly, the optimal P-2CN exhibits an apparent quantum yield of 4.6% at 420 nm for photocatalytic CO2 to CO. Further adjusting the amounts of cyano groups and cocatalysts, the CO selectivity could be obtained in the range of 08-0.5%.
Keyword ：
CO2 Reduction CO2 Reduction Conjugated Polymer Conjugated Polymer Electronic Transmission Channel Electronic Transmission Channel Molecular Design Molecular Design Photocatalysis Photocatalysis
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| GB/T 7714 | Chi, Xu , Lan, Zhi-An , Chen, Qian et al. Electronic Transmission Channels Promoting Charge Separation of Conjugated Polymers for Photocatalytic CO2 Reduction with Controllable Selectivity [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
| MLA | Chi, Xu et al. "Electronic Transmission Channels Promoting Charge Separation of Conjugated Polymers for Photocatalytic CO2 Reduction with Controllable Selectivity" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 22 (2023) . |
| APA | Chi, Xu , Lan, Zhi-An , Chen, Qian , Zhang, Xirui , Chen, Xiong , Zhang, Guigang et al. Electronic Transmission Channels Promoting Charge Separation of Conjugated Polymers for Photocatalytic CO2 Reduction with Controllable Selectivity . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
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In this paper, two types of conjugated, triazine-based covalent organic frameworks (COFs) with different connected linkages (imine bond and sp(2)-carbon-CN bond) are presented. The insignificant difference in the linkages creates a remarkable difference in their performance in visible-light-driven hydrogen generation. The fully pi-conjugated two-dimensional (2D) COF with sp(2)-carbon-CN linkages showed an external quantum efficiency of 13.48% at 450 nm, which is an unprecedented result for COF photocatalysts. In contrast, the imine-linked 2D COF displayed almost no photoactivity. Further photoelectrochemical and quantum chemical studies provide an in-depth understanding of the catalytic mechanism. This finding provides new insight into preparing high-performance organic photocatalysts for solar energy conversion.
Keyword ：
covalent organic frameworks covalent organic frameworks photocatalytic hydrogen generation photocatalytic hydrogen generation pi-conjugated system pi-conjugated system triazine triazine
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| GB/T 7714 | Liu, Hui , Wang, Danbo , Yu, Zefang et al. Fully conjugated two-dimensional sp(2)-carbon covalent organic frameworks for efficient photocatalytic hydrogen generation [J]. | SCIENCE CHINA-MATERIALS , 2023 , 66 (6) : 2283-2289 . |
| MLA | Liu, Hui et al. "Fully conjugated two-dimensional sp(2)-carbon covalent organic frameworks for efficient photocatalytic hydrogen generation" . | SCIENCE CHINA-MATERIALS 66 . 6 (2023) : 2283-2289 . |
| APA | Liu, Hui , Wang, Danbo , Yu, Zefang , Chen, Yajing , Li, Xubing , Zhang, Ruiling et al. Fully conjugated two-dimensional sp(2)-carbon covalent organic frameworks for efficient photocatalytic hydrogen generation . | SCIENCE CHINA-MATERIALS , 2023 , 66 (6) , 2283-2289 . |
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Covalent organic polymers (COPs) have emerged as a promising class of materials for memory devices due to their unique electronic properties and potential for tunability. This review highlights recent advances in the field of COPs-based thin films for memory applications, with a focus on the synthesis and characterization of COP thin films, their electronic properties, and their performance as memory devices. The potential of COPs-based thin films as flexible memory devices is also discussed. Overall, the recent progress in COPs-based thin films for memory applications suggests that these materials may have a significant impact on the development of next-generation memory technologies.
Keyword ：
covalent organic polymers covalent organic polymers memory device memory device memristors memristors resistive random-access memory resistive random-access memory thin films thin films
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| GB/T 7714 | Zhou, Pan-Ke , Yu, Hongling , Li, Yiping et al. Recent advances in covalent organic polymers-based thin films as memory devices [J]. | JOURNAL OF POLYMER SCIENCE , 2023 , 62 (8) : 1536-1553 . |
| MLA | Zhou, Pan-Ke et al. "Recent advances in covalent organic polymers-based thin films as memory devices" . | JOURNAL OF POLYMER SCIENCE 62 . 8 (2023) : 1536-1553 . |
| APA | Zhou, Pan-Ke , Yu, Hongling , Li, Yiping , Yu, Hong , Chen, Qian , Chen, Xiong . Recent advances in covalent organic polymers-based thin films as memory devices . | JOURNAL OF POLYMER SCIENCE , 2023 , 62 (8) , 1536-1553 . |
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