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学者姓名:汪颖
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This work proposes a sigma-pi hyperconjugation strategy to establish interlayer charge transport channels (CTC) in supramolecular organic nanostructures. A series of ullazine-based molecular semiconductors were designed and synthesized successfully by engineering end groups to demonstrate the sigma-pi hyperconjugation that unlocks the quantum confinement of photogenerated charges in pi-conjugated planes. Ullazine grafted with tert-butyl (U-t-Bu) showed a J-cross-stacking model in which the cross-stacked U-t-Bu molecular pair smoothly glides along the elongated dimension, forming a Z-schemed interlayer CTC by sigma-pi hyperconjugations between C-H sigma-bonds of tert-butyl end group and pi-bonds of ullazines in adjacent layers along the stacking dimension. Consequently, upon photoexcitation of ullazine-based supramolecular nanoaggregates in aqueous solution, the formed Frenkel excitons are dissociated to charge-separated excitons by the interlayer charge separation channels, undergoing an ultrafast charge transfer within 0.58 ps and an ultrafast charge separation within 0.67 ps. The Z-schemed charge separation between adjacent layers leads to a significantly enhanced hydrogen yield over U-t-Bu/PVP/Pt, with a hydrogen evolution rate of 369.9 mu molg-1h-1 and an apparent quantum yield of 1.46% at 420 nm. It is 3.8-fold larger than that of ullazine modified with methoxy (U-OMe), without the sigma-pi hyperconjugation.
Keyword :
exciton dynamics exciton dynamics HER HER hyperconjugation effect hyperconjugation effect photocatalysis photocatalysis supramolecule supramolecule
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GB/T 7714 | Yang, Qin , Li, Wanqing , Wang, Ying et al. σ-π Hyperconjugation Unlocks Interlayer Charge Separation of Ullazine-Based Supramolecular Nanostructures for Photocatalytic Hydrogen Evolution [J]. | ACS CATALYSIS , 2025 , 15 (4) : 3267-3275 . |
MLA | Yang, Qin et al. "σ-π Hyperconjugation Unlocks Interlayer Charge Separation of Ullazine-Based Supramolecular Nanostructures for Photocatalytic Hydrogen Evolution" . | ACS CATALYSIS 15 . 4 (2025) : 3267-3275 . |
APA | Yang, Qin , Li, Wanqing , Wang, Ying , Zhuang, Yan , Wu, Shuhong , Wang, Shuo et al. σ-π Hyperconjugation Unlocks Interlayer Charge Separation of Ullazine-Based Supramolecular Nanostructures for Photocatalytic Hydrogen Evolution . | ACS CATALYSIS , 2025 , 15 (4) , 3267-3275 . |
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The persistent threats posed by toxic chemical warfare agents (CWAs) such as mustard gas (bis(2-chloroethyl) sulfide, HD) and bacterial contaminants demand the development of innovative, sustainable mitigation strategies. Photocatalytic processes that generate reactive oxygen species (ROS) offer a promising dual-functional approach for both chemical detoxification and antibacterial defense. In this study, two structurally analogous covalent organic frameworks (COFs), BPY-COF and BD-COF, are synthesized using benzotrithiophene as the donor unit paired with bipyridine and biphenyl, respectively. These COFs exhibit high crystallinity, broad-spectrum light absorption, and efficient charge carrier transport, with BPY-COF demonstrating superior performance due to the incorporation of heteroatoms. BPY-COF achieved ultrafast detoxification of the mustard gas simulant 2-chloroethyl ethyl sulfide (CEES) with a half-life of 35 min and 100% selectivity for 2-chloroethyl sulfoxide (CEESO) under white LED light, outperforming BD-COF. Additionally, electrospun composite fibers containing 40 wt.% BPY-COF maintained comparable CEES degradation rates and exhibited over 99% antibacterial efficiency against Escherichia coli and Bacillus subtilis within 60 min. These findings highlight the potential of BPY-COF as a multifunctional photocatalyst for integrated applications in chemical detoxification and antibacterial defense, addressing critical challenges in public health and safety.
Keyword :
antibacterial antibacterial charge transfer charge transfer covalent organic frameworks covalent organic frameworks photocatalytic degradation photocatalytic degradation
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GB/T 7714 | Zhu, Yongchao , Qin, Liyang , Yang, Mingyuan et al. Dual-Functional Benzotrithiophene-Based Covalent Organic Frameworks for Photocatalytic Detoxification of Mustard Gas Simulants and Antibacterial Defense [J]. | SMALL , 2025 , 21 (12) . |
MLA | Zhu, Yongchao et al. "Dual-Functional Benzotrithiophene-Based Covalent Organic Frameworks for Photocatalytic Detoxification of Mustard Gas Simulants and Antibacterial Defense" . | SMALL 21 . 12 (2025) . |
APA | Zhu, Yongchao , Qin, Liyang , Yang, Mingyuan , Shi, Zhicheng , Chen, Hongxuan , Wen, Na et al. Dual-Functional Benzotrithiophene-Based Covalent Organic Frameworks for Photocatalytic Detoxification of Mustard Gas Simulants and Antibacterial Defense . | SMALL , 2025 , 21 (12) . |
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H2 and O2 evolutions occur simultaneously for conventional particulate photocatalytic overall water splitting (PPOWS), leading to a significant backward reaction and the formation of an explosive H2/O2 gas mixture. This is an issue that must be addressed prior to industrialization of PPOWS. Here, a convenient, cost-effective, and scalable concept is introduced to uncouple hydrogen and oxygen production for PPOWS. Based on this idea, a three-component photocatalyst, Co(5 %)-HPCN/(rGO/Pt), is constructed, consisting of a photoresponsive chip (HPCN), a H2 evolution cocatalyst (rGO/Pt), and a cobalt complex capable of reversibly binding O2 (Co), to achieve the decoupling of PPOWS under alternating UV and visible light irradiations. The asynchronous O2 and H2 evolution strategy have considerable flexibility regarding the photocatalyst structure and light sources suitable for PPOWS.
Keyword :
carbon nitride chips carbon nitride chips overall water splitting overall water splitting photocatalytic photocatalytic PPOWS decoupling PPOWS decoupling reaction mechanism reaction mechanism
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GB/T 7714 | Liu, Dan , Xu, Huihui , Shen, Jinni et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
MLA | Liu, Dan et al. "Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 9 (2025) . |
APA | Liu, Dan , Xu, Huihui , Shen, Jinni , Wang, Xun , Qiu, Chengwei , Lin, Huaxiang et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
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Bacterial infections are a major public health challenge around the world. The development of novel surface coatings that effectively inhibit bacterial adhesion, proliferation and growth is a critical step in addressing this global challenge. Photocatalytic antibacterial therapy has proven to be an effective approach and has received increasing attention. However, it is still a challenge to obtain coatings with both antibacterial adhesion and durable photocatalytic antibacterial functions. Herein, an acridine-based coating with antibacterial adhesion and photocatalytic antibacterial properties was prepared by simple methods (i.e., spin-coating, spray-coating, and drop-coating) and can be applied to various substrates. The bacterial anti-adhesion test results showed that the coating could effectively prevents the adhesion of Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), and Pseudomonas aeruginosa (P. aeruginosa), indicating the strong anti-fouling capability. The acridine-based coating demonstrated durable photocatalytic antimicrobial activity, remaining 99.3 % antibacterial effective against all three bacterial strains even after 30 days exposed to visible light. The coating can significantly reduce or eliminate the risk of contamination and cross-contamination, making it ideal for use in public healthcare environments.
Keyword :
Antibacterial Antibacterial Anti-fouling Anti-fouling Coating Coating Photocatalytic Photocatalytic
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GB/T 7714 | Kang, Linfeng , Peng, Houqian , Yang, Mingyuan et al. Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial [J]. | PROGRESS IN ORGANIC COATINGS , 2024 , 194 . |
MLA | Kang, Linfeng et al. "Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial" . | PROGRESS IN ORGANIC COATINGS 194 (2024) . |
APA | Kang, Linfeng , Peng, Houqian , Yang, Mingyuan , Hu, Ke , Lin, Yihui , Zhu, Yongchao et al. Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial . | PROGRESS IN ORGANIC COATINGS , 2024 , 194 . |
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Converting clean solar energy into chemical energy through artificial photosynthesis is an effective solution to solve the energy and environmental issues. Here, we report a Cs3Bi2Br9/Bi2WO6 (CBB/BWO) Z-scheme heterojunction constructed via electrostatic self-assembly, which facilitates efficient separation of photogenerated carriers and ensures the corresponding redox capacity of both components. By sharing Bi atoms, a Br-Bi-O bond is established between CBB and BWO, serving as an "electron bridge". The electrons generated by BWO are efficiently channeled to CBB through the heterojunction-formed "electron bridge", thereby achieving effective photocatalytic CO2 reduction. Under simulated sunlight conditions, it exhibits the highest CO yield of 72.52 mu mol g(-1) (without the addition of any precious metal, photosensitizers or sacrifices), which is approximately 7-fold and 18-fold greater than that of pure CBB and BWO, respectively. This work provides a more profound comprehension of the regulation of electron transfer through interfacial chemical bonds, thereby proposing a promising strategy for the development of efficient heterojunction photocatalysts for CO2 photoreduction.
Keyword :
Bi2WO6 Bi2WO6 CO2 reduction CO2 reduction Perovskite Perovskite Photocatalysis Photocatalysis Z-scheme Z-scheme
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GB/T 7714 | Liu, Haolan , Sun, Jingjing , Lin, Qianying et al. An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction [J]. | CHEMCATCHEM , 2024 , 16 (22) . |
MLA | Liu, Haolan et al. "An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction" . | CHEMCATCHEM 16 . 22 (2024) . |
APA | Liu, Haolan , Sun, Jingjing , Lin, Qianying , Wang, Ying , Wang, Shuo , Wang, Shuowen et al. An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction . | CHEMCATCHEM , 2024 , 16 (22) . |
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Efficient photocatalytic reduction of CO2 to high-calorific-value CH4, an ideal target product, is a blueprint for C-1 industry relevance and carbon neutrality, but it also faces great challenges. Herein, we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst, which are prepared via a facile impregnation-reduction method, featuring an optimized local electronic structure. It exhibits a superior photocatalytic carbon-based products yield of 30.0 mu mol g(-1) h(-1) and achieves a record CH4 selectivity of up to 94.3%, which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity. Specifically, the synergistic effects of directional migration of photogenerated electrons and strong pi-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO2 -> CH4 pathway. This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.
Keyword :
artificial synthesis of CH4 artificial synthesis of CH4 electronic structure optimization electronic structure optimization Fe species cocatalyst Fe species cocatalyst photocatalytic CO2 reduction photocatalytic CO2 reduction SiC SiC
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GB/T 7714 | Lin, Qianying , Zhao, Jiwu , Zhang, Pu et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation [J]. | CARBON ENERGY , 2024 , 6 (1) . |
MLA | Lin, Qianying et al. "Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation" . | CARBON ENERGY 6 . 1 (2024) . |
APA | Lin, Qianying , Zhao, Jiwu , Zhang, Pu , Wang, Shuo , Wang, Ying , Zhang, Zizhong et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation . | CARBON ENERGY , 2024 , 6 (1) . |
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Photocatalytic CO2 reduction reaction (CO2RR) is a desired solution to overcome current energy and environmental problems. As a main competitive reaction, hydrogen evolution reaction (HER) urgently needs to be restrained to improve the conversion rate and selectivity of CO2RR. Here, we report a Cu2O/MXene-g-C3N4 (Cu2O/MX-CN) p-n heterojunction that achieves highly selective CO2 reduction of 93% (competing with HER) under visible light. CO is the only product of CO2RR, which yielded 28.4 mu mol g(-1) h(-1). The introduction of Ti3C2 MXene in g-C3N4 promotes the energy of photoelectrons and the transport efficiency of photogenerated carriers at the p-n heterojunction interface via hot electron injection induced by the localized surface plasmonic resonance (LSPR) and band structure regulation. Meanwhile, apart from the component of p-n heterojunction, Cu2O also acts as the adsorption site of CO2, inhibiting HER by blocking the adsorption of protons. This study provides a novel strategy to fabricate multifunctional composite for efficient and highly selective CO2 reduction.
Keyword :
CO2 Reduction CO2 Reduction Cu2O Cu2O G-C3N4 G-C3N4 Photocatalysis Photocatalysis Ti3C2 MXene Ti3C2 MXene
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GB/T 7714 | Gao, Yuan , Wang, Ying , Sun, Ruihong et al. Interfacial hot electron injection in Cu2O/MXene-g-C3N4 p-n heterojunction for efficient photocatalytic CO2 reduction [J]. | COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS , 2024 , 684 . |
MLA | Gao, Yuan et al. "Interfacial hot electron injection in Cu2O/MXene-g-C3N4 p-n heterojunction for efficient photocatalytic CO2 reduction" . | COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS 684 (2024) . |
APA | Gao, Yuan , Wang, Ying , Sun, Ruihong , Luo, Yining , Xin, Liantao , Wang, Debao . Interfacial hot electron injection in Cu2O/MXene-g-C3N4 p-n heterojunction for efficient photocatalytic CO2 reduction . | COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS , 2024 , 684 . |
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Polypropylene (PP) nonwovens have been widely used in disposable protective masks and protective clothing, which are essential to protect healthcare workers from highly infectious diseases such as COVID-19. However, realizing the disinfection reusable function of PP nonwovens to reduce carbon emission or white waste pollution after extensive use has been still a great challenge. Herein, Durable Antimicrobial and Anti-fungal Post-disinfection polypropylene nonwovens were developed by co-grafting of Triclosan and Chitosan. The antibacterial performance test results showed that the as-prepared co-grafted polypropylene nonwoven has a > 99.9% of antimicrobial efficiency against E. coli, S. aureus as well as multi-drug-resistant P. aeruginosa, and the excellent anti-fungal performance against fungus (C. albicans) and mold (A. niger). Moreover, it retained excellent Antimicrobial and Anti-fungal Properties after disinfection 3 times with boiling water, 40 x diluted 84 disinfectant and 75% alcohol for 5 min. This work provided ideas for developing more effective pathogen protection and longer-lasting personal protective equipment to reduce the environmental impact of medical masks and personal protective equipment in terms of energy consumption, carbon emissions and waste generation.
Keyword :
Antibacterial Antibacterial Anti-fungal Anti-fungal Polypropylene nonwovens Polypropylene nonwovens UV irradiation modification UV irradiation modification
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GB/T 7714 | Hu, Ke , Chen, Hongxuan , Lin, Yihui et al. Synthesis and Durable Antimicrobial and Anti-fungal Properties of Triclosan and Chitosan Co-grafted Polypropylene Nonwovens [J]. | FIBERS AND POLYMERS , 2024 , 25 (11) : 4245-4256 . |
MLA | Hu, Ke et al. "Synthesis and Durable Antimicrobial and Anti-fungal Properties of Triclosan and Chitosan Co-grafted Polypropylene Nonwovens" . | FIBERS AND POLYMERS 25 . 11 (2024) : 4245-4256 . |
APA | Hu, Ke , Chen, Hongxuan , Lin, Yihui , Han, Shitong , Wang, Qi , Peng, Houqian et al. Synthesis and Durable Antimicrobial and Anti-fungal Properties of Triclosan and Chitosan Co-grafted Polypropylene Nonwovens . | FIBERS AND POLYMERS , 2024 , 25 (11) , 4245-4256 . |
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This work introduces a new strategy of a single-atom nest catalyst, whereby several single atoms are positioned closely, aiming to achieve the dual benefits of high atom-utilization efficiency while avoiding the steric hindrance in the coupling reaction. As a proof of concept, Pt single-atom nests, where the adjacent Pt single atoms are approximately 4 & Aring; apart, are precisely engineered on the TiO2 photocatalyst for photocatalytic non-oxidative coupling of methane. The Pt single-atom nest photocatalyst demonstrates remarkable activity, achieving a C2H6 yield and turnover frequency of 251.6 mu mol g(cat)(-1) h(-1) and 20 h(-1), respectively, representing a 3.2-fold improvement compared to the Pt single-atom photocatalyst. Density functional theory calculations reveal that the Pt single-atom nest can significantly decrease the energy barrier for the activation of both CH4 molecules in the coupling process.
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GB/T 7714 | Zhang, Pu , Li, Junwei , Huang, Haowei et al. Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (34) : 24150-24157 . |
MLA | Zhang, Pu et al. "Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146 . 34 (2024) : 24150-24157 . |
APA | Zhang, Pu , Li, Junwei , Huang, Haowei , Sui, Xiaoyu , Zeng, Haihua , Lu, Haijiao et al. Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (34) , 24150-24157 . |
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Covalent organic frameworks (COFs) are promising materials for converting solar energy into green hydrogen. However, limited charge separation and transport in COFs impede their application in the photocatalytic hydrogen evolution reaction (HER). In this study, the intrinsically tunable internal bond electric field (IBEF) at the imine bonds of COFs was manipulated to cooperate with the internal molecular electric field (IMEF) induced by the donor-acceptor (D-A) structure for an efficient HER. The aligned orientation of IBEF and IMEF resulted in a remarkable H-2 evolution rate of 57.3 mmol center dot g(-1)center dot h(-1) on TNCA, which was approximately 520 times higher than that of TCNA (0.11 mmol center dot g(-1)center dot h(-1)) with the opposing electric field orientation. The superposition of the dual electric fields enables the IBEF to function as an accelerating field for electron transfer, kinetically facilitating the migration of photogenerated electrons from D to A. Furthermore, theoretical calculations indicate that the inhomogeneous charge distribution at the C and N atoms in TNCA not only provides a strong driving force for carrier transfer but also effectively hinders the return of free electrons to the valence band, improving the utilization of photoelectrons. This strategy of fabricating dual electric fields in COFs offers a novel approach to designing photocatalysts for clean energy synthesis. (c) 2024, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
Keyword :
Covalent organic framework Covalent organic framework Hydrogen evolution Hydrogen evolution Internal bond electric field Internal bond electric field Internal molecular electric field Internal molecular electric field Photocatalysis Photocatalysis
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GB/T 7714 | Li, Chao , Wang, Shuo , Liu, Yuan et al. Superposition of dual electric fields in covalent organic frameworks for efficient photocatalytic hydrogen evolution [J]. | CHINESE JOURNAL OF CATALYSIS , 2024 , 63 : 164-175 . |
MLA | Li, Chao et al. "Superposition of dual electric fields in covalent organic frameworks for efficient photocatalytic hydrogen evolution" . | CHINESE JOURNAL OF CATALYSIS 63 (2024) : 164-175 . |
APA | Li, Chao , Wang, Shuo , Liu, Yuan , Huang, Xihe , Zhuang, Yan , Wu, Shuhong et al. Superposition of dual electric fields in covalent organic frameworks for efficient photocatalytic hydrogen evolution . | CHINESE JOURNAL OF CATALYSIS , 2024 , 63 , 164-175 . |
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