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学者姓名：李留义
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Abstract ：
Covalent organic frameworks (COFs) with excellent structural tunability have emerged as fascinating photocatalysts to fulfill future energy demands. Here, we developed a COFs heterostructure by assembling two COFs for photocatalytic overall water splitting. The resulting heterostructure exhibited an effective spatial separation of photoredox sites originating from the efficient separation of photoinduced charge carriers through an orientated interfacial electron transfer pathway. Accordingly, the heterostructure of the COFs displays excellent activity for stoichiometric water splitting into H-2 and O-2 under 5 W white LED light irradiation. Our efficiencies of H-2 and O-2 evolution rates up to 120 and 58 mu mol g(-1) h(-1) are significantly higher than those reported previously. The combination of experiments and theoretical calculations shows that water oxidation proceeds by a metal-free hydration-mediated pathway. This work sheds light on a rational design of the COF heterostructure with spatially separated photoredox for water splitting.
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| GB/T 7714 | Niu, Qing , Chen, Wei , Pan, Guodong et al. Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting [J]. | ACS MATERIALS LETTERS , 2024 , 6 (4) : 1411-1417 . |
| MLA | Niu, Qing et al. "Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting" . | ACS MATERIALS LETTERS 6 . 4 (2024) : 1411-1417 . |
| APA | Niu, Qing , Chen, Wei , Pan, Guodong , Li, Liuyi , Yu, Yan , Bi, Jinhong et al. Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting . | ACS MATERIALS LETTERS , 2024 , 6 (4) , 1411-1417 . |
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Abstract ：
Covalent organic frameworks (COFs) are promising semiconductor photocatalysts but are still limited in overall water splitting mainly owing to a lack of clear design approaches with which to ameliorate catalytic activities. Here, we demonstrate a synergy of exciton dipole orientation and dynamic reactivity of COFs that enables water splitting for stoichiometric evolution of H2 and O2. The exciton dipole orientation is responsible for driving the spatial separation of photoinduced charges, while the dynamic reactivity of imine bonds of COFs with water and holes is proven for initiating water oxidation. Accordingly, a rationally designed BtS-COF with benzotrithiophene and sulfone units exhibits a much-improved performance in H2 and O2 evolution in neutral water under visible light. Its catalytic efficiency is even superior to some photocatalysts with metal-based water oxidation cocatalyst.
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| GB/T 7714 | Niu, Qing , Deng, Wenfeng , Chen, Yanlei et al. Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks [J]. | ACS ENERGY LETTERS , 2024 , 9 (12) : 5830-5835 . |
| MLA | Niu, Qing et al. "Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks" . | ACS ENERGY LETTERS 9 . 12 (2024) : 5830-5835 . |
| APA | Niu, Qing , Deng, Wenfeng , Chen, Yanlei , Lin, Qingqing , Li, Liuyi , Liu, Zheyuan et al. Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks . | ACS ENERGY LETTERS , 2024 , 9 (12) , 5830-5835 . |
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Designing photocatalysts with well-defined structure-function relationships is imperative for propelling the progression of desired photocatalytic oxidation. Herein, the efficient conversion of solar energy to H2O2 and subsequently to hydroxyl radicals (•OH) is achieved through a synergistic interplay between olefin linkage (-C[dbnd]C-) and spatially separated benzene-triazine dual reaction sites within covalent organic frameworks (COFs). The upgraded -C[dbnd]C- can increase the conjugation degree of COFs, which establishes an expanded superstructure for boosting charge separation/transfer and stability. This precise modulation renders more opportunities for the hot electrons to migrate to the benzene site for solar-to-H2O2 generation, and to the triazine site for H2O2-to-•OH, separately. The optimized •OH generation pathway enables remarkable oxidation performances against recalcitrant organic pollutants, and pathogenic microorganisms under visible light irradiation. This work provides new insights for tuning the synergistic interactions of various building blocks within the COFs for the selective generation of highly reactive •OH for environmental remediation. © 2024 Elsevier B.V.
Keyword ：
Benzene Benzene Hot electrons Hot electrons Microorganisms Microorganisms Organic pollutants Organic pollutants Solar energy Solar energy
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| GB/T 7714 | Zhang, Jinpeng , Huang, Guocheng , Chen, Qiaoshan et al. Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation [J]. | Applied Catalysis B: Environmental , 2024 , 356 . |
| MLA | Zhang, Jinpeng et al. "Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation" . | Applied Catalysis B: Environmental 356 (2024) . |
| APA | Zhang, Jinpeng , Huang, Guocheng , Chen, Qiaoshan , Wu, Ling , Li, Liuyi , Bi, Jinhong . Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation . | Applied Catalysis B: Environmental , 2024 , 356 . |
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Photocatalytic reduction of CO 2 with H 2 O is thought as an environment friendly approach for sustainable development. It is highly desirable but remains challenging to develop photocatalyst with metal -free site for CO 2 reduction. Here, we fabricated a heterostructure by integrating azine-based COF with ZnIn 2 S 4 , where the azine unit in COF acts as metal -free sites for CO 2 adsorption and reduction. The as -formed interfused heterointerface in the heterostructure ensures the effective electron transfer from ZnIn 2 S 4 across the interface to the COF, resulting in a spatial separation of redox sites for CO 2 reduction and water oxidation. The hybrid catalyst exhibits remarkably enhanced photocatalytic activity for CO 2 reduction to CO, which is 8 and 6 times than the COF and ZnIn 2 S 4 , respectively, and is even comparable with some metal -catalyzed CO 2 reduction systems. This study provides a new paradigm to mimic natural photosynthesis by using metal -free site for CO 2 reduction. (c) 2024, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
Keyword ：
CO 2 reduction CO 2 reduction Covalent organic framework Covalent organic framework Heterostructure Heterostructure Metal -free site Metal -free site Photocatalysis Photocatalysis
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| GB/T 7714 | Huang, Haoming , Lin, Qingqing , Niu, Qing et al. Metal- free photocatalytic reduction of CO 2 on a covalent organic framework- based heterostructure [J]. | CHINESE JOURNAL OF CATALYSIS , 2024 , 60 : 201-208 . |
| MLA | Huang, Haoming et al. "Metal- free photocatalytic reduction of CO 2 on a covalent organic framework- based heterostructure" . | CHINESE JOURNAL OF CATALYSIS 60 (2024) : 201-208 . |
| APA | Huang, Haoming , Lin, Qingqing , Niu, Qing , Ning, Jiangqi , Li, Liuyi , Bi, Jinhong et al. Metal- free photocatalytic reduction of CO 2 on a covalent organic framework- based heterostructure . | CHINESE JOURNAL OF CATALYSIS , 2024 , 60 , 201-208 . |
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A metal-insulator-semiconductor (MIS) ternary photo-system was intricately crafted through precise amalgamation polyvinylpyrrolidone (PVP)-capped metal Cu with typical covalent triazine framework CTF-1 via electrostatic self-assembly. The 2 % Cu-PVP-CTF exhibited an impressive CH4 yield of 80.7 mu mol & sdot;g � 1 & sdot;h- 1 with selectivity of 96.8 % under visible light, representing a 2.3-fold and 112-fold improvement over Schottky-type Cu-CTF and pristine CTF-1, respectively. In-situ XPS and VASP-diff calculations unfolded that the ultrathin PVP insulating layer significantly expedited interfacial charges tunneling, corroborated by smaller lifetime tau 2 determined via femtosecond transient absorption spectroscopy. The intermediates of paramount importance in CO2 reduction like *COOH and *HCHO were meticulously monitored by in-situ Fourier infrared spectroscopy. DFT calculations elucidated that Cu-PVP-CTF was notably more adept at facillitating the rate-determining step (*COOH -> *CO) to produce CH4 than Cu-CTF. This work tamps the groundwork for conceptional roadmap in designing novel MIS photo-system for CO2 conversion.
Keyword ：
Carbon dioxide reduction Carbon dioxide reduction Covalent triazine-based frameworks Covalent triazine-based frameworks Metal-insulator-semiconductor Metal-insulator-semiconductor Methane evolution Methane evolution Visible-light photocatalysis Visible-light photocatalysis
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| GB/T 7714 | Chen, Qiaoshan , Chen, Yueling , Yu, Mingfei et al. Modulating interfacial charges in CTF-based metal-insulator-semiconductor promotes selective CO2 reduction to CH4 [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
| MLA | Chen, Qiaoshan et al. "Modulating interfacial charges in CTF-based metal-insulator-semiconductor promotes selective CO2 reduction to CH4" . | CHEMICAL ENGINEERING JOURNAL 482 (2024) . |
| APA | Chen, Qiaoshan , Chen, Yueling , Yu, Mingfei , Xu, Bin , Wu, Houyi , Li, Liuyi et al. Modulating interfacial charges in CTF-based metal-insulator-semiconductor promotes selective CO2 reduction to CH4 . | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
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光催化CO2还原制备碳基化学品,是解决能源危机的理想途径之一.以往的研究主要聚焦于金属位点催化,尽管金属催化剂具有显著的应用潜力,但其高昂的成本和金属中心易失活的问题,限制了其广泛应用.因此,模拟植物光合作用,探寻基于非金属位点的光催化剂,为CO2还原提供了新的解决思路.共价有机框架材料(COFs)作为一种新型有机晶态多孔材料,因其高度有序的结构和π共轭体系,通常表现出半导体特性.在COF中引入氮官能团,能有效增强对CO2的吸附和活化能力,有望在COFs上实现非金属光催化CO2还原. 本文利用COF异质结材料研究了非金属位点催化CO2还原过程.采用原位合成方法制备出ZnIn2S4@TAz-COF异质结材料.红外光谱、Raman光谱和X-射线衍射等方法证明了异质结材料的成功合成.扫描电镜和透射电镜观察显示,ZnIn2S4纳米片与COF形成了异质互融界面,这对后续研究电子转移路径和光催化增强机制至关重要.通过紫外-可见光漫反射光谱、紫外光电子能谱和Mott-Schottky表征,分析了复合前后样品在能带结构上发生的变化和单独组分的功函数.由此推断,当两者复合后,在费米能级差的驱动下,TAz-COF表面的电子流向ZnIn2S4,在界面处形成内建电场,这与差分电荷计算结果相一致.进一步的原位光照X射线光电子能谱研究证实,ZnIn2S4@TAz-COF异质结两相之间存在电荷转移,在界面处形成由TAz-COF指向ZnIn2S4的内建电场.这驱动了ZnIn2S4导带上的光生电子与TAz-COF价带上的光生空穴定向迁移和复合,而TAz-COF导带上还原能力较强的光生电子和ZnIn2S4价带上氧化能力较强的光生空穴被空间分离并参与光催化反应.在以水为电子供体的光催化还原CO2反应中,该异质结材料表现出较好的还原CO2到CO活性和良好的稳定性,其转化效率可与部分金属催化的CO2还原体系相当.密度泛函理论计算和原位光谱分析结果表明,吖嗪基团是CO2分子的吸附和活化位点,吖嗪中的氮原子与CO2中的碳原子的强相互作用确保了 CO2向COOH*中间体的转化,最终通过光生电子和质子的协助在COF表面转化为CO. 综上所述,本文制备了ZnIn2S4@TAz-COF异质结光催化材料.在可见光照射下,该材料界面处形成的内建电场有效驱动了光生电子和空穴的定向迁移,使得COF导带上具有较强还原能力的光生电子与ZnIn2S4价带上具有较强氧化能力的光生空穴实现了高效的空间分离.在没有金属助催化剂和空穴牺牲剂的条件下,ZnIn2S4@TAz-COF复合光催化剂表现出较好的光催化CO2还原活性.本工作不仅为深入理解非金属位点催化CO2还原机理提供了新视角,也为设计和构建高效CO2还原光催化材料提供了参考.
Keyword ：
二氧化碳还原 二氧化碳还原 光催化 光催化 共价有机框架 共价有机框架 异质结构 异质结构 非金属位点 非金属位点
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| GB/T 7714 | 黄浩铭 , 林清清 , 牛青 et al. 基于共价有机框架非金属位点的光催化CO2还原 [J]. | 催化学报 , 2024 , 60 (5) : 201-208 . |
| MLA | 黄浩铭 et al. "基于共价有机框架非金属位点的光催化CO2还原" . | 催化学报 60 . 5 (2024) : 201-208 . |
| APA | 黄浩铭 , 林清清 , 牛青 , 宁江淇 , 李留义 , 毕进红 et al. 基于共价有机框架非金属位点的光催化CO2还原 . | 催化学报 , 2024 , 60 (5) , 201-208 . |
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The design of photocatalytic supramolecular systems composing of semiconductors and molecular metal complexes for CO2 reduction has attracted increasing attention. The supramolecular system combines the structural merits of semiconductors and metal complexes, where the semiconductor harvests light and undertakes the oxidative site, while the metal complex provides activity for CO2 reduction. The intermolecular charge transfer plays crucial role in ensuring photocatalytic performance. Here, we review the progress of photocatalytic supramolecular systems in reduction of CO2 and highlight the interfacial charge transfer pathways, as well as their state-of-the-art characterization methods. The remaining challenges and prospects for further design of supramolecular photocatalysts are also presented.
Keyword ：
charge transport charge transport metal complex metal complex photocatalytic CO2 reduction photocatalytic CO2 reduction semiconductor semiconductor supramolecule supramolecule
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| GB/T 7714 | Ning, Jiangqi , Chen, Wei , Niu, Qing et al. Charge Transport Approaches in Photocatalytic Supramolecular Systems Composing of Semiconductor and Molecular Metal Complex for CO2 Reduction [J]. | CHEMSUSCHEM , 2024 , 17 (19) . |
| MLA | Ning, Jiangqi et al. "Charge Transport Approaches in Photocatalytic Supramolecular Systems Composing of Semiconductor and Molecular Metal Complex for CO2 Reduction" . | CHEMSUSCHEM 17 . 19 (2024) . |
| APA | Ning, Jiangqi , Chen, Wei , Niu, Qing , Li, Liuyi , Yu, Yan . Charge Transport Approaches in Photocatalytic Supramolecular Systems Composing of Semiconductor and Molecular Metal Complex for CO2 Reduction . | CHEMSUSCHEM , 2024 , 17 (19) . |
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Metal complex-based photocatalysts are promising for CO2 reduction. Their catalytic performances greatly rely on the synergy of ligands and metal ions. Here, we demonstrate an assembly of covalent organic cage (COC) and metal ions for photocatalytic CO2 reduction. The coordinated metal serves as catalytically active site for CO2 reduction, while the cage not only chelates the metal site, but also enhances the local concentration of CO2 around metal site, and decreases the key intermediate reaction energy barrier, thereby promoting the CO2 reduction reaction kinetically and thermodynamically. Accordingly, a Ni metalized COC exhibited outstanding photocatalytic performance in CO2-to-CO conversion under visible light irradiation. This study highlights the feasibility and advantage of organic cages for the construction of photocatalysts for artificial photosynthesis.
Keyword ：
CO2 reduction CO2 reduction Covalent organic cages Covalent organic cages Metal complex Metal complex Metallization Metallization Photocatalysis Photocatalysis
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| GB/T 7714 | Miao, Rongbin , Niu, Qing , Li, Liuyi et al. Ni-Metalized Covalent Organic Cage as a Photocatalyst for Selective Photoreduction of CO2 to CO [J]. | CHEMSUSCHEM , 2024 . |
| MLA | Miao, Rongbin et al. "Ni-Metalized Covalent Organic Cage as a Photocatalyst for Selective Photoreduction of CO2 to CO" . | CHEMSUSCHEM (2024) . |
| APA | Miao, Rongbin , Niu, Qing , Li, Liuyi , Yu, Yan . Ni-Metalized Covalent Organic Cage as a Photocatalyst for Selective Photoreduction of CO2 to CO . | CHEMSUSCHEM , 2024 . |
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We demonstrate an electrostatic confinement-induced charge transfer pathway in a supramolecular photocatalyst comprising of an ionic covalent organic framework (COF) and cationic metal complexes. The dynamic electrostatic interactions not only attract cations around the COF to accept photogenerated electrons, but also allow for a retention of homogeneous catalytic characters of complexes, making a subtle balance. Accordingly, the electrostatic confinement effect facilitates the forward electron transfer from a photoexcited COF to cationic Co complex, realizing a remarkable photocatalytic CO2 reduction performance. Its catalytic efficiency is far superior to the supramolecular counterparts with Van-der-Waals or hydrogen bonding interactions. This work presents an insight for enhancing charge transfer in supramolecular systems, and provides an effective approach for construction of highly efficient photocatalysts.
Keyword ：
CO2 reduction CO2 reduction covalent organic framework covalent organic framework electrostatic confinement electrostatic confinement photocatalysis photocatalysis single site single site
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| GB/T 7714 | Yu, Mingfei , Chen, Wei , Lin, Qingqing et al. Electrostatic Confinement-Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO2 Reduction [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
| MLA | Yu, Mingfei et al. "Electrostatic Confinement-Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO2 Reduction" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024) . |
| APA | Yu, Mingfei , Chen, Wei , Lin, Qingqing , Li, Liuyi , Liu, Zheyuan , Bi, Jinhong et al. Electrostatic Confinement-Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO2 Reduction . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
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共价有机框架材料(COFs)是由有机单元通过共价键连接而成的晶态多孔有机聚合物.因其具有长程有序、高表面积和结构可预先设计等特点,为解决日益严重的环境和能源问题提供了新兴的材料平台,在光(电)催化领域得到广泛关注.负载型单位点催化剂具有最大的金属原子利用率和明确的活性中心,对提高原子利用效率、揭示催化反应机制和提升催化性能等具有重要意义,成为近年的科研前沿.基于单位点催化和COFs材料的独特优势,利用COFs材料作为支撑材料锚定高度分散的单位点,如单个金属离子、单原子、单个活性位点或金属团簇等,设计和制备基于COFs的单位点光(电)催化材料成为当前催化科学领域的研究热点之一.近年来,国内外研究人员在设计合成COFs基单位点光(电)催化材料方面取得诸多重要进展.本文综述了COFs基单位点光(电)催化材料的结构特点、设计原则、催化机理及其在光-电催化领域的应用.总结了COFs基单位点材料在光(电)催化应用方面的基本依据和适用光(电)催化的COFs材料的一般合成方法,讨论了COFs基单位点光(电)催化材料的设计原则及优缺点.概述了COFs基单位点光(电)催化材料在光催化分解水、光催化制备H_2O_2、光催化CO_2还原、光催化N_2还原、光催化降解污染物、光催化有机转化及电催化分解水、电催化CO_2还原、电催化产氧、氧还原和N_2还原等领域的最新研究进展,并着重介绍了催化机理.此外,介绍了COFs基单位点光(电)催化材料常用的先进原位表征技术,如原位红外和原位X射线光电子能谱,并对其他先进的原位技术如原位X射线吸收光谱和原位电子顺磁共振光谱等在COFs基单位点催化中的应用进行了展望.总结了理论计算在揭示COFs基单位点光(电)催化材料催化活性来源中的重要作用,并提出用于光催化和电催化的修饰策略.同时指出COFs基单位点材料在光(电)催化领域所面临的挑战和未来的发展机遇.综上,期望本文为COFs基单位点材料在光(电)催化领域的应用提供一些借鉴.
Keyword ：
光催化 光催化 共价有机框架材料 共价有机框架材料 单位点催化 单位点催化 电催化 电催化
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| GB/T 7714 | 牛青 , 米林华 , 陈玮 et al. 基于共价有机框架的单位点光(电)催化材料的研究进展（英文） [J]. | Chinese Journal of Catalysis , 2023 , 50 (07) : 45-82 . |
| MLA | 牛青 et al. "基于共价有机框架的单位点光(电)催化材料的研究进展（英文）" . | Chinese Journal of Catalysis 50 . 07 (2023) : 45-82 . |
| APA | 牛青 , 米林华 , 陈玮 , 李秋军 , 钟升红 , 于岩 et al. 基于共价有机框架的单位点光(电)催化材料的研究进展（英文） . | Chinese Journal of Catalysis , 2023 , 50 (07) , 45-82 . |
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