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学者姓名：李留义
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Abstract ：
Covalent organic frameworks (COFs) have significant potential for solar-driven water splitting, yet they face the critical challenge of suppressing rapid charge recombination. Herein, we demonstrate a linker engineering strategy for the construction of COFs that involves polarized pi-spacers to integrate donor and acceptor units into anisotropic skeletons. Under illumination, the polarized pi-spacers induce an intramolecular sequential electron transfer along the linkers, enabling an enhanced charge delocalization and thereby significantly prolonging the charge-separated states compared to the binary-component counterparts. As a result, the designed ternary-ordered COF shows enhanced co-production of H2 and H2O2 from visible-light-driven water splitting, achieving an apparent quantum efficiency of 0.98% at 420 nm, outperforming most reported analogous materials. This strategy of driving sequential electron transfer in COFs by linker design to suppress charge recombination offers a rational approach for developing high-performance photocatalytic systems.
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| GB/T 7714 | Pan, Hongji , Niu, Qing , Yu, Mingfei et al. Polarized π-Spacer Engineering Enables Sequential Electron Transfer for Photocatalytic Water Splitting in Covalent Organic Frameworks [J]. | ACS ENERGY LETTERS , 2025 , 10 (9) : 4580-4588 . |
| MLA | Pan, Hongji et al. "Polarized π-Spacer Engineering Enables Sequential Electron Transfer for Photocatalytic Water Splitting in Covalent Organic Frameworks" . | ACS ENERGY LETTERS 10 . 9 (2025) : 4580-4588 . |
| APA | Pan, Hongji , Niu, Qing , Yu, Mingfei , Li, Liuyi , Yu, Yan . Polarized π-Spacer Engineering Enables Sequential Electron Transfer for Photocatalytic Water Splitting in Covalent Organic Frameworks . | ACS ENERGY LETTERS , 2025 , 10 (9) , 4580-4588 . |
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Photocatalytic CO2 reduction offers a promising approach for solar-to-chemical energy conversion. Achieving CO2 reduction under an aerobic environment is challenging, primarily owing to the competitive O2 reduction reaction at metal active sites. Herein, we demonstrate a hybrid photocatalyst of N3-COF/MoS2, where an azine-linked COF serves as a metal-free active site for CO2 reduction. The hybrid exhibits enhanced catalytic performance in CO2 reduction under aerobic conditions. At 20% O2 concentration, close to the atmospheric O2 content, the CO production rate reaches 28 mu mol g-1 h-1, which is much higher than that obtained using pure CO2. Structural, in situ spectroscopic and computational analyses reveal that the oxidation of azine groups in the COF by O2 induces the formation of highly active radical intermediates, which can suitably and preferentially react with CO2, resulting in the enhanced CO2 reduction performance in the presence of O2. This work provides a fresh insight into designing photocatalysts applied under ambient conditions for solar energy conversion.
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| GB/T 7714 | Ning, Jiangqi , Niu, Qing , Liu, Zheyuan et al. Aerobic oxidation of a covalent organic framework facilitating photocatalytic CO2 reduction with water [J]. | GREEN CHEMISTRY , 2025 , 27 (23) : 6804-6812 . |
| MLA | Ning, Jiangqi et al. "Aerobic oxidation of a covalent organic framework facilitating photocatalytic CO2 reduction with water" . | GREEN CHEMISTRY 27 . 23 (2025) : 6804-6812 . |
| APA | Ning, Jiangqi , Niu, Qing , Liu, Zheyuan , Li, Liuyi . Aerobic oxidation of a covalent organic framework facilitating photocatalytic CO2 reduction with water . | GREEN CHEMISTRY , 2025 , 27 (23) , 6804-6812 . |
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Herein, we report a hydrogen-bonded supramolecular hybrid composed of a cobaloxime complex and a covalent organic framework (COF) that achieves photocatalytic overall water splitting. The designed COF features ternary units and dual linkages, which induce asymmetric linkers. Upon photoexcitation, this asymmetry facilitates directed electron transfer and spatially separated redox sites, resulting in a long-lived charge-separated state. Consequently, the COF, hydrogen-bonded with cobaloxime as a hydrogen (H2) production cocatalyst, enables visible-light photocatalytic overall water splitting, simultaneously producing H2 and hydrogen peroxide (H2O2), outperforming the COFs with symmetric linker structures. This strategy of asymmetric structural design offers new insights for the design of photocatalysts with suppressed charge recombination for photocatalysis.
Keyword ：
Asymmetric structure Asymmetric structure Covalent organic framework Covalent organic framework Overall water splitting Overall water splitting Photocatalysis Photocatalysis Single site Single site
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| GB/T 7714 | Yu, Mingfei , Huang, Junhan , Niu, Qing et al. Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (22) . |
| MLA | Yu, Mingfei et al. "Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 22 (2025) . |
| APA | Yu, Mingfei , Huang, Junhan , Niu, Qing , Li, Liuyi , Yu, Yan , Bi, Jinhong . Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (22) . |
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The photocatalytic ammonia production is fundamentally constrained by the inertness of N2 molecules and the spatial overlap of photo-redox sites that probably leads to competitive by-products and inevitable reverse reactions. Herein, a well-defined S-scheme heterojunction with spatially separated redox centers was constructed by integrating a covalent organic framework (COF-TaTp) with NiFe layered double hydroxide (NiFe-LDH). The resulting inorganic-organic hybrid (NF30) showcased a remarkable NH3 evolution rate of 411.7 mu g center dot L-1 in pure water without sacrificial agents-3.8-and 12.5-fold higher than the individual counterparts. The enhanced performance primarily stems from the reinforced internal electric field (IEF = 10.4) and oriented charge migration via the specific O-H-C/N interfacial channels, as validated by layered charge difference distribution and augmented surface photovoltage. In situ XPS, DRIFTS, and DFT calculations further revealed a typical Sscheme electron transfer mechanism and an alternating N2 reduction pathway with a substantially lowered energy barrier for rate-determining step (*N2 -> *NNH). This work provides mechanistic insights into charge kinetics across inorganic-organic interfaces and COF-based heterojunction design for efficient solar ammonia production.
Keyword ：
Ammonia production Ammonia production Covalent organic framework Covalent organic framework Internal electronic field Internal electronic field Photocatalysis Photocatalysis S -scheme heterojunction S -scheme heterojunction
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| GB/T 7714 | Yu, Mingfei , Chen, Yueling , Song, Xiaoping et al. Achieving spatially separated photo-redox sites via COFs-based inorganic-organic S-scheme heterojunction for boosting solar ammonia production [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
| MLA | Yu, Mingfei et al. "Achieving spatially separated photo-redox sites via COFs-based inorganic-organic S-scheme heterojunction for boosting solar ammonia production" . | CHEMICAL ENGINEERING JOURNAL 522 (2025) . |
| APA | Yu, Mingfei , Chen, Yueling , Song, Xiaoping , Chen, Qiaoshan , Li, Liuyi , Bi, Jinhong . Achieving spatially separated photo-redox sites via COFs-based inorganic-organic S-scheme heterojunction for boosting solar ammonia production . | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
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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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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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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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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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Covalent organic frameworks (COFs) have been regarded as promising photocatalytic materials. However, the sluggish diffusion of photoinduced charges in a single-component COF remains the obstacles that have to be overcome. Here, we demonstrate a synthesis of a COF bearing dual cocatalysts Co(3)O(4 )and Re complex as photocatalyst for water oxidation. The dual cocatalysts are coordinated on the COF, and enable the spatial separation of photoinduced charges. The generated electrons were attracted to Re moiety, while the holes were localized on Co(3)O(4 )cocatalyst for water oxidation to produce O-2 product. The synergy of dual cocatalysts of COF promote the charge separation and redox reaction. Moreover, hydroxyl radicals generated from the hydration of COF contribute to O-O bond formation, which is the key step of O-2 formation. Accordingly, an excellent O-2 production rate of 400 mu mol g(-1) h(-1) under visible light irradiation was obtained. This work may pave the way to the development of highly efficient COF photocatalysts for solar energy conversion.
Keyword ：
Covalent organic frameworks Covalent organic frameworks Dual cocatalysts Dual cocatalysts O-2 evolution O-2 evolution Photocatalysis Photocatalysis Water oxidation Water oxidation
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| GB/T 7714 | Yu, Mingfei , Li, Qiujun , Li, Liuyi et al. Dual Cocatalysts on Covalent Organic Framework as Charge Transfer Mediator Facilitating Photocatalytic Water Oxidation [J]. | CHEMCATCHEM , 2024 , 16 (23) . |
| MLA | Yu, Mingfei et al. "Dual Cocatalysts on Covalent Organic Framework as Charge Transfer Mediator Facilitating Photocatalytic Water Oxidation" . | CHEMCATCHEM 16 . 23 (2024) . |
| APA | Yu, Mingfei , Li, Qiujun , Li, Liuyi , Yu, Yan . Dual Cocatalysts on Covalent Organic Framework as Charge Transfer Mediator Facilitating Photocatalytic Water Oxidation . | CHEMCATCHEM , 2024 , 16 (23) . |
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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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