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学者姓名：蓝志安
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Abstract ：
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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Abstract ：
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 0-80.5 %.
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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Covalent triazine-based frameworks (CTFs) are typically produced by the salt-melt polycondensation of aromatic nitriles in the presence of ZnCl2. In this reaction, molten ZnCl2 salt acts as both a solvent and Lewis acid catalyst. However, when cyclotrimerization takes place at temperatures above 300 degrees C, undesired carbonization occurs. In this study, an ionothermal synthesis method for CTF-based photocatalysts was developed using a ternary NaCl-KCl-ZnCl2 eutectic salt (ES) mixture with a melting point of approximately 200 degrees C. This temperature is lower than the melting point of pure ZnCl2 (318 degrees C), thus providing milder salt-melt conditions. These conditions facilitated the polycondensation process, while avoiding carbonization of the polymeric backbone. The resulting CTF-ES200 exhibited enhanced optical and electronic properties, and displayed remarkable photocatalytic performance in the hydrogen evolution reaction.
Keyword ：
Covalent Triazine Frameworks Covalent Triazine Frameworks Hydrogen Production Hydrogen Production Ionothermal Synthesis Ionothermal Synthesis Photocatalysis Photocatalysis Ternary Eutectic Salts Ternary Eutectic Salts
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| GB/T 7714 | Lan, Zhi-An , Wu, Meng , Fang, Zhongpu et al. Ionothermal Synthesis of Covalent Triazine Frameworks in a NaCl-KCl-ZnCl2 Eutectic Salt for the Hydrogen Evolution Reaction [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2022 , 61 (18) . |
| MLA | Lan, Zhi-An et al. "Ionothermal Synthesis of Covalent Triazine Frameworks in a NaCl-KCl-ZnCl2 Eutectic Salt for the Hydrogen Evolution Reaction" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 61 . 18 (2022) . |
| APA | Lan, Zhi-An , Wu, Meng , Fang, Zhongpu , Zhang, Yongfan , Chen, Xiong , Zhang, Guigang et al. Ionothermal Synthesis of Covalent Triazine Frameworks in a NaCl-KCl-ZnCl2 Eutectic Salt for the Hydrogen Evolution Reaction . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2022 , 61 (18) . |
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Direct photocatalytic water splitting is an attractive strategy for clean energy, in which, organic photocatalytic systems with broad light-harvesting region and efficient charge separation are highly desired and still challenging. In this paper, three multi-branched organic dyes were designed and synthesized with dipolar, V-shaped, and octupolar geometries, respectively. The multiple intramolecular charge transfer processes by electronic pull-push effect along the branches can provide more channels for light-harvesting and carrier transporting. Also, the interactions with polymeric carbon nitride (PCN) can be optimized by multiple anchoring units and defect filling effect, resulting in the gradually enhanced photocatalytic hydrogen evolution performance with the increased number of branches. Accordingly, the highest one of 996.9 mu mol h(-1) was achieved, which is over 40-folders that of PCN/Pt (24.8 mu mol h(-1)) under the same conditions. It provides an efficient strategy for molecular design of organic dyes as photocatalyst, promoting development of PHE system from the molecular level.
Keyword ：
Heterojunction system Heterojunction system Hydrogen evolution Hydrogen evolution Multi-branched structure Multi-branched structure Organic dye Organic dye Polymeric carbon nitride (PCN) Polymeric carbon nitride (PCN)
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| GB/T 7714 | Liu, Siwei , Lin, Peixuan , Wu, Meng et al. Organic dyes with multi-branched structures for highly efficient photocatalytic hydrogen evolution under visible-light irradiation [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 309 . |
| MLA | Liu, Siwei et al. "Organic dyes with multi-branched structures for highly efficient photocatalytic hydrogen evolution under visible-light irradiation" . | APPLIED CATALYSIS B-ENVIRONMENTAL 309 (2022) . |
| APA | Liu, Siwei , Lin, Peixuan , Wu, Meng , Lan, Zhi-An , Zhuzhang, Hangyu , Han, Mengmeng et al. Organic dyes with multi-branched structures for highly efficient photocatalytic hydrogen evolution under visible-light irradiation . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 309 . |
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Abstract ：
Conjugated polymers (CPs) have garnered increasing attention in the field of photocatalysis due to their stability and molecular tunability. Understanding the structure-property relationship in CPs and addressing appropriate molecular design strategies are pivotal to improving the photocatalytic performance of CPs. Herein, a new efficient cyano (CN) engineering approach was proposed to promote the photocatalytic performance of CPs, and three representative CP-based photocatalysts with different CN contents were tailor-made to investigate the relationship between CN functionalization and photocatalytic activity. A series of systematically experimental and theoretical studies reveal that CN functionalization contributes to strengthening the donor-acceptor (D-A) interaction, enhancing the light absorption ability, charge separation/transfer efficiency, and hydrophilicity of CPs, and also facilitating the output of separated photoinduced electrons from CPs to Pt cocatalyst. Thus, the dicyano-functionalized polymer (P-2CN) manifests an attractive photocatalytic performance in hydrogen production. This study provides a facile strategy to develop excellent CP-based photocatalysts for solar fuel production.
Keyword ：
conjugated polymers conjugated polymers cyano functionalization cyano functionalization hydrogen production hydrogen production photocatalysis photocatalysis structure-property relationship structure-property relationship
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| GB/T 7714 | Chi, Xu , Chen, Qian , Lan, Zhi-An et al. Structure-Property Relationship of Cyano-Functionalized Conjugated Polymers for Photocatalytic Hydrogen Production [J]. | CHEMISTRY-A EUROPEAN JOURNAL , 2022 , 29 (2) . |
| MLA | Chi, Xu et al. "Structure-Property Relationship of Cyano-Functionalized Conjugated Polymers for Photocatalytic Hydrogen Production" . | CHEMISTRY-A EUROPEAN JOURNAL 29 . 2 (2022) . |
| APA | Chi, Xu , Chen, Qian , Lan, Zhi-An , Zhang, Xirui , Chen, Xiong , Wang, Xinchen . Structure-Property Relationship of Cyano-Functionalized Conjugated Polymers for Photocatalytic Hydrogen Production . | CHEMISTRY-A EUROPEAN JOURNAL , 2022 , 29 (2) . |
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Abstract ：
Covalent triazine frameworks (CTFs) represent promising polymeric photocatalysts for photocatalytic hydrogen production with visible light. However, the separation and transfer of charges in CTFs are isotropic because of the uniform distribution of donor-acceptor motifs in the skeleton. Herein, to achieve the anisotropic charge carrier separation and migration, thiophene (Th) or benzothiadiazole (BT) unit is selected as the dopant to modify the molecular structure of CTF-based photocatalysts. Both theoretical and experimental studies reveal that the incorporation of Th or BT units induces the anisotropic charge carrier separation and migration at the interface of CTFs. The optimized polymer manifests a much enhanced photocatalytic activity for photocatalytic hydrogen production with visible light, and thus this study provides a useful tool to design conjugated polymer photocatalysts at the molecular level for solar energy conversion.
Keyword ：
anisotropic charge mobility anisotropic charge mobility covalent triazine frameworks covalent triazine frameworks hollow porous structure hollow porous structure photocatalysis photocatalysis solar hydrogen evolution solar hydrogen evolution
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| GB/T 7714 | Lan, Zhi-An , Chi, Xu , Wu, Meng et al. Molecular Design of Covalent Triazine Frameworks with Anisotropic Charge Migration for Photocatalytic Hydrogen Production [J]. | SMALL , 2022 , 18 (16) . |
| MLA | Lan, Zhi-An et al. "Molecular Design of Covalent Triazine Frameworks with Anisotropic Charge Migration for Photocatalytic Hydrogen Production" . | SMALL 18 . 16 (2022) . |
| APA | Lan, Zhi-An , Chi, Xu , Wu, Meng , Zhang, Xirui , Chen, Xiong , Zhang, Guigang et al. Molecular Design of Covalent Triazine Frameworks with Anisotropic Charge Migration for Photocatalytic Hydrogen Production . | SMALL , 2022 , 18 (16) . |
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Charge generation and separation are regarded as the major constraints limiting the photocatalytic activity of polymeric photocatalysts. Herein, two new linear polyarylether-based polymers (PAE-CPs) with distinct linking patterns between their donor and acceptor motifs were tailor-made to investigate the influence of different linking patterns on the charge generation and separation process. Theoretical and experimental results revealed that compared to the traditional single-stranded linker, the double-stranded linking pattern strengthens donor-acceptor interactions in PAE-CPs and generates a coplanar structure, facilitating charge generation and separation, and enabling red-shifted light absorption. With these prominent advantages, the PAE-CP interlinked with a double-stranded linker exhibits markedly enhanced photocatalytic activity compared to that of its single-strand-linked analogue. Such findings can facilitate the rational design and modification of organic semiconductors for charge-induced reactions.
Keyword ：
hydrogen evolution hydrogen evolution hydrogen peroxide evolution hydrogen peroxide evolution linking pattern linking pattern photocatalysis photocatalysis polyarylether polyarylether
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| GB/T 7714 | Lan, Zhi-An , Wu, Meng , Fang, Zhongpu et al. A Fully Coplanar Donor-Acceptor Polymeric Semiconductor with Promoted Charge Separation Kinetics for Photochemistry [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2021 , 60 (30) : 16355-16359 . |
| MLA | Lan, Zhi-An et al. "A Fully Coplanar Donor-Acceptor Polymeric Semiconductor with Promoted Charge Separation Kinetics for Photochemistry" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 60 . 30 (2021) : 16355-16359 . |
| APA | Lan, Zhi-An , Wu, Meng , Fang, Zhongpu , Chi, Xu , Chen, Xiong , Zhang, Yongfan et al. A Fully Coplanar Donor-Acceptor Polymeric Semiconductor with Promoted Charge Separation Kinetics for Photochemistry . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2021 , 60 (30) , 16355-16359 . |
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Conjugated polymers have gathered particular interests in photocatalysis because of their excellent properties such as optimization flexibility, cost-effective, and robust stability. The pyrene-based polymer (PyP), as one of the conjugated polymers, holds a great potential for water splitting because of their suitable band structure, visible light absorption, and high surface area. However, because of the fast charge carrier recombination confined by Frenkel excitons with high exciton binding energy, PyP in its pristine form remains barely active for photoctalytic hydrogen evolution. The concise construction of heterojunction is a feasible way to accelerate the charge separation, increase the lifetime of the photogenerated e(-)/h(+) pair and decrease the activation barriers of hydrogen evolution reaction. In this work, a series of transition metal sulfides as cocatalysts have been deposited on PyP to construct heterojunctions for photocatalytic H-2 evolution reaction (HER). The loading techniques (immersion, in-situ and photodeposition) and the loading contents of cocatalysts have been investigated. The optimized MoS2/PyP sample exhibited a 10-fold increase in comparison with pure PyP without modification. The extended pi-conjugation, high surface area, and widely exposed 2D interface highlight the importance of PyP as effective supports for stabilizing the homogeneously dispersed MoS2, thereby resulting in an efficient photocatalytic activity. This study provides a new idea to construct low-cost, sustainable and efficient hybrid system for photocatalytic hydrogen production.
Keyword ：
H-2 production H-2 production Heterojunction Heterojunction MoS2 MoS2 Photocatalysis Photocatalysis Pyrene-based conjugated polymer Pyrene-based conjugated polymer
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| GB/T 7714 | Zang, Shaohong , Zhang, Guigang , Lan, Zhi-An et al. Enhancement of photocatalytic H-2 evolution on pyrene-based polymer promoted by MoS2 and visible light [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2019 , 251 : 102-111 . |
| MLA | Zang, Shaohong et al. "Enhancement of photocatalytic H-2 evolution on pyrene-based polymer promoted by MoS2 and visible light" . | APPLIED CATALYSIS B-ENVIRONMENTAL 251 (2019) : 102-111 . |
| APA | Zang, Shaohong , Zhang, Guigang , Lan, Zhi-An , Zheng, Dandan , Wang, Xinchen . Enhancement of photocatalytic H-2 evolution on pyrene-based polymer promoted by MoS2 and visible light . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2019 , 251 , 102-111 . |
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Abstract ：
Photo-to-chemical energy conversion requires a systematic and complex molecular design to manage consecutive photochemical processes, including energy harvesting, exciton migration, electron transfer, charge separation, and charge transport. However, such an integrated design remains a substantial challenge. Here, we report a seamless system in managing these photochemical events on the basis of two-dimensional sp(2) carbon-conjugated covalent organic frameworks. The frameworks are designed to be fully pi conjugated for harvesting a wide range of visible to near-infrared light and to constitute built-in donor-acceptor heterojunction interfaces for splitting excitons. The frameworks create dense yet ordered columnar pi arrays that offer pathways to facilitate exciton migration and charge transport. Loading reaction centers in pores or on surface shortens the electron-transfer distance and promotes the accumulation of electrons at the reaction centers. These three molecular mechanisms are seamlessly integrated in the frameworks and render the system able to efficiently produce hydrogen that is driven by low-energy photons.
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| GB/T 7714 | Jin, Enquan , Lan, Zhian , Jiang, Qiuhong et al. 2D sp(2) Carbon-Conjugated Covalent Organic Frameworks for Photocatalytic Hydrogen Production from Water [J]. | CHEM , 2019 , 5 (6) : 1632-1647 . |
| MLA | Jin, Enquan et al. "2D sp(2) Carbon-Conjugated Covalent Organic Frameworks for Photocatalytic Hydrogen Production from Water" . | CHEM 5 . 6 (2019) : 1632-1647 . |
| APA | Jin, Enquan , Lan, Zhian , Jiang, Qiuhong , Geng, Keyu , Li, Guosheng , Wang, Xinchen et al. 2D sp(2) Carbon-Conjugated Covalent Organic Frameworks for Photocatalytic Hydrogen Production from Water . | CHEM , 2019 , 5 (6) , 1632-1647 . |
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Exciton binding energy has been regarded as a crucial parameter for mediating charge separation in polymeric photocatalysts. Minimizing the exciton binding energy of the polymers can increase the yield of charge-carrier generation and thus improve the photocatalytic activities, but the realization of this approach remains a great challenge. Herein, a series of linear donor-acceptor conjugated polymers has been developed to minimize the exciton binding energy by modulating the charge-transfer pathway. The results reveal that the reduced energy loss of the charge-transfer state can facilitate the electron transfer from donor to acceptor, and thus, more electrons are ready for subsequent reduction reactions. The optimized polymer, FSO-FS, exhibits a remarkable photochemical performance under visible light irradiation.
Keyword ：
charge-transfer pathway charge-transfer pathway conjugated polymer conjugated polymer exciton binding energy exciton binding energy hydrogen evolution hydrogen evolution photocatalysis photocatalysis
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| GB/T 7714 | Lan, Zhi-An , Zhang, Guigang , Chen, Xiong et al. Reducing the Exciton Binding Energy of Donor-Acceptor-Based Conjugated Polymers to Promote Charge-Induced Reactions [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2019 , 58 (30) : 10236-10240 . |
| MLA | Lan, Zhi-An et al. "Reducing the Exciton Binding Energy of Donor-Acceptor-Based Conjugated Polymers to Promote Charge-Induced Reactions" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 58 . 30 (2019) : 10236-10240 . |
| APA | Lan, Zhi-An , Zhang, Guigang , Chen, Xiong , Zhang, Yongfan , Zhang, Kai A., I , Wang, Xinchen . Reducing the Exciton Binding Energy of Donor-Acceptor-Based Conjugated Polymers to Promote Charge-Induced Reactions . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2019 , 58 (30) , 10236-10240 . |
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