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核心技术专利：CN118964589B侵权必究
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一种修饰在3D-G上的新型全共轭共价有机框架，以增强氧催化性能中的“D-π-A”电子调控。

A novel fully conjugated COF adorned on 3D-G to boost the "D-π-A" electron regulation in oxygen catalysis performance.

作者信息

Sun Yinggang, Duan Wenjie, Wang Jigang, Sun Peng, Zhuang Yanqiong, Li Zhongfang

机构信息

College of Chemistry and Chemical Engineering, Shandong University of Science and Technology Zibo 255000 Shandong P. R. China

出版信息

Chem Sci. 2025 Apr 22. doi: 10.1039/d5sc02082d.

DOI:10.1039/d5sc02082d
PMID:40336990
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12053216/
Abstract

Covalent organic frameworks (COFs) are promising materials for oxygen catalysis. Here, a novel, highly stable, conjugated two-dimensional poly(benzimidazole porphyrin-cobalt) (PBIPorCo) with a large delocalization energy is synthesized using meso-5,10,15,20-tetra (4-cyano-phenylporphyrin) cobalt (TCNPorCo) and 3,3'-diaminobenzidine (DAB). The decrease in energy between the HOMO and LUMO orbitals of PBIPorCo could enhance the capability for the gain and loss of electrons during the catalytic process. In a nitrogen-rich environment, a benzimidazole (BI) group can transfer electrons to the Co-N site and enhance the protonation process in the oxygen reduction reaction (ORR). The π-π interactions between PBIPorCo and three-dimensional graphene (3D-G) form an "electron donor-π-electron acceptor" structure to boost the bifunctional oxygen catalysis process. PBIPorCo/3D-G exhibits outstanding bifunctional oxygen catalytic performance (Δ = 0.62 V) and outstanding performance in zinc-air batteries. It exhibits satisfactory potential for application in fuel cells (FCs) and overall water splitting (OWS). This work presents a promising strategy for the design of novel COFs as bifunctional oxygen catalysts.

摘要

共价有机框架（COFs）是用于氧催化的有前景的材料。在此，使用中-5,10,15,20-四（4-氰基苯基卟啉）钴（TCNPorCo）和3,3'-二氨基联苯胺（DAB）合成了一种具有大离域能的新型、高度稳定的共轭二维聚（苯并咪唑卟啉-钴）（PBIPorCo）。PBIPorCo的最高占据分子轨道（HOMO）和最低未占据分子轨道（LUMO）之间的能量降低可以增强催化过程中电子得失的能力。在富氮环境中，苯并咪唑（BI）基团可以将电子转移到Co-N位点，并增强氧还原反应（ORR）中的质子化过程。PBIPorCo与三维石墨烯（3D-G）之间的π-π相互作用形成“电子供体-π-电子受体”结构，以促进双功能氧催化过程。PBIPorCo/3D-G表现出出色的双功能氧催化性能（Δ = 0.62 V）以及在锌空气电池中的出色性能。它在燃料电池（FCs）和全水分解（OWS）中展现出令人满意的应用潜力。这项工作为设计新型COFs作为双功能氧催化剂提出了一种有前景的策略。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/b36541a8accf/d5sc02082d-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/05d470f82b03/d5sc02082d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/8c1a366fc9c2/d5sc02082d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/44c3a2dca3fe/d5sc02082d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/4a39852eeab8/d5sc02082d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/a83b4a0b86ec/d5sc02082d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/8eac57c770cf/d5sc02082d-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/b36541a8accf/d5sc02082d-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/05d470f82b03/d5sc02082d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/8c1a366fc9c2/d5sc02082d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/44c3a2dca3fe/d5sc02082d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/4a39852eeab8/d5sc02082d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/a83b4a0b86ec/d5sc02082d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/8eac57c770cf/d5sc02082d-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8dbd/12135826/b36541a8accf/d5sc02082d-f7.jpg

相似文献

[1]
A novel fully conjugated COF adorned on 3D-G to boost the "D-π-A" electron regulation in oxygen catalysis performance.

Chem Sci. 2025-4-22

[2]
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J Colloid Interface Sci. 2025-5-15

[3]
Theory-Guided Design of N-Confused Porphyrinic Covalent Organic Frameworks for Oxygen Reduction Reaction.

J Am Chem Soc. 2025-3-12

[4]
Designing Thiophene-Enriched Fully Conjugated 3D Covalent Organic Framework as Metal-Free Oxygen Reduction Catalyst for Hydrogen Fuel Cells.

Angew Chem Int Ed Engl. 2023-1-23

[5]
Interlayer Polymerization to Construct a Fully Conjugated Covalent Organic Framework as a Metal-Free Oxygen Reduction Reaction Catalyst for Anion Exchange Membrane Fuel Cells.

Small. 2024-8

[6]
Building synergistic multiple active sites in branch-leaf nanostructured carbon nanofiber derived from MOF/COF hybrid for flexible wearable Zn-air battery.

J Colloid Interface Sci. 2024-7-15

[7]
Construction of Catalytic Covalent Organic Frameworks with Redox-Active Sites for the Oxygen Reduction and the Oxygen Evolution Reaction.

Angew Chem Int Ed Engl. 2022-12-5

[8]
Identification of catalytic sites for oxygen reduction and oxygen evolution in N-doped graphene materials: Development of highly efficient metal-free bifunctional electrocatalyst.

Sci Adv. 2016-4-22

[9]
Construction of Bimetallic-Anchored Two-Dimensional Nanosheets on COF for Rechargeable Zinc-Air Batteries.

ACS Appl Mater Interfaces. 2024-4-3

[10]
From Porphyrin-Like Rings to High-Density Single-Atom Catalytic Sites: Unveiling the Superiority of p-CN for Bifunctional Oxygen Electrocatalysis.

ACS Appl Mater Interfaces. 2024-1-10

本文引用的文献

[1]
Task-Driven Tailored Covalent Organic Framework for Dynamic Capture of Trace Radioactive CH I under High-Flow Rate Conditions.

ACS Cent Sci. 2024-10-25

[2]
Stabilizing atomic Ru species in conjugated sp carbon-linked covalent organic framework for acidic water oxidation.

Nat Commun. 2024-6-26

[3]
Instantaneous Thermal Energy for Swift Synthesis of Single-Atom Catalysts for Unparalleled Performance in Metal-Air Batteries and Fuel Cells.

Adv Mater. 2024-8

[4]
Dithiine-linked metalphthalocyanine framework with undulated layers for highly efficient and stable HO electroproduction.

Nat Commun. 2024-1-23

[5]
Covalent-organic framework nanobionics for robust cytoprotection.

Chem Sci. 2023-12-13

[6]
An erythrocyte membrane-camouflaged fluorescent covalent organic framework for starving/nitric oxide/immunotherapy of triple-negative breast cancer.

Chem Sci. 2023-7-28

[7]
Recent advances in the utilization of covalent organic frameworks (COFs) as electrode materials for supercapacitors.

Chem Sci. 2023-11-7

[8]
A Porous Crystalline Nitrone-Linked Covalent Organic Framework.

Angew Chem Int Ed Engl. 2023-9-4

[9]
Geometric frustration of Jahn-Teller order in the infinite-layer lattice.

Nature. 2023-3

[10]
Covalent organic frameworks with Ni-Bis(dithiolene) and Co-porphyrin units as bifunctional catalysts for Li-O batteries.

Sci Adv. 2023-2-3

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