Heterocyclization Strategy for Construction of Linear Conjugated Polymers: Efficient Metal‐Free Electrocatalysts for Oxygen Reduction

Long, Xinggui; Li, Daohao; Wang, Binbin; Jiang, Zhenjie; Xu, Wenjia; Wang, Bingbing; Yang, Dongjiang; Xia, Yanzhi

doi:10.1002/ange.201905468

Cited by 16 publications

(1 citation statement)

References 45 publications

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“…Taking this into consideration, an innovative defect engineering strategy has been developed in recent years to create topological defects in pure nanocarbon, which can promote electrical conductivity and thus electrochemical activity. [28][29][30] In particular, the investigation into the real active sites becomes complicated when there are no heteroatoms in carbon materials. Recent studies have shown that pure carbon nanomaterials with a large number of intrinsic defects can effectively stimulate charge redistribution on a conjugated sp 2 -carbon matrix, thus significantly increasing the ORR activity.…”

Section: Introductionmentioning

confidence: 99%

Defect‐Engineered Mesoporous Undoped Carbon Nanoribbons for Benchmark Oxygen Reduction Reaction

Srinivas

Liu

et al. 2023

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For large‐scale fuel cell applications, it is significant to replace expensive Pt‐based oxygen reduction reaction (ORR) electrocatalysts with nonprecious metal‐ or metal‐free carbon‐based catalysts with high activity. However, it is still challenging to deeply understand the role of intrinsic defects and the origin of ORR activity in pure nanocarbon. Therefore, a novel self‐assembly and a pyrolysis strategy to fabricate defect‐rich mesoporous carbon nanoribbons are presented. Due to the effective regulation of nanoarchitecture, a vast number of defective catalytic sites (edge defects and holes) are exposed, which thereby enhances the electron transfer kinetics and catalytic activity. Such undoped nanoribbons display a large half‐wave potential of 0.837 V, excellent long‐term stability, and exceptional methanol tolerance, surpassing the most undoped ORR catalysts and the commercial Pt/C (20 wt.%) catalyst. Structural characterizations and density functional theory (DFT) calculations confirm that the zigzag edge defects and the armchair pentagon at the hole defect are responsible for outstanding ORR performance.

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Section: Introductionmentioning

confidence: 99%

Defect‐Engineered Mesoporous Undoped Carbon Nanoribbons for Benchmark Oxygen Reduction Reaction

Srinivas

Liu

et al. 2023

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BN‐Embedded Polycyclic Aromatic Hydrocarbon Oligomers: Synthesis, Aromaticity, and Reactivity

Chen

Qiao

et al. 2020

Angewandte Chemie

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BN-embedded oligomers with different pairs of BN units were synthesized by electrophilic borylation. Up to four pairs of BN units were incorporated in the large polycyclic aromatic hydrocarbons (PAHs). Their geometric,p hotophysical, electrochemical, and Lewis acidic properties were investigated by X-ray crystallography,o ptical spectroscopy, and cyclic voltammetry.The B À Nbonds showdelocalized doublebond characteristics and the conjugation can be extended through the trans-orientated aromatic azaborine units.C alculations reveal the relatively lower aromaticity for the inner azaborine rings in the BN-embedded PAHo ligomers.T he frontier orbitals of the longer oligomers are delocalized over the inner aromatic rings.C onsequently,t he inner moieties of the BN-embedded PAHo ligomers are more active than the outer parts.T his is confirmed by as imple oxidation reaction, which has significant effects on the aromaticity and the intramolecular charge-transfer interactions. Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.org/10.1002/anie.202000556. Angewandte Chemie Forschungsartikel Scheme 1. Borylation of oligoanilinesinto BN-embedded PAH oligomers. Scheme 2. Synthetic routes for BN-embedded PAH oligomers BN1-BN4. Angewandte Chemie Forschungsartikel 7189

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Controlled Asymmetric Charge Distribution of Active Centers in Conjugated Polymers for Oxygen Reduction

Yao

Wang

et al. 2021

Angewandte Chemie

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Active center reconstruction is essential for high performance oxygen reduction reaction (ORR) electrocatalysts. Usually, the ORR activity stems from the electronic environment of active sites by charge redistribution. We introduce an asymmetry strategy to adjust the charge distribution of active centers by designing conjugated polymer (CP) catalysts with different degrees of asymmetry. We synthesized asymmetric backbone CP (asy-PB) by modifying B ! N coordination bonds and asymmetric sidechain CP (asy-PB-A) with different alkyl chain lengths. Both CPs with backbone and sidechain asymmetry exhibit superior ORR performance to their symmetric counterparts (sy-P and sy-PB). The asy-PB with greater asymmetry shows higher catalytic activity than asy-PB-A with relatively smaller asymmetry. DFT calculations reveal that the increased dipole moment and non-uniform charge distribution caused by asymmetric structure endows the center carbon atom of bipyridine with efficient catalytic activity.

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Heterocyclization Strategy for Construction of Linear Conjugated Polymers: Efficient Metal‐Free Electrocatalysts for Oxygen Reduction

Cited by 16 publications

References 45 publications

Defect‐Engineered Mesoporous Undoped Carbon Nanoribbons for Benchmark Oxygen Reduction Reaction

Defect‐Engineered Mesoporous Undoped Carbon Nanoribbons for Benchmark Oxygen Reduction Reaction

BN‐Embedded Polycyclic Aromatic Hydrocarbon Oligomers: Synthesis, Aromaticity, and Reactivity

Controlled Asymmetric Charge Distribution of Active Centers in Conjugated Polymers for Oxygen Reduction

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