Covalent-Bridged Heterointerfaces via Grafted Triazine Organic Polymers Enable Directed Charge Transfer for Efficient Oxygen Reduction in Zn–Air Batteries

Covalent triazine framework (CTF) derivatives have emerged as promising metal-free electrocatalysts due to their high nitrogen content and intrinsic porosity. However, their performance remains limited by sluggish interfacial charge transport and the inaccessibility of active sites. Herein, we report an interfacial covalent bridging strategy based on grafting polymerization to construct a carbon heterostructure electrocatalyst, featuring vertically aligned nitrogen-doped nanosheets covalently anchored onto graphene (v-N/CNS/Gr) support. The covalently bridged interface promotes interfacial charge transfer across the heterostructure, activating otherwise dormant nitrogen active sites and amplifying the oxygen reduction reaction (ORR) reactivity. <i>In situ</i> spectroscopic analyses and theoretical simulations reveal that the covalent bridged bonding promotes charge transport and oxygen activation, and optimizes the adsorption/desorption of intermediates, collectively contributing to reduced energy barriers along the 4e<sup>-</sup> ORR pathway. As a result, the v-N/CNS/Gr delivers excellent ORR activity with a half-wave potential of 0.85 V (<i>vs</i> RHE). When employed as the cathode in a Zn-air battery, v-N/CNS/Gr achieves a high-power density and stable operation over 850 h. This work demonstrates a generalizable triazine-polymer-based interfacial bridge strategy for enhancing active site accessibility and charge transport in metal-free electrocatalysts.

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Publication Details

Journal
ACS Nano
Published
2025-08-25
DOI
https://doi.org/10.1021/acsnano.5c11348
Citations
18
Primary Topic
Advanced battery technologies research
Type
article
Field-Weighted Citation Impact
13.15

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article

Covalent-Bridged Heterointerfaces via Grafted Triazine Organic Polymers Enable Directed Charge Transfer for Efficient Oxygen Reduction in Zn–Air Batteries

Yuhang Dai, Tianxi X. Liu, Jiexin Zhu, Jitao Shang et al.
18 citations
ACS Nano
Advanced battery technologies research
13.15
article

Covalent-Bridged Heterointerfaces via Grafted Triazine Organic Polymers Enable Directed Charge Transfer for Efficient Oxygen Reduction in Zn–Air Batteries

Yuhang Dai, Tianxi X. Liu, Jiexin Zhu, Jitao Shang, Yazhou Zhou, Xueying Cao, Feng Peng, Kaibin Chu, Guanjie He, Ivan P. Parkin, Xinliang Fu, Wei Zong, Yong Hui Zheng, Fei Guo, Shan Chen, Ouyang Yue, Zihan Song
article en
18 citations

Abstract

Covalent triazine framework (CTF) derivatives have emerged as promising metal-free electrocatalysts due to their high nitrogen content and intrinsic porosity. However, their performance remains limited by sluggish interfacial charge transport and the inaccessibility of active sites. Herein, we report an interfacial covalent bridging strategy based on grafting polymerization to construct a carbon heterostructure electrocatalyst, featuring vertically aligned nitrogen-doped nanosheets covalently anchored onto graphene (v-N/CNS/Gr) support. The covalently bridged interface promotes interfacial charge transfer across the heterostructure, activating otherwise dormant nitrogen active sites and amplifying the oxygen reduction reaction (ORR) reactivity. <i>In situ</i> spectroscopic analyses and theoretical simulations reveal that the covalent bridged bonding promotes charge transport and oxygen activation, and optimizes the adsorption/desorption of intermediates, collectively contributing to reduced energy barriers along the 4e<sup>-</sup> ORR pathway. As a result, the v-N/CNS/Gr delivers excellent ORR activity with a half-wave potential of 0.85 V (<i>vs</i> RHE). When employed as the cathode in a Zn-air battery, v-N/CNS/Gr achieves a high-power density and stable operation over 850 h. This work demonstrates a generalizable triazine-polymer-based interfacial bridge strategy for enhancing active site accessibility and charge transport in metal-free electrocatalysts.

ACS NanoVol. 19(35)
Jiangnan University (CN), Ministry of Education of the People's Republic of China (CN), VSB - Technical University of Ostrava (CZ), Linyi University (CN), China Three Gorges University (CN), Wuhan University (CN), University of Oxford (GB), Max Planck Institute for Polymer Research (DE), CAS Key Laboratory of Urban Pollutant Conversion (CN), Division of Materials Science and Engineering (AU), Hubei Normal University (CN), University College London (GB), Wuhan Institute of Technology (CN)
UK Research and Innovation, European Commission, National Natural Science Foundation of China, Natural Science Foundation of Hubei Province, Natural Science Foundation of Shandong Province, HORIZON EUROPE Framework Programme, Engineering and Physical Sciences Research Council
Openalex Percentile: Top 1%
Advanced battery technologies research
13.15
DOIOpen Access PDFOpenAlex
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