Construction of symbiotic one-dimensional ionic channels in a cobalt-based covalent organic framework for high-performance oxygen reduction electrocatalysis

Ren, Rong1; Yang, Liting2; Lin, Zhang1; Li, Xiaoyu1; Zhang, Shuomeng1; Zheng, Tianlong1; Wu, Duojie3; Wang, Jian4; Wei, Zidong4; Ding, Wei4; Huang, Ning2; Gu, Meng3; He, Qinggang1,5

2022-09-01

10.1039/d2ta06228c

Journal of Materials Chemistry A   Impact Factor & Quartile

2050-7488

2050-7496

With the advantages of high specific activity and selectivity, molecular catalysts are regarded as burgeoning electrode materials for anion exchange membrane fuel cells (AEMFCs). However, their catalytic performance in the catalyst layer of AEMFCs is often limited by the uneven distribution of triple-phase boundaries due to the agglomeration of the catalyst and the intermittent ionic channels. Herein, we constructed a porphyrin cobalt-based covalent organic framework (TAPPCo COF) composed of symbiotic ordered ionic channels and anchored quaternary ammonium (QA) cationic groups to facilitate the conduction of OH-. Microscopic and spectroscopic analyses confirm that the TAPPCo COF maintains plenty of Co catalytic active sites for the oxygen reduction reaction (ORR) and a reticular porous structure for O-2 reactant permeation. Atomic force microscopy coupled with electrochemical impedance spectroscopy (AFM-EIS) demonstrated nonlinear local variation of double-layer capacitance and ion transportation resistance at the nanoscale on the catalyst surface, as well as a decreased OH- mass transfer barrier with modification of hydrophilic QA groups. Owing to its structural advantages, the TAPPCo-QA COF catalyst exhibited a significantly enhanced ORR turnover frequency and alleviated voltage drop in the high-mass transport region during the single-cell test. This design strategy of "ion channel-in-catalyst" may serve as a platform for the application of versatile molecular catalysts in electrochemical energy conversion applications where both high intrinsic electrocatalytic activity and effective ion transport are required.

SCI

English

Others

National Natural Science Foundation of China["21978260","22178307"]

Chemistry ; Energy & Fuels ; Materials Science

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary

WOS:000869856000001

ROYAL SOC CHEMISTRY

Web of Science

1.Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China
2.Zhejiang Univ, Dept Polymer Sci & Engn, MOE Key Lab Macromol Synth & Functionalizat, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
4.Chongqing Univ, Sch Chem & Chem Engn, State Key Lab Power Transmiss Equipment & Syst Se, Chongqing Key Lab Chem Proc Clean Energy & Resour, Chongqing 400044, Peoples R China
5.Zhejiang Univ, Ningbo Res Inst, Ningbo 315100, Zhejiang, Peoples R China

Ren, Rong,Yang, Liting,Lin, Zhang,et al. Construction of symbiotic one-dimensional ionic channels in a cobalt-based covalent organic framework for high-performance oxygen reduction electrocatalysis[J]. Journal of Materials Chemistry A,2022.

Ren, Rong.,Yang, Liting.,Lin, Zhang.,Li, Xiaoyu.,Zhang, Shuomeng.,...&He, Qinggang.(2022).Construction of symbiotic one-dimensional ionic channels in a cobalt-based covalent organic framework for high-performance oxygen reduction electrocatalysis.Journal of Materials Chemistry A.

Ren, Rong,et al."Construction of symbiotic one-dimensional ionic channels in a cobalt-based covalent organic framework for high-performance oxygen reduction electrocatalysis".Journal of Materials Chemistry A (2022).