TY - JOUR
T1 - Construction of Catalytic Covalent Organic Frameworks with Redox-Active Sites for the Oxygen Reduction and the Oxygen Evolution Reaction
AU - Liu, Minghao
AU - Liu, Sijia
AU - Cui, Cheng Xing
AU - Miao, Qiyang
AU - He, Yue
AU - Li, Xuewen
AU - Xu, Qing
AU - Zeng, Gaofeng
N1 - Funding Information:
Q. Xu acknowledges the financial support from the Natural Science Foundation of Shanghai (20ZR1464000). C. Cui acknowledges the financial support from the China Postdoctoral Science Foundation (2021M692908). G. Zeng acknowledge the supports from the National Natural Science Foundation of China (21878322, 22075309), the Science and Technology Commission of Shanghai Municipality (19ZR1479200, 22ZR1470100).
Publisher Copyright:
© 2022 Wiley-VCH GmbH.
PY - 2022/12/5
Y1 - 2022/12/5
N2 - Construction of catalytic covalent organic frameworks (COFs) for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is significant but rarely demonstrated. In this work, we have first constructed bifunctional COFs towards ORR and OER by integrating diarylamine derivatives into the Co-porphyrin based frameworks. Both of the new COFs (CoTAPP-PATA-COF and CoTAPP-BDTA-COF) have good ordered structures, high surface areas, and robust chemical stability. The diarylamine units, as a typical electron donor and redox-active cores, promote intramolecular electron transport along the frameworks and improve the electrochemically active surface areas. Thus, the COFs showed higher catalytic activities than that of the COF without redox-active units. CoTAPP-PATA-COF had a halfwave potential of 0.80 V towards ORR, and delieved an overpotential of 420 mV for OER in 0.1 M KOH. The theoretical calculation revealed introducing diarylamine unites improved the oxygen electrocatalysis.
AB - Construction of catalytic covalent organic frameworks (COFs) for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is significant but rarely demonstrated. In this work, we have first constructed bifunctional COFs towards ORR and OER by integrating diarylamine derivatives into the Co-porphyrin based frameworks. Both of the new COFs (CoTAPP-PATA-COF and CoTAPP-BDTA-COF) have good ordered structures, high surface areas, and robust chemical stability. The diarylamine units, as a typical electron donor and redox-active cores, promote intramolecular electron transport along the frameworks and improve the electrochemically active surface areas. Thus, the COFs showed higher catalytic activities than that of the COF without redox-active units. CoTAPP-PATA-COF had a halfwave potential of 0.80 V towards ORR, and delieved an overpotential of 420 mV for OER in 0.1 M KOH. The theoretical calculation revealed introducing diarylamine unites improved the oxygen electrocatalysis.
KW - Bifunctional Catalysts
KW - Covalent Organic Frameworks
KW - Oxygen Evolution Reaction
KW - Oxygen Reduction Reaction
KW - Redox-Active Sites
UR - http://www.scopus.com/inward/record.url?scp=85141732526&partnerID=8YFLogxK
U2 - 10.1002/anie.202213522
DO - 10.1002/anie.202213522
M3 - Article
C2 - 36240790
AN - SCOPUS:85141732526
SN - 1433-7851
VL - 61
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 49
M1 - e202213522
ER -