Decarboxylation‐Induced Defects in MOF‐Derived Single Cobalt Atom@Carbon Electrocatalysts for Efficient Oxygen Reduction

Autor:	Xiao Feng, Siwu Li, Wenxiu Yang, Qinghua Zhang, Jiani Li, Jinwei Zhang, Yanan Gao, Shuai Yuan, Lin Gu, Bo Wang, Linyu Hu
Rok vydání:	2021
Předmět:	Chemistry Decarboxylation Inorganic chemistry General Medicine General Chemistry Electrochemistry Catalysis Metal chemistry.chemical_compound Adsorption Transition metal visual_art visual_art.visual_art_medium Carboxylate Zeolitic imidazolate framework
Zdroj:	Angewandte Chemie International Edition. 60:21685-21690
ISSN:	1521-3773 1433-7851
DOI:	10.1002/anie.202107053
Popis:	Developing transition metal single-atom catalysts (SACs) for oxygen reduction reaction (ORR) is of great importance. Zeolitic imidazolate frameworks (ZIFs) as a subgroup of metal-organic frameworks (MOFs) are distinguished as SAC precursors, due to their large porosity and N content. However, the activity of the formed metal sites is limited. Herein, we report a decarboxylation-induced defects strategy to improve their intrinsic activity via increasing the defect density. Carboxylate/amide mixed-linker MOF (DMOF) was chosen to produce defective Co SACs (Co@DMOF) by gas-transport of Co species to DMOF upon heating. Comparing with ZIF-8 derived SAC (Co@ZIF-8-900), Co@DMOF-900 with more defects yet one fifth Co content and similar specific double-layer capacitance show better ORR activity and eight times higher turnover frequency (2.015 e s-1 site-1 ). Quantum calculation confirms the defects can weaken the adsorption free energy of OOH on Co sites and further boost the ORR process.
Databáze:	OpenAIRE
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