Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 40, Pages 21685-21690Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202107053
Keywords
defects; electrochemistry; metal-organic frameworks (MOFs); oxygen reduction reaction; single-atom catalyst
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Funding
- National Key Research and Development Program of China [2020YFB1506300]
- National Natural Science Foundation of China [21625102, 21971017, 21922502, 21802003, 22075018, 51991344, 52025025, 52072400]
- Beijing Institute of Technology Research Fund Program
- Natural Science Foundation of Hainan Province [2019RC166]
- Beijing Natural Science Foundation [Z190010]
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The study focuses on developing transition metal single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) by using a decarboxylation-induced defects strategy to enhance their intrinsic activity. A gas-transport method was used to produce defective Co SACs (Co@DMOF) from carboxylate/amide mixed-linker MOF (DMOF), showing improved ORR activity compared to Co@ZIF-8-900.
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.
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