Journal
CELL REPORTS PHYSICAL SCIENCE
Volume 3, Issue 3, Pages -Publisher
CELL PRESS
DOI: 10.1016/j.xcrp.2022.100804
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Funding
- National Key Research and Development Program of China [2017YFA0204800]
- Natural Science Foundation of Shandong Province [ZR2021QB201]
- Program of Qilu Young Scholars of Shandong University [62460082163005]
- Science Foundation for Outstanding Young Scholars of Shandong Province
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In this study, an iron single-atom catalyst confined in a covalent organic framework exhibited outstanding oxygen evolution reaction (OER) performance, with high mass activity and record-low overpotential and Tafel slope. This work provides design strategies for advanced electrocatalysis through the prudent confinement of unusually coordinated single-atom catalysts.
The exploration of environmentally friendly and highly efficient oxygen evolution reaction (OER) catalysts is vital to large-scale, electrochemical renewable-fuels generation. Here, we report an iron single-atom catalyst (SAC) confined in a covalent organic framework (Fe-SAC@COF), which constitutes an unusual Fe-NO coordination in the skeleton. The as-prepared Fe-SAC@COF exhibits a high mass activity of 9.20 A mg(-1), which is 1.95 times higher than Ni species of the same coordination and 5.05 times higher than nanoparticulate Fe counterpart. Moreover, it shows, to the best of our knowledge, a record-low overpotential (290 mV) and Tafel slope (40 mV dec(-1)) among the reported atomically dispersed Fe-based catalysts and surpasses the benchmark Ir/C catalyst. The density functional theory calculation shows that the Fe-NO coordination exhibits low binding energy of oxygenated intermediates, which leads to an outstanding electrocatalytic OER performance. This work provides design strategies toward unusually coordinated SACs by prudent COF confinement for advanced electrocatalysis.
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