Journal
NATURE COMMUNICATIONS
Volume 11, Issue 1, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-16715-6
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Funding
- NSFC [21725101, 21871244, 21673213, 21521001]
- China Postdoctoral Science Foundation [2019TQ0298, 2019M660151]
- International Partnership Program of CAS [211134KYSB20190109]
- Fundamental Research Funds for the Central Universities [WK2060030029]
- BSRF
- SSRF
- National Synchrotron Radiation Laboratory Foundation [KY2060000160]
- Fujian Institute of Innovation (CAS)
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Canadian Light Source
- supercomputing system in the Supercomputing Center of University of Science and Technology of China
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Single-atom catalysts (SACs) have sparked broad interest recently while the low metal loading poses a big challenge for further applications. Herein, a dual protection strategy has been developed to give high-content SACs by nanocasting SiO2 into porphyrinic metal-organic frameworks (MOFs). The pyrolysis of SiO2@MOF composite affords single-atom Fe implanted N-doped porous carbon (Fe-SA-N-C) with high Fe loading (3.46wt%). The spatial isolation of Fe atoms centered in porphyrin linkers of MOF sets the first protective barrier to inhibit the Fe agglomeration during pyrolysis. The SiO2 in MOF provides additional protection by creating thermally stable FeN4/SiO2 interfaces. Thanks to the high-density Fe-SA sites, Fe-SA-N-C demonstrates excellent oxygen reduction performance in both alkaline and acidic medias. Meanwhile, Fe-SA-N-C also exhibits encouraging performance in proton exchange membrane fuel cell, demonstrating great potential for practical application. More far-reaching, this work grants a general synthetic methodology toward high-content SACs (such as Fe-SA, Co-SA, Ni-SA). Single-atom catalysts (SACs) with high metal loading are highly desired to improve catalytic performance. Here, the authors report a dual protection strategy by nanocasting SiO2 into metal-organic frameworks to prepare high-loading SACs with excellent catalytic performance toward oxygen reduction.
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