Nanocasting SiO2 into metal-organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts

被引:446
作者
Jiao, Long [1 ]
Zhang, Rui [1 ]
Wan, Gang [2 ]
Yang, Weijie [3 ]
Wan, Xin [4 ]
Zhou, Hua [5 ]
Shui, Jianglan [4 ]
Yu, Shu-Hong [1 ]
Jiang, Hai-Long [1 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Collaborat Innovat Ctr Suzhou Nano Sci & Technol, Dept Chem,CAS Key Lab Soft Matter Chem, Hefei 230026, Anhui, Peoples R China
[2] Argonne Natl Lab, Mat Sci Div, Lemont, IL 60439 USA
[3] North China Elect Power Univ, Sch Energy & Power Engn, Baoding 071003, Peoples R China
[4] Beihang Univ, Sch Mat Sci & Engn, Beijing 100083, Peoples R China
[5] Argonne Natl Lab, Xray Sci Div, Adv Photon Source, Lemont, IL 60439 USA
基金
中国博士后科学基金;
关键词
EFFICIENT OXYGEN REDUCTION; ACTIVE-SITES; CARBON; EVOLUTION; CATALYSTS; NANOPARTICLES; GRAPHENE; SURFACE; HYBRID;
D O I
10.1038/s41467-020-16715-6
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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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页数:7
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