Title: Secondary-Atom-Assisted Synthesis of Single Iron Atoms Anchored on N-Doped Carbon Nanowires for Oxygen Reduction Reaction

Abstract

The development of efficient Fe–N–C materials enriched with single-atom Fe sites toward the oxygen reduction reaction (ORR) is still a great challenge because Fe atoms are mobile and easily aggregate into nanoparticles during the high-temperature treatment. Herein, we proposed a facile and universal secondary-atom-assisted strategy to prepare atomic iron sites with high density hosted on porous nitrogen-doped carbon nanowires (Fe–NCNWs). The Fe–NCNWs showed an impressive half-wave potential ($$E$$_1/2) of 0.91 V and average kinetic current density ($$J$$_K) of 6.0 mA cm^–2 at 0.9 V in alkaline media. They also held a high ORR activity in acidic solution with the $$E$$_1/2 of 0.82 V and average $$J$$_K of 8.0 mA cm^–2 at 0.8 V. Density functional theory calculations demonstrated that the high ORR activity achieved is originated from single-atom iron sites that decrease the energy barrier in the reaction path efficiently.

Authors:

Li, Jin-Cheng ^[1]; Xiao, Fei ^[2]; Zhong, Hong ^[3]; Li, Tao ^[4]; Xu, Mingjie ^[5]; Ma, Lu ^[6]; Cheng, Min ^[7]; Liu, Dong ^[3]; Feng, Shuo ^[3]; Shi, Qiurong ^[3]; Cheng, Hui-Ming  ^[7];

• Search DOE PAGES for author "Cheng, Hui-Ming"
• Search DOE PAGES for ORCID "0000-0002-5387-4241"

Liu, Chang ^[7]; Du, Dan  ^[3];

• Search DOE PAGES for author "Du, Dan"
• Search DOE PAGES for ORCID "0000-0003-1952-4042"

Beckman, Scott P. ^[3]; Pan, Xiaoqing  ^[8];

• Search DOE PAGES for author "Pan, Xiaoqing"
• Search DOE PAGES for ORCID "0000-0002-0965-8568"

Lin, Yuehe  ^[3];

• Search DOE PAGES for author "Lin, Yuehe"
• Search DOE PAGES for ORCID "0000-0003-3791-7587"

Shao, Minhua  ^[2]

• Search DOE PAGES for author "Shao, Minhua"
• Search DOE PAGES for ORCID "0000-0003-4496-0057"

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+ Show Author Affiliations

1. Hong Kong Univ. of Science and Technology (Hong Kong). Fok Ying Tung Research Inst.; Washington State Univ., Pullman, WA (United States). School of Mechanical and Materials Engineering; Chinese Academy of Sciences (CAS), Shenyang (China). Shenyang National Lab. for Materials Science, Inst. of Metal Research
2. Hong Kong Univ. of Science and Technology (Hong Kong). Fok Ying Tung Research Inst.
3. Washington State Univ., Pullman, WA (United States). School of Mechanical and Materials Engineering
4. Northern Illinois Univ., DeKalb, IL (United States). Dept. of Chemistry and Biochemistry; Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
5. Hong Kong Univ. of Science and Technology (Hong Kong). Fok Ying Tung Research Inst.; Univ. of California, Irvine, CA (United States). Irvine Materials Research Inst. (IMRI), Dept. of Chemical Engineering and Materials Science
6. Northern Illinois Univ., DeKalb, IL (United States). Dept. of Chemistry and Biochemistry
7. Chinese Academy of Sciences (CAS), Shenyang (China). Shenyang National Lab. for Materials Science, Inst. of Metal Research
8. Univ. of California, Irvine, CA (United States). Irvine Materials Research Inst. (IMRI), Dept. of Chemical Engineering and Materials Science

Publication Date:

Tue May 28 00:00:00 EDT 2019

Research Org.:

Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:

National Key Research and Development Program of China; USDOE Office of Science (SC)

OSTI Identifier:

1570447

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

ACS Catalysis

Additional Journal Information:

Journal Volume: 9; Journal Issue: 7; Journal ID: ISSN 2155-5435

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Fe-N; carbon nanowire; density functional theory; oxygen reduction; single-atom catalysts