High-Performance, Long-Life, Rechargeable Li-CO2 Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

Chuangang Hu; Lele Gong; Ying Xiao; Yifei Yuan; Nicholas M Bedford; Zhenhai Xia; Lu Ma; Tianpin Wu; Yi Lin; John W Connell; Reza Shahbazian-Yassar; Jun Lu; Khalil Amine; Liming Dai

doi:10.1002/adma.201907436

High-Performance, Long-Life, Rechargeable Li-CO₂ Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

Adv Mater. 2020 Apr;32(16):e1907436. doi: 10.1002/adma.201907436. Epub 2020 Feb 28.

Authors

Chuangang Hu^{1

2}, Lele Gong³, Ying Xiao^{1

2}, Yifei Yuan^{4

5}, Nicholas M Bedford⁶, Zhenhai Xia³, Lu Ma⁷, Tianpin Wu⁷, Yi Lin⁸, John W Connell⁹, Reza Shahbazian-Yassar⁴, Jun Lu⁵, Khalil Amine⁵, Liming Dai^{1

2}

Affiliations

¹ Center of Advanced Science and Engineering for Carbon (Case4carbon), Department of Macromolecular Science and Engineering, Case Western Reserve University, 10900 Euclid Avenue, Cleveland, OH, 44106, USA.
² The UNSW-CWRU International Joint Laboratory, School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
³ Department of Materials Science and Engineering, and Department of Chemistry, University of North Texas, Denton, TX, 76203, USA.
⁴ Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL, 60439, USA.
⁵ Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, Chicago, IL, 60607, USA.
⁶ Particle and Catalysis Research Group, School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
⁷ Advanced Photon Source, X-ray Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL, 60439, USA.
⁸ National Institute of Aerospace, 100 Exploration Way, Hampton, VA, 23666, USA.
⁹ Advanced Materials and Processing Branch, NASA Langley Research Center, Hampton, VA, 23681, USA.

PMID: 32108387
DOI: 10.1002/adma.201907436

Abstract

A highly efficient cathode catalyst for rechargeable Li-CO₂ batteries is successfully synthesized by implanting single iron atoms into 3D porous carbon architectures, consisting of interconnected N,S-codoped holey graphene (HG) sheets. The unique porous 3D hierarchical architecture of the catalyst with a large surface area and sufficient space within the interconnected HG framework can not only facilitate electron transport and CO₂ /Li⁺ diffusion, but also allow for a high uptake of Li₂ CO₃ to ensure a high capacity. Consequently, the resultant rechargeable Li-CO₂ batteries exhibit a low potential gap of ≈1.17 V at 100 mA g^-1 and can be repeatedly charged and discharged for over 200 cycles with a cut-off capacity of 1000 mAh g^-1 at a high current density of 1 A g^-1 . Density functional theory calculations are performed and the observed appealing catalytic performance is correlated with the hierarchical structure of the carbon catalyst. This work provides an effective approach to the development of highly efficient cathode catalysts for metal-CO₂ batteries and beyond.

Keywords: 3D carbon; bifunctional catalysis; holey graphene; rechargeable Li-CO 2 batteries; single-atom catalysts.

Abstract

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