Reversible lithium storage in sp2 hydrocarbon frameworks

DOI: 10.1016/j.jechem.2021.07.019

Authors: Zhangxiang Hao (University College London (UCL)) , Junrun Feng (University College London (UCL)) , Yiyun Liu (University College London) , Liqun Kang (University College London (UCL)) , Bolun Wang (University College London (UCL)) , Junwen Gu (University College London) , Lin Sheng (University College London (UCL)) , Ruoyu Xu (University College London) , Sushila Marlow (University College London) , Dan J.l. Brett (University College London) , Yunhui Huang (Huazhong University of Science and Technology) , Feng Ryan Wang (University College London)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of Energy Chemistry , VOL 1

State: Published (Approved)
Published: July 2021
Diamond Proposal Number(s): 22572 , 21641 , 22604 , 26717 , 29407

Abstract: Polymer materials offer controllable structure-dependent performances in separation, catalysis and drug release. Their molecular structures can be precisely tailored to accept Li+ for energy storage applications. Here the design of sp2 carbon-based polyphenylene (PPH) with high lithium-ion uptakes and long-term stability is reported. Linear-PPH (L-PPH) exceeds the performance of crosslink-PPH (C-PPH), due to the fact that it has an ordered lamellar structure, promoting the Li+ intercalation/deintercalation channel. The L-PPH cell shows a clear charge and discharge plateau at 0.35 and 0.15 V vs. Li+/Li, respectively, which is absent in the C-PPH cell. The Li+ storage capacity of L-PPH is five times that of the C-PPH. The reversible storage capacity is further improved to 261 mAh g−1 by functionalizing the L-PPH with the –SO3H groups. In addition, the Li-intercalated structures of C-PPH and L-PPH are investigated via near-edge X-ray absorption fine structure (NEXAFS), suggesting the high reversible Li+ - C=C bond interaction at L-PPH. This strategy, based on new insight into sp2 functional groups, is the first step toward a molecular understanding of the structure storage-capacity relationship in sp2 carbon-based polymer.

Journal Keywords: Lithium-ions battery; Organic anode; Topological structure; sp2 hydrocarbon

Diamond Keywords: Batteries; Lithium-ion

Subject Areas: Materials, Chemistry, Energy

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: B07-C-Versatile Soft X-ray beamline: Ambient Pressure XPS and NEXAFS , E01-JEM ARM 200CF

Added On: 03/08/2021 09:19

Discipline Tags:

Energy Storage Energy Physical Chemistry Energy Materials Chemistry Materials Science Polymer Science

Technical Tags:

Microscopy Spectroscopy Electron Microscopy (EM) Transmission Electron Microscopy (TEM) X-ray Absorption Spectroscopy (XAS) Near Edge X-ray Absorption Fine Structures (NEXAFS) Scanning Transmission Electron Microscopy (STEM)