Institution: | 1. Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Haihe Laboratory of Sustainable Chemical Transformations, Renewable Energy Conversion and Storage Center (RECAST), College of Chemistry, Nankai University, Tianjin, 300071 P. R. China
These authors contributed equally to this work.;2. National Supercomputer Center in Tianjin, Tianjin, 300457 P. R. China
These authors contributed equally to this work.;3. Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Haihe Laboratory of Sustainable Chemical Transformations, Renewable Energy Conversion and Storage Center (RECAST), College of Chemistry, Nankai University, Tianjin, 300071 P. R. China;4. College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083 P. R. China. |
Abstract: | High-capacity small organic materials are plagued by their high solubility. Here we proposed constructing hydrogen bond networks (HBN) via intermolecular hydrogen bonds to suppress the solubility of active material. The illustrated 2, 7- diamino-4, 5, 9, 10-tetraone (PTO-NH2) molecule with intermolecular hydrogen (H) bond between O in ?C=O and H in ?NH2, which make PTO-NH2 presents transverse two-dimensional extension and longitudinal π–π stacking structure. In situ Fourier transform infrared spectroscopy (FTIR) has tracked the reversible evolution of H-bonds, further confirming the existence of HBN structure can stabilize the intermediate 2-electron reaction state. Therefore, PTO-NH2 with HBN structure has higher active site utilization (95 %), better cycle stability and rate performance. This study uncovers the H-bond effect and evolution during the electrochemical process and provides a strategy for materials design. |