A Metal–Organic Framework with Mixed Electron Donor TTF and Electron Acceptor NDI Ligands for High-Performance Hybrid Lithium-Ion Capacitors
Jun-Die Zhang, Ruo-Nan Wang, Wei Liu, Zi-Yi Wang, Yu-Chuan Tan, Qin-Yu Zhu（朱琴玉）*
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123,PR China
Inorg. Chem.2025, 64, 6250−6258
Abstract: Integrating mixed electron donor (D) and electron acceptor (A) ligands intometal−organic frameworks (MOFs) is an effective yet relatively unexplored approach forimproving the anode performance of hybrid lithium-ion capacitors (HLICs). In this study, usingan electron donor 2,6-bis(4’-pyridyl)tetrathiafulvalene and an electron acceptor N,N’-bis(5-isophthalic acid) naphthalene diimide as ligands, a new Zn-TTF/NDI MOF (1) is constructedas a pseudocapacitive anode of HLICs. Crystallographic characterization revealed that MOF 1adopts a two-dimensional (2D) coordination network. Athree-dimensional(3D) supra-molecular framework is formed through face-to-face TTF packing of the adjacent 2D layers. Asa result, the 2D MOF 1 with both electron-donating TTF and electron-accepting NDI units notonly has rich active sites and excellent charge conductivity for reversible Li+ storage but also,owing to its 3D-supramolecular architecture, provides open channels for ion transport, leading to the merits of enhanced capacityutilization and high power density. The MOF 1||activated carbon HLIC exhibited maximum specific energy (133.7 Wh kg−1) andhigh specific power (12.9 kW kg−1) with stable cycling performance. The remarkable performance originates from the synergisticeffect of the mixed electron-donating TTF and electron-withdrawing NDI ligands, interligand charge transfer, and structural stability.
Article information: //doi.org/10.1021/acs.inorgchem.5c00059
