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Highly Crystalline and Semiconducting Imine-Based Two-Dimensional Polymers Enabled by Interfacial Synthesis
2020, Sahabudeen, Hafeesudeen, Qi, Haoyuan, Ballabio, Marco, Položij, Miroslav, Olthof, Selina, Shivhare, Rishi, Jing, Yu, Park, SangWook, Liu, Kejun, Zhang, Tao, Ma, Ji, Rellinghaus, Bernd, Mannsfeld, Stefan, Heine, Thomas, Bonn, Mischa, Cánovas, Enrique, Zheng, Zhikun, Kaiser, Ute, Dong, Renhao, Feng, Xinliang
Single-layer and multi-layer 2D polyimine films have been achieved through interfacial synthesis methods. However, it remains a great challenge to achieve the maximum degree of crystallinity in the 2D polyimines, which largely limits the long-range transport properties. Here we employ a surfactant-monolayer-assisted interfacial synthesis (SMAIS) method for the successful preparation of porphyrin and triazine containing polyimine-based 2D polymer (PI-2DP) films with square and hexagonal lattices, respectively. The synthetic PI-2DP films are featured with polycrystalline multilayers with tunable thickness from 6 to 200 nm and large crystalline domains (100–150 nm in size). Intrigued by high crystallinity and the presence of electroactive porphyrin moieties, the optoelectronic properties of PI-2DP are investigated by time-resolved terahertz spectroscopy. Typically, the porphyrin-based PI-2DP 1 film exhibits a p-type semiconductor behavior with a band gap of 1.38 eV and hole mobility as high as 0.01 cm2 V−1 s−1, superior to the previously reported polyimine based materials. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
Ultrathin positively charged electrode skin for durable anion-intercalation battery chemistries
2023, Sabaghi, Davood, Wang, Zhiyong, Bhauriyal, Preeti, Lu, Qiongqiong, Morag, Ahiud, Mikhailovia, Daria, Hashemi, Payam, Li, Dongqi, Neumann, Christof, Liao, Zhongquan, Dominic, Anna Maria, Nia, Ali Shaygan, Dong, Renhao, Zschech, Ehrenfried, Turchanin, Andrey, Heine, Thomas, Yu, Minghao, Feng, Xinliang
The anion-intercalation chemistries of graphite have the potential to construct batteries with promising energy and power breakthroughs. Here, we report the use of an ultrathin, positively charged two-dimensional poly(pyridinium salt) membrane (C2DP) as the graphite electrode skin to overcome the critical durability problem. Large-area C2DP enables the conformal coating on the graphite electrode, remarkably alleviating the electrolyte. Meanwhile, the dense face-on oriented single crystals with ultrathin thickness and cationic backbones allow C2DP with high anion-transport capability and selectivity. Such desirable anion-transport properties of C2DP prevent the cation/solvent co-intercalation into the graphite electrode and suppress the consequent structure collapse. An impressive PF6−-intercalation durability is demonstrated for the C2DP-covered graphite electrode, with capacity retention of 92.8% after 1000 cycles at 1 C and Coulombic efficiencies of > 99%. The feasibility of constructing artificial ion-regulating electrode skins with precisely customized two-dimensional polymers offers viable means to promote problematic battery chemistries.
Ultrathin positively charged electrode skin for durable anion-intercalation battery chemistries
2023, Sabaghi, Davood, Wang, Zhiyong, Bhauriyal, Preeti, Lu, Qiongqiong, Morag, Ahiud, Mikhailovia, Daria, Hashemi, Payam, Li, Dongqi, Neumann, Christof, Liao, Zhongquan, Dominic, Anna Maria, Nia, Ali Shaygan, Dong, Renhao, Zschech, Ehrenfried, Turchanin, Andrey, Heine, Thomas, Yu, Minghao, Feng, Xinliang
The anion-intercalation chemistries of graphite have the potential to construct batteries with promising energy and power breakthroughs. Here, we report the use of an ultrathin, positively charged two-dimensional poly(pyridinium salt) membrane (C2DP) as the graphite electrode skin to overcome the critical durability problem. Large-area C2DP enables the conformal coating on the graphite electrode, remarkably alleviating the electrolyte. Meanwhile, the dense face-on oriented single crystals with ultrathin thickness and cationic backbones allow C2DP with high anion-transport capability and selectivity. Such desirable anion-transport properties of C2DP prevent the cation/solvent co-intercalation into the graphite electrode and suppress the consequent structure collapse. An impressive PF6−-intercalation durability is demonstrated for the C2DP-covered graphite electrode, with capacity retention of 92.8% after 1000 cycles at 1 C and Coulombic efficiencies of > 99%. The feasibility of constructing artificial ion-regulating electrode skins with precisely customized two-dimensional polymers offers viable means to promote problematic battery chemistries.