Lithium-Ion Dynamic and Storage of Atomically Precise Halogenated Nanographene Assemblies via Bottom-Up Chemical Synthesis.

Graphene has received much scientific attention as an electrode material for lithium-ion batteries because of its extraordinary physical and electrical properties. However, the lack of structural control and restacking issues have hindered its application as carbon-based anode materials for next generation lithium-ion batteries. To improve its performance, several modification approaches such as edge-functionalization and electron-donating/withdrawing substitution have been considered as promising strategies. In addition, group 7A elements have been recognized as critical elements due to their electronegativity and electron-withdrawing character, which are able to further improve the electronic and structural properties of materials. Herein, we elucidated the chemistry of nanographenes with edge-substituted group 7A elements as lithium-ion battery anodes. The halogenated nanographenes were synthesized via bottom-up organic synthesis to ensure the structural control. Our study reveals that the presence of halogens on the edge of nanographenes not only tunes the structural and electronic properties but also impacts the material stability, reactivity, and Li+ storage capability. Further systematic spectroscopic studies indicate that the charge polarization caused by halogen atoms could regulate the Li+ transport, charge transfer energy, and charge storage behavior in nanographenes. Overall, this study provides a new molecular design for nanographene anodes aiming for next-generation lithium-ion batteries.

Dicyanotriphenylamine-Based Polyimides as High-Performance Electrodes for Next Generation Organic Lithium-Ion Batteries.

Aromatic polyimide (PI) derivatives have recently been investigated as redox-active electrode materials for Li-ion batteries because of their high thermal stability and thermo-oxidative stability complemented by excellent solvent resistance, good electrical and mechanical properties, and chemical resistance. In this work, we report two PI derivatives from a newly synthesized 4,4'-diamino-3″,4″-dicyanotriphenylamine (DiCN-TPA) monomer and two dianhydrides, pyromellitic dianhydride (PMDA) and 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA); designated as TPA-PMPI and TPA-NTCPI, respectively, as electrode materials for Li-ion batteries. Characterizations of the PIs reveal excellent thermal stability and bipolar property. The incorporation of DiCN-TPA into the polymer structure resulted to a disordered chain arrangement, thus giving high glass transition temperatures (Tg). Electrochemical performance tests reveal that TPA-NTCPI cathode delivered a reversible specific capacity of 150 mAh g-1 at 0.1 A g-1 and exhibited a stability up to 1000 cycles. On the other hand, TPA-PMPI anode delivered a high specific capacity of up to 1600 mAh g-1 at 0.1 A g-1 after 100 cycles. The electrochemical performance of TPA-NTCPI cathode and TPA-PMPI anode are both among the best compared with other reported aromatic PI-based electrodes. The long cycle lifetime and excellent battery performance further suggest that TPA-NTCPI and TPA-PMPI are promising organic electrode materials for next generation Li-ion batteries.

Development of Magnesium Anode-Based Transient Primary Batteries.

Biodegradable primary batteries, also known as transient batteries, are essential to realize autonomous biodegradable electronic devices with high performance and advanced functionality. In this work, magnesium, copper, iron, and zinc - metals that exist as trace elements in the human body - were tested as materials for biomedical transient electronic devices. Different full cell combinations of Mg and X (where X = Cu, Fe, and Zn and the anodized form of the metals) with phosphate buffered saline (PBS) as electrolyte were studied. To form the cathodes, metal foils were anodized galvanostatically at a current density of 2.0 mA cm-2 for 30 mins. Electrochemical measurements were then conducted for each electrode combination to evaluate full cell battery performance. Results showed that the Mg-Cuanodized chemistry has the highest power density at 0.99 mW/cm2 . Nominal operating voltages of 1.26 V for the first 0.50 h and 0.63 V for the next 3.7 h were observed for Mg-Cuanodized which was discharged at a current density of 0.70 mA cm-2 . Among the materials tested, Mg-Cuanodized exhibited the best discharge performance with an average specific capacity of 2.94 mAh cm-2 , which is comparable to previous reports on transient batteries.