Search for: All records

Conjugated polymers are at the heart of numerous current and emerging technologies. Doping, a process by which charge carriers are introduced, is crucial to their functionality and performance. Despite significant historical context and the exploration of a broad chemical space, doping processes that are activated by formation of a ground-state charge-transfer complex (GS-CTC), which is mediated by the supramolecular hybridization between the frontier molecular orbitals of distinct molecular species, remain poorly understood. There are no clear demonstrations of this phenomena in contemporary donor–acceptor (DA) conjugated polymers (CP). Here, using diketopyrrolopyrrole-based donor–acceptor semiconducting polymers and a -conjugated penta-t-butylpentacyanopentabenzo[25]annulene “cyanostar” macrocycle, we demonstrate the first examples of features that control GS-CTC formation in contemporary DA CP frameworks. Using complementary experimental techniques and theory, we articulate how subtle molecular, electronic, and solid-state features impact supramolecular hybridization of the frontier molecular orbitals and impact the resultant (opto)electronic, magnetic, and transport properties. These studies demonstrate that subtle effects arising from the admixture between distinct -conjugated materials can have dramatic outcomes on properties and performance through modification of the density of states (DOS). These results will enable completely new design rules for organic semiconductors with precise property control. 

A point-of-use electrochemical phosphate sensor is achieved with electrodeposited mixed-valence molybdenum oxide on flexible electrodes, enabling selective detection in complex aqueous environments. 

The main bottlenecks that hinder the performance of rechargeable zinc electrochemical cells are their limited cycle lifetime and energy density. To overcome these limitations, this work studied the mechanism of a dual-ion Zn-Cu electrolyte to suppress dendritic formation and extend the device cycle life while concurrently enhancing the utilization ratio of zinc and thereby increasing the energy density of zinc ion capacitors (ZICs). The ZICs achieved a best-in-class energy density of 41 watt hour per kilogram with a negative-to-positive (n/p) electrode capacity ratio of 3.10. At the n/p ratio of 5.93, the device showed a remarkable cycle life of 22,000 full charge-discharge cycles, which was equivalent to 557 hours of discharge. The cumulative capacity reached ~581 ampere hour per gram, surpassing the benchmarks of lithium and sodium ion capacitors and highlighting the promise of the dual-ion electrolyte for delivering high-performance, low-maintenance electrochemical energy supplies. 

Structural supercapacitors reach high performance with a gradient electrolyte and redox polymer electrodes.