Kottaichamy Alagar Raja, Deebansok Siraprapha, Deng Jie, Nazrulla Mohammed Azeezulla, Zhu Yachao, Bhat Zahid Manzoor, Devendrachari Mruthyunjayachari Chattanahalli, Vinod Chathakudath Prabhakaran, Nimbegondi Kotresh Harish Makri, Fontaine Olivier, Thotiyl Musthafa Ottakam
Indian Institute of Science Education and Research (IISER) Pune Dr Homi Bhabha Road Pashan Pune 411008 India
Molecular Electrochemistry for Energy Laboratory, VISTEC Rayong 21210 Thailand
Chem Sci. 2023 May 17;14(23):6383-6392. doi: 10.1039/d3sc01692g. eCollection 2023 Jun 14.
The essence of any electrochemical system is engraved in its electrical double layer (EDL), and we report its unprecedented reorganization by the structural isomerism of molecules, with a direct consequence on their energy storage capability. Electrochemical and spectroscopic analyses in combination with computational and modelling studies demonstrate that an attractive field-effect due to the molecule's structural-isomerism, in contrast to a repulsive field-effect, spatially screens the ion-ion coulombic repulsions in the EDL and reconfigures the local density of anions. In a laboratory-level prototype supercapacitor, those with β-structural isomerism exhibit nearly 6-times elevated energy storage compared to the state-of-the-art electrodes, by delivering ∼535 F g at 1 A g while maintaining high performance metrics even at a rate as high as 50 A g. The elucidation of the decisive role of structural isomerism in reconfiguring the electrified interface represents a major step forward in understanding the electrodics of molecular platforms.
任何电化学系统的本质都铭刻在其双电层（EDL）中，我们报告了分子结构异构对其进行的前所未有的重组，这对它们的能量存储能力产生了直接影响。电化学和光谱分析与计算和建模研究相结合表明，与排斥场效应相反，分子结构异构产生的吸引场效应在空间上屏蔽了双电层中的离子-离子库仑排斥，并重新配置了阴离子的局部密度。在实验室级原型超级电容器中，具有β-结构异构的超级电容器与最先进的电极相比，储能提高了近6倍，在1 A g下可提供约535 F g的电容，即使在高达50 A g的电流密度下仍能保持高性能指标。阐明结构异构在重新配置带电界面中的决定性作用是理解分子平台电动力学方面向前迈出的重要一步。
