Author Correction: Persistent and reversible solid iodine electrodeposition in nanoporous carbons

Correction to: Nature Communications https://doi.org/10.1038/s41467-020-18610-6, published online 24 September 2020

Critical Discussion of Ex situ and In situ TEM Measurements on Memristive Devices

Memristors are promising candidates for new memory technologies and are capable to mimic synapses in artificial neural networks. The switching in memristive devices occurs typically in few nanometer thin dielectric layers. The direct observation of the switching mechanism is crucial for better comprehension and improvements of memristors. Therefore, in situ experiments are conducted in a transmission electron microscope (TEM). However, sample preparation processes and electron beam irradiation can lead to a chemical and structural modification of the active layers. Moreover, devices may show significant device-to-device variability due to the details of processing parameters. Thus, it is essential to characterize the identical device electrically before microstructural analysis

Persistent and reversible solid iodine electrodeposition in nanoporous carbons

Aqueous iodine based electrochemical energy storage is considered a potential candidate to improve sustainability and performance of current battery and supercapacitor technology. It harnesses the redox activity of iodide, iodine, and polyiodide species in the confined geometry of nanoporous carbon electrodes. However, current descriptions of the electrochemical reaction mechanism to interconvert these species are elusive. Here we show that electrochemical oxidation of iodide in nanoporous carbons forms persistent solid iodine deposits. Confinement slows down dissolution into triiodide and pentaiodide, responsible for otherwise significant self-discharge via shuttling. The main tools for these insights are in situ Raman spectroscopy and in situ small and wide-angle X-ray scattering (in situ SAXS/WAXS). In situ Raman confirms the reversible formation of triiodide and pentaiodide. In situ SAXS/WAXS indicates remarkable amounts of solid iodine deposited in the carbon nanopores. Combined with stochastic modeling, in situ SAXS allows quantifying the solid iodine volume fraction and visualizing the iodine structure on 3D lattice models at the sub-nanometer scale. Based on the derived mechanism, we demonstrate strategies for improved iodine pore filling capacity and prevention of self-discharge, applicable to hybrid supercapacitors and batteries