Dopamine-integrated all-hydrogel multi-electrode arrays for neural activity recording

Investigation of brain neural circuits is essential for deciphering the diagnostics and therapeutics of neurodegenerative diseases. The main concerns with traditional rigid metal electrodes include intrinsic mechanical mismatch between sensing electrodes and tissues, unavoidable foreign body responses, and inadequate spatiotemporal resolution, resulting in a deficiency of sensing performance. All-hydrogel neural electrodes with multi-electrode arrays (MEAs) suggest a viable way to modulate the trade-off between tissue-mechanical compliance and excellent spatiotemporal recording capacity, but still face the issues of insufficient conductivity and unstable interlayer bonding. Herein, we constructed a four-layer all-hydrogel neural electrode, by sandwiching a conductive hydrogel layer within two encapsulation hydrogel layers, with a shielding hydrogel layer located on top. We introduce a dual-strategy treatment to induce controllable phase separation in poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hydrogel, which achieved ultra-high conductivity (up to 4176 S cm-1) comparable to that of metals and precise spatial resolution (similar to 15 mu m) suitable for single neuron recording. In addition, the utilization of polyphenol chemistry mediated adaptive adhesion endowed this neural electrode with flexible and stable interlayer bonding among conductive-encapsulation-shielding layers and the tissue-electrode interface. Consequently, the all-hydrogel neural electrode exhibited a tenfold higher signal-to-noise ratio than a commercial silver electrode, realized the recording of weak neural activity signals within single and multiple neurons in epileptic rats, and applied man-made stimulation to the cerebral cortex of rats during seizures. This work provides a useful tool to understand the development, function and treatment of neurodegenerative diseases. A four-layer all-hydrogel neural electrode, utilizing dual-strategy for PEDOT:PSS phase separation and polyphenol chemistry for interlayer adhesion, captures ECoG in epileptic rats, demonstrating its potential for advanced neuroscience applications.