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|Title:||Synergistic voltaglue adhesive mechanisms with alternating electric fields||Authors:||Singh, Manisha
Yin, Cheong See
Page, Samuel J.
Choudhary, Shyam Kumar
Kulkarni, Giridhar U.
Hanna, John V.
Webster, Richard David
Steele, Terry W. J.
|Keywords:||Engineering::Materials||Issue Date:||2020||Source:||Singh, M., Yin, C. S., Page, S. J., Liu, Y., Wicaksono, G., Pujar, R., . . . Steele, T. W. J. (2020). Synergistic voltaglue adhesive mechanisms with alternating electric fields. Chemistry of Materials, 32(6), 2440-2449. doi:10.1021/acs.chemmater.9b04962||Journal:||Chemistry of Materials||Abstract:||Voltage-activated adhesion is a relatively new discovery that relies on direct currents for initiation of cross-linking. Previous investigations have found that direct currents are linearly correlated to the migration rates of electrocuring, but this is limited by high voltages exceeding 100 V with instances of incomplete curing of voltage-activated adhesives on semiconducting substrates. Practical applications of electrocuring would benefit from lower voltages to mitigate high-voltage risks, especially with regard to potential medical applications. Alternative electrocuring strategies based on alternating current (AC), electrolyte ionic radius, and temperature are evaluated herein. Square-waveform AC electric field is hypothesized to initiate a two-sided curing progression of voltage-activated adhesive (PAMAM-g-diazirine, aka Voltaglue), where initiation occurs at the cathode terminal. Structure–activity relationships of Voltaglue as a function of AC frequency at currents of 1–3 mA are evaluated against direct currents, migration rate, storage modulus, and lap-shear adhesion on ex vivo tissue mimics. Numerous improvements in electrocuring are observed with AC stimulation vs direct current, including a 35% decrease in maximum voltage, 180% improvement in kinetic rates, and 100% increase in lap-shear adhesion at 2 mA. Li+ ion electrolytes and curing at 4 °C shifts curing kinetics by +104% and −22% respectively, with respect to the control ion (Na+ ion at 24 °C), suggesting that electrolyte migration is the rate-limiting step. Li+ ion electrolytes and curing at 50 °C improve storage modulus by 110% and 470%, respectively. Further evaluations of electrocured matrices with 19F NMR, solid-state NMR, and infrared spectroscopy provide insights into the probable cross-linking mechanisms.||URI:||https://hdl.handle.net/10356/142878||ISSN:||0897-4756||DOI:||10.1021/acs.chemmater.9b04962||Rights:||This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.chemmater.9b04962||Fulltext Permission:||embargo_20210331||Fulltext Availability:||With Fulltext|
|Appears in Collections:||MSE Journal Articles|
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