Print-and-Plate Architected Electrodes for Electrochemical Transformations Under Flow

Barber, Dylan M. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000161295779); Edgar, Sofía [Harvard Univ., Cambridge, MA (United States)]; Emanuel, Michael S. [Harvard Univ., Cambridge, MA (United States)] (ORCID:000900091900673X); Nelwood, Michael D. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0009000849723046); Ahn, Bok Yeop [Harvard Univ., Cambridge, MA (United States)]; Román‐Manso, Benito [Harvard Univ., Cambridge, MA (United States)]; Cochard, Thomas [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000301447624); Platero, Justin [Harvard Univ., Cambridge, MA (United States); Navajo Technical University, Crownpoint, NM (United States)]; Amini, Kiana [Harvard Univ., Cambridge, MA (United States); Univ. of British Columbia, Vancouver, BC (Canada)] (ORCID:0000000327497048); Rycroft, Chris H. [Harvard Univ., Cambridge, MA (United States); Univ. of Wisconsin, Madison, WI (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000346776990); Rubinstein, Shmuel [Hebrew Univ. of Jerusalem (Israel)] (ORCID:0000000228972579); Aziz, Michael J. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000196579456); Lewis, Jennifer A. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000202802774)

doi:10.1002/adfm.202419748

DOE OSTI · 2555742

Print-and-Plate Architected Electrodes for Electrochemical Transformations Under Flow

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Abstract

Flow cell electrodes are typically composed of porous carbon materials, such as papers, felts, and cloths. However, their random architecture hinders the fundamental characterization of electrode structure-performance relationships during in situ operation of porous electrochemical flow systems. This work describes a “print-and-plate” method that combines direct ink writing of micro-periodic lattices with a two-step metal plating process that converts them into highly conductive (sheet resistance 40 mΩ sq -1 ) electrodes. Their operando performance is assessed in an anthraquinone disulfonic acid half-cell using widefield electrochemical fluorescence microscopy, where output current and fluorescence intensity are in excellent agreement. The pressure drop associated with flow through three electrode designs is determined via simulations from which the most efficient design is identified and manufactured via print-and-plate. Confocal fluorescence microscopy is then used to create a 3D map of the state of charge (SOC) inside this print-and-plate electrode. The experimental state of the charge map is in good agreement with computational predictions. The rapid design, simulation, and fabrication of print-and-plate electrodes enable fundamental investigations of how architected porosity affects electrochemical performance under flow.

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Barber, Dylan M. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000161295779), Edgar, Sofía [Harvard Univ., Cambridge, MA (United States)], Emanuel, Michael S. [Harvard Univ., Cambridge, MA (United States)] (ORCID:000900091900673X), Nelwood, Michael D. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0009000849723046), Ahn, Bok Yeop [Harvard Univ., Cambridge, MA (United States)], Román‐Manso, Benito [Harvard Univ., Cambridge, MA (United States)], Cochard, Thomas [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000301447624), Platero, Justin [Harvard Univ., Cambridge, MA (United States); Navajo Technical University, Crownpoint, NM (United States)], Amini, Kiana [Harvard Univ., Cambridge, MA (United States); Univ. of British Columbia, Vancouver, BC (Canada)] (ORCID:0000000327497048), Rycroft, Chris H. [Harvard Univ., Cambridge, MA (United States); Univ. of Wisconsin, Madison, WI (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000346776990), Rubinstein, Shmuel [Hebrew Univ. of Jerusalem (Israel)] (ORCID:0000000228972579), Aziz, Michael J. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000196579456), Lewis, Jennifer A. [Harvard Univ., Cambridge, MA (United States)] (ORCID:0000000202802774). 2025-03-10. Print-and-Plate Architected Electrodes for Electrochemical Transformations Under Flow. https://doi.org/10.1002/adfm.202419748

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