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Abstract Natural systems, synthetic materials, and devices almost always feature interphases that control the flow of mass and energy or stabilize interfaces between incompatible materials. With technologies transitioning to non‐planar and 3D mesoscale architectures, novel deposition methods for realizing ultrathin coatings and interphases are required. Polymer networks are of particular interest for their tunable chemical and physical properties combined with their structural integrity. Here, the electrodeposition of polymer networks (EPoN) is introduced as a general approach to uniformly coat non‐planar conductive materials. Conceptually, EPoN utilizes electrochemically activated crosslinkers as polymer end groups to confine their network formation exclusively to the material surface upon charge transfer, yielding a passivating and self‐limiting growth of conformal and uniform coatings with tunable submicron thickness on conductive materials. EPoN is found to result in thin functional films of various polymer backbones and side group chemistries as demonstrated for poly(ether) and poly(acrylamide) based polymers as solid electrolyte and thermally responsive interphases, respectively.
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This content will become publicly available on November 14, 2025
Cathodic electrodeposition of polymer networks as ultrathin films on 3-D micro-architected electrodes
Advances in precision coatings are critical in enhancing the functionality of porous materials and the performance of three-dimensionally (3-D) micro-architected devices in applications ranging from molecular sorption and separation to energy storage and conversion. To address this need, we report the cathodic electrodeposition of polymer networks (EPoN) that utilizes the coupling between pre-synthesized polymers with electrochemically active end groups and a complementary crosslinker to form a step-growth polymer network. The electrochemically mediated crosslinking reaction confines the network formation to the electrode surface in a passivating and self-limiting film growth, preventing uncontrolled precipitation and deposition away from the surface. The cathodic electrodeposition is compatible with a variety of conductive substrates, which is demonstrated for 3-D carbons and metals with micron-scale pores of high aspect ratio. The entire pore surface of the 3-D electrodes is enveloped by a conformal polymer thin film that is free of detectable defects and highly electronically insulating for its potential use as an ultrathin artificial electrolyte interphase or solid polymer electrolyte. Since our EPoN concept decouples the polymer functionality from its electrodeposition chemistry, we envision it to be a widely applicable method to coat various conductive non-planar and micro-architected 3-D substrates with polymers of broad functionalities.
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- Award ID(s):
- 2146597
- PAR ID:
- 10633985
- Publisher / Repository:
- Royal Society of Chemistry
- Date Published:
- Journal Name:
- RSC Applied Polymers
- Volume:
- 2
- Issue:
- 6
- ISSN:
- 2755-371X
- Page Range / eLocation ID:
- 1139 to 1146
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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