The HCS electrodes were made through the typical slurry-making process. The slurry was stirred in N-methylpyrrolidone (Sigma-Aldrich) solvent with 3:1 HCS/polyvinylidene difluoride ratio for 6 hours and then coated onto a Cu current collector through doctor blading. The electrodes were dried in a vacuum oven overnight. Thin-film coatings were applied directly on HCS electrodes using a Savannah S100 ALD system (Ultratech/Cambridge NanoTech) operated under the exposure mode to ensure high uniformity on high–surface area substrates. The Al2O3 deposition consists of alternating pulse and purge of trimethylaluminum (Sigma-Aldrich) and DI water as precursors at a growth temperature of 150°C. A typical pulse, exposure, and purge sequence for trimethylaluminum and DI water was 0.015 s–15 s–40 s–0.015 s–15 s–40 s. The AlF3 deposition consists of alternating pulse and purge of AlCl3 (>99%, Sigma-Aldrich) and TiF4 (grinded before use, Sigma-Aldrich) as precursors at a growth temperature of 200°C. Both AlCl3 and TiF4 precursors were kept at 120° to 130°C. A typical pulse, exposure, and purge sequence for AlCl3 and TiF4 was 1 s–15 s–30 s–1 s–15 s–30 s.

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