Embedded Micro-Interdigitated Flow Fields for Efficient Intercalation-Based Desalination at Seawater Scale

During the past decade, intensifying water crises around the globe have motivated research in electrochemical desalination. Among such technologies, Faradaic deionization (FDI) has shown great promise for seawater desalination with the use of intercalation electrode materials that possess at least ten-fold higher charge storage concentration (~5 M) than seawater salinity (~0.5 M). Despite many efforts focused either on developing electrode materials or modifying flow-cell architectures, the promise of intercalative FDI was not previously realized experimentally. This work demonstrates for the first time salt removal approaching seawater-level salinity by using a flow cell containing symmetric cation intercalation electrodes separated by an anion-exchange membrane [Do et al., Energy Environ. Sci. , 16 , 3025–3039 (2023)]. We show removal of 96% of salt from ~500 mM NaCl feeds with ~50% water recovery at a thermodynamic energy efficiency (TEE) of 7%. In addition, the flow cell readily produces fresh water (< 0.017 M NaCl) from brackish water with 40% TEE and substantially lowered hypersaline brine concentration from 0.78 M down to 0.23 M at 11.7% TEE. We note that (1) scaling up the charge capacity of intercalation electrodes is crucial to improve salt removal in FDI and (2) rational design of flow-through electrodes is equally important to make FDI more energy-efficient by mitigating pumping energy consumption. Upscaling was achieved by using large-area electrodes with high areal loading of nickel hexacyanoferrate (NiHCF), up to 21 mg cm -2 . Pumping energy was drastically reduced by embedding an interdigitated array of 70 µm wide channels into the NiHCF electrodes using laser micromaching to form novel embedded, micro-interdigitated flow fields (eµ-IDFFs). The dimensions of the eµ-IDFFs were tailored for our low-permeability electrodes based on analytical and numerical modeling, resulting in two orders of magnitude improvement in the apparent hydraulic permeability of these electrodes while minimizing active-material loss. Evidence of water transport between diluted and concentrated streams, as well as feed-concentration-dependent charge efficiency were reported, which potentially contributed to energy efficiency and water recovery losses, motivating their investigation to further improve FDI performance. In addition to their application toward desalination, the present eµ-IDFFs show promise for use in electrochemical energy storage and conversion processes that employ nanomaterials