金属离子消耗会影响多个循环中电池电极去离子的稳定性和性能,Environmental Science & Technology - X-MOL

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金属离子消耗会影响多个循环中电池电极去离子的稳定性和性能
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-03-30 , DOI: 10.1021/acs.est.0c08629
Le Shi ₁ , Evan Newcomer ₁ , Moon Son ₁ , Vineeth Pothanamkandathil ₁ , Christopher A. Gorski ₁ , Ahmed Galal ₂ , Bruce E. Logan ₁

Affiliation

普鲁士蓝六氰合铁酸盐（HCF）材料，例如六氰合铁酸铜（CuHCF）和六氰合铁酸镍（NiHCF），由于阳离子嵌入HCF结构中而在电化学水去离子中用作电极材料时，比纯电容材料具有更高的除盐能力。限制HCF材料应用的因素之一是它们在多个循环中的去离子性能下降。通过在多循环去离子测试中检查CuHCF和NiHCF电极在三种不同pH值（2.5、6.3和10.2）下的性能，发现容量损失（CuHCF高达73％，NiHCF高达39％）是有联系的通过分析电极金属的溶解度，将其还原到不同的氧化还原活性中心铜和铁均作为Na ^+的活性中心CuHCF中的铁元素是NiHCF中的活性中心。Na ⁺与活性中心之间的这种相互作用通过将性能下降与在不同pH值（铁的最高0.86±0.14 mg / L和0.42±0.17 mg的多个循环）中收集的污水溶液中这些金属离子的浓度相关联来证明。 / L（对于CuHCF中的铜）和0.38±0.05 mg / L（对于NiHCF中的铁）。当将适当的金属盐（铜或镍）添加到进料溶液中以抑制电极溶解时，两种材料都更稳定（CuHCF的衰减小于11％，NiHCF的衰减没有）。在pH值为2.5时，质子与Na ⁺离子之间的竞争加剧，从而降低了Na ⁺去除量降低了两种电极材料去离子的热力学能量效率。因此，尽管酸性pH提供最稳定的性能，但周围pH可用于在性能和寿命之间取得更好的平衡。

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Metal-Ion Depletion Impacts the Stability and Performance of Battery Electrode Deionization over Multiple Cycles

Prussian blue hexacyanoferrate (HCF) materials, such as copper hexacyanoferrate (CuHCF) and nickel hexacyanoferrate (NiHCF), can produce higher salt removal capacities than purely capacitive materials when used as electrode materials during electrochemical water deionization due to cation intercalation into the HCF structure. One factor limiting the application of HCF materials is their decay in deionization performance over multiple cycles. By examining the performance of CuHCF and NiHCF electrodes at three different pH values (2.5, 6.3, and 10.2) in multiple-cycle deionization tests, losses in capacity (up to 73% for CuHCF and 39% for NiHCF) were shown to be tied to different redox-active centers through analysis of dissolution of electrode metals. Both copper and iron functioned as active centers for Na⁺ removal in CuHCF, while iron was mainly the active center in NiHCF. This interaction of Na⁺ and active centers was demonstrated by correlating the decrease in performance to the concentration of these metal ions in the effluent solutions collected over multiple cycles at different pHs (up to 0.86 ± 0.14 mg/L for iron and 0.42 ± 0.17 mg/L for copper in CuHCF and 0.38 ± 0.05 mg/L for iron in NiHCF). Both materials were more stable (<11% decay for CuHCF and no decay for NiHCF) when the appropriate metal salt (copper or nickel) was added to the feed solutions to inhibit electrode dissolution. At a pH of 2.5, there was an increased competition between protons and Na⁺ ions, which decreased the Na⁺ removal amount and lowered the thermodynamic energy efficiency for deionization for both electrode materials. Therefore, while an acidic pH provided the most stable performance, a circumneutral pH would be useful to produce a better balance between performance and longevity.

更新日期：2021-04-20

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