鋅負極/水電解液界面上存在著一系列常見的寄生副反應，極大的阻礙了水系鋅基器件的大規模儲能開發。在鋅負極上進行人工聚合物涂層人是解決這一問題的有效途徑。然而，大多數親水聚合物層在長期循環過程中存在被水溶液溶解的風險。傳統的與金屬具有較強結合力的涂層，往往具有疏水性，極大增加了鋅電極/水電解液的界面電阻，進一步抑制了界面離子的遷移。
近日，西南石油大學何顯儒團隊與松山湖材料實驗室王欣團隊合作，通過平衡粘結性與親水性，設計了一種丙烯酸酯型的親水粘接性聚合物涂層(HAC)，作用于鋅負極表面。令人鼓舞的是，該涂層不僅可以增強鋅離子遷移動力學，同時可以調節其沉積/溶解行為，最終實現了對枝晶和副反應出色的抑制效果。研究表明，HAC改性后的鋅對稱電池具有長循環穩定性，即使在較大電流密度5 mA cm-2，容量5 mA cm-2 h下仍表現出超過800小時的長循環壽命。此外， 組成的HAC鋅-活性炭 (AC) 混合超級電容器也表現出了優異的電化學性能，包括將工作電壓提高至2.0 V以及出色的循環穩定性，在10 A g-1下，循環14000次后仍可保持100%的初始比電容。
Fig. 1. Physicochemical properties of HAC. (a) and (b) Contact angles between Bare Zn/HAC-modified Zn electrode and aqueous electrolyte at 5 min; (c) FTIR spectra of HAC before and after plating of Zn2+; (d) Nyquist plots of Zn-Zn symmetric cells with Bare Zn/HAC-modified Zn electrode; (e) Transference number of Zn2+ before and after coating HAC; (f) Stress-strain curve of HAC film.
Fig. 2. Electrochemical stabilities between Zn anode (Bare Zn and HAC-modified Zn) and aqueous electrolyte investigated via galvanostatic electro-plating and stripping processes. (a), (b) and (c) Zn-Zn symmetric cells with Bare Zn and HAC-modified Zn cycled at a current density of 5 mA cm-2, 10 mA cm-2, and varying current densities. Insets of (a) and (b) are the magnified view of voltage profiles. (d) and (e) Top-view SEM images of HAC-modified Zn and Bare Zn surface after cycling at a current density of 1 mA cm-2 with a capacity of 1 mA h cm-2 for 100 h. (f) XRD patterns of Bare Zn and HAC-modified Zn anodes before and after cycling at a current density of 1 mA cm-2 with a capacity of 1 mA h cm-2 for 100 h.
Fig. 3. Electrochemical reversibility between Bare Zn and HAC-modified Zn anodes with aqueous electrolyte. (a) Tafel curves of Bare Zn and HAC-modified Zn. (b) Chronoamperograms (CAs) of Bare Zn and HAC-modified Zn under a -200 mV overpotential. (c) Initial nucleation overpotentials of Zn plating on Ti foil in Bare Zn and HAC-modified Zn asymmetric cells at 5 mA cm-2. (d) Coulombic efficiency (CE) of Zn plating/stripping in Bare Zn-Ti and HAC-modified Zn-Ti cells at a current density of 5 mA cm-2 for 10 min and (e,f) corresponding voltage profiles at various cycles.
Fig. 4. Electrochemical performance of Zn-AC ion hybrid supercapacitors. (a) and (b) Galvanostatic capacity-voltage curves of the Zn-AC hybrid capacitors with Bare Zn and HAC-modified Zn anodes showing a 0.1 V increase in electrochemical window with the introduction of HAC. (c) CV curves at scan rates indicated. (d) and (e) Galvanostatic capacity-voltage curves and long-term cycling stability at 10 A g-1.
Fig. 5. (a) Schematic illustration of morphology evolution for both the symmetric cells with different electrodes during stripping/plating. (b) Comparison of performance among coating-modified Zn anode devices (see Table S1 for references). The selected references have a current density greater than 3 mA cm-2. (c) Comparison of electrochemical performance of cells with Bare Zn and HAC-modified Zn anodes.
相關工作以 “Robust Zn anode enabled by a hydrophilic adhesive coating for long-life zinc-ion hybrid supercapacitors”為題發表于《Chemical Engineering Journal》上。論文第一作者為西南石油大學博士研究生牛奔和廈門大學博士研究生李振剛，西南石油大學何顯儒教授和松山湖材料實驗室王欣研究員為論文共同通訊作者。
原文鏈接：https://doi.org/10.1016/j.cej.2022.136217
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