鋅負(fù)極/水電解液界面上存在著一系列常見的寄生副反應(yīng)，極大的阻礙了水系鋅基器件的大規(guī)模儲能開發(fā)。在鋅負(fù)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(shù)親水聚合物層在長期循環(huán)過程中存在被水溶液溶解的風(fēng)險。傳統(tǒng)的與金屬具有較強結(jié)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(xué)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(jié)性與親水性，設(shè)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(fù)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(xué)，同時可以調(diào)節(jié)其沉積/溶解行為，最終實現(xiàn)了對枝晶和副反應(yīng)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(huán)穩(wěn)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(xiàn)出超過800小時的長循環(huán)壽命。此外， 組成的HAC鋅-活性炭 (AC) 混合超級電容器也表現(xiàn)出了優(yōu)異的電化學(xué)性能，包括將工作電壓提高至2.0 V以及出色的循環(huán)穩(wěn)定性，在10 A g-1下，循環(huán)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(guān)工作以 “Robust Zn anode enabled by a hydrophilic adhesive coating for long-life zinc-ion hybrid supercapacitors”為題發(fā)表于《Chemical Engineering Journal》上。論文第一作者為西南石油大學(xué)博士研究生牛奔和廈門大學(xué)博士研究生李振剛，西南石油大學(xué)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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