釩液流電池(VRFB)為目前最有前景的電化學大型儲能系統之一，然而，高生產成本及較低的能量效率仍限制其可行性。因此，發展低成本且有效的電極及觸媒材料為首要條件，為了提高能量密度與作為大型儲能系統的整體性能，人們已經對VRFB的電極改質進行廣泛的研究。
首先，為了增進VRFB中石墨氈(GF)電極對於VO2+/VO2+的電化學活性，我們在GF表面製備一種穩定、高活性且分布均勻的六方晶型的氧化鉭(Ta2O5)，透過掃描式電子顯微鏡(SEM)可以看到Ta2O5均勻分布在GF表面，表面上分布著數量適當且牢固附著的Ta2O5奈米顆粒，能有效提供活性點及提升親水性而使得電解液更容易吸附於電極表面，進而顯著的增進電極的電化學活性。特別的是，從循環伏安法(CV)和交流阻抗譜(EIS)的結果顯示，相較於其他電極，當Ta2O5奈米顆粒與石墨氈重量百分比為0.75 wt%時具有最佳的VO2+/VO2+電化學活性與可逆性，另外，以80 mA cm−2充放電電流密度，單電池能量效率相較於未處理GF約能提升9 %。此外，以相同充放電電流密度循環測試50圈後，並沒有明顯的效率衰減，意味著Ta2O5奈米顆粒依舊牢固地附著在GF表面。
第二，吾人以單一步驟水熱法合成簡單、便宜且導電性佳的W18O49奈米線(W18O49NWs)修飾GF表面用於催化VO2+/VO2+反應，CV及EIS顯示W18O49NWs加速了正極端VO2+/VO2+氧化還原反應的動力學。為了進一步提升W18O49NWs的電化學性能，在氫氣及氬氣的組成氣氛中，調控其比例後高溫燒結，形成富含氧空缺之氫氣處理W18O49NWs(H-W18O49NWs)，作為VRFB單電池之電極。該材料表現出優異的性能，在80 mA cm−2的高電流密度下，分別與W18O49NWs和未處理GF相比，提升約9.1 %與12.5 %的能量效率。H-W18O49NWs擁有如此優越的電化學性能主要歸因於大量的氧空缺，其已被證明為VO2+/VO2+反應的活性點，此外，其均勻性及一維結構促進了電子傳遞的步驟，增加親水性，因此在活性物質的質傳過程中大大降低了極化現象產生，經過一百次充放電的長期穩定性實驗，可以確認其出色的耐久性，且幾乎沒有任何衰退。
最後，我們選用簡單、便宜且有效的氧化鈦鈮-還原氧化石墨烯(TiNb2O7–rGO)奈米複合物於釩液流電池之電化學觸媒，吾人利用分散、混和其前驅物於溶液中並且冷凍乾燥接著退火燒結製備此樣品。TiNb2O7奈米顆粒均勻分散在片狀rGO間，同時TiNb2O7奈米顆粒也分開片狀rGO，此協同效應防止奈米顆粒團聚和片狀rGO的互相堆疊。從循環伏安法和交流阻抗分析得知，在所有製備的樣品中，TiNb2O7–rGO在正極及負極分別對應於VO2+/VO2+和V3+/V2+反應對有最佳的電化學催化活性，促進釩離子反應動力學。相較於原始GF，在80及120 mA cm−2的電流密度下，分別提升了約11.1%及12.34%的能量效率。此優越的電化學性能乃歸因於rGO的高導電性，以及TiNb2O7 和 rGO介面性質所產生的協同效應。此外，經過200圈充放電穩定性測試後，TiNb2O7–rGO幾乎沒有任何活性衰退，證明在長時間測試中TiNb2O7–rGO仍附著在GF表面，足以說明其卓越的電化學活性及穩定性。

As one of the most promising electrochemical energy storage systems, vanadium redox flow battery (VRFB) has received increasing attention due to its attractive features for large-scale storage applications. However, high production cost and the relatively low energy efficiency still limit their feasibility. Therefore, developments of powerful electrocatalyst and electrode materials with low cost are critical for the design of VRFB. To improve the energy density and overall performance for large scale applications, extensive research has been carried out on the electrode modification methods for VRFB.
First, to increase the electrocatalytic activity of graphite felt (GF) electrodes in vanadium redox flow batteries (VRFBs) toward the VO2+/VO2+ redox couple, we prepared stable, high catalytic activity, and uniformly distributed hexagonal Ta2O5 nanoparticles on the surface of GF by varying the Ta2O5 contents. Scanning electron microscopy (SEM) revealed the amount and distribution uniformity of the electrocatalyst on the surface of GF. It was found that the optimum amount and uniformly immobilized Ta2O5 nanoparticles on GF surface provided the active sites, enhanced hydrophilicity and electrolyte accessibility, thus remarkably improved electrochemical performance of GF. In particular, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) results showed that the Ta2O5-GF nanocomposite electrode with weight percentage of Ta2O5 to GF of 0.75 wt% exhibited the best electrochemical activity and reversibility toward the VO2+/VO2+ redox reaction, when compared with the other electrodes. The corresponding energy efficiency was enhanced by ~ 9% at a current density of 80 mA cm−2, as compared with untreated GF. Furthermore, the charge–discharge stability test with 0.75 wt% Ta2O5-GF electrode at 80 mA cm−2 showed that after 50 cycles, there was no obvious attenuation of efficiencies signifying, the best stability of Ta2O5 nanoparticles which strongly adhered on the GF surface.
Second, we synthesized simple, inexpensive, and conductive W18O49 nanowires (W18O49NWs) as electrocatalysts on the surface of GF through the one-step solvothermal process. Cyclic voltammetry and electrochemical impedance spectroscopy studies revealed that W18O49NWs exhibit electrocatalytic effects on a VO2+/VO2+ redox couple on the positive side, which enhance the electrochemical kinetics of the redox reactions. To further improve the electrochemical performance of the W18O49NWs, the sample was thermally annealed with a controlled amount of H2/Ar atmosphere to form oxygen-vacancy–rich hydrogen-treated W18O49NWs (H-W18O49NWs). When used as an electrode in a VRFB single cell, this material demonstrated outstanding performance with 9.1% and 12.5% higher energy efficiency than cells assembled with W18O49NWs and treated GF, respectively, at a high current density of 80 mA cm−2. The superior performance of the H-W18O49NW electrocatalyst-based electrode can be attributed to the presence of numerous oxygen vacancies, which were proven to act as active sites for the VO2+/VO2+ redox reaction. Moreover, the uniformly immobilized and 1D nature of the W18O49NWs facilitated the charge-transport process, enhanced hydrophilicity and electrolyte accessibility, and thus remarkably reduced electrochemical polarization during the mass transfer of active species. The long-term cycling performance confirmed the outstanding durability of the as-prepared H-W18O49NWs–based electrode with negligible activity decay after 100 cycles.
Third, we use a simple, low-cost, and powerful titanium niobium oxide–reduced graphene oxide (TiNb2O7–rGO) nanocomposite electrocatalyst which was synthesized through dispersion and blending in aqueous solution followed by freeze-drying and annealing for all-vanadium redox flow battery (VRFB). The TiNb2O7 nanoparticles are uniformly anchored between the rGO sheets; simultaneously, the rGO sheets are separated using TiNb2O7 nanoparticles. The synergistic effects between them prevent the agglomeration of the nanoparticles and restacking of the rGO sheets. Cyclic voltammetry and electrochemical impedance spectroscopy results reveal that among all prepared samples, the TiNb2O7–rGO nanocomposite electrocatalyst exhibits the most favorable electrocatalytic activity toward VO2+/VO2+ and V3+/V2+ at the positive electrode and the negative electrode, respectively, to facilitate the electrochemical kinetics of the vanadium redox reactions. The corresponding energy efficiency is improved by ~11.1% and 12.34% at current densities of 80 and 120 mA cm−2, respectively, compared with pristine graphite felt. The superior performance of the TiNb2O7–rGO nanocomposite electrode may have been due to the synergistic effects related to the high electronic conductivity of rGO nanosheets and the interfacial properties created within TiNb2O7 and rGO. Furthermore, the charge-discharge stability test demonstrates the outstanding stability of the TiNb2O7–rGO electrodes. The TiNb2O7–rGO-based VRFB exhibits negligible activity decay after 200 cycles. The remarkable electrocatalytic activity and mechanical stability are achieved due to the TiNb2O7–rGO nanocomposite being strongly anchored on the graphite felt surface for a substantial time during repetitive cycling.

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