應用於染料敏化太陽能電池的光致變色銅(I)錯合物染料合成及性質探討

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题名:	應用於染料敏化太陽能電池的光致變色銅(I)錯合物染料合成及性質探討
作者:	沈正皓;Shen, Jen-Hao
贡献者:	化學學系
关键词:	光致變色材料;銅(I)錯合物;染料敏化太陽能電池;螺噁嗪;金屬-配位基電荷轉移;Photochromic materials;Copper(I) complex;Dye-sensitized solar cells (DSCs));Spirooxazine;Metal-to-Ligand charge transfer
日期:	2025-08-26
上传时间:	2025-10-17 11:39:28 (UTC+8)
出版者:	國立中央大學
摘要:	應用光致變色材料於染料敏化太陽電池(Dye-Sensitized Solar Cells (DSCs))，可藉光照後共軛結構改變且顏色改變的特性，實現理想的建築整合式太陽能電池(Building-Integrated Photovoltaics (BIPV))。儘管如此，迄今具光致變色特性的金屬錯合物染料尚未被成功應用於染料敏化太陽能電池，因此本研究將光致變色基團螺噁嗪(Spirooxazine)導入銅(I)錯合物中，合成具光致變色特性的銅(I)錯合物染料(Pre-CYC-61-Cu和CYC-65-Cu)。為避免Spirooxazine開環處結構重組(Rearrangement)導致光致變色特性消失，透過加入NaOH至L61m THF溶液，或將L65m MeOH溶液避光靜置12小時的方式，使Spirooxazine在配位時穩定在合環形式，成功合成Pre-CYC-61-Cu和CYC-65-Cu。開環形式的CYC-65-Cu DMSO溶液展現出優異的光響應特性，照射波長597 nm的暖白光僅1分鐘即快速合環(遠小於L65m的20分鐘)，且於波長617 nm的吸收度可大幅減少64%，並可在照光結束後60秒內快速回復至初始值，此外，CYC-65-Cu與Pre-CYC-61-Cu的DMSO溶液，在5至8次光照循環皆維持高回復速率，顯見兩光致變色材料優異的抗疲勞性。最終，CYC-65-Cu敏化元件在模擬太陽光照射下展現顯著的顏色變化，是世界上首個成功應用於染料敏化太陽能電池的光致變色金屬錯合物染料，其敏化元件在照射模擬太陽光15分鐘後即由深綠色變為淡黃色，並在照光結束1小時內顏色回復至綠色。CYC-65-Cu敏化元件的短路電流密度與光電轉換效率在照光過程中顯著提高，最終在光穩態時，CYC-65-Cu敏化元件光電轉換效率達0.78%。;Photochromic materials integrated into Dye-Sensitized Solar Cells (DSCs) render a promising strategy for realizing smart building-integrated photovoltaics (BIPVs), relying on their ability to change color and absorption upon irradiation. However, to date, the successful application of photochromic metal complex dyes in DSCs has remained elusive. This study addresses this gap by introducing a photochromic spirooxazine moiety into copper(I) complexes, resulting in the synthesis of two novel photochromic copper(I) complexes, Pre-CYC-61-Cu and CYC-65-Cu. To prevent the rearrangement of the spirooxazine ring-opening structure, which can cause a loss of photochromism, we stabilized spirooxazine in its closed form during coordination. This was achieved by adding NaOH to the THF solution of L61m and keeping the MeOH solution of L65m in dark for 12 hours, respectively. Pre-CYC-61-Cu and CYC-65-Cu complexes exhibited outstanding photoresponsive properties. The open form of CYC-65-Cu DMSO solution demonstrated a rapid photo-induced ring-closing reaction, with a 64% decrease of absorbance at 617 nm just after one minute irradiation (597 nm warm white LED light). It’s significantly faster than 20 minutes L65m required. Both CYC-65-Cu and Pre-CYC-61-Cu DMSO solutions showed high reversibility, with the initial absorbance recovering within 60 seconds after irradiation. They also maintained a fast recovery rate after 5 to 8 irradiation cycles, indicating remarkable fatigue resistance. Remarkably, the CYC-65-Cu-sensitized device demonstrated a prominent color change upon exposure to simulated sunlight, transitioning from deep green to light yellow within 15 minutes. This makes it the first successful application of a photochromic metal complex dye in DSCs. The device′s color reverted to green within one hour after switching off the incident light. During irradiation, both short-circuit current density and power conversion efficiency of the CYC-65-Cu-sensitized device significantly increased, reaching a maximum power conversion efficiency of 0.78% under photostationary state.
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