無鉛且空氣穩定之銻系列鈣鈦礦電觸媒應用於染料敏化太陽能電池：鈍化劑立體障礙之影響
No Thumbnail Available
Date
2022
Authors
Journal Title
Journal ISSN
Volume Title
Publisher
Abstract
空氣且電化學穩定之銻系列無鉛鈣鈦礦（烷基胺鈍化和芳香胺鈍化的FA3(Sb2-xGex)(Br9-yIy)薄膜）可通過簡單的一步滴塗法成功製備。透過不同的表面鈍化劑，包括三種烷基胺（單正丁基溴化銨、二正丁基溴化銨和四正丁基溴化銨）和四種芳香胺（2,2’-聯吡啶、4,4’-聯吡啶、1,10-菲咯啉和三苯胺），這些空氣穩定之FA3(Sb2-xGex)(Br9-yIy)薄膜主要由結晶相或非晶相的二維三方FA3Sb2Br9組成，且含有少量二維三方和零維六方FA3Sb2I9結晶。在不同的烷基胺中，表面鈍化劑上的正丁基取代基越少，可促使越多二維鈣鈦礦顆粒之形成，且提供較低的立體障礙，誘導二維鈣鈦礦顆粒沿著更嚴格的一維方向組裝。單正丁基溴化銨鈍化之NF/TiO2/FA3(Sb2-xGex)(Br9-yIy)電極提供了8.82%的電池效率，可歸因於：(1)一級胺的有效鈍化、(2)高薄膜粗糙度/電催化活性位點、(3）可自組裝一維之微米柱進行良好的電子傳輸。在不同的芳香胺中，1,10-菲咯啉鈍化之NF/TiO2/FA3(Sb2-xGex)(Br9-yIy)電極達到了8.38%的電池效率，可歸因於：(1)剛性的銻-1,10-菲咯啉配位化合物的有效鈍化、(2)高薄膜粗糙度/電催化活性位點、(3）三維微米立方體有利於電子轉移。這兩種成功鈍化之NF/TiO2/FA3(Sb2-xGex)(Br9-yIy)電極可媲美傳統的白金電極（8.78%），顯示著空氣穩定的銻系列鈣鈦礦具備應用於多種電化學元件之巨大潛力。關鍵字 : 空氣穩定、電催化劑、無鉛、表面鈍化、二維結構
Air-stable and electrochemical sustainable lead-free perovskites, the alkyl-amine-passivated and aryl-amine-passivated FA3(Sb2-xGex)(Br9-yIy), were successfully prepared via a one-step drop-coating process. With the present of various surfacts, including three alkyl-amines (mono-n-butylammonium bromide, di-n-butylammonium bromide, and tetra-n-butylammonium bromide) and four aryl-amines (2,2’-bipyridine, 4,4’-bipyridine, 1,10-phenanthroline, and triphenylamine), the decent air-stability were obtained in several FA3(Sb2-xGex)(Br9-yIy) filmes, which were all mainly composed of 2D trigonal FA3Sb2Br9 (in good crystalline or in amorphous phase) with minor 2D-trigonal/0D-hexagonal FA3Sb2I9 crystalline. Among different alkyl-amines, the fewer n-butyl substitutions on the surfactant not only caused the more formation of 2D perovskite particles, but also induced the assembly of the 2D perovskite particles through the more restrict 1D direction due to the less steric hindrance. Then the MBAB-passivated NF/TiO2/FA3(Sb2-xGex)(Br9–yIy) electrode provided the optimal cell efficiency of 8.82% due to (1) efficient passivation by primary amine, (2) high film roughness/electro-catalytic active sites, and (3) good charge transfer via the self-assembled 1D micro-rod. Among different aryl amines, the 1,10-Phen-passivated NF/TiO2/FA3(Sb2-xGex)(Br9–yIy) electrode reached the optimal cell efficiency of 8.38% due to (1) efficient passivation by rigid Sb-1,10-Phen coordinated compound, (2) high film roughness/electro-catalytic active sites, and (3) good charge transfer via the 3D micro-cube. Both of the MBAB-passivated and 1,10-Phen-passivated NF/TiO2/FA3(Sb2-xGex)(Br9–yIy) electrodes showed a comparable performance to the NF/Pt electrode (8.78%), implying a great potential of air-stable Sb-based perovskite for multiple electrochemical applications.Keywords: Air-stability, Electro-catalyst, Lead-free, Surface passivation, Two-dimensional structure
Air-stable and electrochemical sustainable lead-free perovskites, the alkyl-amine-passivated and aryl-amine-passivated FA3(Sb2-xGex)(Br9-yIy), were successfully prepared via a one-step drop-coating process. With the present of various surfacts, including three alkyl-amines (mono-n-butylammonium bromide, di-n-butylammonium bromide, and tetra-n-butylammonium bromide) and four aryl-amines (2,2’-bipyridine, 4,4’-bipyridine, 1,10-phenanthroline, and triphenylamine), the decent air-stability were obtained in several FA3(Sb2-xGex)(Br9-yIy) filmes, which were all mainly composed of 2D trigonal FA3Sb2Br9 (in good crystalline or in amorphous phase) with minor 2D-trigonal/0D-hexagonal FA3Sb2I9 crystalline. Among different alkyl-amines, the fewer n-butyl substitutions on the surfactant not only caused the more formation of 2D perovskite particles, but also induced the assembly of the 2D perovskite particles through the more restrict 1D direction due to the less steric hindrance. Then the MBAB-passivated NF/TiO2/FA3(Sb2-xGex)(Br9–yIy) electrode provided the optimal cell efficiency of 8.82% due to (1) efficient passivation by primary amine, (2) high film roughness/electro-catalytic active sites, and (3) good charge transfer via the self-assembled 1D micro-rod. Among different aryl amines, the 1,10-Phen-passivated NF/TiO2/FA3(Sb2-xGex)(Br9–yIy) electrode reached the optimal cell efficiency of 8.38% due to (1) efficient passivation by rigid Sb-1,10-Phen coordinated compound, (2) high film roughness/electro-catalytic active sites, and (3) good charge transfer via the 3D micro-cube. Both of the MBAB-passivated and 1,10-Phen-passivated NF/TiO2/FA3(Sb2-xGex)(Br9–yIy) electrodes showed a comparable performance to the NF/Pt electrode (8.78%), implying a great potential of air-stable Sb-based perovskite for multiple electrochemical applications.Keywords: Air-stability, Electro-catalyst, Lead-free, Surface passivation, Two-dimensional structure
Description
Keywords
空氣穩定, 電催化劑, 無鉛, 表面鈍化, 二維結構, Air-stability, Electro-catalyst, Lead-free, Surface passivation, Two-dimensional structure