隨著綠色能源需求量的上升，太陽能電池的發展已成為被關注且日趨重要的議題。近年來，鈣鈦礦太陽能電池(Perovskite solar cells, PSCs)被視為極具潛力，以相對低的製造成本，將太陽光有效地轉換成電能的一種新興科技。然而，PSCs欲走向商業化，必須克服幾項重大挑戰，其困境也成為本研究三大研究目的之動機: (I) 研製石墨烯(reduced graphene oxide, rGO)作為鈣鈦礦太陽能電池之低成本電洞傳輸材料；(II) 混摻維他命C (vitamin C)於CH3NH3PbI3¬層，以增加PSCs的操作穩定性；(III) 發展再活化廢棄PSCs的新穎方法，以減少其原料中「鉛」對於環境危害的疑慮及影響。

以簡單、低成本的方式製備石墨烯，並以掃描式電子顯微鏡(SEM)、穿透式電子顯微鏡(TEM)、X光繞射(XRD)、拉曼光譜(Raman)、傅立葉轉換光譜(FTIR)及X光電子能譜(XPS)進行材料特性分析。當混摻0.05 wt% rGO於CH3NH3PbI3¬層中，電池的光電轉換效率可達9%，顯著優於沒加入石墨烯的PSCs (6%)。加入石墨烯，會促使CH3NH3PbI3結晶性的增加及電子電洞再結合率的下降，其可能成為混摻石墨烯PSCs效率提高的主要原因。

當PSCs於空氣中進行連續照光的穩定性測試，可觀察到未混摻維他命C的CH3NH3PbI3迅速地被分解，且在光照3小後轉換效率便下降到原本的一半。而當混摻2.5 wt% vitamin C於¬主動層中，CH3NH3PbI3有較佳的操作穩定性，在光照11小後光電轉換效率僅下降約10%。因此，活性氧化物種(ROS)可能在分解CH3NH3PbI3前，能有效被維他命C去除。

利用碳電極具孔洞結構的特性，發展以簡單製程再活化廢棄PSCs的方法。在廢棄的PSCs上滴入CH3NH3I溶液後，可復原被分解的CH3NH3PbI3結晶，且在400-800 nm可見光波段的吸收值，相似於未老化的PSCs。 因此，再活化PSCs的光電轉換效率可達初始的70%以上 。

本研究發展PSCs新穎技術，以石墨烯為電洞傳輸層在空氣中製備較穩定且具環境友善性的PSCs。並以此研究為基石，期望未來將PSCs採全固態塗佈方式，大幅應用於已存在之室外向陽屋頂、牆壁及窗戶，大面積製備太陽能牆或屋頂，突破傳統太陽能板昂貴、土地遮蔽的缺點，大幅提升綠色能源產電比率。

The development of photovoltaic cells has been becoming much more important with the increasing world’s green energy demand. Recently, perovskite solar cells (PSCs) have been considered as the promising photovoltaic technology with high energy conversion efficiencies and low fabrication costs. Nevertheless, some challenges need to be overcome when PSCs are considered on a mass-production scale, which therefore motivated three major objectives of this research: (I) to prepare graphene (rGO) for the PSCs as a cost-effective hole conductor；(II) to enhance the operational stability of PSCs by adding a small amount of vitamin C antioxidant in the CH3NH3PbI3；(III) to develop a novel method to reactivate spent PSCs to reduce the negative concerns of the use of lead.

Graphene was prepared from graphite and characterized by SEM, TEM, TGA, XRD, Raman, FTIR, and XPS spectroscopy. Compared to the power conversion efficiency (PCE) of 6% for the PSCs without the incorporation of rGO, the solar cells with 0.05 wt% of rGO in the perovskite layer demonstrate a better PCE up to 9%. The improved efficiencies of the rGO/perovskite hybrid solar cells may be mainly attributed to the increased crystallinity of perovskite and the reduced recombination of electrons and holes.

When exposed to both light and air, the solar cells with CH3NH3PbI3 as a photoactive layer rapidly degrade and exhibit a 50% drop in PCE from its initial value within 3 h. In the presence of 2.5wt% of vitamin C in perovskite layer, the PSC with significantly improved stability shows a relatively small 10% drop in PCE over the 11 h aging period, suggesting that the vitamin C antioxidant may be able to scavenge the reactive oxygen species (ROS) from the perovskite film before ROS discompose CH3NH3PbI3.

Taking the advantage of porous structure in the carbon electrodes, a simple approach for reactivation of spent PSCs was newly developed. After the CH3NH3I solution infiltrated through carbon electrodes, the crystallinity of the aged CH3NH3PbI3 films can be restored. Furthermore, the reactivated perovskite film possesses good light absorption at the wavelength range from 400-800 nm, which is similar the fresh sample. The reactivated PSCs can retain about 70% at least of their original efficiency.

These observations offer a novel method to fabricate relatively stable and environmental-friendly PSCs in air with rGO as the low-cost hole-transporting material. It may also pave a way for layer-by-layer coating of PSCs on any unrestricted substrates in the near future, such as outdoor roofs, walls, and windows. By overcoming the limitations of silicon solar cells, PSCs may make substantial progress towards ubiquitous green energy generation.

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