The organic molecular 2,2',7,7'-tetrakis(4,4'-dimethoxy-3-methyldiphenylamino)-9,9'-spirobifluorene (Spiro-MeOTAD) is known as a typical hole transport material in the development of an all-solid-state perovskite solar cell (PSC). Spiro-MeOTAD requires additives of lithium bifurflimide (LiTFSI) and 4--butylpyridine (tBP) to increase the conductivity and solubility for enhancing the photovoltaic performance of PSCs. However, those additives have an adverse effect on the thermal stability. We report on the origin of instability of additive-containing Spiro-MeOTAD at 85 °C and the methodology to solve the thermal instability. We have found that the interaction of LiTFSI with the underneath perovskite surface facilitated by diffusive tBP is responsible for thermal degradation. Degasification of tBP from the Spiro-MeOTAD film is found to be the key to achieving thermally stable PSCs, where the optimal degassing process achieves 90% of the initial power conversion efficiency (PCE) at 85 °C after 1000 h.
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