“…In order to address this shortcoming, solid-state hole-transporting material (HTM) 2,2′,7,7′-tetrakis( N , N -di- p -methoxyphenyl-amine)-9,9′-spirobifluorene (Spiro-OMeTAD) was employed as an alternative to liquid electrolyte to successfully construct the first all solid-state mesoscopic heterojunction PSCs featuring a FTO/c-TiO 2 /m-TiO 2 /perovskite/HTM/Au cell configuration that was stable for 500 h, developed by Park and co-workers in 2012, in which the HTM is the key component for extracting/transporting the photogenerated hole from the perovskite to the back contact metal electrode, effectively minimizing charge-recombination loss at the perovskite/HTM interface and thus achieving good device performance in PSCs. − As reported so far, the commercially available Spiro-OMeTAD has been proven to be the most efficient and widely used HTM in most of the highly performing PSCs yielding the record power conversion efficiency (PCE) of PSCs over 25% . However, Spiro-OMeTAD shows low intrinsic hole mobility of about ∼10 –6 cm 2 ·V –1 ·s –1 in its pristine form, resulting in poor photovoltaic performances in devices. − Thus, it is extremely important to improve its hole-transfer ability by introducing some chemical additives such as Li-bis(trifluoromethanesulfonyl)imide (Li-TFSI) into the Spiro-OMeTAD-based film. It has been reported that inclusion of the additive Li-TFSI can promote the oxidative reaction of pristine Spiro-OMeTAD into Spiro-OMeTAD + in the presence of oxygen and accordingly improve hole mobility by at least 2 orders of magnitude and thus obtain high device performance. , Currently, a great number of new HTMs as alternatives to Spiro-OMeTAD have been extensively developed and applied in PSCs because of tedious synthesis and expensive cost of Spiro-OMeTAD; Li-TFSI was found to be a necessary additive in these HTMs for good device photovoltaic performances. − However, the Li-TFSI additive has been identified as the main component heavily responsible for the deterioration of the PSCs performance and stability.…”