Reliable stability is a prerequisite for the commercialization of PSCs. To explore the self-stability of our devices, highly efficient PSCs in
Fig. 5b (with spiro-OMeTAD as HTL) were stored in a N
2-filled glovebox at room temperature under dark without encapsulation. As shown in
Fig. 5g and Fig. S18a (Supporting information), after 3200 h ambient storage, the CCC modified device retained 102.8% of its original efficiency, whereas the control device remained 98.9% of its initial efficiency. XRD, UV–vis absorption and SEM were conducted to study the aged perovskite films in Fig. S19 (Supporting information). Although the morphology in SEM images and UV–vis absorption of both the films did not change significantly with aging, there was a strong signal of
δ-FAPbI
3 appeared in the XRD pattern of the control device, while the CCC modified sample remained almost unchanged, indicating that the phase stability of perovskites can be significantly enhanced by CCC modification. In order to investigate the resistance of our device to thermal stress, the PSCs with and without CCC treatment were placed on a hotplate at 60 ℃. As shown in
Fig. 5h and Fig. S18b (Supporting information), after 3840 h thermal aging, the CCC modified device retained 84.0% of its original efficiency, more than that of the control one (73.5%). In addition, to exclude the effect of unstable spiro-OMeTAD on the device performance, PTAA was also used instead of spiro-OMeTAD to study the thermostability of PSCs [
71,
72]. As shown in
Fig. 5i and Fig. S18c (Supporting information), after 3024 h thermal aging at 60 ℃, CCC modified device remained a 92.4% of its original efficiency, more than that of the control one (81.5%). The XRD patterns of control perovskite films exhibited stronger signals of
δ-FAPbI
3 and PbI
2 phases than that of the CCC modified perovskite films during thermal tests. But UV–vis absorption of both the films did not change obviously, which could be ascribed to the amount of the perovskite main phase more than that of the decomposition products to a large extent. Moreover, the SEM images of control perovskite films displayed much more holes on the surface compared with the target perovskite films (Figs. S20 and S21 in Supporting information). These results indicate that the decomposition of perovskite under thermal aging can be significantly inhibited by CCC modification. The CCC bound to GBs/surface terminal groups could contribute to the enhanced stability of perovskites by strengthening binding forces and decreasing the surface energy of perovskite films [
30,
73]. Our results manifested that, due to the passivation effect of CCC on different defects, the stability of PSCs can be significantly improved along with the efficiency. Furthermore, in order to investigate the influence of different functional groups on the stability of the perovskite films, we also conducted accelerated aging tests at 100 ℃ for pristine and passivated perovskite films by CC or CCC treatment. As shown in the XRD pattern of Fig. S22 (Supporting information), after 4 days of thermal aging, obvious PbI
2 phase appeared in the unmodified perovskite film, while the main peak (001) of perovskites at 13.99 was significantly reduced. Compared with the aging perovskite films, XRD pattern of one with CC treatment changed only a little. Thus, it is speculated that the alcohol hydroxyl group on CC has the effect of accelerating the decomposition of perovskites (Fig. S1 in Supporting information), which counteracts the effect of enhancing stability due to defect passivation by CC. Surprisingly, after CCC modification, the PbI
2 phase was significantly weakened and the perovskite phase also retained a strong signal, demonstrating that CCC without hydroxyl group can significantly enhance the thermal stability of perovskites. To confirm this, PSCs with or without passivators were heated at a high temperature of 85 ℃ for 2496 h. As shown in Fig. S23a (Supporting information), the control device only retained 65.2% of its initial efficiency, while CC and CCC modified devices maintained 83.3% and 92.0% of their initial efficiency, respectively, demonstrating that CCC modification is superior to CC in improving device stability. The XRD patterns of the CCC modified perovskite films indeed presented weaker signals of
δ-FAPbI
3 and PbI
2 phases than that of other perovskite films after thermal aging, and UV–vis absorption of films did not change apparently (Figs. S23b and c in Supporting information). Moreover, the SEM images of the CCC modified perovskite films hardly did not display holes on the surface compared with the control and CC modified films (Fig. S24 in Supporting information). To confirm the CCC as an effective and universal passivator for different cells, we fabricated the perovskite films
via sequential deposition and then adopted the CCC as a passivator on their surface. In accordance with the PSCs prepared by one-step spin-coating method, we also got a positive result in sequential deposited PSCs as shown in Fig. S25a (Supporting information). In addition, we also used the CCC as a passivator in inverted PSCs (p-i-n) prepared by one-step spin-coating method, which also gave a surprising improvement in PCE (Fig. S25b in Supporting information). We have also tried to use CCC to modify the buried interface of perovskites, but have not got the desired results. The
J-V performance of the devices with CCC modification were displayed in Fig. S26 and Table S7 (Supporting information). It is speculated that the SnO
2 nanocrystals that we fabricated were highly crystalline and coated by Cl
−, which can promote the perovskite crystal growth and improve the charge transfer [
72]. Therefore, this interface could not need to be passivated like the upper interface of perovskite layer. In addition, as an organic compound, CCC may affect the contact and spread of the perovskite precursor solution on the substrate and be not conducive to the crystal growth of perovskite films.