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Crystallization of perovskite is monitored in carbon-electrode based, low-temperature, mesoscopic perovskite solar cells. Crystallographic and morphological properties of the perovskite are examined through changes in the film thickness of carbon-electrode or the volume of perovskite precursor. It is observed that, when a relatively thin carbon-electrode or large volume of perovskite precursor is used, perovskite crystallites mainly form on the device surface, leaving the bottom part of the device un-wetted. However, if a thicker carbon-electrode or less perovskite precursor is used, crystallization could be seen in the whole porous skeleton, and relative uniform distribution of perovskite crystallites is achieved. As such, uneven crystallization is observed. Such behavior is due to solvent evaporation on the surface, which facilitates nucleation processes on the surface, while retards crystallization on the bottom due to the Ostwald ripening effect. Charge transfer/recombination processes and photo-to-electric power conversion properties are studied. As expected, uneven crystallization results in retarded charge transfer and increased risk of recombination, and poor power conversion efficiency, for example, ∼3%. In contrast, uniform crystallization accelerates charge transfer and reduces recombination risk, and increases the efficiency to higher than 11% (AM1.5G, 100 mW/cm2). 

SnO2 modified mesoporous ZrO2 is used to replace the mesoporous TiO2 layer and serves as a kind of mesoporous electron-transport layer during the low-temperature fabrication of mesoscopic perovskite solar cells that are based on carbon electrode. X-ray/ultraviolet photoelectron spectroscopy studies and electrical test observe that SnO2 modification brought down the work function while increasing the conductivity of the mesoporous ZrO2. Transient photovoltage/photocurrent decay curves, impedance spectroscopy, and photoluminescence mapping show that after the bottom layer of ZrO2 is modified by SnO2, the charge extraction process is accelerated while recombination is retarded. This modification helps to increase the power conversion efficiency from 4.70 (±0.85)% to 10.15 (±0.35)%, along with the optimized efficiency at 13.37% (AM1.5G, 100 mW/cm2) for the low-temperature devices. In addition, the effects of modification layers of SnO2 on the power conversion properties are carefully studied. This study shows that SnO2 modified mesoporous ZrO2 could serve as an efficient electron-transport layer for the low-temperature mesoscopic devices. 

Abstract “Perovskite/carbon” interface is a bottle‐neck for hole‐conductor‐free, carbon‐electrode basing perovskite solar cells due to the energy mismatch and concentrated defects. In this article, in‐situ healing strategy is proposed by doping octylammonium iodide into carbon paste that used to prepare carbon‐electrode on perovskite layer. This strategy is found to strengthen interfacial contact and reduce interfacial defects on one hand, and slightly elevate the work function of the carbon‐electrode on other hand. Due to this effect, charge extraction is accelerated, while recombination is obviously reduced. Accordingly, power conversion efficiency of the hole‐conductor‐free, planar perovskite solar cells is upgraded by ≈50%, or from 11.65 (± 1.59) % to 17.97 (± 0.32) % (AM1.5G, 100 mW cm⁻²). The optimized device shows efficiency of 19.42% and open‐circuit voltage of 1.11 V. Meanwhile, moisture‐stability is tested by keeping the unsealed devices in closed chamber with relative humidity of 85%. The “in‐situ healing” strategy helps to obtain T₈₀time of >450 h for the carbon‐electrode basing devices, which is four times of the reference ones. Thus, a kind of “internal encapsulation effect” has also been reached. The “in situ healing” strategy facilitates the fabrication of efficient and stable hole‐conductor‐free devices basing on carbon‐electrode.