Boron Doping of Multiwalled Carbon Nanotubes Significantly Enhances Hole Extraction in Carbon-Based Perovskite Solar Cells

Compared to the conventional perovskite solar cells (PSCs) containing hole-transport materials (HTM), carbon materials based HTM-free PSCs (C-PSCs) have often suffered from inferior power conversion efficiencies (PCEs) arising at least partially from the inefficient hole extraction at the perovskite–carbon interface. Here, we show that boron (B) doping of multiwalled carbon nanotubes (B-MWNTs) electrodes are superior in enabling enhanced hole extraction and transport by increasing work function, carrier concentration, and conductivity of MWNTs. The C-PSCs prepared using the B-MWNTs as the counter electrodes to extract and transport hole carriers have achieved remarkably higher performances than that with the undoped MWNTs, with the resulting PCE being considerably improved from 10.70% (average of 9.58%) to 14.60% (average of 13.70%). Significantly, these cells show negligible hysteretic behavior. Moreover, by coating a thin layer of insulating aluminum oxide (Al₂O₃) on the mesoporous TiO₂ film as a physical barrier to substantially reduce the charge losses, the PCE has been further pushed to 15.23% (average 14.20%). Finally, the impressive durability and stability of the prepared C-PSCs were also testified under various conditions, including long-term air exposure, heat treatment, and high humidity

Colloidal Precursor-Induced Growth of Ultra-Even CH₃NH₃PbI₃ for High-Performance Paintable Carbon-Based Perovskite Solar Cells

Carbon-based hole transport material (HTM)-free perovskite solar cells (PSCs) have attracted intense attention due to their relatively high stability. However, their power conversion efficiency (PCE) is still low, especially for the simplest paintable carbon-based PSCs (C-PSCs), whose performance is greatly limited by poor contact at the perovskite/carbon interface. To enhance interface contact, it is important to fabricate an even-surface perovskite layer in a porous scaffold, which is not usually feasible due to roughness of the crystal precursor. Herein, colloidal engineering is applied to replace the traditional crystal precursor with a colloidal precursor, in which a small amount of dimethyl sulfoxide (DMSO) is added into the conventional PbI₂ dimethylformamide (DMF) solution. After deposition, PbI₂(DMSO) adduct colloids (which are approximately tens of nanometers in size) are stabilized and dispersed in DMF to form a colloidal film. Compared with PbI₂ and PbI₂(DMSO) adduct crystal precursors deposited from pure DMF and DMSO solvents, respectively, the PbI₂(DMSO) adduct colloidal precursor is highly mobile and flexible, allowing an ultra-even surface to be obtained in a TiO₂ porous scaffold. Furthermore, this ultra-even surface is well-maintained after chemical conversion to CH₃NH₃PbI₃ in a CH₃NH₃I solution. As a result, the contact at the CH₃NH₃PbI₃/carbon interface is significantly enhanced, which largely boosts the fill factor and PCE of C-PSCs. Impressively, the achieved champion PCE of 14.58% is among the highest reported for C-PSCs