RESUMO
Hole-transporting layer-free carbon-based perovskite solar cells (HTL-free C-PSCs) hold great promise for photovoltaic applications due to their low cost and outstanding stability. However, the low power conversion efficiency (PCE) of HTL-free C-PSCs mainly results from grain boundaries (GBs). Here, epitaxial growth is proposed to rationally design a hybrid nanostructure of PbI2 nanosheets/perovskite with the desired photovoltaic properties. A post-treatment technique using tri(2,2,2-trifluoromethyl) phosphate (TFEP) to induce in situ epitaxial growth of PbI2 nanosheets at the GBs of perovskite films realizes high-performance HTL-free C-PSCs. The structure model and high-resolution transmission electron microscope unravel the epitaxial growth mechanism. The epitaxial growth of oriented PbI2 nanosheets generates the PbI2 /perovskite heterojunction, which not only passivates defects but forms type-I band alignment, avoiding carrier loss. Additionally, Fourier-transform infrared spectroscopy, 31 P NMR, and 1 H NMR spectra reveal the passivation effect and hydrogen bonding interaction between TFEP and perovskite. As a result, the VOC is remarkably boosted from 1.04 to 1.10 V, leading to a substantial gain in PCE from 14.97% to 17.78%. In addition, the unencapsulated PSC maintains the initial PCE of 80.1% for 1440 h under air ambient of 40% RH. The work offers a fresh perspective on the rational design of high-performance HTL-free C-PSCs.