The synergistic effect of high-quality NiO
x
hole transport layers (HTLs) deposited by ion beam sputtering on ITO substrates and the Ti3C2T
x
MXene doping of CH3NH3PbI3 (MAPI) perovskite layers is investigated in order to improve the power conversion efficiency (PCE) of p-i-n perovskite solar cells (PSCs). The 18 nm thick NiO
x
layers are pinhole-free and exhibit large-scale homogeneous surface morphology as revealed by the atomic force microscopy (AFM). The grazing-incidence x-ray diffraction showed a 0.75% expansion of the face-centered cubic lattice, suggesting an excess of oxygen as is typical for non-stoichiometric NiO
x
. The HTLs were used to fabricate the PSCs with MXene-doped MAPI layers. A PSC with undoped MAPI layer served as a control. The size of MAPI polycrystalline grains increased from 430 ± 80 nm to 620 ± 190 nm on the doping, as revealed by AFM. The 0.15 wt% MXene doping showed a 14.3% enhancement in PCE as compared to the PSC with undoped MAPI. The energy-resolved electrochemical impedance spectroscopy revealed one order of magnitude higher density of defect states in the band gap of MXene-doped MAPI layer, which eliminated beneficial effect of reduced total area of larger MAPI grain boundaries, decreasing short-circuit current. The PCE improvement is attributed to a decrease of the work function from −5.26 eV to −5.32 eV on the MXene doping, which increased open-circuit voltage and fill factor.
In this study, inorganic stannite quaternary Cu2M(M = Ni, Co)SnS4 (CMTS) is explored as a low-cost, earth abundant, environmentally friendly and chemically stable hole transport material (HTM). CMTS nanoparticles were synthesized via a facile and mild solvothermal method and processed into aggregated nanoparticle inks, which were applied in n-i-p perovskite solar cells (PSCs). The results show that Cu2NiSnS4 (CNiTS) is more promising as an HTM than Cu2CoSnS4 (CCoTS), showing efficient charge injection as evidenced by considerable photoluminescence quenching and lower series resistance from Nyquist plots, as well as higher power conversion efficiency (PCE). Moreover, the perovskite layer coated by the CMTS HTM showed superior environmental stability after 200 h light soaking in 50% relative humidity, while organic HTMs suffer from a severe drop in perovskite absorption. Although the obtained PCEs are modest, this study shows that the cost effective and stable inorganic CMTSs are promising HTMs, which can contribute towards PSC commercialization, if the field can further optimize CMTS energy levels through compositional engineering.
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