Efficient Bulk Heterojunction CH3NH3PbI3-TiO2 Solar Cells with TiO2 Nanoparticles at Grain Boundaries of Perovskite by Multi-Cycle-Coating Strategy

perovskite grains act as donor and the TiO2 nanoparticles act as acceptor, is reported. This efficient BHJ PSC was simply solution processed from a mixed precursor of CH3NH3PbI3 (MAPbI(3)) and TiO2 nanoparticles. With dissolution and recrystallization by multi-cycle-coating, a unique composite structure ranging from a MAPbI(3) TiO2-dominated layer on the substrate side to a pure perovskite layer on the top side is formed, which is beneficial for the blocking of possible contact between TiO2 and the hole transport material at the interface. Scanning electron microscopy clearly shows that TiO2 nanoparticles accumulate along the grain boundaries (GBs) of perovskite. The TiO2 nanoparticles at the GBs quickly extract and reserve photogenerated electrons before they transport into the perovskite phase, as described in the multitrapping model, retarding the electron hole recombination and reducing the energy loss, resulting in increased V-oc and fill factor. Moreover, the pinning effect of the TiO2 nanoparticles at the GBs from the strong bindings between TiO2 and MAPbI(3) suppresses massive ion migration along the GBs, leading to improved operational stability and diminished hysteresis. Photoluminescence (PL) quenching and PL decay confirm the efficient exciton dissociation on the heterointerface. Electrochemical impedance spectroscopy and open-circuit photovoltage decay measurements show the reduced recombination loss and improved carrier lifetime of the BHJ PSCs. This novel strategy of device design effectively combines the benefits of both planar and mesostructured architectures whilst avoiding their shortcomings, eventually leading to a high PCE of 17.42% under 1 Sun illumination. The newly proposed approach also provides a new way to fabricate a TiO2-containing perovskite active layer at a low temperature.