Control of Crystal Structures and Optical Properties with Hybrid Formamidinium and 2-Hydroxyethylammonium Cations for Mesoscopic Carbon-Electrode Tin-Based Perovskite Solar Cells

Abstract

Alcohol-based bifunctional ammonium cations, 2-hydroxyethylammonium (HEA(+)), HO(CH2)(2)NH3+, were introduced into formamidinium (FA(+)) tin-based perovskites (HEA(x)FA(1-x)Snl(3); x = 0-1) to absorb light in carbon-based mesoscopic solar cells. We found that HEAP cations play a key role to control the crystal structures, the lattice structures altered from orthorhombic (x = 0) to rhombohedral (x = 0.2-0.4) with greater symmetry. When x was increased to 0.6-1.0, tin and iodide vacancies were formed to generate 3D-vacant perovskites (HEA(x)FA(1-x)Sn(0.6)I(2.33), x >= 0.6) with a tetragonal structure. Tin-based perovskites in this series were fabricated into mesoporous solar cells using one-step drop-cast (DC), two-step solvent-extraction (SE), and SE + 3% ethyl-enediammonium diiodide (EDAI(2)) as an additive. After optimization of device performance with the SE + 3% EDAI2 approach, the HEA(0.4)FA(0.6)SnI(3) (HEAT = 40%) device gave the best photovoltaic performance with J(sc) = 18.52 mA cm(-2)) V-OC 371 mV, FF = 0.562, and overall efficiency 17 = 3.9% after the device was stored for a period of 340 h.