Xiaomeng Hou

Synergy of ammonium chloride and moisture on perovskite crystallization for efficient printable mesoscopic solar cells

Organometal lead halide perovskites have been widely used as the light harvester for high-performance solar cells. However, typical perovskites of methylammonium lead halides (CH3NH3PbX3, X=Cl, Br, I) are usually sensitive to moisture in ambient air, and thus require an inert atmosphere to process. Here we demonstrate a moisture-induced transformation of perovskite crystals in a triple-layer scaffold of TiO2/ZrO2/Carbon to fabricate printable mesoscopic solar cells. An additive of ammonium chloride (NH4Cl) is employed to assist the crystallization of perovskite, wherein the formation and transition of intermediate CH3NH3X·NH4PbX3(H2O)2 (X=I or Cl) enables high-quality perovskite CH3NH3PbI3 crystals with preferential growth orientation. Correspondingly, the intrinsic perovskite devices based on CH3NH3PbI3 achieve an efficiency of 15.6% and a lifetime of over 130 days in ambient condition with 30% relative humidity. This ambient-processed printable perovskite solar cell provides a promising prospect for mass production, and will promote the development of perovskite-based photovoltaics.

Enhanced electronic properties in CH3NH3PbI3via LiCl mixing for hole-conductor-free printable perovskite solar cells

By mixing perovskite MAPbI3 (MA = CH3NH3+) with LiCl, an effective one-step drop-coating approach was developed to improve the performance of hole-conductor-free printable perovskite solar cells. The LiCl-mixed perovskite exhibited superior electronic properties because of the improved conductivity of the perovskite layer enabling faster electron transport. LiCl-mixing also improved the crystallinity and morphology of the perovskite layer. As a consequence, perovskite solar cells prepared using the LiCl-mixed perovskite as the light harvester produced higher performances compared with the unmixed perovskite, improving the power conversion efficiency from 10.0% to 14.5%.

Tunable hysteresis effect for perovskite solar cells

Perovskite solar cells (PSCs) usually suffer from a hysteresis effect in current–voltage measurements, which leads to an inaccurate estimation of the device efficiency. Although ion migration, charge trapping/detrapping, and accumulation have been proposed as a basis for the hysteresis, the origin of the hysteresis has not been apparently unraveled. Herein we reported a tunable hysteresis effect based uniquely on open-circuit voltage variations in printable mesoscopic PSCs with a simplified triple-layer TiO2/ZrO2/carbon architecture. The electrons are collected by the compact TiO2/mesoporous TiO2 (c-TiO2/mp-TiO2) bilayer, and the holes are collected by the carbon layer. By adjusting the spray deposition cycles for the c-TiO2 layer and UV-ozone treatment, we achieved hysteresis-normal, hysteresis-free, and hysteresis-inverted PSCs. Such unique trends of tunable hysteresis are analyzed by considering the polarization of the TiO2/perovskite interface, which can accumulate positive charges reversibly. Successfully tuning of the hysteresis effect clarifies the critical importance of the c-TiO2/perovskite interface in controlling the hysteretic trends observed, providing important insights towards the understanding of this rapidly developing photovoltaic technology.

Improved Performance of Printable Perovskite Solar Cells with Bifunctional Conjugated Organic Molecule

A bifunctional conjugated organic molecule 4-(aminomethyl) benzoic acid hydroiodide (AB) is designed and employed as an organic cation in organic-inorganic halide perovskite materials. Compared with the monofunctional cation benzylamine hydroiodide (BA) and the nonconjugated bifunctional organic molecule 5-ammonium valeric acid, devices based on AB-MAPbI3 show a good stability and a superior power conversion efficiency of 15.6% with a short-circuit current of 23.4 mA cm-2 , an open-circuit voltage of 0.94 V, and a fill factor of 0.71. The bifunctional conjugated cation not only benefits the growth of perovskite crystals in the mesoporous network, but also facilitates the charge transport. This investigation helps explore new approaches to rational design of novel organic cations for perovskite materials.

Effect of guanidinium on mesoscopic perovskite solar cells

Hole-conductor-free printable mesoscopic perovskite solar cells based on a TiO2/ZrO2/carbon architecture have attracted much attention due to their low material cost and simple fabrication process. However, the micron-thick mesoporous scaffold always challenges the filling of the perovskite absorber and causes significant charge carrier loss. We employ a multifunctional additive of guanidinium chloride (GuCl) to improve the quality of the CH3NH3PbI3 perovskite absorber, and suppress the recombination reaction in the device. It is found that GuCl effectively enhances the charge carrier lifetimes of the perovskite, and suppresses charge carrier loss in the hole-conductor-free devices. Correspondingly, the open-circuit voltage (VOC) of the device is significantly enhanced from 0.88 V to 1.02 V.

Boron-Doped Graphite for High Work Function Carbon Electrode in Printable Hole-Conductor-Free Mesoscopic Perovskite Solar Cells

Work function of carbon electrodes is critical in obtaining high open-circuit voltage as well as high device performance for carbon-based perovskite solar cells. Herein, we propose a novel strategy to upshift work function of carbon electrode by incorporating boron atom into graphite lattice and employ it in printable hole-conductor-free mesoscopic perovskite solar cells. The high-work-function boron-doped carbon electrode facilitates hole extraction from perovskite as verified by photoluminescence. Meanwhile, the carbon electrode is endowed with an improved conductivity because of a higher graphitization carbon of boron-doped graphite. These advantages of the boron-doped carbon electrode result in a low charge transfer resistance at carbon/perovskite interface and an extended carrier recombination lifetime. Together with the merit of both high work function and conductivity, the power conversion efficiency of hole-conductor-free mesoscopic perovskite solar cells is increased from 12.4% for the pristine graphite electrode-based cells to 13.6% for the boron-doped graphite electrode-based cells with an enhanced open-circuit voltage and fill factor.

Spacer improvement for efficient and fully printable mesoscopic perovskite solar cells

Highly dispersible TiO2@ZrO2 nanoparticles are synthesized to prepare an ultra-flat and crack-free spacer film, leading to an enhanced insulating ability compared to a conventional spacer. The average power conversion efficiency of fully printable mesoscopic perovskite solar cells is improved from 10.2% to 12.5%, and the highest steady output power conversion efficiency is 13.8%.