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      Efficient ambient-air-stable HTM-free carbon-based perovskite solar cells with hybrid 2D–3D lead halide photoabsorbers

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          Abstract

          HTM-free carbon-based perovskite solar cells (C-PSCs) with over 11.88% efficiency employing the 2D–3D hybrid perovskite photoabsorber achieve the best ambient-air-stable performance among those of all low-temperature carbon electrode-based PSCs reported so far.

          Abstract

          Hole transport material (HTM)-free carbon-based perovskite solar cells (C-PSCs) have shown much promise because of their excellent stability and low cost. However, the most commonly used three-dimensional (3D) MAPbI 3 photoabsorber is ambient-unstable and incompatible with the low-cost mass-production of C-PSCs. Considering the proven operational stability of two-dimensional (2D) perovskites, we herein attempt to use a series of new 2D–3D hybrid (EA) 2(MA) n−1Pb nI 3n+1 perovskites in C-PSCs. We find that the fabricated (EA) 2(MA) n−1Pb nI 3n+1 films ( n = 20, 10, and 6) exhibit extremely improved ambient and photo-stability under 60 day-ambient conditions. The HTM-free C-PSCs with a structure of ITO/C 60/(EA) 2(MA) n−1Pb nI 3n+1/C retain outstanding power conversion efficiency over 11.88%. Particularly, by tuning the stoichiometry of (EA) 2(MA) n−1Pb nI 3n+1 to n = 6, the n 6-2D device maintains a long-term stability of 93% under ambient conditions after 2160 hours, a thermal stability of 80% after heating at 80 °C over 100 hours, and a photo-stability of 92% under continuous 1 sun illumination over 300 hours, which are apparently superior to those of the MAPbI 3 device ( i.e. ambient stability of 73%; thermal stability of 9%; photo-stability of 67% after 83 hours). To the best of our knowledge, our fabricated C-PSC with the 2D–3D halide photoabsorber exhibits the best ambient-air-stable performance among all low-temperature carbon electrode-based PSCs reported so far.

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          Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c5ee03874j Click here for additional data file.

          Today's best perovskite solar cells use a mixture of formamidinium and methylammonium as the monovalent cations. Adding cesium improves the compositions greatly.
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            Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells

            The formation of a dense and uniform thin layer on the substrates is crucial for the fabrication of high-performance perovskite solar cells (PSCs) containing formamidinium with multiple cations and mixed halide anions. The concentration of defect states, which reduce a cell's performance by decreasing the open-circuit voltage and short-circuit current density, needs to be as low as possible. We show that the introduction of additional iodide ions into the organic cation solution, which are used to form the perovskite layers through an intramolecular exchanging process, decreases the concentration of deep-level defects. The defect-engineered thin perovskite layers enable the fabrication of PSCs with a certified power conversion efficiency of 22.1% in small cells and 19.7% in 1-square-centimeter cells.
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              High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells

              Three-dimensional organic-inorganic perovskites have emerged as one of the most promising thin-film solar cell materials owing to their remarkable photophysical properties, which have led to power conversion efficiencies exceeding 20 per cent, with the prospect of further improvements towards the Shockley-Queisser limit for a single‐junction solar cell (33.5 per cent). Besides efficiency, another critical factor for photovoltaics and other optoelectronic applications is environmental stability and photostability under operating conditions. In contrast to their three-dimensional counterparts, Ruddlesden-Popper phases--layered two-dimensional perovskite films--have shown promising stability, but poor efficiency at only 4.73 per cent. This relatively poor efficiency is attributed to the inhibition of out-of-plane charge transport by the organic cations, which act like insulating spacing layers between the conducting inorganic slabs. Here we overcome this issue in layered perovskites by producing thin films of near-single-crystalline quality, in which the crystallographic planes of the inorganic perovskite component have a strongly preferential out-of-plane alignment with respect to the contacts in planar solar cells to facilitate efficient charge transport. We report a photovoltaic efficiency of 12.52 per cent with no hysteresis, and the devices exhibit greatly improved stability in comparison to their three-dimensional counterparts when subjected to light, humidity and heat stress tests. Unencapsulated two-dimensional perovskite devices retain over 60 per cent of their efficiency for over 2,250 hours under constant, standard (AM1.5G) illumination, and exhibit greater tolerance to 65 per cent relative humidity than do three-dimensional equivalents. When the devices are encapsulated, the layered devices do not show any degradation under constant AM1.5G illumination or humidity. We anticipate that these results will lead to the growth of single-crystalline, solution-processed, layered, hybrid, perovskite thin films, which are essential for high-performance opto-electronic devices with technologically relevant long-term stability.
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                Author and article information

                Contributors
                Journal
                JMCAET
                Journal of Materials Chemistry A
                J. Mater. Chem. A
                Royal Society of Chemistry (RSC)
                2050-7488
                2050-7496
                November 20 2018
                2018
                : 6
                : 45
                : 22626-22635
                Affiliations
                [1 ]Beijing Advanced Innovation Center for Soft Matter Science and Engineering
                [2 ]Beijing University of Chemical Technology
                [3 ]Beijing 100029
                [4 ]China
                [5 ]State Key Laboratory of Organic-Inorganic Composites
                [6 ]Research Center of the Ministry of Education for High Gravity Engineering & Technology
                Article
                10.1039/C8TA07836J
                8383c8cf-0a26-45af-815d-63e625c09798
                © 2018

                http://rsc.li/journals-terms-of-use

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