Benign‐by‐Design Solventless Mechanochemical Synthesis of Three‐, Two‐, and One‐Dimensional Hybrid Perovskites

Jodlowski, Alexander D.; Yepez, Alfonso; Luque, Rafael; Camacho, Luis; Miguel, Gustavo de

doi:10.1002/anie.201607397

Cited by 153 publications

(141 citation statements)

References 53 publications

(49 reference statements)

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“…It should be noted that a number of recent publications report on the synthesis Cs 2 [AgIn]Cl 6 [9,10], but its bromide analogue has, to the best of our knowledge, not been reported so far. We used a mechanochemical approach that previously been used successfully for the synthesis of lead halide perovskite materials [11][12][13][14][15]. This technique is advantageous for the formation of compounds with narrow existence region [16].…”

Section: Introductionmentioning

confidence: 99%

Mechanochemical synthesis of the lead-free double perovskite Cs₂[AgIn]Br₆ and its optical properties

et al. 2019

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Hitting hard on the binary halides yields in the formation of Cs 2 [AgIn]Br 6 . The lead-free double perovskite marks, although not usable itself, a further step forward in finding sustainable and durable perovskite materials for photovoltaic applications. Cs 2 [AgIn]Br 6 is one of the prominent examples of double perovskites materials that have been suggested to circumvent the use of lead compounds in perovskite solar cells. We herein report the successful synthesis of the material as bulk powder using a mechanochemical approach. It crystallises in an elpasolite-type structure, an ordered perovskite superstructure, with a cell parameter of a = 11.00 Å. However, the compound exhibits a relatively large optical bandgap of 2.36 eV and is unstable under illumination, which impedes its use as solar absorber material at this early stage. Still, substitution of lead and the potential of this synthesis method are promising as well as the fruitful combination of theoretical considerations with experimental materials discovery.

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Section: Introductionmentioning

confidence: 99%

Mechanochemical synthesis of the lead-free double perovskite Cs₂[AgIn]Br₆ and its optical properties

et al. 2019

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“…More broadly, to increase diversity, it would be necessary to develop methods for integrating insoluble additives into multiple-cation perovskites. Mechanochemical synthesis has recently emerged as a straightforward, solvent-free method for preparing highly pure perovskites, providing rapid access to a variety of simple hybrid iodide and bromide perovskites 23,24,25,26 as well as phase pure mixed-cation perovskites. 27 Here, we show that CsCl, which is insoluble in DMSO and DMF, can be integrated as a new source of Cs into a triple-cation perovskite composition using mechanochemistry.…”

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confidence: 99%

One-step mechanochemical incorporation of an insoluble cesium additive for high performance planar heterojunction solar cells

et al. 2018

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“…The guanidinium cation (Gua) has a Goldschmidt tolerance factor of ≈1.04, and indeed, GuaPbI 3 is a 1D system with no suitable properties for photovoltaics . However, the partial incorporation of Gua into MAPbI 3 has been demonstrated using XRD studies (see Figure 6 ).…”

Section: D Perovskites With Abx3 Formulamentioning

confidence: 99%

Alternative Perovskites for Photovoltaics

Jodlowski

Rodríguez‐Padrón

Luque

et al. 2018

Advanced Energy Materials

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include an optimal band gap energy of ≈1.55 eV, high absorption coefficient (10 4 -10 5 cm −1 ) due to the direct band gap transition, reduced exciton binding energy (10-30 meV) enabling free carrier generation, high charge-carrier mobilities due to low charge effective masses (m h * or m e * ≈ 0.1m 0 ) derived from the large band dispersion, good defect tolerance that avoids the formation of deep trap states and long charge-carrier diffusion lengths. [11][12][13][14][15][16][17][18][19] Additionally, 3D MAPbI 3 is a solutionprocessable material constituted by earthabundant raw materials, which minimizes fabrication costs. [20][21][22][23][24][25] However, there are two important limitations for the further industrial application of these solar devices: the high toxicity of Pb, which poses a risk to humans and causes environmental contamination, and the low stabilities of perovskite materials, which is derived from degradation to its initial precursors due to thermal, moisture and operational effects. [26][27][28][29][30][31][32][33][34][35] Conventional perovskites utilized in photovoltaics exhibit a stoichiometric formula of ABX 3 , where A is a monovalent cation, B is a divalent cation, and X is a halide anion. The perovskite structure is comprised of corner-sharing BX 6 octahedra with in between voids occupied by A cations to achieve charge neutrality (see Figure 1). The perovskite crystal lattice is formed by a 3D network of inorganic octahedra that are primarily responsible for the outstanding optoelectronic properties of this material, including the low binding energy and isotropic charge transport. [12][13][14]36] The size of the A cation suitable for the octahedral voids is experimentally defined by the Goldschmidt tolerance factor t =and R x are the ionic radii for each component. Only A cations with tolerance factors between 0.8 < t < 1.0 give rise to valuable 3D perovskite materials. [37][38][39][40] The main architecture of solar devices fabricated with perovskites is a mesoporous scaffold configuration; however, a planar arrangement offers rivaling PCE values. [36,41] The mesoporous layer is predominately formed by TiO 2 acting as an electrontransport layer (ETL), while the typical solid-state hole-transport layer (HTL) is the organic compound, 2,2′,7,7′-tetrakis(N,N′-di-pmethoxyphenylamine)-9,9′-spirobifluorene (Spiro-OMeTAD). [2,3] In the planar configuration, the ETL layer is usually formed by compact, thin layers of TiO 2 or SnO 2 deposited through different methods. The deposition of the perovskite layer is usually performed by a spin-coating technique from a solution containing the precursors (PbI 2 + MAI for the MAPbI 3 perovskite) and further annealing at ≈120 °C. [5,42] The use of the so-called "antisolvent" method consisting of the addition of a nonpolar solvent during the spin-coating process has been found to provide optimum solar efficiencies. [43,44] The typical layer configuration is The discovery of unique optoelectronic properties of 3D ABX 3 perovskites has produced a great impact ...

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Benign‐by‐Design Solventless Mechanochemical Synthesis of Three‐, Two‐, and One‐Dimensional Hybrid Perovskites

Cited by 153 publications

References 53 publications

Mechanochemical synthesis of the lead-free double perovskite Cs₂[AgIn]Br₆ and its optical properties

Mechanochemical synthesis of the lead-free double perovskite Cs₂[AgIn]Br₆ and its optical properties

One-step mechanochemical incorporation of an insoluble cesium additive for high performance planar heterojunction solar cells

Alternative Perovskites for Photovoltaics

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Benign‐by‐Design Solventless Mechanochemical Synthesis of Three‐, Two‐, and One‐Dimensional Hybrid Perovskites

Cited by 153 publications

References 53 publications

Mechanochemical synthesis of the lead-free double perovskite Cs2[AgIn]Br6 and its optical properties

Mechanochemical synthesis of the lead-free double perovskite Cs2[AgIn]Br6 and its optical properties

One-step mechanochemical incorporation of an insoluble cesium additive for high performance planar heterojunction solar cells

Alternative Perovskites for Photovoltaics

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Mechanochemical synthesis of the lead-free double perovskite Cs₂[AgIn]Br₆ and its optical properties

Mechanochemical synthesis of the lead-free double perovskite Cs₂[AgIn]Br₆ and its optical properties