Air- and water-stable and photocatalytically active germanium-based 2D perovskites by organic spacer engineering

Romani, Lidia; Speltini, Andrea; Chiara, Rossella; Morana, Marta; Coccia, Clarissa; Tedesco, Costanza; Armenise, Vincenza; Colella, Silvia; Milella, Antonella; Listorti, Andrea; Profumo, Antonella; Ambrosio, Francesco; Mosconi, Edoardo; Pau, Riccardo; Pitzalis, Federico; Simbula, Angelica; Ricciarelli, Damiano; Saba, Michele; Medina-Llamas, María; Angelis, Filippo De; Malavasi, Lorenzo

doi:10.1016/j.xcrp.2022.101214

Cited by 7 publications

(10 citation statements)

References 38 publications

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“…Recently Romani and co‐workers demonstrated the photocatalytic activity of water and air‐stable lead‐free PhBz 2 GeBr 4 and PhBz 2 GeI 4 (PhBz = 4‐phenylbenzilammonium) layered perovskites. [ 273 ] The germanium‐based 2D perovskites were tested for simulated solar‐light‐induced hydrogen evolution from water and aqueous solutions of glucose and starch. Further, the heterostructure of the 2D perovskites with graphitic carbon nitride (g‐C 3 N 4 ) enhanced the photocatalytic activity due to the effective charge transfer at the heterojunction between the two semiconductors.…”

Section: Applicationsmentioning

confidence: 99%

Recent Advances and Opportunities in Low‐Dimensional Layered Perovskites for Emergent Applications beyond Photovoltaics

Ghosh

Parveen

Sellin

et al. 2023

Adv Materials Technologies

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Layered metal halide perovskites have attracted enormous research attention over the last few years, befitting their unique optical and electronic properties. Low‐dimensional layered perovskites demonstrate great potential for various optoelectronic and sensing applications beyond photovoltaics. Herein, the recent progress and opportunities in 2D and quasi‐2D perovskites for light‐emitting diodes (LEDs), lasers, memristors, neuromorphic/synaptic applications, UV–vis photodetection, X‐ray detection, scintillators, and photocatalytic applications are reviewed. First, the crystal structure, characteristics, and fundamental properties of 2D layered perovskites are discussed. Recent efforts and developments of 2D and quasi‐2D metal halide perovskite for light‐emitting applications with excellent luminescence properties are reviewed. Unique properties of 2D perovskites, such as negligible leakage current due to restricted carrier transport, high stability, and hydrophobicity, make them viable for memristor devices. After discussing the memristor and neuromorphic devices using 2D perovskites, the outstanding performance of 2D perovskites in UV–vis photodetection including polarization‐sensitive photodetection is discussed. 2D perovskites recently proved as a superior candidate in X‐ray detection with high stability. Further, the scintillation properties of 2D perovskites for the detection of ionizing radiation are discussed. Finally, some of the very recent achievements and present future outlook, including exciting opportunities in this burgeoning field are highlighted.

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Section: Applicationsmentioning

confidence: 99%

Recent Advances and Opportunities in Low‐Dimensional Layered Perovskites for Emergent Applications beyond Photovoltaics

Ghosh

Parveen

Sellin

et al. 2023

Adv Materials Technologies

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“…2D metal halide perovskites (MHPs) are widely investigated for their possible applications in several fields ranging from photovoltaics and photodetection to photocatalysis. [1][2][3][4][5][6] From a structural point of view, both Ruddlesden-Popper and Dion-Jacobson families, of general formula A′2An-1MnX3n+1 and A′An-1MnX3n+1, respectively (where A′ and A= organic cations and n = number of staggered inorganic layers made of metal M and halide X), can be seen as composed by inorganic slabs with octahedrally coordinated metal ions (usually Pb), separated by ammonium organic ligands coordinated to the halides of the octahedra. 1 One of the most appealing characteristics of 2D MHPs is their vast chemical (and in turn structural) tunability which can be modulated by changing the organic spacer, the central atom, and the halide.…”

Section: Introductionmentioning

confidence: 99%

“…However, Ge-containing 2D or even 3D perovskites have been very scarcely considered in the current literature even though some encouraging and interesting properties have been demonstrated in several applicative fields. 6,[11][12][13][14][15][16] Such lack of investigation strongly limits the establishment of solid structure-property correlation in Gebased perovskites which is a pre-requisite to design optimized and novel materials. We recently tried to fill this gap by computationally and experimentally exploring a series of germanium 2D MHPs including aromatic monoammonium cations clarifying the role of different structural distortion parameters on the optical properties.…”

Section: Introductionmentioning

confidence: 99%

“…16 Such work allowed us, for example, to further design air and water stable 2D Ge perovskites for photocatalytic applications or to modulate a broad-band emission through external pressure application. 6,17 In order to provide novel compositions and understanding the role of metal nature and halide alloying on the structural and optical properties of low-dimensional perovskites, we report here the investigation of a novel series of 2D Ge-containing MHPs including decylammonium (DA) as organic spacer.…”

Section: Introductionmentioning

confidence: 99%

“…We afforded since some time a through engineering of stable lead free perovskites trying to provide more environment resistant samples. 5,6,25,26 In this respect, we report here the structural and optical results obtained by exposing the samples for one month to laboratory air (RH around 45%). Figures 7a-h The data clearly demonstrate that iodide-based samples undergo an extended degradation as demonstrated by the XRD patterns showing the appearance of different diffraction patterns (which, at present cannot be assigned to any known phase).…”

Section: Introductionmentioning

confidence: 99%

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Halide Alloying and Role of Central Atom on the Structural and Optical Properties of Decylammonium Germanium 2D Perovskites

Malavasi

Chiara

Accorsi

et al. 2023

Preprint

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We report here a novel series of halide alloyed Ge-containing 2D perovskites including decylammonium as organic spacer, namely DA2Ge(Br1-xIx)4. This system forms a continuous solid solution on the halide site with a modulation of the band gap from 2.74 to 2.17 eV with a rapid decrease up to x=0.5 followed by a plateau. Iodide-rich compositions show enhanced broad RT photoluminescence (PL) which narrows at low temperature with maximum quantum yields for mixed compositions. The replacement of Ge with Pb and Sn in DA2GeBr4 and DA2GeI4 provides a tuning of the band gap in the whole visible spectrum with a marked blue-shift when lead is present and, opposite, a red-shift for Sn replacement. The RT PL progressively broadens moving from Pb to Sn and to Ge covering an emission range from 400 to 800 nm. Finally, the air stability of lead-free 2D perovskites of this work has been determined indicating its improvement by increasing the hardness of the halide.

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Stereo‐Active Lone Pairs Induced Second Harmonic Generation Responses and Electrocatalytic Activity in Hybrid Material

Ding,

Zhuang,

Deng

et al. 2024

Chemistry A European J

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The lone pair electrons in the electronic structure of molecules have been a prominent research focus in chemistry for more than a century. Stable s2lone pair electrons significantly influence material properties, including thermoelectric properties, nonlinear optical properties, ferroelectricity, and electro(photo)catalysis.While major advances have been achieved in understanding the influence of lone pair electrons on material characteristics, research on this effect in organic‐inorganic hybrid materials is in its initial stage. In this work, we successfully obtained a novel organic‐inorganic hybrid material incorporating Ge with 4s2 lone pair electrons, (MeHDabco)2[GeBr3]4‐H2O (MeHDabco = N‐methyl‐1,4‐diazabicyclo[2.2.2]octane) (1). Driven by the stereochemically active lone pair electrons on the Ge2+, 1 crystallizes in the noncentrosymmetric space group P21 at room temperature and exhibits good second harmonic generation (SHG) responses. Interestingly, 1 also shows electrocatalytic activity for the hydrogen evolution reaction due to the existence of lone pair electrons on Ge2+ cations. The electrochemical experiment combined with the DFT calculations revealed the lone pair electrons act as both an active site for proton adsorption and facilitate the ionization of water. This work not only emphasizes the important role of lone pair electrons in material properties and functions but also provides new insight for designing novel Ge‐based hybrid materials.

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Air- and water-stable and photocatalytically active germanium-based 2D perovskites by organic spacer engineering

Cited by 7 publications

References 38 publications

Recent Advances and Opportunities in Low‐Dimensional Layered Perovskites for Emergent Applications beyond Photovoltaics

Recent Advances and Opportunities in Low‐Dimensional Layered Perovskites for Emergent Applications beyond Photovoltaics

Halide Alloying and Role of Central Atom on the Structural and Optical Properties of Decylammonium Germanium 2D Perovskites

Stereo‐Active Lone Pairs Induced Second Harmonic Generation Responses and Electrocatalytic Activity in Hybrid Material

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