Lead-Free Semiconductors : Phase-Evolution and Superior Stability of Multinary Tin Chalcohalides
Roth, Alison N. (Iowa State University)
Porter, Andrew P. (Iowa State University)
Horger, Sarah (Iowa State University)
Ochoa-Romero, Kerly (Universitat Autònoma de Barcelona. Departament de Química)
Guirado López, Gonzalo (Universitat Autònoma de Barcelona. Departament de Química)
Rossini, Aaron J. (Iowa State University)
Vela, Javier (Iowa State University)

Data:	2024
Resum:	Tin-based semiconductors are highly desirable materials for energy applications due to their low toxicity and biocompatibility relative to analogous lead-based semiconductors. In particular, tin-based chalcohalides possess optoelectronic properties that are ideal for photovoltaic and photocatalytic applications. In addition, they are believed to benefit from increased stability compared with halide perovskites. However, to fully realize their potential, it is first necessary to better understand and predict the synthesis and phase evolution of these complex materials. Here, we describe a versatile solution-phase method for the preparation of the multinary tin chalcohalide semiconductors SnSbSI, SnBiSI, SnBiSI, and SnSI. We demonstrate how certain thiocyanate precursors are selective toward the synthesis of chalcohalides, thus preventing the formation of binary and other lower order impurities rather than the preferred multinary compositions. Critically, we utilized 119 Sn ssNMR spectroscopy to further assess the phase purity of these materials. Further, we validate that the tin chalcohalides exhibit excellent water stability under ambient conditions, as well as remarkable resistance to heat over time compared to halide perovskites. Together, this work enables the isolation of lead-free, stable, direct band gap chalcohalide compositions that will help engineer more stable and biocompatible semiconductors and devices.
Ajuts:	European Commission 101115182
Drets:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, i la comunicació pública de l'obra, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original. No es permet la creació d'obres derivades.
Llengua:	Anglès
Document:	Article ; recerca ; Versió publicada
Matèria:	Inorganic carbon compounds ; Nuclear magnetic resonance spectroscopy ; Perovskites ; Precursors ; Semiconductors
Publicat a:	Chemistry of materials, Vol. 36, Issue 9 (April 2024) , p. 4542-4552, ISSN 1520-5002

DOI: 10.1021/acs.chemmater.4c00209
PMID: 38764751

11 p, 7.5 MB

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