Sulfur-Donor Solvents Strongly Coordinate Pb2+ in Hybrid Organic–Inorganic Perovskite Precursor Solutions

Hamill, Jr., J. Clay; Romiluyi, Oluwaseun; Thomas, Sara A.; Cetola, Jacquelyn; Schwartz, Jeffrey; Toney, Michael F.; Clancy, Paulette; Loo, Yueh-Lin

doi:10.1021/acs.jpcc.0c03465

Sulfur-Donor Solvents Strongly Coordinate Pb²⁺ in Hybrid Organic–Inorganic Perovskite Precursor Solutions

Journal Article · Thu Jun 11 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c03465· OSTI ID:1658860

Hamill, Jr., J. Clay ^[1]; Romiluyi, Oluwaseun ^[2]; ^[3]; Cetola, Jacquelyn ^[4]; ^[3]; ^[5]; ^[2]; ^[3]

Princeton Univ., NJ (United States); Princeton University
Johns Hopkins Univ., Baltimore, MD (United States)
Princeton Univ., NJ (United States)
Princeton Univ., NJ (United States); Univ. of Florida, Gainesville, FL (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Strong coordination between Lewis-basic processing additives and the Lewis-acidic lead halide in hybrid organic–inorganic perovskite (HOIP) precursor solutions is required to solubilize the lead halide, and subsequently access the appropriate crystallization kinetics and attain the desired morphology of perovskite active layers. While oxygen-donor solvents and additives, such as dimethylformamide and dimethyl sulfoxide, are widely used for perovskite processing, we demonstrate here that “soft” sulfur-donor solvents exhibit stronger coordination to the “borderline soft” Lewis acid Pb²⁺ center of PbI₂ relative to “hard” O-donor solvents in the precursor solution. The stronger coordination of S-donor solvents compared to O-donor solvents to Pb²⁺ implies that such compounds can be useful additives to HOIP precursor solutions. Density-functional calculations of the enthalpy change resulting from the coordination of solvents to Pb²⁺ provide direct numerical comparison of the strength of O-donor and S-donor coordination with Pb²⁺ and expands the library of candidate S-donor compounds. Our results provide a roadmap for processing additive selection and expand the previously limited choice of perovskite processing additives to include strongly coordinating S-donor compounds.

View Accepted Manuscript (DOE)

Research Organization:: Princeton Univ., NJ (United States); SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Princeton Catalysis Initiative; USDOD; Andlinger Center for Energy and the Environment

Grant/Contract Number:: EE0008560; AC02-76SF00515

OSTI ID:: 1658860

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 27 Vol. 124; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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