Spectacular Enhancement of the Thermal and Photochemical Stability of MAPbI3 Perovskite Films Using Functionalized Tetraazaadamantane as a Molecular Modifier
Abstract:Perovskite solar cells represent a highly promising third-generation photovoltaic technology. However, their practical implementation is hindered by low device operational stability, mostly related to facile degradation of the absorber materials under exposure to light and elevated temperatures. Improving the intrinsic stability of complex lead halides is a big scientific challenge, which might be addressed using various “molecular modifiers”. These modifiers are usually represented by some additives undergoin… Show more
“…CH 2 Cl 2 and Et 3 N were distilled over CaH 2 ; THF was distilled over LiAlH 4 ; other solvents were distilled without drying agents. TAAD, 23 TAAD·HCl, 58 (3β)-21-bromo-20-oxopregna-5,16-dien-3-yl acetate ( 2a ), 59 quaternary salt 4a , 57 2-bromoacetyl chloride 60 and polymer PS-CH 2 -TAAD 27 were prepared according to previously described protocols. 1,4,7-Triazacyclononane trihydrochloride (TACN·3HCl), 1,8-bis(dimethylamino)naphthalene (proton sponge), glycylglycylglycine, p -thiocresol, n -heptanethiol, glutathione and all inorganic reagents were commercial grade and used as received.…”
4,6,10-Trihydroxy-1,4,6,10-tetraazaadamantane (TAAD) has been shown to form a stable Fe(IV) complex having a diamantane cage structure, in which the metal center is coordinated by three oxygen atoms of the deprotonated...
“…CH 2 Cl 2 and Et 3 N were distilled over CaH 2 ; THF was distilled over LiAlH 4 ; other solvents were distilled without drying agents. TAAD, 23 TAAD·HCl, 58 (3β)-21-bromo-20-oxopregna-5,16-dien-3-yl acetate ( 2a ), 59 quaternary salt 4a , 57 2-bromoacetyl chloride 60 and polymer PS-CH 2 -TAAD 27 were prepared according to previously described protocols. 1,4,7-Triazacyclononane trihydrochloride (TACN·3HCl), 1,8-bis(dimethylamino)naphthalene (proton sponge), glycylglycylglycine, p -thiocresol, n -heptanethiol, glutathione and all inorganic reagents were commercial grade and used as received.…”
4,6,10-Trihydroxy-1,4,6,10-tetraazaadamantane (TAAD) has been shown to form a stable Fe(IV) complex having a diamantane cage structure, in which the metal center is coordinated by three oxygen atoms of the deprotonated...
“…THF was distilled over LiAlH 4 ; other solvents were distilled without drying agents. TAAD, 23 TAAD•HCl, 43 (3β)-21-Bromo-20-oxopregna-5,16-dien-3-yl acetate (2a), 44 quaternary salt 4a, 40 2-bromoacetyl chloride 45 and polymer PS-CH 2 -TAAD 27 were prepared according to previously described protocols. 1,4,7-Triazacyclononane trihydrochloride (TACN•3HCl), 1,8-bis(dimethylamino)naphthalene (proton sponge), glycylglycylglycine, p-thiocresol, n-heptanethiol, glutathione and all inorganic reagents were commercial grade and used as received.…”
Section: General Methods and Instrumentationmentioning
4,6,10-Trihydroxy-1,4,6,10-tetraazaadamantane (TAAD) has been shown to form a stable Fe(IV) complex having a diamantane cage structure, in which the metal center is coordinated by three oxygen atoms of the deprotonated ligand. The complex was characterized by X-ray, HRMS, NMR, FT-IR, Mössbauer spectroscopy and DFT calculations, which supported d4 configuration of iron. The Fe(IV)-TAAD complex showed excellent performance in dioxygen activation under mild conditions serving as a mimetic of the thiol oxidase enzyme. The nucleophilicity of the bridge-head nitrogen atom in TAAD provides a straightforward way for conjugation of Fe(IV)-TAAD complexes to various functional molecules. Using this approach, steroidal and peptide molecules having an iron(IV) label have been prepared for the first time. Also, the Fe(IV)-TAAD complex was covalently bounded to a polystyrene matrix and the resulting material was shown to serve as a heterogeneous catalyst for aerobic oxidation of thiols to disulfides.
“…To date, different methods have been reported to alleviate the vulnerability of QD, such as surface ligand modification, encapsulating in particle, coating of shell, binding with matrix, and packaging engineering. Some researchers found more stable and proper ligands for QD [7][8][9], such as moisture-tolerant molecules. Others encapsulated QD in silicon dioxide (SiO 2 ) particles [10][11][12], waterproof aerogels [13], mesoporous particles [14,15], and so on.…”
Quantum dot (QD) features many exceptional optical performances but is also vulnerable to moisture which results in structural damage and luminescent decrease. This work provided and fabricated a novel superior hydrophobic methylated core/shell silica-coated QD (MSQ) for high water stability. QD was coated with a silica shell and then surface-methylated by trimethyl silane. Mercaptopropyl trimethoxy silane, tetraethyl orthosilicate, and ethoxy trimethyl silane were utilized as the ligand exchanger, the raw material of silica, and the surface modification, respectively. Characterization results illustrated the core/shell structure of MSQ. In addition, its water contact angle was up to 159.6º. QD-, silica-coated QD(SQ)-, and MSQ-silicone were made and displayed similar absorption, emission, and excitation spectra but different water stabilities. The photoluminescence intensity and photoluminescence quantum yield of MSQ-silicone hardly changed during 15 days of water immersion, in contrast to the dramatical decrease of other two kinds of composite silicone. Specifically, the photoluminescence quantum yield decreases of MSQ-, SQ-, and QD-silicone were 1%, 40%, and 43 %, respectively. Therefore, MSQ had a much better water stability. The superior hydrophobic methylated silica-coated QD has a great potential to realize the long-term working stability in a humid environment and the wider application in diverse fields.
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