Organic−inorganic halide perovskites feature excellent optoelectronic properties but poor chemical stability. While passivating perovskite grain boundary (GB) by polymers shows prospects on long-term performance of perovskite solar cells (PSCs), its detailed impact on the ion migration phenomenon, which largely deteriorates the PSC stability, remains less probed. Here, we introduce a new polar polymer, polycaprolactone (PCL), to passivate GBs of methylammonium lead triiodide (MAPbI 3 ) perovskite with only 1−2 polymer monolayers via direct backbone attachment. The PSCs with passivated MAPbI 3 , using a classic but less stable Spiro-OMeTAD (2,2′,7,7′tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9′-spirobifluorene) hole transport layer (HTL), exhibit improved power conversion efficiencies up to 20.1%, with 90% of the initial PCE being preserved after 400 h ambient storage, and 80% even after 100 h, 85 °C aging. The improved PSC stability indicates critical roles of PCL GB passivation in retarding moisture-induced decomposition and suppressing ion migration within the perovskite. Time-of-flight secondary ion mass spectrometry reveals that I − ions can actively migrate into the electrode, HTL, and their interface in nonpassivated PSCs, even without an externally applied electric field, while such migration is significantly mitigated in PCL-passivated PSCs. This effective GB passivation by PCL suggests an important potential of polymer additives toward the development of stable high-performance PSCs.

We have designed and engineered an environmentally sustainable ternary polymer blend with the mechanical properties comparable to high impact resistant conventional polymers under the guidance of the lattice self-consistent field model. In this blend system, poly­(methyl methacrylate) (PMMA) was used as the compatibilizer for the poly­(lactic acid) (PLA)/poly­(butylene adipate-co-butylene terephthalate) (PBAT) blend. We characterized the compatibility of those components and found PMMA was miscible with PLA and partially compatible with PBAT, which allowed it to self-assemble to a nanoscale interfacial layer on the PLA/PBAT interface. This PMMA layer can significantly decrease the interfacial energy and strongly entangle with either PLA or PBAT, resulting in the strengthening of the interface and dramatically enhancement of the impact resistance of the ternary blend. The optimal mechanical performance was achieved when the total PMMA concentration was less than 10 wt %. Higher PMMA content embrittled the blend since the additional PMMA did not contribute to the minimization of the interfacial energy but remained in the PLA phase, increasing the glass transition temperature of the matrix.

"Green" polymer nanocomposites were made by melt blending biodegradable poly(lactic acid) (PLA) and poly(butylene adipate-co-butylene terephthalate) (PBAT) with either montmorillonite clays (Cloisite Na(+)), halloysite nanotubes (HNTs), the resorcinol diphenyl phosphate (RDP)-coated Cloisite Na(+), and coated HNTs. A technique for measuring the work of adhesion (Wa) between nanoparticles and their matrixes was used to determine the dispersion preference of the nanoparticles in the PLA/PBAT blend system. Transmission electron microscopy (TEM) images of thin sections indicated that even though both RDP-coated nanotubes and clay platelets segregated to the interfacial regions between the two immiscible polymers, only the platelets, having the larger specific surface area, were able to reduce the PBAT domain sizes. The ability of clay platelets to partially compatibilize the blend was further confirmed by the dynamic mechanical analysis (DMA) which showed that the glass transition temperatures of two polymers tended to shift closer. No shift was observed with either coated or uncoated HNTs samples. Izod impact testing demonstrated that the rubbery PBAT phase greatly increased the impact strength of the unfilled blend, but addition of only 5% of treated clay decreased the impact strength by nearly 50%. On the other hand, an increase of 9% relative to the unfilled blend sample was observed with the addition of 5% treated nanotubes. TEM cross-section analysis confirmed that the RDP-coated clay platelets covered most of the interfacial area. On one hand, this enabled them to reduce the interfacial tension effectively; on the other hand, it prevented chain entanglements across the phase boundary and increased the overall brittleness, which was confirmed by rheology measurements. In contrast, the RDP-coated HNTs were observed to lie perpendicular to the interface, which made them less effective in reducing interfacial tension but encouraged interfacial entanglements across the interface, resulting in "stitching" of the interface and an increase in the Izod impact of the blend.

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