Tin (Sn)-based and mixed tin−lead (Sn−Pb) perovskites have attracted increased attention as promising candidates for new generation lead-free perovskite and all-perovskite tandem solar cells. However, as an inevitably critical issue, Sn(II) induced serious defects and oxidation and caused poor photovoltaic performance and unsatisfactory stability for Sn-based and mixed Sn−Pb perovskites. Herein, a comprehensive understanding on defect classification, defect formation, defect effect on performance, and defect passivation strategies is reviewed on the Sn(II) induced defects. The Sn(II)-based defects can be classified from the aspects of defect dimensions and shallow/deep levels in energy structure according to three main origins, i.e. low defect tolerance, oxidation, and fast crystallization. Then, the state-of-the-art defect passivation strategies including surface Lewis acid/base coordination, low/mixed dimensional perovskite design, composition regulation and crystal orientation modulation, and reducing agent assistance are summarized systematically. Lastly, several key scientific issues and future research prospectives are proposed for achieving stable and high-performance Sn-related perovskite photovoltaics.
Recent synthetic advances have made available very monodisperse zincblende CdSe/CdS quantum dots having near-unity photoluminescence quantum yields. Because of the absence of nonradiative decay pathways, accurate values of the radiative lifetimes can be obtained from time-resolved PL measurements. Radiative lifetimes can also be obtained from the Einstein relations, using the static absorption spectra and the relative thermal populations in the angular momentum sublevels. One of the inputs into these calculations is the shell thickness, and it is useful to be able to determine shell thickness from spectroscopic measurements. We use an empirically corrected effective mass model to produce a "map" of exciton wavelength as a function of core size and shell thickness. These calculations use an elastic continuum model and the known lattice and elastic constants to include the effect of lattice strain on the band gap energy. The map is in agreement with the known CdSe sizing curve and with the shell thicknesses of zincblende core/shell particles obtained from TEM images. If selenium−sulfur diffusion is included and lattice strain is omitted from the calculation then the resulting map is appropriate for wurtzite CdSe/CdS quantum dots synthesized at high temperatures, and this map is very similar to one previously reported (J. Am. Chem. Soc. 2009, 131, 14299). Radiative lifetimes determined from time-resolved measurements are compared to values obtained from the Einstein relations, and found to be in excellent agreement. For a specific core size (2.64 nm diameter, in the present case), radiative lifetimes are found to decrease with increasing shell thickness. This is similar to the size dependence of one-component CdSe quantum dots and in contrast to the size dependence in type-II quantum dots.
The shape and composition effects of platinum-palladium (Pt-Pd) alloy nanoparticle cocatalysts on visible-light photocatalytic hydrogen evolution from an aqueous ammonium sulphite solution have been reported and discussed. The activity of Pt-Pd nanoparticles loaded Pt-Pd/CdS photocatalysts are affected based on both the Pt-Pd alloy nanoparticles' shape and their compositions. In this research, two shapes of Pt-Pd nanoparticles have been studied. One is Pt-Pd nanocubes enclosed by {100} crystal planes and the other is nano-octahedra covered with {111} crystal facets. Results show that the photocatalytic turnover frequency (TOF), defined as moles of hydrogen produced per surface mole of Pt-Pd metal atom per second, for Pt-Pd nanocubes/CdS (Pt-Pd NCs/CdS) photocatalyst can be 3.4 times more effective than Pt-Pd nano-octahedra/CdS (Pt-Pd NOTa/CdS) nanocomposite photocatalyst. Along with the shape effect, the atomic ratio of Pt to Pd can also impact the efficiency of Pt-Pd/CdS photocatalysts. When the Pt to Pd atomic ratio changes from 1:0 to about 2:1, the rate of hydrogen production increases from 900 μmol/h for Pt NCs/CdS catalyst to 1837 μmol/h for Pt-Pd (2:1) NCs/CdS photocatalyst-a 104% rate increase. This result suggests that the 33 mol % of more expensive Pt can be replaced with less costly Pd, resulting in a more than 100% hydrogen production rate increase. The finding of this research will lead to the research and development of highly effective catalysts for photocatalytic hydrogen production using solar photonic energy.
High-efficiency and low-cost perovskite solar cells (PSCs) are desirable candidates for addressing the scalability challenge of renewable solar energy.
Despite Sn‐based perovskite solar cells (PSCs) prevailing over lead‐free candidates, the Sn vacancies (VSn) and Sn4+ defects seriously deteriorate device photovoltaic performance. The presently reported methods can only effectively achieve surface defect passivation, and it is of great challenge and fundamental importance to develop efficient strategy to deal with the intrinsic defects located inside the lattice. Herein, a novel bulk defect suppression strategy is proposed, introducing large organic piperazine cations (PZ2+) into the lattice of 3D FASnI3 perovskite to restrain the generation of bulk defects. The incorporation of PZ2+ results in forming a FA1−2yPZ2ySn1−yI3 (0 ≤ y ≤ 0.25) structure with no reduction in dimensionality, which guarantees the continuity of [SnI6] octahedral structures with unobstructed carrier transport and reduced charged defects. The potent interactions between PZ2+ and [SnI6] structures enhance VSn formation energy and effectively suppress bulk defect formation. As a result, the FASnI3+1%PZ films exhibit optimized crystalline quality, decreased background carrier density, lower p‐type self‐doping, and reduced trap state density. Benefiting from the above advantages, the FASnI3+1%PZ device achieves an optimal PCE of 9.15% and unencapsulated device maintains over 95% of initial PCE after aging for 1000 h in N2 golvebox. The bulk defect suppression strategy provides fire‐new building bricks toward high‐performance Sn‐based PSCs.
Open-circuit voltage loss and instability from surface Sn(II) oxidation and high-density Sn vacancies pose great hurdles for developing highperformance Sn-based perovskite solar cells (PSCs). Turning attention from the bulk microstructure to surface reconstruction is promising to push the performance enhancement of Sn-based PSCs. Herein, a surface-modulation strategy based on 6-maleimidohexanehydrazide trifluoroacetate is rationally designed to reconstruct the surface structure of FASnI 3 films to manage the Fermi level and passivate defects. The electronic state evolution results in an n-type Fermi level shift of the shallow surface, thereby forming an extra back-surface field for electron extraction. Meanwhile, the ion-pairing agent affords passivating cationic and anionic defects, thereby nullifying the charged-defect-rich surface. In particular, the reductive hydrazide group and carboxyl groups alleviate superficial Sn(IV) and inhibit Sn(IV) formation, homogenizing surface potential and prolonging carrier lifetime. Accordingly, devices deliver a champion power conversion efficiency (PCE) of 13.64% and an elongated lifespan, with over 75% of the original PCE after 1000 h of illumination (O 2 < 50 ppm). This work presents a new insight on the surface reconstruction strategy for developing high-performance Sn-based PSCs.
Inorganic CsPbI 2 Br perovskites have witnessed incredible advances as a promising representative for translucent and tandem solar cells, but unfortunately, they are still plagued by serious energy losses and undesired phase instability. Herein, a new type of π-conjugated small molecule of 4-guanidinobenzoic-acidhydrochloride (4-GBACl) is demonstrated to effectively cross-link the Pb-X framework of perovskites. The strong coordination between 4-GBACl and the [PbX 6 ] 4− octahedron of perovskites effectively stiffens the Pb-X framework to suppress the ion migration, thus stabilizing the perovskite phase structure against light and thermal conditions. Apart from the physical barrier for phase instability resulting from the hydrophobic benzene ring at grain boundaries (GBs), guanidinium cations and −COOH and Cl − groups can simultaneously afford the passivation of positively and negatively charged defects at the GBs and surface, including undercoordinated halide species and undercoordinated Pb 2+ ions, thereby effectively inhibiting the charge trapping/recombination centers. Two-dimensional confocal-fluorescence mapping images provide a visualized sight into the significantly suppressed nonradiative recombination and the prolonged carrier lifetime. It is suggested that the 4-GBACl additive plays multiple roles in grain cross-linking to regulate crystallization, distinctly reducing the trapstate density, ion migration inhibition, and moisture barrier in CsPbI 2 Br films. Consequently, the 4-GBACl-treated device exhibits a champion power conversion efficiency (PCE) of 15.59% accompanied with a considerably improved V oc of 1.28 V and maintains 88% of the initial PCE value after 1200 h aging under 20% relative humidity.
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