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CsPbI3 perovskite is a promising light absorber in perovskite solar cells (PSCs) due to its suitable bandgap (Eg) and high chemical stability, but the perovskite phase is metastable in ambient atmosphere and prone to defect formation. To enhance phase stability and reduce defects, forming a low dimensional (LD) perovskite on CsPbI3 has proved effective. However, the energy levels for most of low‐conductivity LD perovskites are not very compatible with those of CsPbI3, which will impair charge separation and device performance. Herein, a new 1D perovskite (5‐Azaspiro[4.4]nonan‐5‐ium lead triiodide, ASNPbI3) with compatible energy levels and a large Eg is reported as a capping layer. The p‐type ASNPbI3 forms a p‐n heterojunction with n‐CsPbI3 with a staggered band alignment, considerably enhancing the carrier separation. Besides, by pre‐forming a ASNPbI3 at an intermediate stage, defects are suppressed in perovskite film. Consequently, the CsPbI3 PSCs based on carbon electrode without hole transporter (C‐PSCs) achieves a PCE of 18.34%, which is among the highest‐reported values for inorganic C‐PSCs. Furthermore, the hydrophobic ASNPbI3 capping layer has a high thermal stability that greatly enhances perovskite phase stability. Hence, the CsPbI3 C‐PSCs maintains 68% of its initial PCE after 400 h aging at 85°C in a N2 glovebox. [ABSTRACT FROM AUTHOR]

Precisely regulating surface reconstruction of copper (Cu) chalcogenides‐based catalysts to promote the multicarbon (C2+)selectivity of the electrochemical CO2 reduction reaction (CO2RR) is hampered by the challenging control of the intractable anions and the optimal Cuδ+ reduction (0 < δ < 1). Herein, a porous carbon‐supported copper selenides electrocatalyst that can remarkably improve the C2‐product yield and especially unveil the time‐revolved electrochemical CO2RR reconstruction process to enable the high C2‐selectivity, most notably for ethanol is constructed. The Faradic efficiency (FE) of C2‐products achieved is as high as ≈85.2% with a partial current density of 229.5 mA cm−2. Operando infrared spectroscopy and density functional theory (DFT) calculations unravel that the surface Se vacancies (VSe) formation brings closer the neighboring Cu+ atoms and activates the Cu sites, thereby rendering efficient generation of the key intermediates (*CO and *CHO) and lowering the C–C coupling barrier for C2 production. The appearance of metallic Cu can shorten the next‐nearest Cu0–Cu+ distance for O atom to bridge in, leading to the preferential formation of *OC2H4 towards ethanol instead of C–O bond cleavage to form ethylene. This work opens the avenue of designing suitable local atomic structures catalysts to engage the intermediates for targeted CO2RR products. [ABSTRACT FROM AUTHOR]

Hole transport material free carbon‐based all‐inorganic CsPbBr3 perovskite solar cells (PSCs) are promising for commercialization due to its low‐cost, high open‐circuit voltage (Voc) and superior stability. Due to the different solubility of PbBr2 and CsBr in conventional solvents, CsPbBr3 films are mainly obtained by multi‐step spin‐coating through the phase evolution from PbBr2 to CsPb2Br5 and then to CsPbBr3. The scalable fabrication of high‐quality CsPbBr3 films has been rarely studied. Herein, an inkjet‐printing method is developed to prepare high‐quality CsPbBr3 films. The formation of long‐range crystalline CsPb2Br5 phase can effectively improve phase purity and promote regular crystal stacking of CsPbBr3. Consequently, the inkjet‐printed CsPbBr3 C‐PSCs realized PCEs up to 9.09%, 8.59% and 7.81% with active areas of 0.09, 0.25, and 1 cm2, respectively, demonstrating the upscaling potential of our fabrication method and devices. This high performance is mainly ascribed to the high purity, strong crystal orientation, reduced surface roughness and lower trap states density of the as‐printed CsPbBr3 films. This work provides insights into the relationship between the phase evolution mechanisms and crystal growth dynamics of cesium lead bromide halide films. [ABSTRACT FROM AUTHOR]

Chalcogen vacancy has long been recognized as a detrimental deep‐level defect that can induce severe charge recombination and diminish the quasi‐Fermi‐level splitting in Sb2S3 and Sb2Se3, especially when they are prepared by physical vapor deposition in vacuum. In order to counter this limitation, a sulfur‐supplemented vapor transport deposition technique is proposed, which intentionally introduces low pressure sulfur vapor and can thus afford low‐defect‐density antimony chalcogenide films. The resultant photocathodes modified with conformal TiO2 protection layer and Pt cocatalyst demonstrate a photocurrent as high as 20 mA cm−2 along with a much improved fill factor and onset potential, achieving an applied bias photoconversion efficiency above 1%. This work highlights the importance of the vacancy defect passivation and the preferential crystalline orientation in the film in promoting the photocathode performance. [ABSTRACT FROM AUTHOR]