Multifunctional Perovskite Photodetectors: From Molecular-Scale Crystal Structure Design to Micro/Nano-scale Morphology Manipulation.

Multifunctional photodetectors boost the development of traditional optical communication technology and emerging artificial intelligence fields, such as robotics and autonomous driving. However, the current implementation of multifunctional detectors is based on the physical combination of optical lenses, gratings, and multiple photodetectors, the large size and its complex structure hinder the miniaturization, lightweight, and integration of devices. In contrast, perovskite materials have achieved remarkable progress in the field of multifunctional photodetectors due to their diverse crystal structures, simple morphology manipulation, and excellent optoelectronic properties. In this review, we first overview the crystal structures and morphology manipulation techniques of perovskite materials and then summarize the working mechanism and performance parameters of multifunctional photodetectors. Furthermore, the fabrication strategies of multifunctional perovskite photodetectors and their advancements are highlighted, including polarized light detection, spectral detection, angle-sensing detection, and self-powered detection. Finally, the existing problems of multifunctional detectors and the perspectives of their future development are presented.

Temperature-Induced Low-Coordinate Ni Single-Atom Catalyst for Boosted CO2 Electroreduction Activity.

Single-atom catalysts (SACs) exhibit remarkable potential for electrochemical reduction of CO2 to value-added products. However, the commonly pursued methods for preparing SACs are hard to scale up, and sometimes, lack general applicability because of expensive raw materials and complex synthetic procedures. In addition, the fine tuning of coordination environment of SACs remains challenging due to their structural vulnerability. Herein, a simple and universal strategy is developed to fabricate Ni SACs with different nitrogen coordination numbers through one-step pyrolysis of melamine, Ni(NO3 )∙6H2 O, and polyvinylpyrrolidone at different temperatures. Experimental measurements and theoretical calculations reveal that the low-coordinate Ni SACs exhibit outstanding CO2 reduction performance and stability, achieving a Faradic efficiency (FECO ) of 98.5% at -0.76 V with CO current density of 24.6 mA cm-2 , and maintaining FECO of over 91.0% at all applied potential windows from -0.56 to -1.16 V, benefiting from its coordinatively unsaturated structure to afford high catalytic activity and low barrier for the formation of *COOH intermediate. No significant performance degradation is observed over 50 h of continuous operation. Additionally, several other metallic single-atom catalysts are successfully prepared by this synthetic method, demonstrating the universality of this strategy.

Yb-doped SnO2 electron transfer layer assisting the fabrication of high-efficiency and stable perovskite solar cells in air.

To date, most preparation processes of polycrystalline perovskite films still have to be performed in a glovebox filled with inert gas, limiting the application due to their high cost and complexity. In this work, we exploit a facile processing technique for the preparation of perovskite solar cells (PSCs) under ambient conditions by the Yb3+ doping effect for SnO2 electron transfer layer. This remarkable and facile interface doping strategy promotes all-air processed planar PSCs, giving enhanced power conversion efficiency (PCE) from 15.69% to 17.31% with a decreasing hysteresis effect. Moreover, the heating and illumination stability of modified devices by virtue of defect suppression located at electron transfer layer (ETL)/perovskite interface has been effectively improved, retaining over 85% of its initial PCE after 7 h heating at 100 °C in ambient condition and 85% of its initial PCE under 7 h continuous light illumination without any encapsulation. Therefore, it is believed that this Yb-doping strategy for SnO2 ETL can provide a novel way of promoting the efficiency and stability of devices prepared in the air.

Prussian Blue Microcrystals with Morphology Evolution as a High-Performance Photo-Fenton Catalyst for Degradation of Organic Pollutants.

The morphology-dependent property of crystal materials has aroused extensive attention and raised high requirements for subtly tailoring the morphology of micro-/nanocrystals. Herein, we develop an in situ etching method for preparation of Prussian blue (PB) microcrystals with morphology evolution by progressively increasing the concentration of chloroplatinic acid in the reaction system. These PB microcrystals with controllable morphologies are employed as photo-Fenton reagents to degrade organic pollutants. PB hexapods (PB-hpds) and PB hexapod stars present superior catalytic performance to pristine PB microcubes and other PB intermediates with truncated corners or edges because of their high specific surface areas and adequate exposure of FeIII-NC coordination active sites. In the reusability test, the reused PB-hpds present more efficient catalytic performance for rhodamine B decomposition compared with the pristine catalyst. According to more investigations, the reasonable mechanism is proposed that FeIII-NC exhibits higher catalytic activity than FeII-CN in the specific coordination environment. The increased content of surface FeIII-NC coordination active sites is the key factor in accelerating the decomposition of H2O2 and enhancing the photo-Fenton performance of PB-hpds. Several operating parameters including catalyst dosage, H2O2 concentration, pH value, and reaction temperature are evaluated in detail. Classical quenching experiments and electron paramagnetic resonance measurements further reveal that HO• should be responsible for high performance of catalysts. This work will be significant for tailoring the morphology of the materials and arousing more attention to enhance the stability and reusability of catalysts.

Fabrication of thorny Au nanostructures on polyaniline surfaces for sensitive surface-enhanced Raman spectroscopy.

Here we demonstrate, for the first time, the fabrication of Au nanostructures on polyaniline (PANI) membrane surfaces for surface enhanced Raman spectroscopy (SERS) applications, through a direct chemical reduction by PANI. Introduction of acids into the HAuCl(4) solution leads to homogeneous Au structures on the PANI surfaces, which show only sub-ppm detection levels toward the target analyte, 4-mercaptobenzoic acid (4-MBA), because of limited surface area and lack of surface roughness. Thorny Au nanostructures can be obtained through controlled reaction conditions and the addition of a capping agent poly (vinyl pyrrolidone) (PVP) in the HAuCl(4) solution and the temperature kept at 80 °C in an oven. Those thorny Au nanostructures, with higher surface areas and unique geometric feature, show a SERS detection sensitivity of 1 × 10(-9) M (sub-ppb level) toward two different analyte molecules, 4-MBA and Rhodamine B, demonstrating their generality for SERS applications. These highly sensitive SERS-active substrates offer novel robust structures for trace detection of chemical and biological analytes.