Stabilizing Top Interface by Molecular Locking Strategy with Polydentate Chelating Biomaterials toward Efficient and Stable Perovskite Solar Cells in Ambient Air.

The instability of top interface induced by interfacial defects and residual tensile strain hinders the realization of long-term stable n-i-p regular perovskite solar cells (PSCs). Herein, one molecular locking strategy is reported to stabilize top interface by adopting polydentate ligand green biomaterial 2-deoxy-2,2-difluoro-d-erythro-pentafuranous-1-ulose-3,5-dibenzoate (DDPUD) to manipulate the surface and grain boundaries of perovskite films. Both experimental and theoretical evidence collectively uncover that the uncoordinated Pb2+ ions, halide vacancy, and/or I─Pb antisite defects can be effectively healed and locked by firm chemical anchoring on the surface of perovskite films. The ingenious polydentate ligand chelating is translated into reduced interfacial defects, increased carrier lifetimes, released interfacial stress, and enhanced moisture resistance, which should be liable for strengthened top interface stability and inhibited interfacial nonradiative recombination. The universality of the molecular locking strategy is certified by employing different perovskite compositions. The DDPUD modification achieves an enhanced power conversion efficiency (PCE) of 23.17-24.47%, which is one of the highest PCEs ever reported for the devices prepared in ambient air. The unsealed DDPUD-modified devices maintain 98.18% and 88.10% of their initial PCEs after more than 3000 h under a relative humidity of 10-20% and after 1728 h at 65 °C, respectively.

Polydentate Ligand Reinforced Chelating to Stabilize Buried Interface toward High-Performance Perovskite Solar Cells.

The instability of the buried interface poses a serious challenge for commercializing perovskite photovoltaic technology. Herein, we report a polydentate ligand reinforced chelating strategy to strengthen the stability of buried interface by managing interfacial defects and stress. The bis(2,2,2-trifluoroethyl) (methoxycarbonylmethyl)phosphonate (BTP) is employed to manipulate the buried interface. The C=O, P=O and two -CF3 functional groups in BTP synergistically passivate the defects from the surface of SnO2 and the bottom surface of the perovskite layer. Moreover, The BTP modification contributes to mitigated interfacial residual tensile stress, promoted perovskite crystallization, and reduced interfacial energy barrier. The multidentate ligand modulation strategy is appropriate for different perovskite compositions. Due to much reduced nonradiative recombination and heightened interface contact, the device with BTP yields a promising power conversion efficiency (PCE) of 24.63 %, which is one of the highest efficiencies ever reported for devices fabricated in the air environment. The unencapsulated BTP-modified devices degrade to 98.6 % and 84.2 % of their initial PCE values after over 3000 h of aging in the ambient environment and after 1728 h of thermal stress, respectively. This work provides insights into strengthening the stability of the buried interface by engineering multidentate chelating ligand molecules.

Interface Coordination Engineering of P-Fe3O4/Fe@C Derived from an Iron-Based Metal Organic Framework for pH-Universal Water Splitting.

Developing electrocatalysts with high energy conversion efficiency is urgently needed. In this work, P-Fe3O4/Fe@C electrodes with rich under-coordinated Fe atom interfaces are constructed for efficient pH-universal water splitting. The introduction of under-coordinated Fe atoms into the P-Fe3O4/Fe@C interface can increase the local charge density and polarize the 3d orbital lone electrons, which promotes water adsorption and activation to release more H*, thus elevating electrocatalytic activity. As a donor-like catalyst, P-Fe3O4/Fe@C displays excellent electrocatalytic performance with overpotentials of 160 mV and 214 mV in acidic and alkaline electrolytes at 10 mA cm-2, in addition to pH-universal long-term stability.

1-Adamantanamine Hydrochloride Resists Environmental Corrosion to Obtain Highly Efficient and Stable Perovskite Solar Cells.

Passivating the defective surface of perovskite film is a promising strategy to improve the stability and efficiency of perovskite solar cells (PSCs). Herein, 1-adamantanamine hydrochloride (ATH) is introduced to the upper surface of the perovskite film to heal the defects of the perovskite surface. The best-performance ATH-modified device has a higher efficiency (23.45%) than the champion control device (21.53%). The defects are passivated, interfacial nonradiative recombination is suppressed, and interface stress is released by the ATH deposited on the perovskite film, leading to longer carrier lifetimes and enhancement in open-circuit voltage (VOC) and fill factor (FF) of the PSCs. With obvious improvement, VOC and FF of 1.159 V and 0.796 for the control device are raised to 1.178 V and 0.826 for the ATH-modified device, respectively. Finally, during an operational stability measurement of more than 1000 h, the ATH-treated PSC exhibited better moisture resistance, thermal persistence, and light stability.

Application of Natural Molecules in Efficient and Stable Perovskite Solar Cells.

Perovskite solar cells (PSCs), one of the most promising photovoltaic technologies, have been widely studied due to their high power conversion efficiency (PCE), low cost, and solution processability. The architecture of PSCs determines that high PCE and stability are highly dependent on each layer and the related interface, where nonradiative recombination occurs. Conventional synthetic chemical materials as modifiers have disadvantages of being toxic and costly. Natural molecules with advantages of low cost, biocompatibility, and being eco-friendly, and have improved PCE and stability by modifying both functional layers and interface. In this review, we discuss the roles of natural molecules on PSCs devices in terms of the perovskite active layer, interface, carrier transport layers (CTLs), and substrate. Finally, the summary and outlook for the future development of natural molecule-modified PSCs are also addressed.

Precise modulation strategies of 2D/3D perovskite heterojunctions in efficient and stable solar cells.

2D/3D perovskite heterojunctions exhibit promising prospects in the improvement of efficiency and stability of perovskite solar cells (PSCs). However, many challenges remain in the development of high-quality 2D/3D heterojunctions, such as a reliable pathway to control the perovskite phase and generally poor performance in inverted (p-i-n) devices, which limit their commercialization. Fortunately, many excellent works have proposed lots of strategies to solve these challenges, which have triggered a new wave of research on 2D/3D perovskite heterojunctions in recent years. In this paper, the latest research progress and the critical factors involved in the modulating mechanisms of PSCs with 2D/3D heterojunctions have been summarized and laid out systematically. The advantages of constructing 2D/3D perovskite heterojunctions in PSCs are highlighted, and the problems and related solutions of low-dimensional perovskites as passivation layers towards high-performance PSCs are also discussed in depth. Finally, the prospects of 2D/3D perovskite heterojunctions utilized in the passivation strategies to further improve the photovoltaic performance of PSCs in the future have been presented.

Spontaneous Interface Healing by a Dynamic Liquid-Crystal Transition for High-Performance Perovskite Solar Cells.

Low-temperature solution processing of thin-film semiconductors is more cost-effective than traditional vacuum processing; however, it leads to more defects during fast bulk crystallization and residual tensile stress. Herein, a new strategy of dynamic liquid-crystal transition (DLCT) is developed to solve these problems in one step. The design principle is used to suggest that the DLCT molecule should firstly interact with the perovskite grains in the bulk and meanwhile go through a dynamic transition to spontaneously heal the interface. A thermotropic LC molecule (CBO6SS6OCB) is then designed to demonstrate the strategy. The LC interacting with perovskite colloid forms an intermediate adduct to retard the crystallization. The annealing processes stimulate the concentrated LC solid, causing it to flow to the electron transport layer to release the residual stress to attain improved electron extraction. Consequently, the device efficiency is increased to 24.38%, where its VOC of 1.184 V is among the best for the formamidine-based perovskite solar cells. Furthermore, the ambient stability (93.0% of initial efficiency after 2000 h of aging) and light stability (96.3% of initial efficiency after 500 h of aging) are much improved. This work conceives a new engineering of additive phase transition for high-performance perovskite solar cells.

Stabilizing Perovskite Precursor by Synergy of Functional Groups for NiOx -Based Inverted Solar Cells with 23.5 % Efficiency.

Perovskite solar cells suffer from poor reproducibility due to the degradation of perovskite precursor solution. Herein, we report an effective precursor stabilization strategy via incorporating 3-hydrazinobenzoic acid (3-HBA) containing carboxyl (-COOH) and hydrazine (-NHNH2 ) functional groups as stabilizer. The oxidation of I- , deprotonation of organic cations and amine-cation reaction are the main causes of the degradation of mixed organic cation perovskite precursor solution. The -NHNH2 can reduce I2 defects back to I- and thus suppress the oxidation of I- , while the H+ generated by -COOH can inhibit the deprotonation of organic cations and subsequent amine-cation reaction. The above degradation reactions are simultaneously inhibited by the synergy of functional groups. The inverted device achieves an efficiency of 23.5 % (certified efficiency of 23.3 %) with an excellent operational stability, retaining 94 % of the initial efficiency after maximum power point tracking for 601 hours.

Simultaneous Passivation of Bulk and Interface Defects with Gradient 2D/3D Heterojunction Engineering for Efficient and Stable Perovskite Solar Cells.

Minimizing bulk and interfacial nonradiative recombination losses is key to further improving the photovoltaic performance of perovskite solar cells (PSC) but very challenging. Herein, we report a gradient dimensionality engineering to simultaneously passivate the bulk and interface defects of perovskite films. The 2D/3D heterojunction is skillfully constructed by the diffusion of an amphiphilic spacer cation from the interface to the bulk. The 2D/3D heterojunction engineering strategy has achieved multiple functions, including defect passivation, hole extraction improvement, and moisture stability enhancement. The introduction of tertiary butyl at the spacer cation should be responsible for increased film and device moisture stability. The device with 2D/3D heterojunction engineering delivers a promising efficiency of 22.54% with a high voltage of 1.186 V and high fill factor of 0.841, which benefits from significantly suppressed bulk and interfacial nonradiative recombination losses. Moreover, the modified devices demonstrate excellent light, thermal, and moisture stability over 1000 h. This work paves the way for the commercial application of perovskite photovoltaics.

Crystal Orientation Modulation and Defect Passivation for Efficient and Stable Methylammonium-Free Dion-Jacobson Quasi-2D Perovskite Solar Cells.

Dion-Jacobson (DJ) quasi-2D perovskite solar cells (PSCs) have received increasing attention due to their greater potentials in realizing efficient and stable quasi-2D PSCs relative to their Ruddlesden-Popper counterpart. The substitution of methylammonium (MA+) with formamidinium is expected to be able to further increase the stability and power conversion efficiency (PCE) of DJ quasi-2D PSCs. Herein, we report a multifunctional additive strategy for preparing high-quality MA-free DJ quasi-2D perovskite films, where 1,1'-carbonyldi(1,2,4-triazole) (CDTA) molecules are incorporated into the perovskite precursor solution. CDTA modification can control phase distribution, enlarge grain size, modulate crystallinity and crystal orientation, and passivate defects. After CDTA modification, more favorable gradient phase distribution and accordingly gradient band alignment are formed, which is conducive to carrier transport and extraction. The improved crystal orientation can facilitate carrier transport and collection. The enlarged grain size and effective defect passivation contribute to reduced defect density. As a result, the CDTA-modified device delivers a PCE of 16.07%, which is one of the highest PCEs ever reported for MA-free DJ quasi-2D PSCs. The unencapsulated device with CDTA maintains 92% of its initial PCE after aging under one sun illumination for 360 h and 86% after aging at 60 °C for 360 h.

CuS/RGO hybrid photocatalyst for full solar spectrum photoreduction from UV/Vis to near-infrared light.

To make full use of the solar energy, it remains a great challenge for semiconductor photocatalysts to harvest the full solar light spectrum from ultraviolet (UV) to visible even the near infrared (NIR) wavelength. Here we show firstly the CuS/RGO (reduced graphene oxide) hybrid photocatalyst synthesized via a microwave assisted method with full solar light (UV-Vis-NIR) active for efficient Cr(VI) reduction. The CuS/RGO displays high absorption and catalytic activity in the UV, visible and even the NIR light regions. As co-catalyst, RGO can separate and inhibit the recombination of charge carriers, consequently improving the catalytic activity. Only 1wt% RGO emersions can reduce 90% of Cr(VI) under the radiation of light over the full spectrum. Findings may provide a new strategy and substance to expand the utilization range of solar light from UV to visible even the NIR energy.

Hierarchical layered Ni(3)S(2)-graphene hybrid composites for efficient photocatalytic reduction of Cr(VI).

Exploring visible light responsive media remains a challenge for solar energy photocatalysis applications. We report the Ni3S2-reduced graphene oxide (NG) hybrid composites with sheet-on-sheet structures synthesized by a facile microwave-assisted method. Their morphology, structure and photocatalytic activity in the reduction of Cr(VI) were characterized by scanning electron microscopy, X-ray diffraction, UV-Vis absorption spectroscopy, and electrochemical impedance spectra, respectively. The results show that NG hybrid composites show excellent visible light photocatalytic activity in the reduction of Cr(VI) compared to pure Ni3S2. The Cr(VI) reduction rate of higher than 90% has been achieved with 1wt.% reduced graphene oxide under visible light irradiation at 180min. Improvement is attributed to its efficient charge separation and more active sites due to the integrative effect and good interfacial contact between Ni3S2 and reduced graphene oxide.

Hexagonal 2H-MoSe2 broad spectrum active photocatalyst for Cr(VI) reduction.

To make full use of the solar energy, exploring broad spectrum active photocatalysts has become one of the core issues for photocatalysis. Here we report a novel hexagonal 2H-MoSe2 photocatalyst with ultraviolet (UV)-visible-near infrared (NIR) light response for the first time. The results indicate that the MoSe2 displays excellent photo-absorption and photocatalytic activity in the reduction of Cr(VI) under UV and visible even NIR light irradiation. MoSe2 synthesized at pH value of 2 achieves the highest Cr(VI) reduction rates of 99%, 91% and 100% under UV, visible and NIR light irradiation, respectively, which should be attributed to its comparatively higher light absorption, efficient charge separation and transfer as well as relatively large number of surface active sites. The excellent broad spectrum active photocatalytic activity makes the MoSe2 to be a promising photocatalyst for the effective utilization of solar energy.