A Comprehensive Review on Perovskite Solar Cells Integrated Photo-supercapacitors and Perovskites-Based Electrochemical Supercapacitors.

Perovskite solar cells (PSCs) have rapidly become a prevalent photovoltaic technology owing to their simple structure, low processing cost, and remarkable increase in solar-to-electric power conversion efficiency (PCE). However, the intermittent nature of solar radiation induces some technical and financial challenges for its practical applications as a reliable power source. To address this issue, the integration of PSCs with supercapacitors (SCs) in the form of integrated photo-supercapacitors (IPSs) has gathered significant attention. This integration can balance energy availability and demand, reduce energy wastage, and stabilize power output for portable and wearable electronics. Meanwhile, the excellent optoelectronic properties with mixed electronic and ionic conductivity of metal halide perovskites (MHPs) have expanded their application as electrode and electrolyte materials for SCs and photo-supercapacitors (PSs) applications. This review provides an all-inclusive summary of the current state-of-the-art research progress of PSCs-IPSs and MHPs-based SCs and PSs by highlighting their basics and integration approaches. It also discusses the challenges and prospects of these materials and technologies.

Self-Assembled Molecules with Asymmetric Backbone for Highly Stable Binary Organic Solar Cells with 19.7 % Efficiency.

The hole-transporting material (HTM), poly (3,4-ethylene dioxythiophene) poly(styrene sulfonate) (PEDOT : PSS), is the most widely used material in the realization of high-efficiency organic solar cells (OSCs). However, the stability of PEDOT : PSS-based OSCs is quite poor, arising from its strong acidity and hygroscopicity. In addition, PEDOT : PSS has an absorption in the infrared region and high highest occupied molecular orbital (HOMO) energy level, thus limiting the enhancement of short-circuit current density (Jsc) and open-circuit voltage (Voc), respectively. Herein, two asymmetric self-assembled molecules (SAMs), namely BrCz and BrBACz, were designed and synthesized as HTM in binary OSCs based on the well-known system of PM6 : Y6, PM6 : eC9, PM6 : L8-BO, and D18 : eC9. Compared with BrCz, BrBACz shows larger dipole moment, deeper work function and lower surface energy. Moreover, BrBACz not only enhances photon harvesting in the active layer, but also minimizes voltage losses as well as improves interface charge extraction/ transport. Consequently, the PM6 : eC9-based binary OSC using BrBACz as HTM exhibits a champion efficiency of 19.70 % with a remarkable Jsc of 29.20 mA cm-2 and a Voc of 0.856 V, which is a record efficiency for binary OSCs so far. In addition, the unencapsulated device maintains 95.0 % of its original efficiency after 1,000 hours of storage at air ambient, indicating excellent long-term stability.

An Ideal Molecular Construction Strategy for Ultra-Narrow-Band Deep-Blue Emitters: Balancing Bathochromic-Shift Emission, Spectral Narrowing, and Aggregation Suppression.

Narrowband emissive multiple resonance (MR) emitters promise high efficiency and stability in deep-blue organic light-emitting diodes (OLEDs). However, the construction of ideal ultra-narrow-band deep-blue MR emitters still faces formidable challenges, especially in balancing bathochromic-shift emission, spectral narrowing, and aggregation suppression. Here, DICz is chosen, which possesses the smallest full-width-at-half-maximum (FWHM) in MR structures, as the core and solved the above issue by tuning its peripheral substitution sites. The 1-substituted molecule Cz-DICz is able to show a bright deep-blue emission with a peak at 457 nm, an extremely small FWHM of 14 nm, and a CIE coordinate of (0.14, 0.08) in solution. The corresponding OLEDs exhibit high maximum external quantum efficiencies of 22.1%-25.6% and identical small FWHMs of 18 nm over the practical mass-production concentration range (1-4 wt.%). To the best of the knowledge, 14 and 18 nm are currently the smallest FWHM values for deep-blue MR emitters with similar emission maxima under photoluminescence and electroluminescence conditions, respectively. These discoveries will help drive the development of high-performance narrowband deep-blue emitters and bring about a revolution in OLED industry.

Molecularly Engineered Multifunctional Bridging Layer Derived from Dithiafulavene Capped Spiroxanthene for Stable and Efficient Perovskite Solar Cells.

This study introduces a novel approach centered around the design and synthesis of an interfacial passivating layer in perovskite solar cells (PSCs). This architectural innovation is realized through the development of a specialized material, termed dithiafulvene end-capped Spiro[fluorene-9,9'-xanthene], denoted by the acronym AF32. In this design architecture, dithiafulvene is thoughtfully attached to the spiroxanthene fluorene core with phenothiazine as the spacer unit, possessing multiple alkyl chains. AF32 passivates interfacial defects by coordinating the sulfur constituents of the phenothiazine and dithiafulvene frameworks to the uncoordinated Pb2+ cations on the surface of the perovskite film, and the alkyl chains construct a hydrophobic environment, preventing moisture from entering the hydrophilic perovskite layer and improving the long-term stability of PSCs. Furthermore, this conductive interlayer facilitates hole transport in PSCs due to its well-aligned molecular orbital levels. Such improvements translated into an enhanced power conversion efficiency (PCE) of 22.6% for the device employing 1.5 mg/mL AF32, and it maintained 85% of its initial PCE after more than 1800 h under ambient conditions [illumination and 45 ± 5% relative humidity (RH)]. This study not only marks progress in photovoltaic technology but also expands our understanding of manipulating interfacial properties for optimized device performance and stability.

Improving the Efficiency and Stability of Perovskite Solar Cells by Refining the Perovskite-Electron Transport Layer Interface and Shielding the Absorber from UV Effects.

This study aims to enhance the performance of perovskite solar cells (PSCs) by optimizing the interface between the perovskite and electron transport layers (ETLs). Additionally, we plan to protect the absorber layer from ultraviolet (UV) degradation using a ternary oxide system comprising SnO2, strontium stannate (SrSnO3), and strontium oxide (SrO). In this structure, the SnO2 layer functions as an electron transport layer, SrSnO3 acts as a layer for UV filtration, and SrO is employed to passivate the interface. SrSnO3 is characterized by its chemical stability, electrical conductivity, extensive wide band gap energy, and efficient absorption of UV radiation, all of which significantly enhance the photostability of PSCs against UV radiation. Furthermore, incorporating SrSnO3 into the ETL improves its electronic properties, potentially raising the energy level and improving alignment, thereby enhancing the electron transfer from the perovskite layer to the external circuit. Integrating SrO at the interface between the ETL and perovskite layer reduces interface defects, thereby reducing charge recombination and improving electron transfer. This improvement results in higher solar cell efficiency, reduced hysteresis, and extended device longevity. The benefits of this method are evident in the observed improvements: a noticeable increase in open-circuit voltage (Voc) from 1.12 to 1.16 V, an enhancement in the fill factor from 79.4 to 82.66%, a rise in the short-circuit current density (Jsc) from 24.5 to 24.9 mA/cm2 and notably, a marked improvement in the power conversion efficiency (PCE) of PSCs, from 21.79 to 24.06%. Notably, the treated PSCs showed only a slight decline in PCE, reducing from 24.15 to 22.50% over nearly 2000 h. In contrast, untreated SnO2 perovskite devices experienced a greater decline, with efficiency decreasing from 21.79 to 17.83% in just 580 h.

Recent Progress of Layered Perovskite Solar Cells Incorporating Aromatic Spacers.

Layered two dimensional (2D) or quasi-2D perovskites are emerging photovoltaic materials due to their superior environment and structure stability in comparison with their 3D counterparts. The typical 2D perovskites can be obtained by cutting 3D perovskites along < 100 > orientation by incorporation of bulky organic spacers, which play a key role in the performance of 2D perovskite solar cells (PSCs). Compared with aliphatic spacers, aromatic spacers with high dielectric constant have the potential to decrease the dielectric and quantum confinement effect of 2D perovskites, promote efficient charge transport and reduce the exciton binding energy, all of which are beneficial for the photovoltaic performance of 2D PSCs. In this review, we aim to provide useful guidelines for the design of aromatic spacers for 2D perovskites. We systematically reviewed the recent progress of aromatic spacers used in 2D PSCs. Finally, we propose the possible design strategies for aromatic spacers that may lead to more efficient and stable 2D PSCs.

Mild construction of robust FeS-based electrode for pH-universal hydrogen evolution at industrial current density.

The development of fast and mild preparation of transition metal electrocatalysts for efficient and ultra-stable water electrolysis in wide pH range electrolytes is essential for hydrogen energy supply. Herein, ultrathin and metastable FeS nanolayer self-supported on 3D porous iron foam (IF) substrate is fabricated via one-step mild sulfurization etching for only 2 h to obtain FeS@IF electrode, which achieves efficient and long-term hydrogen evolution in alkaline simulated seawater (1.0 M KOH + 0.5 M NaCl), neutral electrolyte (1.0 M PBS) and other corrosive systems. The overpotentials are only 63 mV and 78 mV to drive 10 mA cm-2 during hydrogen evolution in 1.0 M KOH + 0.5 M NaCl and 1.0 M PBS, respectively. Additionally, the FeS@IF electrode continuously catalyzes for over 600 h at 0.2-0.4 A cm-2 in 1.0 M PBS with negligible performance loss, partly attributed to FeS nanolayer firmly etching on the surface and the formation of corrosion-resistant ultrathin nano fan-like iron sulfide oxide (FeOxSy). This uniformly-distributed morphology helps to facilitate the interfacial electron transmission between active species and substrate, expose more active sites, and provide moderate channels for the rapid liberation of gas bubbles and mass transfer. This work proposes a novel strategy for developing efficient and stable catalysts for hydrogen production in wide pH range systems.

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.

Area-Scalable Zn2SnO4 Electron Transport Layer for Highly Efficient and Stable Perovskite Solar Modules.

The development of a scalable chemical bath deposition (CBD) process facilitates the realization of electron-transporting layers (ETLs) for large-area perovskite solar modules (PSMs). Herein, a method to prepare a uniform and scalable thick Zn2SnO4 ETL by CBD, which yielded high-performance PSMs, is reported. This Zn2SnO4 ETL exhibits excellent electrical properties and enhanced optical transmittance in the visible region. Moreover, the Zn2SnO4 ETL influences the perovskite layer formation, yielding enhanced crystallinity, increased grain size, and a smoother surface, thus facilitating electron extraction and collection from the perovskite to the ETL. Zn2SnO4 thereby yields PSMs with a remarkable photovoltaic performance, low hysteresis index, and high device reproducibility. The champion PSM exhibited a power conversion efficiency (PCE) of 22.59%, being among the highest values published so far. In addition, the CBD Zn2SnO4-based PSMs exhibit high stability, retaining more than 88% of initial efficiency over 1000 h under continuous illumination. This demonstrates that CBD Zn2SnO4 is an appropriate ETL for high-efficiency PSMs and a viable new process for their industrialization.

Lead-Free Halide Double Perovskite Nanocrystals for Light-Emitting Applications: Strategies for Boosting Efficiency and Stability.

Lead-free halide double perovskite (HDP) nanocrystals are considered as one of the most promising alternatives to the lead halide perovskite nanocrystals due to their unique characteristics of nontoxicity, robust intrinsic thermodynamic stability, rich and tunable optoelectronic properties. Although lead-free HDP variants with highly efficient emission are synthesized and characterized, the photoluminescent (PL) properties of colloidal HDP nanocrystals still have enormous challenges for application in light-emitting diode (LED) devices due to their intrinsic and surface defects, indirect band, and disallowable optical transitions. Herein, recent progress on the synthetic strategies, ligands passivation, and metal doping/alloying for boosting efficiency and stability of HDP nanocrystals is comprehensive summarized. It begins by introducing the crystalline structure, electronic structure, and PL mechanism of lead-free HDPs. Next, the limiting factors on PL properties and origins of instability are analyzed, followed by highlighting the effects of synthesis strategies, ligands passivation, and metal doping/alloying on the PL properties and stability of the HDPs. Then, their preliminary applications for LED devices are emphasized. Finally, the challenges and prospects concerning the development of highly efficient and stable HDP nanocrystals-based LED devices in the future are proposed.

Novel Quasi-2D Perovskites for Stable and Efficient Perovskite Solar Cells.

Compared to three-dimensional (3D) organic-inorganic hybrid perovskites, two-dimensional (2D) ones possess great possibilities to realize stable cost-effective perovskite solar cells (PSCs). However, studies indicated that PSCs with 2D perovskites exhibited poor power conversion efficiencies (PCEs). In this study, we report novel propargylamine cation (PPA+)-based quasi-2D perovskites. PPA+ employed as an organic spacer is for enhancing charge-carrier transport of quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin films, consequently boosting PCEs of PSCs. To further boost PCEs of PSCs with quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin films, a quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin film is processed with Pb(SCN)2 additives. Systematical studies indicate that the quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin film processed with Pb(SCN)2 additives exhibits superior film morphology and crystallinity, larger crystals, reduced nonradiative charge-carrier recombination, and enhanced and balanced charge-carrier mobilities compared to the pristine quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin film. As a result, PSCs with the quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin film processed with Pb(SCN)2 additives exhibit a PCE of 15.20%, which is an over 25% enhancement compared to those (12.16%) with a pristine quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin film. In addition, PSCs with the quasi-2D (PPA)2(CH3NH3)2Pb3I10 thin film processed with Pb(SCN)2 additives possess dramatically suppressed photocurrent hysteresis and significantly boosted stability. All these results indicate that we have developed a facile way to synthesize novel 2D perovskite thin films for realizing stable and efficient PSCs with dramatically suppressed photocurrent hysteresis.

Toward Perovskite Solar Cell Commercialization: A Perspective and Research Roadmap Based on Interfacial Engineering.

High-efficiency and low-cost perovskite solar cells (PVKSCs) are an ideal candidate for addressing the scalability challenge of solar-based renewable energy. The dynamically evolving research field of PVKSCs has made immense progress in solving inherent challenges and capitalizing on their unique structure-property-processing-performance traits. This review offers a unique outlook on the paths toward commercialization of PVKSCs from the interfacial engineering perspective, relevant to both specialists and nonspecialists in the field through a brief introduction of the background of the field, current state-of-the-art evolution, and future research prospects. The multifaceted role of interfaces in facilitating PVKSC development is explained. Beneficial impacts of diverse charge-transporting materials and interfacial modifications are summarized. In addition, the role of interfaces in improving efficiency and stability for all emerging areas of PVKSC design are also evaluated. The authors' integral contributions in this area are highlighted on all fronts. Finally, future research opportunities for interfacial material development and applications along with scalability-durability-sustainability considerations pivotal for facilitating laboratory to industry translation are presented.