Abstract Self-assembled monolayers (SAMs) have emerged as efficient hole-transport layers for inverted perovskite solar cells (PSCs), yet molecular self-aggregation during assembly limits interfacial homogeneity and device performance. Here we report an indole-carbazole co-adsorption strategy by incorporating N-indoleacetic acid (Nd) into (4-(3,6-diphenyl-9H-carbazol-9-yl)butyl)phosphonic acid (Ph-4PACz) to construct phase-homogeneous monolayers. Nd interacts with Ph-4PACz via synergistic π–π stacking and hydrogen bonding, resulting in a uniform alternating Ph-4PACz/Nd molecular arrangement. This co-adsorbed structure enables optimized interfacial energy alignment, enhances perovskite film uniformity, and suppresses trap-assisted non-radiative recombination. As a result, devices achieve an efficiency of 26.95% (certified 26.57%) on 0.0717 cm2 and 25.61% on 1 cm2, retaining 93.36% of their initial efficiency after 1500 h of maximum power point tracking under continuous illumination and 91.10% after 1200 h at 85 °C. The strategy is broadly applicable to carbazole-based SAMs and wide-bandgap PSCs, offering a general co-adsorption route toward efficient and stable devices.

High-efficiency perovskite-silicon tandem solar cells require effective charge recombination at the interconnecting junction. On textured silicon bottom cells, conventional alkyl-chain-based self-assembled molecules (SAMs) tend to aggregate, limiting device performance. To overcome this, we synthesized a conjugated linker SAM, (4-(7H-dibenzo[c,g]carbazol-7-yl)phenyl)phosphonic acid (Bz-PhpPACz), enabling efficient charge transport. Our molecular design included controlling bromine (Br) impurities in the SAM precursors, as chemical analysis revealed that commercial 4PADCB contains trace bromine species that passivate interface defects. We optimized the molecular mixture by precisely blending brominated and non-brominated counterparts. The conjugated framework promotes charge transport on rough surfaces, while bromine improves energy alignment, passivates defects, and relieves lattice strain in the perovskite layer. This approach yielded perovskite-silicon tandem cells on Czochralski (CZ) silicon with 31.4% efficiency, highlighting the critical role of molecular design and impurity control in achieving high-performance tandem devices.

Perovskite solar cells (PSCs) experience mechanical damage and failure (i.e. degradation and fracture) induced by temperature changes under thermal cycling. However, few studies have been able to simultaneously suppress interface delamination and delay chemical degradation to ensure the mechanical integrity of perovskite film under thermal shock, making it challenging to improve the thermal cycling stability of PSCs. We report a universal interlocking strategy via the modification of polymethyl(hydro)/polymethylvinylsilazane (PHVS), which achieves interfacial interlocking through the condensation reactions with substrates, hydrogen bonding with the perovskite film, and a self-crosslinking reaction. The interlocked interface significantly enhances the interfacial adhesion toughness and releases the residual stress of the perovskite film, thereby suppressing the interface delamination and delaying the chemical degradation under thermal cycling. The PHVS-modified PSCs exhibit a certified efficiency of 26.82%. The encapsulated PSCs retain 96% of their original efficiency after 200 cycles of thermal cycling testing, and the perovskite modules maintain 95% of their original efficiency after 1000 h, day and night, outdoor testing. This work highlights the significance of enhancing the mechanical integrity of perovskite films under thermal cycling and provides a promising approach for achieving thermal cycling-stable PSCs with high efficiency.

Interfacial charge extraction is the kinetic bottleneck governing the open-circuit voltage (V OC) in perovskite solar cells (PSCs), yet it is conventionally modeled as a static process characterized by a constant extraction velocity. Here, we demonstrate that interfacial extraction is inherently dynamic and self-limiting, driven by a negative feedback loop where accumulating charges generate a transient electric field that suppresses subsequent carrier transfer. Using interface-sensitive transient reflectance (TR) spectroscopy combined with a field-modified diffusion-extraction model, we resolve the time-dependent extraction velocity, S F(t), at ITO/perovskite and ITO/SAM/perovskite buried interfaces. We uncover a fundamental trade-off: efficient interfaces (e.g., SAM-functionalized) exhibit high initial extraction rates (S 0) but suffer from rapid field saturation (short tau), leading to a sharp decay in extraction efficacy. This self-generated field mechanism is corroborated by Kelvin probe force microscopy and explains the performance disparity in operational devices. To quantify this dynamic behavior, we introduce the time-integrated extraction capacity, , as a robust descriptor of sustained performance. This metric accurately reflects the superior V OC (1.18 V versus 1.13 V) and efficiency (26.47% versus 25.45%) of optimized SAM-based devices, establishing a new paradigm for designing interfaces that minimize field-induced losses.

Self-assembled monolayers serve as hole-selective contacts in perovskite solar cells, but their scalable fabrication remains challenging. Here we report a rapid (<= 5 min) soak-coating strategy for self-assembled monolayer fabrication, enabled by molecular design and solvent engineering. The unsymmetric self-assembled monolayer material (4-(10-methoxy-7H-benzo[c]carbazol-7-yl)phenyl)phosphonic acid was rationally designed with dual-functional molecular segments to inhibit molecular aggregation in solution and enhance interfacial charge transport. Concurrently, an ethanol-based solvent system containing 1.5 vol% water was engineered to improve material dispersity and strengthen surface anchoring on transparent conducting oxide substrates. The soak-coated self-assembled monolayers exhibit dense and uniform coverage, yielding perovskite solar cells with a certified power conversion efficiency of 27.23%. This methodology demonstrates good scalability, successfully extending to large-area devices, mini-modules and flexible architectures, all of which maintain stable operation. Notably, both the soak-coating solutions and modified transparent conducting oxide substrates can be reused, substantially improving resource efficiency. This work provides a scalable and cost-efficient route for fabricating stable perovskite solar cells.

The surfaces of MXene etched via chemical etching feature randomly diverse terminals, which creates an uneven surface potential. The non-uniform potential promotes disordered stacking of nanosheets, which in turn precipitates a rapid deterioration in the electrochemical performance of MXene-based electrodes at high mass loadings (ML). In this study, L-ascorbic acid (AA) is used to block polymerization of dopamine (DA), forming a uniform polydopamine (PDA) coating on MXene surfaces, which corrects the surface potential distribution. And we add borax to do a further modification to increase stabilization. Characterization results demonstrate that introducing AA creates a more uniform PDA coating and surface potential distribution, which not only increases the interlayer spacing but also improves the in-plane stacking orderliness of the nanosheets, which is beneficial for electrolyte transport. The as-prepared electrode retains high areal capacitance (5.6 F cm- 2) at 10.0 mg cm- 2, and the resulting symmetric device exhibits outstanding cycling stability. This study offers an insight for optimizing the surface potential and orientation of MXene, paving the way toward high ML electrode applications.

Despite rapid advances in perovskite solar cells (PSCs), interfacial losses at the SnO2/perovskite buried contact continue to limit the efficiency and operational stability of n–i–p devices. Here, we introduce trace...

Perovskite solar cells (PSCs) based on poly[bis(4-phenyl) (2,4,6-trimethylphenyl) amine] (PTAA) as the hole transport material offer excellent thermal stability but still suffer from open-circuit voltage (V OC) losses that limit their power conversion efficiency (PCE). These losses are primarily attributed to interfacial defects, energy level mismatches, and suboptimal contact with charge transport layers, which induce non-radiative recombination. Here, a conjugated ionic additive designed to synergistically integrate interfacial engineering and bulk passivation is reported. The cationic pi-conjugated moiety localizes at grain boundaries and the perovskite/PTAA interface, enabling energy level tuning, defect passivation, and enhanced hole extraction, while the anionic counterpart preferentially resides at the buried perovskite/SnO2 interface, passivating interfacial defects and improving film quality. This dual-site modulation yields high-quality perovskite films with suppressed energetic disorder and improved charge extraction. As a result, n-i-p structured PSCs employing PTAA achieve PCEs of (25.73 +/- 0.35)%, alongside a 15.17 cm2 mini-module delivering (22.96 +/- 0.61)% efficiencies. The devices exhibit outstanding stability, retaining 86% of the original PCE following 960 h of thermal aging at 85 degrees C in nitrogen. This work demonstrates that rationally designed conjugated ionic additives can simultaneously optimize bulk and interfacial properties, offering a viable route toward high-efficiency, stable PSCs compatible with scalable manufacturing.

Electrocatalytic nitrate reduction reaction (NO3-RR) to ammonia is a promising approach for ammonia synthesis under ambient conditions. However, most studies have focused on nitrate reduction using alkaline wastewater, neglecting the large amount of acidic wastewater. Although many catalysts exhibit excellent NO3-RR performance in alkaline environment, they do not perform well in acidic conditions (with ammonia yield rate <= 1 mmol h-1 cm- 2 ) owing to poor stability, strong competition from hydrogen evolution reaction (HER), and inadequate nitrate hydrogenation kinetics in acidic solution. In this study, we prepared an acidic-stable and HER-inert catalyst based on bimetallic copper-iron phthalocyanine molecules (Cu1Fe3Pc) that exhibits ammonia Faradaic efficiency over 89% and yield rate over 2.4 mmol h-1 cm- 2 at all pH conditions. We employed deuterium labelling and operando Fourier-transform infrared spectroscopy to investigate promoted nitrate hydrogenation behaviors on Cu1Fe3Pc. Density functional theory simulations further demonstrate that electrons concentrated near FePc in Cu1Fe3Pc promote nitrate hydrogenation to ammonia in both acidic and alkaline conditions. Our research suggests a material strategy for the practical ammonia electrosynthesis for nitrate waste across a wide pH range.

Perovskite solar cells (PSCs) have emerged as a promising candidate for low‐cost and high‐efficiency photovoltaic solutions, poised to rival conventional photovoltaic technologies. Despite their potential, the path to commercialization is impeded by the significant defect state density present within the films. In this work, a phthalocyanine derivative, tetra‐2‐(benzyloxy)ethoxy substituted Zn(II) phthalocyanine (BE‐ZnPc), characterized by multiple binding sites, is introduced into the perovskite precursor solution. This innovative approach is designed to modulate the crystallization process of the perovskite and to passivate defects through a strategic doping mechanism. The BE‐ZnPc molecule, with its planar macrocyclic structure and electron‐donating attributes, engages effectively with the undercoordinated Pb 2+ ions, thereby diminishing the defect density and enhancing the overall film quality. The resultant PSCs, optimized with BE‐ZnPc, have achieved power conversion efficiencies (PCE) as high as 26% (with a certified PCE of 26.05%), marking a significant milestone in PSC performance. Moreover, these devices maintain an impressive 92% of their initial PCE following 550 h of operation at the maximum power point. This study delineates a novel strategy for bolstering both the efficiency and durability of PSCs through the utilization of functional phthalocyanines, charting a new course for the advancement of PSC technology.

Electrochemical acetamide synthesis under ambient conditions offers a sustainable route for converting waste nitrate into valuable chemicals. Conventional methods, limited to standalone reduction or oxidation processes, typically achieve low Faradaic efficiencies (<40

Fabricating high-quality perovskite layers is essential for achieving high-performance solar cells. Considering the significant advancements made in additive engineering for optimizing perovskite crystallization using single additive, exploring the collaborative effect of dual additives on precursor for perovskite crystallization may be an effective way for further advancing device performance. Herein, a binary additives strategy is proposed, where phenylmethylammonium iodide (PMAI) and [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) are introduced into the precursor. Compared with the precursor with no additives or a single additive (PMAI or 2PACz), the use of dual additives more effectively cleaves edge-shared Pb-I octahedra to expedite the transformation from PbI2 to PbI3 - complexes as prenucleation clusters and produces much larger colloidal particles with accelerated nucleation. Concurrently, the crystallization in both spin-coating and annealing processes is significantly retarded due to the stronger interaction between perovskite and binary additives. Benefiting from such rapid nucleation and slow crystallization, high-quality perovskite layer with larger-sized crystals and fewer defects is formed, resulting in mitigated microstrain, enhanced charge extraction, and suppressed nonradiative recombination. Consequently, the device derived from the use of dual additives could achieve an impressive efficiency of 26.05% (certified 25.49%) and retained 90% of its initial efficiency after 1200 h of maximum power point tracking.

Self-assembled molecules (SAMs) as hole-selective layers have achieved tremendous success in perovskite solar cells. However, the effective modulation of the adsorption configuration of hybrid SAMs on indium tin oxide (ITO) substrates remains a challenge, which essentially influences the SAM's orientation and homogeneity. Herein, the adsorption configuration of [4-(3,6-diphenyl-9H-carbazol-9-yl)butyl]phosphonic acid (Ph-4PACz) on the ITO surface is modulated with co-assembled molecules 2,3,5,6-tetrafluoroterephthalic acid (BCA) or 2,3,5,6-tetrafluoro-4-sulfanylbenzoic acid (BSCA). Specifically, planar BCA molecules anchored via bi-carboxylic groups stabilize Ph-4PACz in a tilted configuration, forming an angle of approximately 54.03° relative to the ITO surface, whereas tilted BSCA molecules anchored via mono-carboxylic groups induce Ph-4PACz to adopt an almost perpendicular orientation relative to the ITO surface. Upon BSCA introduction, the Ph-4PACz film becomes more uniform with better energy level alignment, which further results in the enhanced homogeneity of the buried surface of perovskite films with enhanced charge transport and reduced interfacial non-radiative recombination losses. Consequently, the resultant BSCA-based devices achieve a high efficiency of 26.72% (certified 26.75%) for devices with the active area of 0.0717 cm2 and 25.21% for 1 cm2, respectively, maintaining over 90% of their initial efficiencies after 1,500 h operational tracking under illumination or 1000 h at 85 °C heating.

The synthesis of stable helically chiral dinuclear Pd(II) diacetylide complexes exhibiting intramolecular Pd···Pd interactions in both fluid and solid states is reported, utilizing foldable bis(arylacetylide) as electron-donating ligands. A systematic investigation of the substitution effect of chiral oxazolinyl-type C^N^N moieties and foldable bis(arylacetylide) ligands, with and without alkoxy linker groups, on the molecular configuration and circularly polarized luminescence (CPL) properties of the chiral dinuclear Pd(II) complexes has been conducted. The emission peak maximum was found to be tunable from 650 to 715 nm, and CPL dissymmetry factors (|glum|) up to 3.0 × 10-3 have been obtained. The metal-metal-to-ligand charge transfer (MMLCT) nature of the phosphorescence was assigned through analysis of the photophysical properties and TDDFT calculations. Additionally, circularly polarized organic light-emitting diode (OLED) devices employing the helically chiral Pd(II) complexes as phosphorescent emitters have been successfully fabricated, achieving a maximum |gEL| value of approximately 3.0 × 10-3.

Self-assembled monolayer (SAM) materials have emerged as promising materials for interface engineering in perovskite solar cells. However, achieving an optimal balance between molecular packing density, charge transport efficiency, and defect passivation remains a challenge. In this work, we propose a SAM material design strategy that synergizes flexible head groups with rigid linking groups. Using (4-(diphenylamino)phenyl)phosphonic acid as a model molecule, Compared to traditional materials such as (4-(9H-carbazol-9-yl)phenyl)phosphonic acid and (4-(diphenylamino)phenethyl)phosphonic acid, our material generates a high-quality perovskite layer. This design achieves superior energy level alignment, improved hole extraction, and enhanced charge transport efficiency, effectively reducing non-radiative recombination. (4-(diphenylamino)phenyl)phosphonic acid-based device achieve power conversion efficiency of 26.21% and 24.49% for small- (0.0715 cm2) and large-area (1 cm2), respectively. This work establishes an effective approach to SAM molecular design, providing a clear pathway for improving both the efficiency and long-term stability of perovskite solar cells through interface engineering.

While self-assembled material based inverted perovskite solar cells have surpassed power conversion efficiencies of 26%, enhancing their performance in large-area configurations remains a significant challenge. In this work, we report a self-assembled material based hole-selective layer 4-(7H-dibenzo[c,g]carbazol-7-yl)phenyl)phosphonic acid, with a π-expanded conjugation. The enhanced intermolecular π–π interactions facilitate the self-assembly of 4-(7H-dibenzo[c,g]carbazol-7-yl)phenyl)phosphonic acid molecules to form an ordered bilayer with a hydrophilic surface, which passivates the buried perovskite interface defect and enables high-quality and large-area perovskite preparation, while simultaneously enhancing interfacial charge extraction and transport. The certified efficiency of 4-(7H-dibenzo[c,g]carbazol-7-yl)phenyl)phosphonic acid based small-area (0.0715 cm2) device is 26.39% with high stability. Furthermore, a certified efficiency of 25.21% is achieved for a 99.12 mm2 large area device. Qu et al. report a self-assembled material with π-expanded conjugation to form hydrophilic ordered bilayer as hole selective layer for inverted perovskite solar cells. The enhanced interfacial charge extraction and transport enable certified efficiency of 26.39% and 25.21% for 7.15 mm2 - and 99.12 mm2 -devices, respectively.

The conventional fabrication of perovskite solar cells (PSCs) has historically relied on toxic solvents, such as dimethylformamide (DMF), N-methyl-2-pyrrolidone (NMP), and chlorobenzene, a practice that is now yielding to more sustainable and economically viable alternatives. A one-step antisolvent-free methodology is developed, guided by the strategy of minimizing solvent toxicity and enhancing device performance. This method employs N,N-dimethylacetamide (DMAc) and N,N'-dimethylpropyleneurea (DMPU) as alternatives to DMF/NMP in antisolvent-free perovskite fabrication, along with ethanol for the hole transport layer. However, formamidinium (FA)-based perovskite films prepared via an antisolvent-free process often suffer from severe crystallization issues at the buried interface, which lacks rapid solvent removal and leads to a high concentration of defects such as uncoordinated Pb2+ ions. To surmount this challenge, a strategy is devised that paired the use of mixed solvents (DMAc/DMPU) with the incorporation of stable radical additives, featuring Cl, methoxy, or methylthio groups. This approach effectively modulates the crystallization dynamics, diminishes defect concentrations, and enhances the extraction of charge carriers. Employing this method, an efficiency of 25.02% is achieved, along with exceptional operational stability. This breakthrough represents a pivotal leap forward in the realm of sustainable photovoltaics, offering a promising path toward a greener energy future.

The rationale for low performances in perovskite solar cells with buried interface still needs to be clarified, owing to the complicated physiochemistry of metal oxides/perovskite interface, and literature offers a meager knowledge about the reactions at this interface. While exploring the SnO2/perovskite interfacial interactions, the reasons behind deteriorating perovskite at the interface are comprehensively investigated, and it is revealed that the PbI2 residue and metallic Pb-0 are the byproducts of this decomposed perovskite. Introducing an optimized amount of Ti3C2TX at the SnO2/perovskite interface detaches the SnO2 hydroxyls, which are found to be responsible for interfacial ion migrations. In addition, Ti3C2TX passivates the interface defects via its functional groups and establishes ballistic pathways for electrons with high chances of non-radiative recombination. Thus, 25.19% (certified as 24.41%) of efficiency with superior long-term operational stability is achieved.

To make supercapacitors a viable commercial product, it is necessary to increase the mass loading (ML) of the electrodes. However, current research on high ML MXene electrodes mainly focuses on internal structure optimization, often neglecting the importance of surface texture in the electrodes, which plays a crucial role in mediating interactions between the internal structure and the electrolyte. This study reports on a simple ion-intercalation process that can reduce charge transfer resistance and improve cycling stability. Through the integration of 3D visualization models and wide-angle X-ray scattering techniques, a comprehensive investigation of the electrode's surface structure and MXene flake arrangement is conducted. The results showed that pre-oriented aggregates induced by ion-intercalation create a sophisticated surface structure with rich hills and valleys, promoting electrolyte permeation and ion exchange. This work highlights the significance of surface texture in films and electrodes, guiding the design of high-performance materials.

We report a highly crystalline self-assembled multilayer (SAMUL) that is fundamentally different from the conventional monolayer or disordered bilayer used for hole-extraction in inverted perovskite solar cells (PSCs). The SAMUL can be easily formed on ITO substrate to establish better surface coverage to enhance the performance and stability of PSCs. A detailed structure-property-performance relationship of molecules used for SAMUL is established through a systematic study of their crystallinity, molecular packing, and hole-transporting properties. These SAMULs are rationally optimized by varying their molecular structures and deposition methods through thermal evaporation or spin-coating for fabricating PSCs. The CbzNaphPPA-based SAMUL was chosen for fabricating inverted PSCs due to it exhibiting the highest crystallinity and hole mobility which is derived from the ordered H-aggregation. This resulted in a remarkably high fill factor of 86.45 %, which enables a very impressive power conversion efficiency (PCE) of 26.07 % to be achieved along with excellent device stability (94 % of its initial PCE retained after continuous operation for 1200 h under 1-sun irradiation at maximum power point at 65 °C). Additionally, a record-high PCE of 23.50 % could be achieved by adopting a thermally evaporated SAMUL. This greatly simplifies and broadens the scope for SAM to be used for large-area devices on diverse substrates.