Green hydrogen production driven by intermittent renewable energy poses significant challenges to alkaline hydrogen evolution reaction (HER) in achieving high-efficiency and durability. An all-in-one nanostructured electrochemical reactor (NER) was newly designed and synthesized for the HER electrode to tackle the challenges by enabling continuous electron transport and intensified gas-liquid transport in NER, thereby maximizing the interfacial charge-transfer reaction capability of the catalyst electrode under large and varying currents. This was realized by designing an all-in-one catalyst P-CoPt3/P-CoMoO4, featuring a self-supported structure, a heterostructure, and a super-hydrophilic nanoarray. This all-in-one catalyst functions as a built-in NER with finely-tailored critical interfaces. Self-supported structure and heterostructure form strong couplings at electron-conducting heterointerfaces, enabling continuous electron transport across these interfaces and thus in the NER. Super-hydrophilic nanoarray allows continuous gas-liquid transport at electrode/electrolyte interfaces, intensifying the gas-liquid transport process in the NER. Consequently, P-CoPt3/P-CoMoO4 displayed a >30-fold increase in mass activity for alkaline HER compared to the P-CoPt3 catalyst electrode. It exhibited an impressively low overpotential of 132 mV at 1 A cm-2. Stable operation for over 750 h at 100 and 500 mA cm-2 and notable durability under varying currents were also obtained. Overall water-splitting of P-CoPt3/P-CoMoO4 || RuO2 outperformed the commercial Pt/C || RuO2, especially at higher currents.
Alkaline hydrogen evolution reaction (HER) is limited by sluggish water dissociation kinetics. Herein, Ru nanoparticles supported on an oxygen-vacancy-rich amorphous/crystalline MoO2 heterostructure (Ru/ac-MoO2@NC) are developed to promote HER in alkaline media. The amorphous phase provides a distribution of active sites that facilitates water adsorption and dissociation, while the crystalline phase ensures efficient charge transport. Experimental results combined with theoretical calculations reveal that the interfacial interaction between Ru and MoO2 reduces the energy barrier for water dissociation and optimizes hydrogen adsorption/desorption. As a result, the catalyst achieves a low overpotential of 13 mV at 10 mA cm-2 with a Tafel slope of 12 mV dec-1, outperforming commercial Pt/C, along with good stability.
Wide-bandgap (WBG) perovskites are essential components for all-perovskite tandem solar cells, yet they often suffer from substantial open-circuit voltage (V OC) deficits and uncontrolled crystallization kinetics. Herein, we employ a coordination engineering strategy with a multifunctional additive, 4-(Trifluoromethyl) benzene-1-sulfonyl chloride (BSCF3), to optimize 1.77 eV WBG perovskite films. Detailed spectroscopic characterizations reveal that the -SO2Cl group acts as a Lewis base to coordinate with Pb2+ ions and the strongly electronegative -CF3 group forms hydrogen bonds with formamidinium (FA+) cations. These synergistic effects regulate the subsequent nucleation and crystallization kinetics. Driven by this controlled growth process, the resulting films exhibit enlarged grain sizes and suppressed residual PbI2 phases. This enhanced structural integrity, in turn, minimizes the trap-state density and significantly mitigates nonradiative recombination at the grain boundaries. As a result, the inverted 1.77 eV WBG perovskite solar cells achieve a champion power conversion efficiency (PCE) of 19.81% with a high V OC of 1.32 V. Furthermore, the optimized monolithic all-perovskite tandem cells deliver a remarkable PCE of 27.26%. Under continuous 1-sun illumination in a nitrogen atmosphere, both the single-junction and tandem devices retain approximately 80% of their initial efficiencies after 1000 and 300 h aging, respectively.
Annealing, while indispensable for achieving high-quality perovskite crystals, introduces strain into the material, undermining the stability of perovskite solar cells. Here we incorporate 1,4-butanesultam as an additive into the perovskite precursor film to address this issue. During annealing, the additive liquifies and promotes grain boundary reconstruction and crystal reorganization, resulting in large, strain-free perovskite grains. The liquid state also facilitates the conformal deposition of the self-assembled molecules that serve as a hole transport layer at the bottom surface of the perovskite, further minimizing tensile strain. The resulting solar cell achieves a power conversion efficiency of 26.79% and retains 95% of its initial efficiency after 1,000 h of ISOS-V-2 testing, as well as 98% after 1,500 h of diurnal cycling between dark at 20 degrees C and light at 85 degrees C.
Atomic-layer-deposited (ALD) tin oxide (SnO2) electron-transport layers (ETLs) generally underperform in n-i-p structured perovskite solar cells (PSCs) compared to solution-processed counterparts. The inherent organic residues in ALD-SnO2 disrupt crystallinity and obstruct charge transfer, while they accelerate perovskite interfacial degradation. To address this, an invasive solution bath post-treatment is introduced by using sodium 2,3-dimercapto-1-propanesulfonate (DMPS) as the additive in the solution bath. DMPS, bearing thiol and sulfonate groups, simultaneously chelates the surface and the inner layer of the SnO2 layer, successfully removing organic residues from the bulk and surface while suppressing water-induced morphological damage. Consequently, this synergistic modification yields champion efficiencies of 25.26% for small-size cells and 22.42% for 12.5 cm2 mini-modules, alongside significantly enhanced operational stability. Our work offers a scalable route for integrating high-performance ALD-SnO2 in large-area n-i-p solar modules.
Semitransparent perovskite solar cells require top electrodes that are transparent, conductive, and stable, yet bare AgNW networks suffer from high junction resistance and oxidation in air. Here, we combine spray-coated AgNWs with a sputtered indium zinc oxide overlayer on an ALD-SnOx buffer layer to create an oxidation-retarded AgNWs/IZO composite electrode. By tuning AgNW coverage and IZO thickness, the electrode can be adjusted over a broad optoelectronic window, with an average near-infrared transmittance of 85.4-88.8%, a sheet resistance of 5-15 Ω/□, and a maximum figure of merit of 383.5. The IZO overlayer bridges nanowire junctions, smooths the surface, and retards air-induced degradation. As a result, haze is reduced to 1.53%, and resistance increases by less than 10% after 3 months in air. Using the optimized electrode, 1.68 eV semitransparent devices achieved a power conversion efficiency of 18.4%, while 2T perovskite/TOPCon tandems reach 28.3% with T90 ≥ 800 h.
This study demonstrates how an interaction between the additive BrFBN and a perovskite precursor results in a perovskite film with fewer defect states. This work provides insights on the feasibility of manufacturing stable, high-performance PSCs.
The commercial viability of perovskite photovoltaics hinges on developing efficient and stable solar modules, with high-quality, large-area perovskite films being crucial but hindered by uncontrolled crystallization of perovskite. This challenge can be effectively addressed through a perovskite-solvent complex intermediate phase strategy. To elucidate the molecular-level design principles of solvent additives, a systematic exploration of various solvent additives has been conducted. It reveals that complexation with nitrogen can boost the nucleation rate of the intermediate phase. On this basis, and guided by DFT calculations, two N-methyl groups are incorporated into the commonly used amide structure to elevate the electronegativity of nitrogen above that of oxygen. Consequently, N,N '-dimethyl-2-imidazolone is chosen as a solvent additive to enable the effective printing of high-quality perovskite films, thereby realizing efficient and stable perovskite solar cells. When scaled up to 30 x 30 cm2, the perovskite solar modules achieve a champion efficiency of 20.19 %.
Flexible perovskite solar cells have broader prospects for application over their rigid counterparts. However, they are normally prepared by the spin coating process, which is not conducive to scaling up. One of the considerable barriers to scaling up stems from the printing of electron transport layers (ETLs), with tin oxide (SnO 2 ) being a commonly used material. Here, poly(acrylic acid) (PAA) is introduced into the SnO 2 nanocrystals ink to engineer the ink to enhance the dispersion of nanocrystals and slow down solvent evaporation, ensuring the printed ETLs having optimized coverage and morphology. Concurrently, the buried interface is refined by PAA, which enhances charge transfer and suppresses nonradiative recombination. The flexible device modified by PAA achieves a high efficiency of 22.46% (certified at 21.56%) and retains 89.3% of its initial value after 3000 bending cycles and 92.4% after 2000 hours of storage. The printed 30 centimeter–by–30 centimeter flexible module attains an impressive efficiency of 16.40% (certified at 16.28%).
The metal halide (BX6)4- octahedron, where B represents a metal cation and X represents a halide anion, is regarded as the fundamental structural and functional unit of metal halide perovskites. However, the influence of the way the (BX6)4- octahedra connect to each other has on the structural stability and optoelectronic properties of metal halide perovskite is still unclear. Here, the octahedral connectivity, including corner-, edge-, and face-sharing, of various CsxFA1-xPbI3 (0 ≤ x ≤ 0.3) perovskite films is tuned and reliably characterized through compositional and additive engineering, and with ultralow-dose transmission electron microscopy. It is found that the overall solar cell device performance, the charge carrier lifetime, the open-circuit voltage, and the current density-voltage hysteresis are all improved when the films consist of corner-sharing octahedra, and non-corner sharing phases are suppressed, even in films with the same chemical composition. Additionally, it is found that the structural, optoelectronic, and device performance stabilities are similarly enhanced when non-corner-sharing connectivities are suppressed. This approach, combining macroscopic device tests and microscopic material characterization, provides a powerful tool enabling a thorough understanding of the impact of octahedral connectivity on device performance, and opens a new parameter space for designing high-performance photovoltaic metal halide perovskite devices.
Buried interface engineering is crucial to improve the performance and stability of perovskite solar cells (PSCs). Although coordination materials have been widely used for buried interface modification, they are generally engineered on one surface of the interface through monodentate or bidentate molecules. Here, we propose that a multidentate polymer, sodium alginate (SA), acts with both surfaces via numerous C & boxH;O groups to reinforce buried interfaces. SA effectively reduces buried interface defects, adjusts the energy level alignment, and refines carrier dynamics. Notably, it also induces the growth of a perovskite film that is less tensile stressed and free of voids. Consequently, the champion device efficiency after SA treatment increased from 23.05% to 24.98%, along with significant improvements in both light and thermal stability. This work offers insights into efficiency and stability improvement from the perspective of multidentate polymer anchoring.
Poly[bis(4‐phenyl)(2,4,6‐trimethylphenyl)amine] (PTAA), as an extensively used hole transport material in inverted perovskite solar cells (PSCs), has given reason for concern due to its hydrophobicity for a long time. Herein, buried interface engineering is applied for the scalable deposition of perovskite films by introducing an amphiphilic molecule hexadecyltrimethylammonium chloride on the PTAA surface, which improves the interfacial wettability of the perovskite precursor solution on the organic hole transport layer (HTL), facilitates the nucleation and growth of perovskites, and reduces the nonradiative recombination at the perovskite/HTL interface. As a result, all photovoltaic parameters of the inverted PSCs are improved significantly. The champion devices demonstrate power conversion efficiencies (PCEs) of 22.04% and 20.47% with aperture areas of 0.148 and 1.0 cm2, respectively. Moreover, the encapsulated 1.0 cm2 device exhibits excellent stability and maintains over 70% of its initial PCE after 1200 h under continuous 1 sun illumination at 65 °C in a nitrogen environment.
The low‐cost perovskite solar cell has become the next‐generation photovoltaic. However, compared to the high efficiency of the small‐area perovskite solar cells, the large‐area perovskite solar modules (PSMs) have still been struggling for the performance. In addition to preventing the decline in quality of each functional layer after upscaling, another key point is to construct a high geometric filling factor (GFF) for an efficient PSM. Herein, a “back‐scribing” technique is developed by using a low‐cost nanosecond laser scribing from the back side of substrates. The “back‐scribing” technology can clean up the scribing channels greatly, enabling an effective connection with a small damaged area. With precise control of the laser parameters for the scribing of P1, P2, and P3, a high GFF of 96% is achieved, resulting in a high power conversion efficiency of 19.97% with an aperture area of 16 cm 2 for the PSM. By this means, the efficiency loss is minimized (<10%) when upscaling a small device to a large‐area solar module.
AbstractTin oxide has made a major breakthrough in high‐efficiency perovskite solar cells (PSCs) as an efficient electron transport layer by the low‐temperature chemical bath deposition method. However, tin oxide often contains pernicious defects, resulting in unsatisfactory performance. Herein, we develop high‐quality tin oxide films via a nitrogen‐doping strategy for high‐efficiency and stable planar PSCs. The aligned energy level at the interface of doped SnO2/perovskite, more excellent charge extraction and reduced nonradiative recombination contribute to the enhanced efficiency and stability. Correspondingly, the power conversion efficiency of the devices based on N‐SnO2 film increases to 23.41% from 20.55% of the devices based on the pristine SnO2. The N‐SnO2 devices show an outstanding stability retaining 97.8% of the initial efficiency after steady‐state output at a maximum power point for 600 s under standard AM1.5G continuous illumination without encapsulation, while less than 50% efficiency remains for the devices based on pristine SnO2. This simple scalable strategy has shown great promise toward highly efficient and stable PSCs.
Metal‐halide perovskite solar cells (PSCs) exhibit outstanding power conversion efficiencies (PCEs) when fabricated as mm‐sized devices, but creation of high‐performing large‐area modules that are stable on a sufficiently long timescale still presents a significant challenge. Herein, the quality of large‐area perovskite film is improved by using ionic liquid additives via forming a new Pb‐N bonding between the ionic liquid and Pb 2+ . This new bond can be modulated by a critical screening of the anion structure of the ionic liquid. The selected ionic liquid effectively reduces the defects of the perovskite films and markedly elongate their carrier lifetimes. As a result, a champion PCE of 24.4% for small‐area (0.148 cm 2 ) devices and 20.4% for larger‐area (10.0 cm 2 ) modules under AM 1.5G irradiation is achieved. More importantly, the modified devices retain 90% of their peak PCE after aging for 1900 h at 65 ± 5 ° C (ISOS‐T‐1) and 80% after continuous light soaking for 750 h. The non‐encapsulated modules maintained 80% of their peak PCE after 1100 h of aging in the air with a relative humidity of 35 ± 5% and temperature of 25 ± 5 ° C under dark (ISOS‐D‐1), showing great potential for future commercialization.
Suppressing nucleation over large areas Although formamidinium-based lead iodide (PbI 2 ) perovskites have a favorable bandgap and good thermal stability, the difficulty in controlling nucleation makes it difficult to grow high-quality, large-area films compared with methylammonium counterparts. Bu et al. show that adding N -methyl-2-pyrrolidone to the perovskite precursors forms an adduct with PbI 2 that promotes the formation of the desired black α-phase at room temperature. The addition of potassium hexafluorophosphate eliminated hysteresis by passivating interfacial defects and promoted long-term thermal stability at 85°C in unencapsulated devices. Large-area modules (17 square centimeters) achieved power conversion efficiencies of 20.4%. Science , abh1035, this issue p. 1327
With the high efficiencies achieved, perovskite solar cells are showing promise for commercial applications. Exploring scale-up technology for perovskite solar modules is becoming the next focus. The scaling-up not only requires the development of methods for fabrication of large-area perovskite films but also needs to develop functional materials for high-efficiency modules. To evaluate the materials for modules, a mature module fabrication process shall be established. However, few research groups know how to fabricate modules, especially the large-area perovskite films, which is often difficult to learn or requires expensive instruments. This will slow down the research in perovskite solar modules. Herein, a detailed description for the fabrication of high-efficiency mini-modules in lab is elaborated. Using spin-coater and multi-tip pipette, repeatable 5 x 5 cm(2) modules with efficiency exceeding 16% are easily fabricated. Thus, a simple way to fabricate modules in labs is demonstrated, providing a platform for modules research.
A green approach is employed to prepare mechanically enhanced composites by adding noncovalently proanthocyanidin (PC)-modified graphene (PC-rGO) into poly(vinyl alcohol) (PVA). Ascorbic acid (AA) is used as the reducing agent, and PC is used as a dispersant to synthesize low-defect and fully dispersed graphene. After static treatment, the PC-rGO sheets in the composite form a horizontally arranged structure. Compared with neat PVA, the Young's modulus of the graphene-modified composites is significantly enhanced by approximately 79.3% with incorporation of 0.9 wt% PC-rGO. The composites incorporated with GO or AA-rGO (without PC) have randomly distributed GO structures and apparent rGO agglomeration, resulting in a weaker mechanical property. The dispersibility, degree of defects, distribution state of graphene, and interactions with the polymer matrix are directly related to the final mechanical performance. This new approach to mechanically enhance graphene-embedded PVA composites provides the possibility for large-scale production of graphene-reinforced composite materials.
The gas-liquid membrane contactor forms a gas-solid-liquid interface and has a high potential for the applications in gas adsorption, catalysis, energy exchange, and so on. Porous superhydrophobic membranes show a great gas separation/adsorption ability. However, the complicated device architecture and the durability issue are normally concerned especially for the continuous circulation of gas and liquid. In this work, we present a free-standing gas-conductive circuit simply formed by connecting the superamphiphobic porous monoliths (SAPMs) to achieve an efficient under-liquid gas adsorption. The porous worm-like SAPM is prepared with low-temperature expandable graphite and polyvinylidenefluoride, exhibiting superamphiphobicity and superaerophilicity after fluoridation. The as-made SAPM circuits can be used as a reliable gas conductor under numerous liquids, such as water, alkaline, acidic, and oily solutions. In this work, the CO2 adsorption capacities of the SAPM circuits are evaluated under NaOH and methyldiethanolamine solutions and the mass transfer rate can reach up to 9.61 mmol m-2 s-1. Moreover, the effective human blood oxygenation process is also demonstrated using SAPM circuits. Thus, the reported SAPM provides an alternative gas-liquid exchanging method and the simplified process could be of great benefit to the cost-effectively large-scale CO2 capture or gas exchanging applications.