Continuous Light Illumination Research Articles

Aluminum Carboxylate Modification Enabled Efficient and Stable Perovskite-Polystyrene Thin Films for Light-Emitting Applications.

Lead halide perovskite nanocrystals (PNCs) have demonstrated great potential in emerging display technologies. However, the practical application of PNCs is hindered by the inherent instability of their ionic surface. Here, we proposed a surface modification approach to enhance the stability of CsPbBr3 PNCs by postsynthetic treatment with aluminum phenylbutyrate (Al(PA)3). Our study reveals that Al(PA)3 displaces ammonium ligands and binds tightly on surface halide, providing excellent air and moisture resistance while preserving a high quantum efficiency of 81.6%. The modified PNCs maintain a constant photoluminescence intensity under continuous UV light illumination for 500 h. Additionally, the Al(PA)3 ligand is compatible with styrene, enabling homogeneous dispersion of PNCs in polystyrene matrices to form bright and uniform PNC-PS thin films. We demonstrated the application of the composite films for display backlighting, which exhibits a wide color gamut of 125% NTSC. The result highlights the potential of AlPA-modified PNCs in light-emitting and other optoelectronic devices.

Transition‐Metal‐Doped TiO2 Nanorods with High‐Visible‐Light Response via a Simple Hydrothermal Method

Transition‐metal‐ion doping is an effective method to shorten bandgap and enhance visible‐light absorption of TiO2, but there are still some serious challenges for most doping technologies, such as nonuniform doping, severe lattice damages, metal atoms agglomeration, and inactivated impurities. Herein, a simple and universal hydrothermal method is developed to realize the effective transition‐metal ions doping of TiO2 (including Fe, Co, Mn, Cu, V, and Cr). The photoelectrochemical water splitting performances of Cr‐doped TiO2 nanorods with multifarious Cr ion valence states (Cr3+ or Cr6+ ions), various Cr‐ion concentrations, with or without oxygen vacancy activation are emphatically and systematically studied. Experiments and theoretical calculations demonstrate that the remarkably enhanced carrier separation and injection efficiencies are the key factors to improve the visible‐light photoactivity, benefiting from the homogeneous distribution of impurity atoms and the incorporation of oxygen vacancies. The Cr3+‐ion‐doped TiO2 nanorod arrays with oxygen vacancy activation (Cr3+/Ov–TiO2) displays an impressive incident photon‐to‐electron conversion efficiency of 5.4% at 450 nm visible light, far superior to the pure TiO2 of 0.03%. Furthermore, no obvious photocurrent decay is observed in the Cr3+/Ov–TiO2 photoanode after 12 h continuous light illumination.

Aluminium-doped Carbon Dots for the Simultaneous Selective Detection of Five Tetracycline Antibiotics.

In this paper, the aluminium-doped carbon dots (Al-CDs) were developed for simultaneous selective detection of five tetracycline antibiotics (TCs), including minocycline (MC), tetracycline (TC), oxytetracycline (OTC), doxycycline (DOC) and chlortetracycline (CTC). With the bright blue fluorescence, Al-CDs displayed excellent stability and showed no obvious fluorescence intensity changes under different ionic strength, acidic or alkaline environment, continuous ultraviolet light illumination, and even longtime storage at room temperature. As adding different antibiotics, the fluorescence of Al-CDs was strongly quenched by five TCs and showed no distinguished changes with the addition of other kinds of antibiotics. The presence of interferential metal ions, anions and small organic molecules imposed no effect on the simultaneous selective detection of five TCs. A good linear relationship was achieved for five TCs in the range of 0-100μM, and the limit of detection for MC, TC, OTC, DOC, and CTC were 13.91 (0-100μM), 15.54 (0-100μM), 14.26 (0-100μM), 13.48 (0-100μM) and 13.88nM (0-100μM), respectively. Moreover, Al-CDs was successfully used to the detection of five TCs in real samples with recovery ranging from 92.47% to 122.05%, confirming a bright future for the practical applications in the assays of foods, medicines, and environments.

Evaluation of Microalgae Chlorella vulgaris and Tetradesmus bernardii for Cultivation and Nutrient Removal in Palm Oil Mill Effluent

The palm oil industry is one of the key players in contributing to Malaysia’s economy. Palm oil mill effluent (POME), a significant by-product of the oil extraction process, requires mandatory remediation to ensure proper treatment and disposal. Bioremediation using microalgae is a cost-effective and sustainable approach. This study aims to utilise pure and mixed microalgal species, Chlorella vulgaris and Tetradesmus bernardii, in phycoremediation and biomass production in different concentrations of POME (20%, 40%, 60%, and 80%). Cultivation of microalgae was carried out in 200 mL medium with pH 7–7.8, room temperature of 25±1°C for 21 days and continuous light illumination at 2000 lux. The highest biomass productivity was observed in 20% POME for mixed microalgae (mean = 0.1733 mg.mL-1 ± 0.0057), followed by C. vulgaris (0.1633 mg.mL-1 ± 0.0057) and T. bernardii (0.1603 mg.mL-1 ± 0.0020). Similarly, the highest nutrient removal was observed in 20% POME for mixed microalgae (COD:66.9801%, TN:86.9565%, TP:86.9655%), followed by C. vulgaris and T. bernardii. The results showed positive effects on growth, increased biomass production, and nutrient removal, with 20% POME being the optimal concentration for microalgae. Valuable by-products, such as high-quality pigments and biomass, are also generated by applying microalgae for remediation. Mixed microalgae are superior in the remediation of POME compared to single-culture algae. Treating wastewater through microalgal bioremediation is highly efficient in nutrient removal. This research has contributed towards the use of mixed microalgae to achieve effective nutrient removal and biomass for future industrial applications.

“Light battery” role of long afterglow phosphor for round-the-clock environmental photocatalysis

Owing to its convenient, sustainable and green process, photocatalysis has become a feasible technique for solving environmental pollution issues. So far, significant achievements have been realized in photocatalytic pollutant elimination. Nevertheless, photocatalytic processes require a continuous external light illumination to drive photoredox reactions, seriously prohibiting their applications in darkness. In this context, exploring a photocatalyst with reliable photocatalytic activity in dark condition is therefore highly meaningful and an ultimate target of photocatalysis technique. Recently, long afterglow phosphor has aroused great attention due to its “light battery” role for driving catalytic reactions in dark conditions. To be specific, long-afterglow phosphor or long-afterglow phosphor/semiconductor composite can be used as a photocatalyst to simultaneously promote the photoredox processes and store extra photoexcited charges in the trapping states upon light irradiation. When the light illumination terminates, a gradual release of the charges from trapping states occurs in long-afterglow phosphor, which can continuously spur photoredox reactions under the dark environment and even maintains the photocatalysis around the clock. In this work, we comprehensively reviewed the recent advances of long afterglow phosphor based round-the-clock photocatalysts in environmental pollutant elimination. Meanwhile, the inherent mechanism of long afterglow photocatalysis was discussed in depth. More importantly, the relationship between the improved long afterglow photocatalytic capability and the engineering of long afterglow system is correlated systematically. Finally, the ongoing challenges and future prospects for the mass production and commercial utilization of round-the-clock photocatalysts are analyzed and outlooked.

Tailoring the Buried Interface by Dipolar Halogen-Substituted Arylamine for Efficient and Stable Perovskite Solar Cells.

Improving the quality of the buried interface is decisive for achieving stable and high-efficiency perovskite solar cells. Herein, we report the interface engineering by using dipolar 2,4-difluoro-3,5-dichloroaniline (DDE) as the adhesive between titanium dioxide (TiO2) and MAPbI3. By manipulation of the anchoring groups of DDE, this molecule not only passivated defects of TiO2 but also optimized the energy level alignment. Furthermore, the perovskite film on the modified TiO2 surface showed improved crystallinity, released residual stress, and reduced trap states. Therefore, these benefits directly contribute to achieving a power conversion efficiency of up to 22.10%. The unencapsulated device retained 90% of initial power conversion efficiencies (PCE) after continuous light illumination for 1000 h and 93% of initial PCE after exposure to air with a relative humidity of 30-40% for over 3000 h. Moreover, the performance of PSCs based on FA0.15MA0.85PbI3 has also increased from 20.48 to 23.51%. Our results demonstrate the effectiveness and universality of dipolar halogen-substituted arylamine (DDE) for enhancing PSC performance.

Growth of a Sub-Centimeter-Sized CsPbBr3 Bulk Single Crystal Using an Anti-Solvent Precipitation Method

A facile and low-cost strategy to fabricate CsPbBr3 single crystals is essential for developing perovskite optoelectronic devices. Herein, we have presented a room temperature anti-solvent precipitate method for growing sub-centimeter-sized CsPbBr3 single crystals. The as-prepared CsPbBr3 single crystal has an orthorhombic structure, and phase transition occurs as the measured temperature increases. The as-grown CsPbBr3 single crystal also shows abundant surface morphologies including footsteps, precipitated crystals, cracks, and pits. Subsequently, a metal–semiconductor–metal (MSM)-structured photodetector was fabricated based on the CsPbBr3 single crystal. Under 525 nm green light illumination, the photodetector exhibits an obvious response and the photocurrent linearly increases with the increase in the light intensity. The rise time of the photodetector increases from 0.82 s to 2.19 s as the light intensity is enhanced from 15 mW/cm2 to 160 mW/cm2, indicating that more time is required to reach to a stable photocurrent. However, the decay time is as fast as ~0.82 ms, irrelevant of the light intensity. The photocurrent, under continuous light illumination, was further studied and this indicates that a stronger light intensity can accelerate the attenuation of the device.

Facile Tailoring of Metal-Organic Frameworks for Förster Resonance Energy Transfer-Driven Enhancement in Perovskite Photovoltaics.

Förster resonance energy transfer (FRET) has demonstrated its potential to enhance the light energy utilization ratio of perovskite solar cells by interacting with metal-organic frameworks (MOFs) and perovskite layers. However, comprehensive investigations into how MOF design and synthesis impact FRET in perovskite systems are scarce. In this work, nanoscale HIAM-type Zr-MOF (HIAM-4023, HIAM-4024, and HIAM-4025) is meticulously tailored to evaluate FRET's existence and its influence on the perovskite photoactive layer. Through precise adjustments of amino groups and acceptor units in the organic linker, HIAM-MOFs are synthesized with the same topology, but distinct photoluminescence (PL) emission properties. Significant FRET is observed between HIAM-4023/HIAM-4024 and the perovskite, confirmed by spectral overlap, fluorescence lifetime decay, and calculated distances between HIAM-4023/HIAM-4024 and the perovskite. Conversely, the spectral overlap between the PL emission of HIAM-4025 and the perovskite's absorption spectrum is relatively minimal, impeding the energy transfer from HIAM-4025 to the perovskite. Therefore, the HIAM-4023/HIAM-4024-assisted perovskite devices exhibit enhanced EQE via FRET processes, whereas the HIAM-4025 demonstrates comparable EQE to the pristine. Ultimately, the HIAM-4023-assisted perovskite device achieves an enhanced power conversion efficiency (PCE) of 24.22% compared with pristine devices (PCE of 22.06%) and remarkable long-term stability under ambient conditions and continuous light illumination.

Anomalous spectral shift of localized surface plasmon resonance.

We report the first observation of spectral blue shift of plasmon resonance of synthesized silver nanoparticles (AgNPs) due to a negative optical nonlinearity of a local ambient medium, i.e., indigo carmine (IC) solution at around 420 nm wavelength. The blue shift occurred at a larger concentration of AgNPs or at a larger concentration of IC solution, being in obvious contrast to spectral red shift which was widely witnessed in plasmon spectral shift in a linear regime. Plasmon-enhanced local fields could excite the third-order optical nonlinearity for blue shift even under continuous (non-pulsed) light illumination. We also found that the plasmon-excited nonlinearity could allow for differential nonlinear response of the IC solution to be even greater than its differential linear response, though appearing to be somewhat inconsistent with what was generally known in light-matter interaction. The demonstrated properties of such anomalous shift of plasmon spectral peaks and its accompanying properties indicated that plasmon technologies could be exploited not only in linear but also in nonlinear aspects for critical optimization in plasmon-energy harvesting systems such as in surface enhanced spectroscopy/microscopy, biomedical imaging/sensing, laser frequency conversion, ultrashort pulse generation, and all-optical switching.

Buried-Interface Engineering Enables Efficient and 1960-HourISOS-L-2I Stable Inverted Perovskite Solar Cells.

High-performance perovskite solar cells (PSCs) typically require interfacial passivation, yet this is challenging for the buried interface, owing to the dissolution of passivation agents during the deposition of perovskites. Here, this limitation is overcome with in situ buried-interface passivation-achieved via directly adding a cyanoacrylic-acid-based molecular additive, namely BT-T, into the perovskite precursor solution. Classical and ab initio molecular dynamics simulations reveal that BT-T spontaneously may self-assemble at the buried interface during the formation of the perovskite layer on a nickel oxide hole-transporting layer. The preferential buried-interface passivation results in facilitated hole transfer and suppressed charge recombination. In addition, residual BT-T molecules in the perovskite layer enhance its stability and homogeneity. A power-conversion efficiency (PCE) of 23.48% for 1.0cm2 inverted-structure PSCs is reported. The encapsulated PSC retains 95.4% of its initial PCE following 1960h maximum-power-point tracking under continuous light illumination at 65°C (i.e., ISOS-L-2I protocol). The demonstration of operating-stable PSCs under accelerated ageing conditions represents a step closer to the commercialization of this emerging technology.

Light-induced micro-strain regulation and charge carrier dynamics of (FA0.83MA0.17)0.95Cs0.05Pb(I0.83Br0.17)3 hybrid perovskite films

Light-induced strategies are crucial for deciding the physical and chemical properties of organometal halide perovskite materials and their photovoltaic devices. Herein, the triple cation ((FA0.83MA0.17)0.95Cs0.05Pb(I0.83Br0.17)3) hybrid perovskite films have been fabricated using a simple solution-processed method. These films were illuminated by blue light (417 nm) for different time durations and characterized for structural, surface morphological, optical, and charge carrier dynamics. Under illumination conditions, a reduction in lattice micro-strain has been observed. The enhanced optical absorbance and reduced non-radiative recombination have also been monitored in light-illuminated perovskite films. Further, time-resolved photoluminescence (TRPL) and ultra-fast transient absorption spectroscopy (TAS) measurements have been performed to study the charge carrier dynamics. TRPL results show that the average lifetime of charge carriers has increased from 3 ns to 19 ns upon continuous light illumination conditions. Further, the recombination time of the charge carriers decreased from 226 ps to 66 ps upon continuous light illumination for 30 min. This study suggests that light-induced experiments on perovskite films can be utilized for micro-strain regulation and modulation of their charge carrier dynamics for future perovskite solar cell applications.

Thiol-Functionalized Conjugated Metal-Organic Frameworks for Stable and Efficient Perovskite Photovoltaics.

Metal-organic frameworks (MOFs) have been investigated recently in perovskite photovoltaics owing to their potential to boost optoelectronic performance and device stability. However, the impact of variations in the MOF side chain on perovskite characteristics and the mechanism of MOF/perovskite film formation remains unclear. In this study, three nanoscale thiol-functionalized UiO-66-type Zr-based MOFs (UiO-66-(SH)2 , UiO-66-MSA, and UiO-66-DMSA) are systematically employed and examined in perovskite solar cells (PSCs). Among these MOFs, UiO-66-(SH)2 , with its rigid organic ligands, exhibited a strong interaction with perovskite materials with more efficient suppression of perovskite vacancy defects. More importantly, A detailed and in-depth discussion is provided on the formation mechanism of UiO-66-(SH)2 -assisted perovskite film upon in situ GIWAXS performed during the annealing process. The incorporation of UiO-66-(SH)2 additives substantially facilitates the conversion of PbI2 into the perovskite phase, prolongs the duration of stage I, and induces a delayed phase transformation pathway. Consequently, the UiO-66-(SH)2 -assisted device demonstrates reduced defect density and superior optoelectronic properties with optimized power conversion efficiency of 24.09% and enhanced long-term stability under ambient environment and continuous light illumination conditions. This study acts as a helpful design guide for desired MOF/perovskite structures, enabling further advancements in MOF/perovskite optoelectronic devices.

Fine-tuned photochromic sulfonylureas for optical control of beta cell Ca2+ fluxes.

We previously developed, synthesized and tested light-activated sulfonylureas for optical control of KATP channels and pancreatic beta cell activity in vitro and in vivo. Such technology relies on installation of azobenzene photoswitches onto the sulfonylurea backbone, affording light-dependent isomerization, alteration in ligand affinity for SUR1 and hence KATP channel conductance. Inspired by molecular dynamics simulations and to further improve photoswitching characteristics, we set out to develop a novel push-pull closed ring azobenzene unit, before installing this on the sulfonylurea glimepiride as a small molecule recipient. Three fine-tuned, light-activated sulfonylureas were synthesized, encompassing azetidine, pyrrolidine and piperidine closed rings. Azetidine-, pyrrolidine- and piperidine-based sulfonylureas all increased beta cell Ca2+ -spiking activity upon continuous blue light illumination, similarly to first generation JB253. Notably, the pyrrolidine-based sulfonylurea showed superior switch OFF performance to JB253. As such, third generation sulfonylureas afford more precise optical control over primary pancreatic beta cells, and showcase the potential of pyrrolidine-azobenzenes as chemical photoswitches across drug classes.

Enhancing the Photoelectrochemical Performance of a Nanoporous Silicon Photocathode through Electroless Nickel Deposition.

Renewable energy sources, particularly solar energy, are key to our efforts to decarbonize. This study investigates the photoelectrochemical (PEC) behavior of nanoporous silicon (NPSi) and its Ni-coated hybrid system. The methods involve the application of a Ni coating to NPSi, a process aimed at augmenting catalytic activity, light absorption, and carrier transport. Scanning electron microscopy was used to analyze the morphological changes on NPSi surfaces due to the Ni coating. Results demonstrate that the Ni coating creates unique structures on NPSi surfaces, with peak PEC performance observed at 15 min of coating time and 60 °C. These conditions were found to promote electron-hole pair separation and uniform Ni coverage. A continuous 50-min white light illumination experiment confirmed stable PEC fluctuations, showing the interplay of NPSi's characteristics and Ni's catalytic effect. This study provides practical guidance for the design of efficient water-splitting catalysts, contributing to the broader field of renewable energy conversion.

Trivalent Europium Doped CsCl Quantum Dots for MA-free Perovskite Solar Cells with Inherent Bandgap through Lattice Strain Compensation.

Cesium-formamidinium (Cs-FA) perovskites have garnered widespread interest owing to their excellent thermal- and photostability in achieving stable formamidinium lead iodide (FAPbI3 ) perovskite solar cells (PSCs). However, Cs-FA perovskite typically suffers from Cs+ and FA+ mismatches, affecting the Cs-FA morphology and lattice distortion, resulting in an enlarged bandgap (Eg). To address these issues, we developed "upgraded" CsCl-Eu3+ -doped CsCl quantum dots (QDs) for FAPbI3 PSCs to solve the key issues in Cs-FA PSCs and also exploit the advantage of Cs-FA PSCs on stability. The introduction of Eu3+ promoted the formation of high-quality Cs-FA films by adjusting the Pb-I cluster structure. CsCl:Eu3+ also offsets the local strain and lattice contraction induced by Cs+ , which maintains the inherent Eg of FAPbI3 and decreases the trap density. Finally, we obtained a power conversion efficiency (PCE) of 24.13% with an excellent short-circuit current density (Jsc ) of 26.10mA/cm2 , which are among the highest in methylammonium (MA)-free PSCs. The unencapsulated devices showed excellent humidity and storage stability owing to the relieved lattice strain and ligand protection. We achieved an initial PCE of 92.2% within 500h under continuous light illumination of 1.5 G and bias voltage conditions, demonstrating excellent operational stability. This study provides a universal strategy to address the inherent issues of Cs-FA devices and maintain the stability of MA-free PSCs to satisfy future commercial criteria. This article is protected by copyright. All rights reserved.

Synergetic Effect of Aluminum Oxide and Organic Halide Salts on Two‐Dimensional Perovskite Layer Formation and Stability Enhancement of Perovskite Solar Cells

AbstractLong‐chain organic halide salts are widely used in perovskite‐based optoelectronic devices for surface passivation owing to their capability to interact with the surface defects of perovskites. Here, aluminum oxide (AlOx) is introduced via atomic layer deposition onto octylammonium iodide (OAI) to exploit the benefits of organic halide salts without generating undesired defects. The devices incorporating AlOx on OAI‐treated perovskite (OAI/AlOx) show enhancement in both device performance and photo‐stability compared to those with only treatment. A diffusion of aluminum from AlOx into the perovskite through surface characterization contributes to a uniform photo‐generated carrier transport in both the surface and the bulk of the perovskite absorber. In addition, it is revealed that light‐induced two‐dimensional perovskite formation on OAI/AlOx. This may be ascribed to preventing the loss of OA cations due to the presence of AlOx, leading to a decrease in the number of iodine anions which suppresses the light‐induced degradation of corresponding devices. Consequently, the devices show over 24% efficiency and retain their efficiency over 1000 hours under continuous light illumination.

Quantum dots decorated photoanodes in bioelectrochemical fuel cells: Enhanced electricity generation using green algae.

The power performance of the bio-electrochemical fuel cells (BEFCs) depends mainly on the energy harvesting ability of the anode material. The anode materials with low bandgap energy and high electrochemical stability are highly desirable in the BEFCs. To address this issue, a novel anode is designed using indium tin oxide (ITO) modified by chromium oxide quantum dots (CQDs). The CQDs were synthesized using facile and advanced pulsed laser ablation in liquid (PLAL) technique. The combination of ITO and CQDs improved the optical properties of the photoanode by exhibiting a broad range of absorption in the visible to UV region. A systematic study has been performed to optimize the amount of CQDs and green Algae (Alg) film grown using the drop casting method. Chlorophyll (a, b, and total) content of algal cultures (with different concentrations) were optimized to investigate the power generation performance of each cell. The BEFC cell (ITO/Alg10/Cr3//Carbon) with optimized amounts of Alg and CQDs demonstrated enhanced photocurrent generation of 120 mA cm-2 at a photo-generated potential of 24.6 V m-2 . The same device exhibited a maximum power density of 7 W m-2 under continuous light illumination. The device also maintained 98% of its initial performance after 30 repeated cycles of light on-off measurements.

On-Chip Light-Incorporated In Situ Transmission Electron Microscopy of Metal Halide Perovskite Materials

We report an on-chip light-incorporated in situ transmission electron microscopy (LI2ST) approach for probing metal halide perovskites (MHPs) at the nanoscale, realizing the real-time, site-specific tracking of the light-triggered structure transformation. This in situ platform is based on a specifically designed microelectromechanical systems (MEMS) chip that offers the capability of light illumination with adjustable intensity and tailorable multiwavelength. The excellent operational reliability of the platform allows for the continuous observation of nanoscale regions of interest, recording the morphological and structural evolutions of perovskite grains and grain boundaries. A proof-of-concept demonstration shows a polycrystalline MHP film undergoing decomposition upon continuous light illumination. Counterintuitively, the decomposition starts and expands within the intragrain regions rather than at the grain boundaries. This work demonstrates an unprecedented ability to reveal light-triggered structural-phase variation for illuminating the dynamic behaviors of MHPs with implications for various energy applications.

Ultralong Carrier Lifetime Exceeding 20 µs in Lead Halide Perovskite Film Enable Efficient Solar Cells.

The carrier lifetime is one of the key parameters for perovskite solar cells (PSCs). However, it is still a great challenge to achieve long carrier lifetimes in perovskite films that are comparable with perovskite crystals owning to the large trap density resulting from the unavoidable defects in grain boundaries and surfaces. Here, by regulating the electronic structure with the developed 2-thiopheneformamidinium bromide (ThFABr) combined with the unique film structure of 2D perovskite layer caped 2D/3D polycrystalline perovskite film, an ultralong carrier lifetime exceeding 20 µs and carrier diffusion lengths longer than 6.5µm are achieved. These excellent properties enable the ThFA-based devices to yield a champion efficiency of 24.69% with a minimum VOC loss of 0.33V. The unencapsulated device retains ≈95% of its initial efficiency after 1180h by max power point (MPP) tracking under continuous light illumination. This work provides important implications for structured 2D/(2D/3D) perovskite films combined with unique FA-based spacers to achieve ultralong carrier lifetime for high-performance PSCs and other optoelectronic applications.

Rationally Designed Eco-Friendly Solvent System for High-Performance, Large-Area Perovskite Solar Cells and Modules.

The important but remained issue to be addressed to achieve the mass production of perovskite solar modules include a large-area fabrication of high-quality perovskite film with eco-friendly, viable production methods. Although several efforts are made to achieve large-area fabrication of perovskite, the development of eco-friendly solvent system, which is precisely designed to be fit to scale-up methods are still challenging. Herein, this work develops the eco-friendly solvent/co-solvent system to produce a high-quality perovskite layer with a bathing in eco-friendly antisolvent. The new co-solvent/additive, methylsulfonylmethane (MSM), efficiently improves the overall solubility and has a suitable binding strength to the perovskite precursor, resulting in a high-quality perovskite film with antisolvent bathing method in large area. The resultant perovskite solar cells showed high power conversion efficiency of over 24% (in reverse scan), with a good long-term stability under continuous light illumination or damp-heat condition. MSM is also beneficial to produce a perovskite layer at low-temperature or high-humidity. MSM-based solvent system is finally applied to large-area, resulting in highly efficiency perovskite solar modules with PCE of 19.9% (by aperture) or 21.2% (by active area) in reverse scan. These findings contribute to step forward to a mass production of perovskite solar modules with eco-friendly way.