Light-driven, bias-free nitrogenase-based bioelectrochemical cell for ammonia generation.

Nitrogen fixation is a key process that sustains life on Earth. Nitrogenase is the sole enzyme capable of fixing nitrogen under ambient conditions. Extensive research efforts have been dedicated to elucidating the enzyme mechanism and its artificial activation through high applied voltage, photochemistry, or strong reducing agents. Harnessing light irradiation to minimize the required external bias can lower the process's high energy investment. Herein, we present the development of photo-bioelectrochemical cells (PBECs) utilizing BiVO4/CoP or CdS/NiO photoanodes for nitrogenase activation toward N2 fixation. The constructed PBEC based on BiVO4/CoP photoanode requires minimal external bias (200 mV) and suppresses O2 generation that allows efficient activation of the nitrogenase enzyme, using glucose as an electron donor. In a second developed PBEC configuration, CdS/NiO photoanode was used, enabling bias-free activation of the nitrogenase-based cathode to produce 100 µM of ammonia at a faradaic efficiency (FE) of 12%. The ammonia production was determined by a commonly used fluorescence probe and further validated using 1H-NMR spectroscopy. The presented PBECs lay the foundation for biotic-abiotic systems to directly activate enzymes toward value-added chemicals by light-driven reactions.

Progress in electrochemically empowered C-O bond formation: Unveiling the pathway of efficient green synthesis.

(C-X) bonds (X= C, N, O) are the main backbone for making different skeleton in the organic synthetic transformations. Among all the sustainable techniques, electro-organic synthesis for    C-X bond formation is the advanced tool as it offers a greener and more cost-effective approach to chemical reactions by utilizing electrons as reagents.  In this review, we want to explore the recent advancements in electrochemical C-O bond formation. The electrochemically driven C-O bond formation represents an emerging and exciting area of research.  In this context, electrochemical techniques offers numerous advantages, including higher yields, cost-efficient production, and simplified work-up procedures. This method enables the continuous and consistent formation of C-O bonds in molecules, significantly enhancing overall reaction yields. Furthermore, both intramolecular and intermolecular C-O bond forming reaction provided valuable products of O-containing acyclic/cyclic analogue. Hence, carbonyl (C=O), ether (-O-), and ester (-COOR) functionalization in both cyclic/acyclic analogues have been prepared continuously via this innovative pathway. In this context, we want to discuss one-decade electrochemical synthetic pathways of various C-O bond contains functional group in chronological manner. This review focused on all the synthetic aspects including mechanistic path and has also mentioned overall critical finding regarding the C-O bond formation via electrochemical pathways.

Suppression of Resistive Coupling in Nanogap Electrochemical Cell: Resolution of Dual Pathways for Dopamine Oxidation.

A nanogap cell involves two working electrodes separated by a nanometer-wide solution to enable unprecedented electrochemical measurements. The powerful nanogap measurements, however, can be seriously interfered with by resistive coupling between the two electrodes to yield erroneous current responses. Herein, we employ the nanogap cell based on double carbon-fiber microelectrodes to suppress resistive coupling for the assessment of intrinsic current responses. Specifically, we modify a commercial bipotentiostat to compensate the Ohmic potential drop shared by the two electrodes through the common current pathway with a fixed resistance in the solution. Resistive coupling through both non-Faradaic and Faradaic processes is suppressed to eliminate erroneous current responses. Our approach is applied to investigate the mechanism of dopamine oxidation at carbon-fiber microelectrodes as important electrochemical sensors for the crucial neurotransmitter. Resistive coupling is suppressed to manifest the intrinsic current responses based on the oxidation of both adsorbed and non-adsorbed forms of dopamine to the respective forms of dopamine-o-quinone. The simultaneous dual oxidation pathways are observed for the first time and can be mediated through either non-concerted or concerted mechanisms of adsorption-coupled electron transfer. The two mechanisms are not discriminated for the two-electron oxidation of dopamine because it can not be determined whether the intermediate, dopamine semi-quinone, is adsorbed on the electrode surface. Significantly, our approach will be useful to manifest intrinsic current responses without resistive coupling for nanogaps and microgaps, which are too narrow to eliminate the common solution resistance by optimizing the position of a reference electrode.

Biosynthesis of silver nanoparticles by banana pulp extract: Characterizations, antibacterial activity, and bioelectricity generation.

Here, green banana pulp extract (PE) has been used as a bio-reducing agent for the reduction of silver ions to silver nanoparticles (AgNPs). Bio-synthesized AgNPs were characterized by using UV, XRD, FEEM, TEM, and FTIR analysis. The face-centered cubic structures of AgNPs were formed with an average crystallite size of 31.26 nm and an average particle size of 42.97 nm. In this report, the electrical activities of green synthesized AgNPs have been evaluated along with the antibacterial activities. The antibacterial activities of AgNPs were evaluated against two pathogenic bacteria: Escherichia coli (gram-negative) and Staphylococcus epidermidis (gram-positive). AgNPs were added to the electrochemical cell and results demonstrated the improvement of power of the electrochemical cell. Green synthesized AgNPs showed excellent antibacterial activities against both gram-positive and negative bacteria and most importantly the NPs played an important role as an effective catalyst to enhance the electrical performance of bio-electrochemical cells. These significant findings may help in the advancement of nanotechnology in biomedical applications as well as in the creation of cheap and eco-friendly power generation devices.

Efficiency Roll-Off in Light-Emitting Electrochemical Cells.

Understanding "efficiency roll-off" (i.e., the drop in emission efficiency with increasing current) is critical if efficient and bright emissive technologies are to be rationally designed. Emerging light-emitting electrochemical cells (LECs) can be cost- and energy-efficiently fabricated by ambient-air printing by virtue of the in situ formation of a p-n junction doping structure. However, this in situ doping transformation renders a meaningful efficiency analysis challenging. Herein, a method for separation and quantification of major LEC loss factors, notably the outcoupling efficiency and exciton quenching, is presented. Specifically, the position of the emissive p-n junction in common singlet-exciton emitting LECs is measured to shift markedly with increasing current, and the influence of this shift on the outcoupling efficiency is quantified. It is further verified that the LEC-characteristic high electrochemical-doping concentration renders singlet-polaron quenching (SPQ) significant already at low drive current density, but also that SPQ increases super-linearly with increasing current, because of increasing polaron density in the p-n junction region. This results in that SPQ dominates singlet-singlet quenching for relevant current densities, and significantly contributes to the efficiency roll-off. This method for deciphering the LEC efficiency roll-off can contribute to a rational realization of all-printed LEC devices that are efficient at highluminance.

Recent advances in electrochemical cell-based biosensors for food analysis: Strategies for sensor construction.

Owing to their advantages such as great specificity, sensitivity, rapidity, and possibility of noninvasive and real-time monitoring, electrochemical cell-based biosensors (ECBBs) have been a powerful tool for food analysis encompassing the areas of nutrition, flavor, and safety. Notably, the distinctive biological relevance of ECBBs enables them to mimic physiological environments and reflect cellular behaviors, leading to valuable insights into the biological function of target components in food. Compared with previous reviews, this review fills the current gap in the narrative of ECBB construction strategies. The review commences by providing an overview of the materials and configuration of ECBBs, including cell types, cell immobilization strategies, electrode modification materials, and electrochemical sensing types. Subsequently, a detailed discussion is presented on the fabrication strategies of ECBBs in food analysis applications, which are categorized based on distinct signal sources. Lastly, we summarize the merits, drawbacks, and application scope of these diverse strategies, and discuss the current challenges and future perspectives of ECBBs. Consequently, this review provides guidance for the design of ECBBs with specific functions and promotes the application of ECBBs in food analysis.

Catalytic valorization of Kraft lignin into feedstock chemicals with methyltrioxorhenium (MTO) catalyst in microbial electrochemical cell.

In this study, the authors investigate a novel approach to valorize Kraft lignin using the catalyst Methyltrioxorhenium (MTO) in tandem with in-situ produced H2O2 in a Microbial Electrochemical Cell (MEC). This study demonstrates the in-situ oxidation of Kraft lignin using different concentrations of MTO catalyst (2 mM to 8 mM) and H2O2 (5.24 ± 0.40 mM to 8.91 ± 0.70 mM) in three MECs. The depolymerized Kraft lignin samples were characterized using FTIR, CHNS/O, and 1H NMR analysis. The MTO/H2O2 combination showed high selectivity towards the oxidation of Kraft lignin, resulting in both aromatic ring and side chain cleavage reactions and the production of valuable feedstock chemicals. The oxidation also led to a reduction of 68.42 % to 78.18 % in Chemical Oxygen Demand (COD) of lignin. The selective oxidation favored the recovery of Guaiacyl (G) unit-derived feedstock chemicals, with Guaiacol being the most abundant compound (45.04 mg/mL) among the quantified products by HPLC. Additionally, the system demonstrated high efficiency in anodic wastewater treatment, achieving BOD and COD removal rates ranging from 67.68 % to 72.55 %. This method showcases the use of a sustainable system in combination with a selective catalyst to produce valuable products from usually discarded Kraft lignin while simultaneously treating wastewater.

Long-Range SECCM Enables High-Throughput Electrochemical Screening of High Entropy Alloy Electrocatalysts at Up-To-Industrial Current Densities.

High-entropy alloys (HEAs), especially in the form of compositional complex solid solutions (CCSS), have gained attention in the field of electrocatalysis. However, exploring their vast composition space concerning their electrocatalytic properties imposes significant challenges. Scanning electrochemical cell microscopy (SECCM) offers high-speed electrochemical analysis on surface areas with a lateral resolution down to tens of nm. However, high-precision piezo positioners often used for the motion of the tip limit the area of SECCM scans to the motion range of the piezo positioners which is typically a few tens of microns. To bridge this experimental gap, the study proposes a long-range SECCM system with a rapid gas-exchange environmental cell for high-throughput electrochemical characterization of 100 mm diameter HEA thin-film material libraries (ML) obtained by combinatorial co-sputtering. Due to the gas-liquid interface at the positioned SECCM droplet on the sample, high-throughput evaluation under industrial current density conditions becomes feasible. This allows the direct correlation between electrocatalytic activity and material composition with high statistical reliability. The multidimensional data obtained accelerates materials discovery, development, and optimization.

Green synthesis of silver nanoparticles by using Allium sativum extract and evaluation of their electrical activities in bio-electrochemical cell.

An electrical application of green synthesized silver nanoparticles (Ag NPs) by developing a unique bio-electrochemical cell (BEC) has been addressed in the report. Here, garlic extract (GE) has been used as a reducing agent to synthesize Ag NPs, and as a bio-electrolyte solution of BEC. Ag NPs successfully formed into face-centered cubic structures with average crystallite and particle sizes of 8.49 nm and 20.85 nm, respectively, according to characterization techniques such as the UV-vis spectrophotometer, XRD, FTIR, and FESEM. A broad absorption peak at 410 nm in the UV-visible spectra indicated that GE played a vital role as a reducing agent in the transformation of Ag+ions to Ag NPs. After that four types of BEC were developed by varying the concentration of GE, CuSO4. 5H2O, and Ag NPs electrolyte solution. The open circuit voltage and short circuit current of all cells were examined with the time duration. Moreover, different external loads (1 Ω, 2 Ω, 5 Ω, and 6 Ω) were used to investigate the load voltage and load current of BEC. The results demonstrated that the use of Ag NPs on BEC played a significant role in increasing the electrical performance of BEC. The use of GE-mediated Ag NPs integrated the power, capacity, voltage efficiency, and energy efficiency of BEC by decreasing the internal resistance and voltage regulation. These noteworthy results can take a frontier forward to the development of nanotechnology for renewable and low-cost power production applications.

Precision Synthesis of Bimetallic Nanoparticles via Nanofluidics in Nanopipets.

Bimetallic nanoparticles often show properties superior to their single-component counterparts. However, the large parameter space, including size, structure, composition, and spatial arrangement, impedes the discovery of the best nanoparticles for a given application. High-throughput methods that can control the composition and spatial arrangement of the nanoparticles are desirable for accelerated materials discovery. Herein, we report a methodology for synthesizing bimetallic alloy nanoparticle arrays with precise control over their composition and spatial arrangement. A dual-channel nanopipet is used, and nanofluidic control in the nanopipet further enables precise tuning of the electrodeposition rate of each element, which determines the final composition of the nanoparticle. The composition control is validated by finite element simulation as well as electrochemical and elemental analyses. The scope of the particles demonstrated includes Cu-Ag, Cu-Pt, Au-Pt, Cu-Pb, and Co-Ni. We further demonstrate surface patterning using Cu-Ag alloys with precise control of the location and composition of each pixel. Additionally, combining the nanoparticle alloy synthesis method with scanning electrochemical cell microscopy (SECCM) allows for fast screening of electrocatalysts. The method is generally applicable for synthesizing metal nanoparticles that can be electrodeposited, which is important toward developing automated synthesis and screening systems for accelerated material discovery in electrocatalysis.

Multiscale Analysis of Electrocatalytic Particle Activities: Linking Nanoscale Measurements and Ensemble Behavior.

Nanostructured electrocatalysts exhibit variations in electrochemical properties across different length scales, and the intrinsic catalytic characteristics measured at the nanoscale often differ from those at the macro-level due to complexity in electrode structure and/or composition. This aspect of electrocatalysis is addressed herein, where the oxygen evolution reaction (OER) activity of ß-Co(OH)2 platelet particles of well-defined structure is investigated in alkaline media using multiscale scanning electrochemical cell microscopy (SECCM). Microscale SECCM probes of ∼50 µm diameter provide voltammograms from small particle ensembles (ca. 40-250 particles) and reveal increasing dispersion in the OER rates for samples of the same size as the particle population within the sample decreases. This suggests the underlying significance of heterogeneous activity at the single-particle level that is confirmed through single-particle measurements with SECCM probes of ∼5 µm diameter. These measurements of multiple individual particles directly reveal significant variability in the OER activity at the single-particle level that do not simply correlate with the particle size, basal plane roughness, or exposed edge plane area. In combination, these measurements demarcate a transition from an "individual particle" to an "ensemble average" response at a population size of ca. 130 particles, above which the OER current density closely reflects that measured in bulk at conventional macroscopic particle-modified electrodes. Nanoscale SECCM probes (ca. 120 and 440 nm in diameter) enable measurements at the subparticle level, revealing that there is selective OER activity at the edges of particles and highlighting the importance of the three-phase boundary where the catalyst, electrolyte, and supporting carbon electrode meet, for efficient electrocatalysis. Furthermore, subparticle measurements unveil heterogeneity in the OER activity among particles that appear superficially similar, attributable to differences in defect density within the individual particles, as well as to variations in electrical and physical contact with the support material. Overall this study provides a roadmap for the multiscale analysis of nanostructured electrocatalysts, directly demonstrating the importance of multilength scale factors, including particle structure, particle-support interaction, presence of defects, etc., in governing the electrochemical activities of ß-Co(OH)2 platelet particles and ultimately guiding the rational design and optimization of these materials for alkaline water electrolysis.

Investigating the effects of solution viscosity on the stability and success rate of SECCM imaging.

Due to the capability of simultaneously detecting the morphology and electrochemical information of samples and limiting the electrochemical reaction to a range approximately the size of the inner diameter of the pipette tip opening, scanning electrochemical cell microscopy (SECCM) enables higher precision local electrochemical measurement and surface material delivery and has been demonstrating unique advantages and broad application prospects. However, the meniscus droplet at the pipette tip of SECCM is equivalent to the opening radius of the pipette tip, which is usually tens of nanometers to hundreds of nanometers. The tiny meniscus droplet makes it susceptible to evaporation and crystallization, which increases the likelihood of the pipette colliding with the sample during the scanning process, resulting in the failure of scanning. In this paper, the influence of solution viscosity on the shape variation of the droplet at the tip during the movement of the pipette of SECCM was studied by finite element analysis. It is proved that the increase of solution viscosity is helpful in reducing the shape variation of the droplet at the tip during the movement of the pipette. Then scanning experiments were carried out using a flat Au substrate and Au substrates with rounded triangle and rounded rectangular convex structures as the samples. According to the experimental results, increasing solution viscosity improves scanning success rates and scanning quality and effectively lowers the MSE of the scanning results. The experimental results also show that SECCM can image at a higher speed when the solution's viscosity increases since the deformation of the droplet at the tip is less than with a typical solution.

Microscale Electrochemical Corrosion of Uranium Oxide Particles.

Understanding the corrosion of spent nuclear fuel is important for the development of long-term storage solutions. However, the risk of radiation contamination presents challenges for experimental analysis. Adapted from the system for analysis at the liquid-vacuum interface (SALVI), we developed a miniaturized uranium oxide (UO2)-attached working electrode (WE) to reduce contamination risk. To protect UO2 particles in a miniatured electrochemical cell, a thin layer of Nafion was formed on the surface. Atomic force microscopy (AFM) shows a dense layer of UO2 particles and indicates their participation in electrochemical reactions. Particles remain intact on the electrode surface with slight redistribution. X-ray photoelectron spectroscopy (XPS) reveals a difference in the distribution of U(IV), U(V), and U(VI) between pristine and corroded UO2 electrodes. The presence of U(V)/U(VI) on the corroded electrode surface demonstrates that electrochemically driven UO2 oxidation can be studied using these cells. Our observations of U(V) in the micro-electrode due to the selective semi-permeability of Nafion suggest that interfacial water plays a key role, potentially simulating a water-lean scenario in fuel storage conditions. This novel approach offers analytical reproducibility, design flexibility, a small footprint, and a low irradiation dose, while separating the α-effect. This approach provides a valuable microscale electrochemical platform for spent fuel corrosion studies with minimal radiological materials and the potential for diverse configurations.

Root Cause Analysis of Degradation in Protonic Ceramic Electrochemical Cell with Interfacial Electrical Sensors Using Data-Driven Machine Learning.

Protonic ceramic electrochemical cells (PCECs) offer promising paths for energy storage and conversion. Despite considerable achievements made, PCECs still face challenges such as physiochemical compatibility between componenets and suboptimal solid-solid contact at the interfaces between the electrolytes and electrodes. In this study, a novel approach is proposed that combines in situ electrochemical characterization of interfacial electrical sensor embedded PCECs and machine learning to quantify the contributions of different cell components to total degradation, as well as to predict the remaining useful life. The experimental results suggest that the overpotential induced by the oxygen electrode is 48% less than that of oxygen electrode/electrolyte interfacial contact for up to 1171 h. The data-driven machine learning simulation predicts the RUL of up to 2132 h. The root cause of degradation is overpotential increase induced by oxygen electrode, which accounts for 82.9% of total cell degradation. The success of the failure diagnostic model is demonstrated by its consistency with degradation modes that do not manifest in electrolysis fade during early real operations. This synergistic approach provides valuable insights into practical failure diagnosis of PCECs and has the potential to revolutionize their development by enabling improved performance prediction and material selection for enhanced durability and efficiency.

Development of a versatile electrochemical cell for in situ grazing-incidence X-ray diffraction during non-aqueous electrochemical nitrogen reduction.

In situ techniques are essential to understanding the behavior of electrocatalysts under operating conditions. When employed, in situ synchrotron grazing-incidence X-ray diffraction (GI-XRD) can provide time-resolved structural information of materials formed at the electrode surface. In situ cells, however, often require epoxy resins to secure electrodes, do not enable electrolyte flow, or exhibit limited chemical compatibility, hindering the study of non-aqueous electrochemical systems. Here, a versatile electrochemical cell for air-free in situ synchrotron GI-XRD during non-aqueous Li-mediated electrochemical N2 reduction (Li-N2R) has been designed. This cell not only fulfills the stringent material requirements necessary to study this system but is also readily extendable to other electrochemical systems. Under conditions relevant to non-aqueous Li-N2R, the formation of Li metal, LiOH and Li2O as well as a peak consistent with the α-phase of Li3N was observed, thus demonstrating the functionality of this cell toward developing a mechanistic understanding of complicated electrochemical systems.

Probing charge transfer through antifouling polymer brushes by electrochemical methods: The impact of supporting self-assembled monolayer chain length.

Ultrathin surface-tethered polymer brushes represent attractive platforms for a wide range of sensing applications in strategically vital areas such as medicine, forensics, or security. The recent trends in such developments towards "real world conditions" highlighted the role of zwitterionic poly(carboxybetaine) (pCB) brushes which provide excellent antifouling properties combined with bio-functionalization capacity. Highly dense pCB brushes are usually prepared by the "grafting from" polymerization triggered by initiators on self-assembled monolayers (SAMs). Here, multi-methodological experimental studies are pursued to elucidate the impact of the alkanethiolate SAM chain length (C6, C8 and C11) on structural and functional properties of antifouling poly(carboxybetaine methacrylamide) (pCBMAA) brush. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) in a custom-made 3D printed cell employing [Ru(NH3)6]3+/2+ redox probe were used to investigate penetrability of SAM/pCBMAA bilayers for small molecules and interfacial charge transfer characteristics. The biofouling resistance of pCBMAA brushes was characterized by surface plasmon resonance; ellipsometry and FT-IRRAS spectroscopy were used to determine swelling and relative density of the brushes synthesized from initiator-bearing SAMs with varied carbon chain length. The SAM length was found to have a substantial impact on all studied characteristics; the highest value of charge transfer resistance (Rct) was observed for denser pCBMAA on longer-chain (C11) SAM when compared to shorter (C8/C6) SAMs. The observed high value of Rct for C11 implies a limitation for the analytical performance of electrochemical sensing methods. At the same time, the pCBMAA brushes on C11 SAM exhibited the best bio-fouling resistance among inspected systems. This demonstrates that proper selection of supporting structures for brushes is critical in the design of these assemblies for biosensing applications.

Acidic Hydrogen Evolution Electrocatalysis at High-Entropy Alloys Correlates with its Composition-Dependent Potential of Zero Charge.

The vast possibilities in the elemental combinations of high-entropy alloys (HEAs) make it essential to discover activity descriptors for establishing rational electrocatalyst design principles. Despite the increasing attention on the potential of zero charge (PZC) of hydrogen evolution reaction (HER) electrocatalyst, neither the PZC of HEAs nor the impact of the PZC on the HER activity at HEAs has been described. Here, we use scanning electrochemical cell microscopy (SECCM) to determine the PZC and the HER activities of various elemental compositions of a Pt-Pd-Ru-Ir-Ag thin-film HEA materials library (HEA-ML) with high statistical reliability. Interestingly, the PZC of Pt-Pd-Ru-Ir-Ag is linearly correlated with its composition-weighted average work function. The HER current density in acidic media positively correlates with the PZC, which can be explained by the preconcentration of H+ in the electrical double layer at potentials negative of the PZC.

Tracking drugged waters from various sources to drinking water-its persistence, environmental risk assessment, and removal techniques.

Pharmaceuticals have become a major concern due to their nature of persistence and accumulation in the environment. Very few studies have been performed relating to its toxicity and ill effects on the aquatic/terrestrial flora and fauna. The typical wastewater and water treatment processes are not efficient enough to get these persistent pollutants treated, and there are hardly any guidelines followed. Most of them do not get fully metabolized and end up in rivers through human excreta and household discharge. Various methods have been adopted with the advancement in technology, sustainable methods are more in demand as they are usually cost-effective, and hardly any toxic by-products are produced. This paper aims to illustrate the concerns related to pharmaceutical contaminants in water, commonly found drugs in the various rivers and their existing guidelines, ill effects of highly detected pharmaceuticals on aquatic flora and fauna, and its removal and remediation techniques putting more emphasis on sustainable processes.

1T/1H-SnS2 Sheets for Electrochemical CO2 Reduction to Formate.

Understanding the catalytic mechanism of highly active two-dimensional electrocatalysts is crucial to their rational design. Herein, we reveal the element dependence of the reactivity of two-dimensional metal dichalcogenide sheets for electrocatalytic CO2 reduction. We found that tin(IV) disulfide (SnS2) and molybdenum(IV) disulfide (MoS2) sheets exhibited Faradaic efficiencies of 63.3% and ∼0%, respectively, for formic acid. Scanning electrochemical cell microscopy and theoretical calculations were used to identify the catalytically active sites of SnS2 as terraces and edges. Owing to the effective utilization of the entire surface area, SnS2 can effectively accelerate catalytic reactions. This finding provides a direction for material research in two-dimensional electrocatalysts for energy-efficient chemical production from electrochemical CO2 reduction, as well as for other energy devices.

Mathematical Model-Assisted Ultrasonic Spray Coating for Scalable Production of Large-Sized Solid Oxide Electrochemical Cells.

Thin solid oxide films are crucial for developing high-performance solid oxide-based electrochemical devices aimed at decarbonizing the global energy system. Among various methods, ultrasonic spray coating (USC) can provide the throughput, scalability, quality consistency, roll-to-roll compatibility, and low material waste necessary for scalable production of large-sized solid oxide electrochemical cells. However, due to the large number of USC parameters, systematic parameter optimization is required to ensure optimal settings. However, the optimizations in previous literature are either not discussed or not systematic, facile, and practical for scalable production of thin oxide films. In this regard, we propose an USC optimization process assisted with mathematical models. Using this method, we obtained optimal settings for producing high-quality, uniform 4 × 4 cm2 oxygen electrode films with a consistent thickness of ∼27 µm in 1 min in a facile and systematic way. The quality of the films is evaluated at both micrometer and centimeter scales and meets desirable thickness and uniformity criteria. To validate the performance of USC-fabricated electrolytes and oxygen electrodes, we employ protonic ceramic electrochemical cells, which achieve a peak power density of 0.88 W cm-2 in the fuel cell mode and a current density of 1.36 A cm-2 at 1.3 V in the electrolysis mode, with minimal degradation over a period of 200 h. These results demonstrate the potential of USC as a promising technology for scalable production of large-sized solid oxide electrochemical cells.