Perovskite solar cells (PSCs) offer a potentially large-scale method for producing low-cost renewable energy. However, stability challenges currently limit their practical application. Consequently, alternative methods for increasing the PSC stability are urgently needed. Compared with three-dimensional (3D) perovskites, low-dimensional (LD) perovskites have been shown to have higher stability. In this study, a LD/3D hybrid perovskite strategy is used that involves post-treating the Cs(FAMA)Pb(IBr) perovskite with a neutral allyl 1H-imidazole-1-carboxylate (AImC) ligand. We show that this neutral organic spacer molecule has two key roles. AImC acts as a solvent and triggers localized reconstruction to produce a LD capping layer in one postprocessing step. AImC prolongs the carrier lifetime and reduces trap-assisted recombination. As a result, the PSCs containing AImC achieve a maximum power conversion efficiency (PCE) of 21.42% compared to 20.27% for the control device and show significantly decreased hysteresis. AImC also greatly increased the stability of the films and devices to air, moisture, and heat. The results of this study imply that neutral amine liquids that have the correct solvating and ligating properties have good potential to improve the PCE and stability of the PSCs.

In this study, we propose a practical approach for producing a heterobimetallic Ni(II)-Ce(III) diimine complex from an extended salen-type ligand (HL) to serve as an electrocatalyst for CO reduction and demonstrate an outstanding overall efficiency of 99.6% of the cerium-nickel complex and integrate it into applicable cell assemblies. We optimize not only the catalyst, but the operational conditions enabling successful CO electrolysis over extended periods at different current densities. A comparison of electrochemical behavior in H-cell and zero-gap cell electrolyzers suggests potential applications for industrial scale-up. In the H-cell electrolyzer configuration, the most elevated efficiency in CO production was achieved with a selectivity of 56.96% at -1.01 V vs RHE, while HCOO formation exhibited a selectivity of 32.24% at -1.11 V vs RHE. The highest TON was determined to be 14657.0 for CO formation, followed by HCOO with a TON of 927.8 at -1.11 V vs RHE. In the zero-gap electrolyzer configuration, the most efficient setup toward CO production was identified at a current density (CD) of 75 mA cm, a flow rate of 10 mL min, operating at 60 °C and utilizing a low KOH concentration of 0.1 M to yield a maximum faradaic efficiency (FE) of 82.1% during 24 h of stable electrocatalysis.

Solid-state batteries with lithium metal anodes are considered the next major technology leap with respect to today's lithium-ion batteries, as they promise a significant increase in energy density. Expectations for solid-state batteries from the automotive and aviation sectors are high, but their implementation in industrial production remains challenging. Here, we report a solid-state lithium-metal battery enabled by a polymer electrolyte consisting of a poly(DMADAFSI) cationic polymer and LiFSI in PyrFSI as plasticizer. The polymer electrolyte is infiltrated and solidified in the pores of a commercial LiNiMnCoO (NMC811) cathode with up to 2.8 mAh cm nominal areal capacity and in the pores of a 25 μm thin commercial polypropylene separator. Cathode and separator are finally laminated into a cell in combination with a commercial 20 μm thin lithium metal anode. Our demonstration of a solid-state polymer battery cycling at full nominal capacity employing exclusively commercially available components available at industrial scale represents a critical step forward toward the commercialization of a competitive all-solid-state battery technology.

Nitrate electroreduction reaction (NORR) to ammonia (NH) still faces fundamental and technological challenges. While Cu-based catalysts have been widely explored, their activity and stability relationship are still not fully understood. Here, we systematically monitored the dynamic alterations in the chemical and morphological characteristics of CuO nanocubes (NCs) during NORR in an alkaline electrolyte. In 1 h of electrolysis from -0.10 to -0.60 V vs RHE, the electrocatalyst achieved the maximum NH faradaic efficiency (FE) and yield rate at -0.3 V (94% and 149 μmol h cm, respectively). Similar efficiency could be found at a lower overpotential (-0.20 V vs RHE) in long-term electrolysis. At -0.20 V vs RHE, the catalyst FE increased from 73% in the first 2 h to ∼90% in 10 h of electrolysis. Electron microscopy revealed the loss of the cubic shape with the formation of sintered domains. Raman, X-ray diffraction (XRD), and Cu K-edge X-ray absorption near-edge spectroscopy (XANES) indicated the reduction of CuO to oxide-derived Cu (OD-Cu). Nevertheless, a remaining CuO phase was noticed after 1 h of electrolysis at -0.3 V vs RHE. This observation indicates that the activity and selectivity of the initially well-defined CuO NCs are not solely dependent on the initial structure. Instead, it underscores the emergence of an OD-Cu-rich surface, evolving from near-surface to underlying layers over time and playing a crucial role in the reaction pathways. By employing differential electrochemical mass spectrometry (DEMS) and Fourier transform infrared spectroscopy (FTIR), we experimentally probed the presence of key intermediates (NO and NHOH) and byproducts of NORR (N and NH ) for NH formation. These results show a complex relationship between activity and stability of the nanostructured CuO oxide catalyst for NORR.

Improving the photostability of the light-harvesting blend film in organic photovoltaics is crucial to achieving long-term operational lifetimes that are required for commercialization. However, understanding the degradation factors which drive instabilities is complex, with many variables such as film morphology, residual solvents, and acceptor or donor design all influencing how light and oxygen interact with the blend film. In this work, we show how blend films comprising a donor polymer (PBDB-T) and small molecule acceptor (PCBM or ITIC) processed with solvent additive (DIO) yield very different film morphologies, device performance, and photostability. We show that DIO is retained approximately 10 times more effectively in ITIC based films compared to PCBM. Unexpectedly, we see that while high volumes of DIO reduce photostability for encapsulated ITIC devices, when oxygen is introduced DIO can improve the lifetime of PBDB-T:ITIC based cells. Here, the addition of 3% DIO doubles the compared to ITIC based devices without DIO, suggesting that DIO-induced morphological changes interfere with or reduce photo-oxidative reactions.

Triboelectric nanogenerators (TENGs) have emerged as potential energy sources, as they are capable of harvesting energy from low-frequency mechanical actions such as biological movements, moving parts of machines, mild wind, rain droplets, and others. However, periodic mechanical motion can have a detrimental effect on the triboelectric materials that constitute a TENG device. This study introduces a self-healable triboelectric layer consisting of an Ecoflex-coated self-healable polydimethylsiloxane (SH-PDMS) polymer that can autonomously repair mechanical injury at room temperature and regain its functionality. Different compositions of bis(3-aminopropyl)-terminated PDMS and 1,3,5-triformylbenzene were used to synthesize SH-PDMS films to determine the optimum healing time. The SH-PDMS films contain reversible imine bonds that break when the material is damaged and are subsequently restored by an autonomous healing process. However, the inherent stickiness of the SH-PDMS surface itself renders the material unsuitable for application in TENGs despite its attractive self-healing capability. We show that spin-coating a thin layer (≈32 μm) of Ecoflex on top of the SH-PDMS eliminates the stickiness issue while retaining the functionality of a triboelectric material. TENGs based on Ecoflex/SH-PDMS and nylon 6 films show excellent output and fatigue performance. Even after incisions were introduced at several locations in the Ecoflex/SH-PDMS film, the TENG spontaneously attained its original output performance after a period of 24 h of healing. This study presents a viable approach to enhancing the longevity of TENGs to harvest energy from continuous mechanical actions, paving the way for durable, self-healable mechanical energy harvesters.

In recent years, hydrogels have been demonstrated as simple and cheap additives to improve the optical properties and material stability of organometal halide perovskites (OHPs), with most research centered on the use of hydrophilic, petrochemical-derived polymers. Here, we investigate the role of a peptide hydrogel in passivating defect sites and improving the stability of methylammonium lead iodide (MAPI, CHNHPbI) using closely controlled, X-ray photoelectron spectroscopy (XPS) techniques under realistic pressures. Optical measurements reveal that a reduction in the density of defect sites is achieved by incorporating peptide into the precursor solution during the conventional one-step MAPI fabrication approach. Increasing the concentration of peptide is shown to reduce the MAPI crystallite size, attributed to a reduction in hydrogel pore size, and a concomitant increase in the optical bandgap is shown to be consistent with that expected due to quantum size effects. Encapsulation of MAPI crystallites is further evidenced by XPS quantification, which demonstrates that the surface stoichiometry differs little from the expected nominal values for a homogeneously mixed system. XPS demonstrates that thermally induced degradation in a vacuum is reduced by the inclusion of peptide, and near-ambient pressure XPS (NAP-XPS) reveals that this enhancement is partially retained at 9 mbar water vapor pressure, with a reduced loss of methylammonium (MA) from the surface following heating achieved using 3 wt % peptide loading. A maximum power conversion efficiency (PCE) of 16.6% was achieved with a peptide loading of 3 wt %, compared with 15.9% from a 0 wt % device, the former maintaining 81% of its best efficiency over 480 h storage at 35% relative humidity (RH), compared with 48% maintained by a 0 wt % device.

Polymeric carbon nitride (PCN) and PCN-ZnO nanocomposites are promising candidates for catalysis, particularly for hydrogen evolution reactions (HER). However, their catalytic efficiency requires enhancement to fully realize their potential. This study aims to improve the HER performance of PCN by synthesizing PCN-ZnO nanocomposites using melamine as a precursor. Two synthesis methods were employed: thermal condensation (Method 1) and liquid exfoliation (Method 2). Method 1 resulted in a composite with a 2.44 eV energy gap and reduced particle size, with significantly enhanced performance as a bifunctional electrocatalyst for simultaneous hydrogen and oxygen production. In contrast, Method 2 produced a nanocomposite with an enhanced surface area and a minor alteration in the band gap. In alkaline electrolytes, the PCN-ZnO nanocomposite synthesized with Method 1 exhibited high HER performance with an overpotential of 281 mV, outperforming pristine PCN (382 mV) and ZnO (302 mV), along with improved oxygen evolution reaction (OER) activity. Further analysis in a two-electrode alkaline electrolyzer using PCN-ZnO nanocomposite as both the anode and cathode demonstrated its promise as a bifunctional electrocatalyst. Density functional theory (DFT) calculations explained the enhanced catalytic activity of the PCN-ZnO nanocomposite, confirming that hydrogen evolution occurs through the Heyrovsky process, consistent with experimental results. Notably, the solar-to-hydrogen (STH) efficiency of the PCN-ZnO nanocomposite was four times greater, at 21.7% compared to 5.2% for the PCN monolayer, underscoring its potential for efficient solar-driven hydrogen production. This work paves the way for future advancements in the design of high-performance electrocatalysts for sustainable energy applications.

Maintaining the electrochemically and mechanically stable solid electrolyte interphase (SEI) is of highest importance for the performance of high-capacity anode materials such as silicon (Si). Applying flexible Li-ion permeable coatings to the electrode surface using molecular layer deposition (MLD) offers a strategy to improve the properties of the SEI and greatly contributes to an increase in the cycle life and capacity retention of Si electrodes. In this study, the long-term cycling of Si electrodes with an MLD alucone coating is investigated in the context of more stable SEI formation. When the joined strategy introducing both MLD coating and anFEC electrolyte additive was realized, high performance of Si anodes was achieved, capable of delivering more than 1500 mAh g even after 400 cycles. The reason for the significantly improved longevity is the ability of the alucone layer to react with HF present in LiPF-based electrolytes already under OCV-like conditions, fluorinating most of the available -OH groups in the alucone structure. This reaction not only partially scavenges hydrofluoric acid but also does not disturb the confining effect of alucone-like fluorinated artificial SEI. This study shows the significance of searching for synergetic solutions, such as a combination of electrode surface modification and electrolyte composition, for maximizing the capacity retention of Si as an active material or as a capacity-enhancing additive to graphite electrodes, and as well can be applied to other high-energy battery materials with large volume changes during cycling.

Understanding the vertical compositional homogeneity and defect distribution is of paramount importance in elucidating and maximizing the performance of halide-perovskite-based optoelectronic devices. This work reports the depth-dependent study of the chemical composition and metallic Pb content of all-inorganic CsPbIBr perovskite films undertaken using lab-based hard X-ray photoelectron spectroscopy and soft X-ray photoelectron spectroscopy. The presence of elemental or metallic Pb (Pb), in the bulk and at the surface of the perovskite films highlights the formation of defect or recombination centers throughout the analyzed depth. The Pb content was found to be of higher concentration in the bulk of the CsPbIBr films compared to that at the surface. Engineering the CsPbIBr film growth using appropriate antisolvents resulted in the overall reduction and/or complete elimination of Pb at the surface and at the bulk of the perovskite films. However, the effect of antisolvent treatment was significantly pronounced in the bulk-like region as compared to that at the surface. Pb is synonymous with defect states/recombination centers in perovskite films and this reduction in defect density due to the antisolvent treatment corroborates the enhanced phase stability and improved solar cell performance of the corresponding CsPbIBr devices.

Stress-relieving and electrically conductive single-walled carbon nanotubes (SWNTs) and conjugated polymer, poly[3-(potassium-4-butanoate)thiophene] (PPBT), wrapped silicon microparticles (Si MPs) have been developed as a composite active material to overcome technical challenges such as intrinsically low electrical conductivity, low initial Coulombic efficiency, and stress-induced fracture due to severe volume changes of Si-based anodes for lithium-ion batteries (LIBs). The PPBT/SWNT protective layer surrounding the surface of the microparticles physically limits volume changes and inhibits continuous solid electrolyte interphase (SEI) layer formation that leads to severe pulverization and capacity loss during cycling, thereby maintaining electrode integrity. PPBT/SWNT-coated Si MP anodes exhibited high initial Coulombic efficiency (85%) and stable capacity retention (0.027% decay per cycle) with a reversible capacity of 1894 mA h g after 300 cycles at a current density of 2 A g, 3.3 times higher than pristine Si MP anodes. The stress relaxation and underlying mechanism associated with the incorporation of the PPBT/SWNT layer were interpreted by quasi-deterministic and quantitative stress analyses of SWNTs through Raman spectroscopy. PPBT/SWNT@Si MP anodes can maintain reversible stress recovery and 45% less variation in tensile stress compared with SWNT@Si MP anodes during cycling. The results verify the benefits of stress relaxation a protective capping layer and present an efficient strategy to achieve long cycle life for Si-based anodes for next-generation LIBs.

Improving the energy alignment between charge-transport layers and the perovskite is crucial for further enhancing the photovoltaic performance of tin-based perovskite solar cells (PSCs). Herein, the role of TiCT MXene in a poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hole transport layer (HTL) on the photovoltaic properties of PSCs is investigated as a function of its concentration. An improved perovskite film formation with reduced pinhole density and a more uniform contact potential difference is noted when MXene is embedded in the PEDOT:PSS HTL. The work function of the HTL is increased according to photoelectronic measurements, leading to a favorable energy alignment with the HOMO of PEAFASnI perovskite. PSCs fabricated using a MXene-embedded PEDOT:PSS HTL delivered a power conversion efficiency (PCE) of 8.35% compared to 7.35% from the pristine counterpart, while retaining ∼90% of its initial PCE after 450 h of storage in a N atmosphere.

Gallocyanine () was recently introduced as a promising aqueous-soluble electroactive molecule for preparing two-electron storage alkaline flow battery (FB) negolytes. The development of a cost-effective FB electrolyte is limited by the unexpectedly low solubility of . In this work, the compound 7-amino-4-hydroxy-2-naphthalenesulfonic acid was introduced as a molecular spectator to modulate the solubility of in KOH; this formulation allowed the preparation of a negolyte with a theoretical volumetric capacity of 32.00 Ah L. The cycling stability of an improved electrolyte was demonstrated by operating a FB cell outside of the glovebox (bubbling N in the tanks). The cell exhibited a Coulombic efficiency close to 98% and began operating with 72.1% of its theoretical capacity (16.06 Ah L), retaining 88% of it after 110 cell cycles. This work demonstrates that significant improvement in electrolyte performance can be obtained with suitable additives and electrolyte engineering.

Silver is the metal of choice for the fabrication of highly transparent grid electrodes for photovoltaics because it has the highest electrical conductivity among metals together with high stability toward oxidation in air. Conventional methods for fabricating silver grid electrodes involve printing the metal grid from costly colloidal solutions of nanoparticles, selective removal of metal by etching using harmful chemicals, or electrochemical deposition of the silver, an inherently chemical intensive and slow process. This Spotlight highlights an emerging approach to the fabrication of transparent and patterned silver electrodes that can be applied to glass and flexible plastic substrates or directly on top of a device, based on spatial modulation of silver vapor condensation. This counterintuitive approach has been possible since the discovery in 2019 that thin films of perfluorinated organic compounds are highly resistant to the condensation of silver vapor, so silver condenses only where the perfluorinated layer is not. The beauty of this approach lies in its simplicity and versatility because vacuum evaporation is a well-established and widely available deposition method for silver and the shape and dimensions of metallized regions depend only on the method used to pattern the perfluorinated layer. The aim of this Spotlight is to describe this approach and summarize its electronic applications to date with particular emphasis on organic photovoltaics, a rapidly emerging class of thin-film photovoltaics that requires a flexible alternative to the conventional conducting oxide electrodes currently used to allow light into the device.

To enable the greater installed capacity of proton exchange membrane water electrolysis (PEMWE) for clean hydrogen production, associated costs must be lowered while achieving high current density performance and durability. Scarce and expensive iridium (Ir) required for the oxygen evolution reaction (OER) is a large contributor to the overall cost, yet high loadings of Ir (1-2 mg cm) are currently needed in commercial systems to maintain sufficient activity, conductivity, and durability. To meet the aggressive targets for low Ir loadings, we introduce a composite anode approach using a conductive additive that is less expensive than Ir to facilitate robust, high-performance operation with low Ir loading by retaining electrode thickness and in-plane electrical conductivity. In this demonstration, we use platinum (Pt) black as the conductive additive given its high electrical conductivity, acid stability, and current price one-fifth that of Ir. Using a high-activity commercial Ir oxide (IrO ) catalyst, we present a 95% Ir loading reduction and 80% cost reduction of the anode catalyst materials while maintaining equal current density performance at a cell voltage of 1.8 V. Furthermore, we show enhanced stability of a composite anode compared to an IrO anode with loadings of 0.10 mg cm via accelerated stress test (AST) and postmortem imaging. With this approach, we show promising results toward lowering Ir loadings and material costs, addressing a significant barrier to the widespread adoption of PEMWE for clean hydrogen production.

Although lithium-sulfur (Li-S) batteries offer a high theoretical energy density, shuttling of dissolved sulfur and polysulfides is a major factor limiting the specific capacity, energy density, and cyclability of Li-S batteries with a liquid electrolyte. Cathode host materials with a microstructure to restrict the migration of active material may not totally eliminate the shuttling effect or may create additional problems that limit the full dissolution and redox conversion of all active cathode materials. Selecting a cathode coating binder with a multifunctional role offers a universal solution suitable for various cathode hosts. PEDOT:PSS is investigated as such a binder in this study via experimental testing and material characterization as well as multiscale modeling. The study is based on Li-S cells with a sulfur cathode in hollow porous particles as the cathode host and the 10 wt % PEDOT:PSS binder and electrolyte 1 M LiTFSI in 1:1 DOL:DME 1:1 v/v. A reference supercapacitor cell with the same electrolyte and electrodes comprising a coating of the same hollow porous particles and 10 wt % PEDOT:PSS revealed the pseudocapacitive effect of PEDOT:PSS following a surface redox mechanism that dominates the charge phase, which is equivalent to the discharge phase of the Li-S battery cell. A multipore continuum model for supercapacitors and Li-S cells is extended to incorporate the pseudocapacitive effects of PEDOT:PSS with the Li ions and the adsorption effects of PEDOT:PSS with respect to sulfur and lithium sulfides in Li-S cells, with the adsorption energies determined via molecular and simulations in this study. Experimental data and predictions of multiscale simulations concluded a 7-9% extension of the specific capacity of Li-S battery cells due to the surface redox effect of PEDOT:PSS and elimination of lithium sulfides from the anode by slowing down their migration and shuttling via their adsorption by the PEDOT:PSS binder.

In pursuit of commercial viability for carbon dioxide (CO) electrolysis, this study investigates the operational challenges associated with membrane electrode assembly (MEA)-type CO electrolyzers, with a focus on CO loss into the solution phase through bicarbonate (HCO ) and carbonate (CO ) ion formation. Utilizing a silver electrode known for selectively facilitating CO to CO conversion, the molar production of CO, CO, and H is measured across a range of current densities from 0 to 600 mA/cm, while maintaining a constant CO inlet flow rate of 58 mL/min. The dynamics of CO loss are monitored through measurements of pH changes in the electrolyte and carbon elemental balance analysis. Employing the concept of conservation of elemental carbon, a chemical reaction analysis is conducted, identifying the critical role of the hydroxide (OH) ion. At lower current densities below 125 mA/cm, where CO reduction predominates, it is observed that CO loss is proportional to current density, reaching up to 0.18 mmol/min, and directly correlates with the rate of OH ion production, indicative of HCO /CO ion formation. Conversely, at higher current densities above 450 mA/cm, where hydrogen evolution is the dominant process, CO loss is shown to decouple from the OH ion production rate with a constant limit condition of 0.12 mmol/min, regardless of the current density. This suggests that electrolyte-induced cathode flooding restricts CO access to cathode sites. Additionally, pH change in the electrolyte during the electrolysis further infers differing ion populations in the CO reduction and hydrogen evolution regimes, and their movement across the membrane. Continued monitoring of the pH change after the cessation of electricity offers insights into the accumulation of HCO /CO ion at the cathode, influencing salt formation.

Perovskite solar cells (PSCs) are receiving renewed interest since they have reached high power conversion efficiency (PCE) and show potential for application not only on rigid and flexible substrates but also on mechanically deformable substrates for integration on nonplanar curvilinear surfaces. Here we demonstrate PSCs fabricated on transparent conducting oxide-free ultrathin polyethylene terephthalate substrates capable of efficiently harvesting indoor light even under compressive strain. Interface engineering with poly(bis(4-phenyl)(2,4,6-trimethylphenyl)amine) improved the shunt resistance and band alignment at the perovskite-hole transport layer interface, which resulted in enhanced charge extraction, leading to 114% improvement in PCE from 5.57 to 11.91% under 500 lx indoor white LED (4000 K) illumination. The champion device exhibited a PCE of 18.37% under 250 lx cool white LED (4000 K) light. The maximum power output ( ) of the devices varied from 13.78 to 25.38 μW/cm by changing the indoor light illumination from 250 to 1000 lx, respectively. Moreover, the devices showed impressive performance even after mechanical deformation and retained 83 and 76% for 1 sun and indoor light, respectively, under 30% compressive strain. Our approach paves the way for fabrication of efficient indoor light harvesting PSCs on mechanically deformable substrates for integration on nonplanar surfaces prone to compressive strain.

Finding green energy resources that contribute to the battle against global warming and the pollution of our planet is an urgent challenge. Thermoelectric electricity production is a clean and efficient method of producing energy; consequently, scientists are currently researching and creating thermoelectric materials to increase the efficiency of thermoelectric electricity production and expand the potential of the thermoelectric effect for clean energy production. This work focuses on a comprehensive study of the thermoelectric properties of two-dimensional ScYCBr. We report here a computational analysis of this Janus-like MXene, which is predicted to exhibit outstanding thermoelectric properties. The study uses density-functional theory to provide evidence of the important role played by symmetry breaking to promote low-thermal transport by favoring certain phonon scattering channels. Compared to its symmetric parent compounds, the asymmetric Janus-type ScYCBr displays additional phonon scattering channels reducing the thermal conductivity. An exhaustive investigation of the dynamical stability for both zero-temperature and high-temperature conditions was also performed to support the stability of ScYCBr. Our analysis shows that thanks to its asymmetric structure, the ScYCBr MXene has thermoelectric properties that largely surpass those of its parent symmetric counterpart ScCBr, being a material with a remarkable thermoelectric high figure of merit. Another advantage of ScYCBr is its high carrier mobility. This work not only demonstrates that this material is a promising thermoelectric material but also shows that ScYCBr can operate efficiently at high temperatures up to 1200 K.

For conductive polymers to be competitive with carbon-based electrode materials, it is critical to increase their surface area and electroactivity. In this work, a thick nanofibrous polypyrrole (PPy) membrane with communicating interfiber spaces was prepared through one-pot interfacial polymerization for the first time. The electrochemical properties and conductivity of the membrane were studied with cyclic voltammetry, electrochemical impedance spectroscopy, and a four-point probe. Its morphology, chemistry, and thermostability were evaluated by scanning electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and thermogravimetric analysis. The areal specific capacitances measured between 0.0 and 0.8 V at 1 mA/cm were 19179, 13264, 7238, and 4458 mF/cm for the membranes doped with docusate sodium (AOT), camphor-10-sulfonic acid (β) (CSA), Cl, and poly(sodium 4-styrenesulfonate) (PSS), respectively. The capacity retentions after 1000 cycles were 83, 74, 67, and 61% for the AOT-, CSA-, PSS-, and Cl-doped membranes, respectively. The Coulombic efficiency was above 99% for all of the membranes. They showed energy densities of 1.7, 1.2, 0.7, and 0.4 mWh/cm and power densities of 0.61, 0.75, 0.66, and 0.62 mW/cm for the AOT-, CSA-, Cl-, and PSS-doped membranes, respectively. The ultrahigh areal specific capacitance of PPy-AOT is due to its nanofibrous structure. A mechanism has been proposed to explain how this structure is formed based on the role of AOT as the surfactant. This nanofibrous PPy membrane is easy to prepare and metal-free and offers a very high areal specific capacitance, making it an excellent candidate to construct electrodes in pseudosupercapacitors.

Nickel phosphides are an emerging class of earth-abundant catalysts for hydrogen generation through water electrolysis. However, the hydrogen evolution reaction (HER) activity of NiP is lower than that of benchmark Pt group catalysts. To address this limitation, an integrated theoretical and experimental study was performed to enhance the HER activity and stability of hexagonal NiP through doping with synergistic transition metals. Among the nine dopants computationally studied, zinc emerged as an ideal candidate due to its ability to modulate the hydrogen binding free energy (Δ ) closer to a thermoneutral value. Consequently, phase pure hexagonal Ni Zn P nanocrystals (NCs) with a solid spherical morphology, variable compositions ( = 0-17.14%), and size in the range of 6.8 ± 1.1-9.1 ± 1.1 nm were colloidally synthesized to investigate the HER activity and stability in alkaline electrolytes. As predicted, the HER performance was observed to be composition-dependent with Zn compositions () of 0.03, 0.07, and 0.15 demonstrating superior activity with overpotentials (η) of 188.67, 170.01, and 135.35 mV, respectively at a current density of -10 mA/cm, in comparison to NiP NCs (216.2 ± 4.4 mV). Conversely, Ni Zn P NCs with = 0.01, 0.38, 0.44, and 0.50 compositions showed a notable decrease in HER activity, with corresponding η of 225.3 ± 3.2, 269.9 ± 4.3, 276.4 ± 3.7 and 263.9 ± 4.9 mV, respectively. The highest HER active catalyst was determined to be NiZnP NCs, featuring a Zn concentration of 5.24%, consistent with composition-dependent Δ calculations. The highest performing NiZnP NCs displayed a Heyrovsky HER mechanism, enhanced kinetics and electrochemically active surface area (ECSA), and superior corrosion tolerance with a negligible increase of η after 10 h of continuous HER. This study provides critical insights into enhancing the performance of metal phosphides through doping-induced electronic structure variation, paving the way for the design of high-efficiency and durable nanostructures for heterogeneous catalytic studies.