ACS Applied Energy Materials

In this work, tin sulfide nanosheets decorated on face-mask-derived activated carbon have been explored as electrode material for electrochemical supercapacitors. A hydrothermal route was employed to grow tin sulfide on the surface and inside of high-surface-area face-mask-derived activated carbon, activated at 850 °C, to produce a hierarchical interconnected porous composite (ACFM-850/TS) structure. The presence of tin sulfide in the porous carbon framework exposed the surface active sites for rapid adsorption/desorption of electrolyte ions and ensured high utilization of the porous carbon surface...

Li-ion batteries have a pivotal role in the transition toward electric transportation. Ni-rich layered transition metal oxide (LTMO) cathode materials promise high specific capacity and lower cost but exhibit faster degradation compared with lower Ni alternatives. Here, we employ high-resolution electron microscopy and spectroscopy techniques to investigate the nanoscale origins and impact on performance of intragranular cracking (within primary crystals) in Ni-rich LTMOs. We find that intragranular cracking is widespread in charged specimens early in cycle life but uncommon in discharged samples even after cycling...

Transition metal oxynitrides are a promising class of functional materials for photoelectrochemical (PEC) applications. Although these compounds are most commonly synthesized via ammonolysis of oxide precursors, such synthetic routes often lead to poorly controlled oxygen-to-nitrogen anion ratios, and the harsh nitridation conditions are incompatible with many substrates, including transparent conductive oxides. Here, we report direct reactive sputter deposition of a family of zirconium oxynitride thin films and the comprehensive characterization of their tunable structural, optical, and functional PEC properties...

The use of precious metal electrocatalysts in clean electrochemical energy conversion and storage applications is widespread, but the sustainability of these materials, in terms of their availability and cost, is constrained. In this research, iron triad-based bimetallic nitrogen-doped carbon (M-N-C) materials were investigated as potential bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The synthesis of bimetallic FeCo-N-C, CoNi-N-C, and FeNi-N-C catalysts involved a precisely optimized carbonization process of their respective metal-organic precursors...

Forward-bias bipolar membrane (BPM) CO2 coelectrolysis (CO2ELY) aims at overcoming the issues of salt precipitation and CO2 crossover in anion exchange membrane CO2ELY. Increasing the stability of BPM-CO2ELY is crucial for widespread application of the technique. In this study, we employ time-resolved X-ray tomographic microscopy to elucidate the structural dynamics that occur within the electrochemical cell during operation under various conditions. Using advanced image processing methods, including custom 4D machine learning segmentation, we can visualize and quantify damages in the membrane and anode catalyst layer (CL)...

Electrochemical CO2 reduction (CO2 R) using heterogenized molecular catalysts usually yields 2-electron reduction products (CO, formate). Recently, it has been reported that certain preparations of immobilized cobalt phthalocyanine (CoPc) produce methanol (MeOH), a 6-electron reduction product. Here, we demonstrate the significant role of intermediate mass transport in CoPc selectivity to methanol. We first developed a simple, physically mixed, polymer (and polyfluoroalkyl, PFAS)-free preparation of CoPc on multiwalled carbon nanotubes (MWCNTs) which can be integrated onto Au electrodes using a poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT:PSS) adhesion layer...

An increasing number of studies focus on organic flow batteries (OFBs) as possible substitutes for the vanadium flow battery (VFB), featuring anthraquinone derivatives, such as anthraquinone-2,7-disulfonic acid (2,7-AQDS). VFBs have been postulated as a promising energy storage technology. However, the fluctuating cost of vanadium minerals and risky supply chains have hampered their implementation, while OFBs could be prepared from renewable raw materials. A critical component of flow batteries is the electrode material, which can determine the power density and energy efficiency...

Porous composite battery electrode performance is influenced by a large number of manufacturing decisions. While it is common to evaluate only finished electrodes when making process adjustments, one must then make inferences about the fabrication process dynamics from static results, which makes process optimization very costly and time-consuming. To get information about the dynamics of the manufacturing processes of these composites, we have built a miniature coating and drying apparatus capable of fabricating lab-scale electrode laminates while operating within an X-ray beamline hutch...

A hydrogen-organic hybrid flow battery (FB) has been developed using methylene blue (MB) in an aqueous acid electrolyte with a theoretical positive electrolyte energy storage capacity of 65.4 A h L-1 . MB paired with the versatile H2 /H+ redox couple at the negative electrode forms the H2 -MB rechargeable fuel cell, with no loss in capacity (5 sig. figures) over 30 100% discharge cycles of galvanostatic cycling at 50 mA cm-2 , which shows excellent stability. A peak power density of 238 mW cm-2 has also been demonstrated by utilizing 1...

Two-dimensional (2D) transition-metal dichalcogenides have shown great potential for energy storage applications owing to their interlayer spacing, large surface area-to-volume ratio, superior electrical properties, and chemical compatibility. Further, increasing the surface area of such materials can lead to enhanced electrical, chemical, and optical response for energy storage and generation applications. Vertical silicon nanowires (SiNWs), also known as black-Si, are an ideal substrate for 2D material growth to produce high surface-area heterostructures, owing to their ultrahigh aspect ratio...

One of the main challenges to expand the use of titanium dioxide (titania) as a photocatalyst is related to its large band gap energy and the lack of an atomic scale description of the reduction mechanisms that may tailor the photocatalytic properties. We show that rutile TiO2 single crystals annealed in the presence of atomic hydrogen experience a strong reduction and structural rearrangement, yielding a material that exhibits enhanced light absorption, which extends from the ultraviolet to the near-infrared (NIR) spectral range, and improved photoelectrocatalytic performance...

Voltaic pile, the very first battery built by humanity in 1800, plays a seminal role in battery development history. However, the premature design leads to the inevitable copper ion dissolution issue, which dictates its primary battery nature. To address this issue, solid-state electrolytes, ion exchange membranes, and/or sophisticated electrolytes are widely utilized, leading to high costs and complicated cell configuration. Herein, we build a rechargeable zinc-copper voltaic battery from simple and cheap electrolyte/separator materials, thus eliminating the need to use the above components...

This work aims to understand the spin-coating growth process of BiVO4 photoanodes from a photon absorption and conversion perspective. BiVO4 layers with thicknesses ranging from 7 to 48 nm and the role of a thin (<5 nm) SnO2 hole-blocking layer have been studied. The internal absorbed photon-to-current efficiency (APCE) is found to be nonconstant, following a specific dependence of the internal charge separation and extraction on the increasing thickness. This APCE variation with BiVO4 thickness is key for precise computational simulation of light propagation in BiVO4 based on the transfer matrix method...

Solid-state batteries (SSBs) that incorporate the argyrodite-Li6 PS5 Cl (LPSCl) electrolyte hold potential as substitutes for conventional lithium-ion batteries (LIBs). However, the mismatched interface between the LPSCl electrolyte and electrodes leads to increased interfacial resistance and the rapid growth of lithium (Li) dendrites. These factors significantly impede the feasibility of their widespread industrial application. In this study, we developed a composite electrolyte of the LPSCl/polymer to enhance the contact between the electrolyte and electrodes and suppress dendrite formation at the grain boundary of the LPSCl ceramic...

Mesoscopic carbon-based perovskite solar cells (CPSCs) are often cited as a potential frontrunner to perovskite commercialization. Infiltration, the extent to which perovskite fills the mesoporous scaffold, is critical for optimum performance and stability. However, infiltration data are usually presented as qualitative photographic comparisons of samples with extreme infiltration variation. This work examines how small infiltration defects impact performance using an optical microscopy examination of the base TiO2 layer to identify issues and develop targeted techniques for infiltration enhancement...

An inorganic wide-bandgap hole transport layer (HTL), copper(I) thiocyanate (CuSCN), is employed in inorganic planar hydrothermally deposited Sb2 S3 solar cells. With excellent hole transport properties and uniform compact morphology, the solution-processed CuSCN layer suppresses the leakage current and improves charge selectivity in an n-i-p-type solar cell structure. The device without the HTL (FTO/CdS/Sb2 S3 /Au) delivers a modest power conversion efficiency (PCE) of 1.54%, which increases to 2.46% with the introduction of CuSCN (FTO/CdS/Sb2 S3 /CuSCN/Au)...

Herein, we systematically examined how composition influenced the properties of vinyl addition polynorbornene anion exchange membranes (AEMs) prepared from 5 -n -hexyl-2-norbornene and 5-(4-bromobutyl)-2-norbornene. Copolymerization kinetics revealed that 5 -n -hexyl-2-norbornene is consumed faster than 5-(4-bromobutyl)-2-norbornene, leading to a portion of the chain being richer in bromoalkyl groups. The alkyl halide pendants can then be converted to either trimethylammonium or tetrakis(dialkylamino)phosphonium cations through straightforward substitution with trimethylamine or a tris(dialkylamino)phosphazene...

Ni-Xides (X = B, P, or S) exhibit intriguing properties that have endeared them for electrocatalytic water splitting. However, the role of B, P, and S, among others, in tailoring the catalytic performance of the Ni-Xides remains vaguely understood, especially if they are studied in unpurified KOH (Un-KOH) because of the renowned impact of incidental Fe impurities. Therefore, decoupling the effect induced by Fe impurities from inherent material reconstruction processes necessitates investigation of the materials in purified KOH solutions (P-KOH)...

Despite the progress made in Li-ion battery components, technology still faces major challenges. Among them, the development of novel electrolytes with promising characteristics is required for next-generation energy storage devices. In this work, rigid hybrid electrolytes have been prepared by infiltration of an ionic liquid solution (Pyr14 TFSI) with a lithium salt (LiTFSI) into a sintered LATP ion-conducting porous ceramic. The porous ceramic 3D network was obtained via solid-state sintering of LATP powders mixed with a small amount of corn starch as pore former...

Recent developments in Sb2 Se3 van der Waals material as an absorber candidate for thin film photovoltaic applications have demonstrated the importance of surface management for improving the conversion efficiency of this technology. Sb2 Se3 thin films' versatility in delivering good efficiencies in both superstrate and substrate configurations, coupled with a compatibility with various low-temperature deposition techniques (below 500 °C and often below 350 °C), makes them highly attractive for advanced photovoltaic applications...