Active Cathode Research Articles

High‐Capacity, Long‐Life All‐Solid‐State Lithium–Selenium Batteries Enabled by Lithium Iodide Active Additive

AbstractSelenium (Se) shows promise as a cathode candidate for all‐solid‐state lithium (Li) batteries due to its impressive theoretical volumetric energy density, much higher electronic conductivity, and improved safety in comparison to those for sulfur (S). An active cathode additive, lithium iodide (LiI) is demonstrated, to address the major challenge for all‐solid‐state Li–Se batteries, namely the sluggish redox kinetics resulting from the huge solid‐state conversion barrier. The LiI additive enhances Li+ transport and provides catalytic sites for Se cathode, thus endowing the batteries with accelerated reaction kinetics and extra capacity. DFT calculation and experimental analysis clearly reveal that LiI additive efficiently accelerates the conversion between polyselenide intermediates and Li2Se. With the above advantages, the battery with LiI using Li6PS5Br electrolyte gives an outstanding capacity of 862 mAh gSe−1 beyond the theoretical specific capacity of Se and a superlong life over 1800 cycles at 1C under room temperature. This work offers a simple strategy to facilitate the kinetics of all‐solid‐state Se cathodes and paves the way for the practicality of high‐capacity and long‐life all‐solid‐state Li–Se batteries.

Multiple enhancement effects of dipoles within polyimide cathode promoting highly efficient energy storage of lithium-ion batteries

Polyimide (PI) has been recognized as a potential organic cathode for Li-ion batteries (LIBs) due to its programmable structural design, high theoretical capacity, and resource availability. However, the poor intrinsic electrical conductivity of PI means that PI-based cathodes of LIBs have inefficient energy storage performance, especially at high current densities. In this work, the molecular structure of PI is optimized to obtain a layer-stacked crystalline PI with significantly enhanced dipoles, denoted NT-B for the first time. The dipoles in this PI are induced by the electronegative carbonyl groups from the monomer biuret and further enhanced via a π-π layer stacking effect. This work is the first to verify that the co-directional dipole enhancement effect of biuret is surprisingly different from that of monomer urea. A series of ex-situ/in-situ and theoretical DFT simulations are carried out to understand the functional mechanism of such effects. The multiple enhancement effects of the dipoles synergistically promoting the generation of a strong built-in electric field (BIEF) within NT-B are proposed based on the results obtained. It is confirmed that this BIEF plays a significant role in accelerating electron transport, which enhances the electrochemical activity of LIB cathodes. This work provides a new idea for the structural design of high-performance PI cathodes for LIBs.

Construction of more oxygen vacancies of BaCo0.4Fe0.4Zr0.2O3-δ for high-performance proton-conducting solid oxide fuel cell cathodes

The cathodic catalytic activity for the oxygen reduction reaction (ORR) plays a critical role in determining the performance of proton-conducting solid oxide fuel cells (P-SOFCs). BaCo0.4Fe0.4Zr0.2O3-δ (BCFZ) has emerged as a promising cathode for P-SOFCs due to its triple-phase conductivity. Nevertheless, its suboptimal proton conductivity and hydration ability at intermediate temperatures prevent it from achieving the anticipated ORR catalytic activity. To address these limitations, this study explores the enhancement of electrocatalytic activity in BCFZ through alkali metal doping and A-site defect construction. The effects of such modifications on oxygen surface exchange kinetics and ORR catalytic activity are systematically investigated. The findings reveal that BCFZ exhibits relatively low parameters in terms of electronic conductivity, oxygen ion conductivity, oxygen vacancy concentration, kchem, and Dchem. Conversely, these parameters are markedly improved in A-site deficient BCFZ (D-BCFZ) and Na/K-doped BCFZ. Consequently, the enhancement of these properties yields a significant increase in ORR catalytic activity, with D-BCFZ demonstrating the best electrochemical performance. Specifically, P-SOFC with D-BCFZ cathode achieves an Rp value of just 0.073 Ω cm2 and a Pmax value of 0.928 W cm−2 at 650 °C. This study provides theoretical insight into the mechanisms by how alkali metal doping and defect construction enhance the ORR catalytic activity of BCFZ. These findings offer valuable guidance for the development and optimization of high-performance P-SOFC cathodes.

Engineering active and robust alloy-based electrocatalyst by rapid Joule-heating toward ampere-level hydrogen evolution

Rational design of bimetallic alloy is an effective way to improve the electrocatalytic activity and stability of Mo-based cathode for ampere-level hydrogen evolution. However, it is still critical to realise desirable syntheses due to the wide reduction potentials between different metal elements and uncontrollable nucleation processes. Herein, we propose a rapid Joule heating method to effectively load RuMo alloy onto MoOx matrix. As-prepared catalyst exhibits excellent stability (2000 h @ 1000 mA cm−2) and ultralow overpotential (9 mV, 18 mV and 15 mV in 1 M KOH, 1 M PBS, 0.5 M H2SO4 solution, respectively) at 10 mA cm−2. Based on first-principle simulations and operando measurements, the impressive electrocatalytic stability and activity are investigated. And the role of rapid Joule heating method is highlighted and discussed in details. This study showcases rapid Joule heating as a feasible strategy to construct highly efficient alloy-based electrocatalysts.

Effect of Extrusion Process on Microstructure, Corrosion Properties, and Mechanical Properties of Micro-Alloyed Mg-Zn-Ca-Zr Alloy.

The effect of the extrusion process on the microstructure, corrosion, and mechanical properties of Mg-Zn-Ca-Zr alloy has been investigated. Zn and Ca were both in a solid solution and only the Zr-rich phase was observed in the homogenized and extruded alloys. The Zr-rich phase was obviously refined after extrusion. The corrosion rate of the homogenized alloy decreased by about 25% after extrusion. This is because the refined Zr-rich phase was easier to cover with the deposited corrosion products, which reduced the cathodic reaction activity of the Zr-rich phase. The corrosion rate is similar for the alloys extruded at 320 °C and 350 °C since the size and distribution of the Zr-rich phase were not different in the two conditions. The alloy extruded at 320 °C has a smaller grain size and better comprehensive mechanical properties.

Non-metal doping enhsances oxygen reduction kinetics and CO2 tolerance of SrFeO3-δ perovskite as high-performance cathodes for solid oxide fuel cells

The sluggish of the oxygen reduction reaction (ORR) kinetics and the susceptibility to CO2 interactions are major barriers to the widespread application of solid oxide fuel cells (SOFCs). In this study, a non-metal cation doping strategy was employed to enhance the ORR catalytic activity and CO2 tolerance of SrFeO3-δ cathode. SrFe1-xPxO3-δ (SFPx, x = 0, 0.05, 0.1, 0.15, 0.2) materials were synthesized by substituting phosphorus (P) for Fe in SrFeO3-δ. The doping of P facilitated the formation of oxygen vacancies in SrFeO3-δ, enhancing oxygen adsorption, dissociation, diffusion, and charge transfer processes, leading to a notable increase in ORR catalytic activity. At 800 ℃, the polarization resistance of SFP0.15 was 0.08 Ω cm2, a reduction of 42.86 % compared to undoped SrFeO3-δ. Additionally, SFP0.15 achieved a peak power density of 749.36 mW cm2, representing a 91.99 % enhancement over SrFeO3-δ. These findings suggest that non-metal cation doping is an effective approach to boost the performance of SrFeO3-δ perovskite cathode.

Investigating PEDOT:PSS Binder as an Energy Extender in Sulfur Cathodes for Li-S Batteries.

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 ab initio 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.

Enhancing Benzylamine Electro-oxidation and Hydrogen Evolution through in-situ Electrochemical Activation of CoC2O4 Nanoarray.

The sluggish anodic oxygen evolution reaction (OER) seriously restricts the overall efficiency of water splitting. Here, we present an environmentally friendly and efficient aniline oxidation (BOR) to replace the sluggish OER, accomplishing the co-production of H2 and high value-added benzonitrile (BN) at low voltages. Cobalt oxalates grown on cobalt foam (CoC2O4·2H2O/CF) are adopted as the pre-catalysts, which further evolve into working electrocatalysts active for BOR and HER after appropriate electrochemical activation. Thereinto, cyclic voltammetry activation at positive potentials is performed to reconstruct cobalt oxalate via extensive oxidation, resulting in enriched Co(III) species and nanoporous structures beneficial for BOR, while chronoamperometry at negative potentials is introduced for the cathodic activation toward efficient HER with obvious improvement. The two activated electrodes can be combined into a two-electrode system, which achieves a high current density of 75 mA cm-2 at the voltage of 1.95 V, with the high Faraday efficiencies of both BOR (90.0%) and HER (90.0%) and the satisfactory yield of BN (76.8%).

A self-driven solar coupling system with activated carbon felt cathode for resourcefully purifying uranium and organic contaminated water

With the continuous development of nuclear energy, it becomes increasingly important to recover uranium from the radioactive wastewater, in which various organics may combine with uranyl ions (UO22+) to form refractory complexes. Developing highly active cathode materials for uranium reduction is essential to improve the performance of self-driven solar coupling system (SSCS) in treating complex radioactive wastewater. In this study, an activated carbon felt (ACF) cathode is prepared by anodizing carbon felt (CF) in NaOH solution to adjust the surface morphology and functional groups. The ACF is then used in a SSCS combined with a TiO2 nanorods array (TNA) photoanode for the efficient recovery of uranium and the rapid degradation of organic pollutants with simultaneous electricity generation. Compared to CF, the functionalized ACF with oxygen-containing functional groups, provides sufficient sites for UO22+ adsorption and facilitates the charge separation. The SSCS with the ACF cathode exhibits removal ratios of approximately 99.9 % for tetracycline hydrochloride (TCH) and UO22+, with removal rates of ∼ 0.025 and ∼ 0.154 min−1, respectively. In contrast, the SSCS with the CF cathode achieves removal rates of ∼ 0.006 and ∼ 0.026 min−1. Additionally, a maximum power density of 0.94 mW·cm−2 with a fill factor of 23.36 % is achieved. After 20 cycles, the system maintains removal ratios of 99.1 % for TCH and 98.2 % and UO22+. Intensive investigation also reveals that the system functions robustly in treating complex wastewater with a complicated condition of pH, co-exited ions, and various pollutant concentrations. Furthermore, efficient removal of organics and uranium is also achieved from polluted seawater or under real sunlight illumination. This paper presents a simple method to prepare low-cost, highly active and stable cathodes for uranium reduction in an easy-to-operated, energy-saving and economical solar-driven system.

A strategy to reutilize silver nanoparticles on silicon nanowires via photocathodic activation for enhanced and sustainable hydrogen evolution

The development of electrodes for hydrogen evolution via water splitting in a neutral electrolyte is highly desirable, especially considering that natural water resources such as seawater typically have a neutral pH. In this study, silicon nanowires (SiNWs) arrays with uniform silver (Ag) decoration are prepared as a cathode material, which exhibits excellent and stable electrochemical performance for neutral water electrolysis. Ag ions, utilized in the preparation of SiNWs through metal-assisted chemical etching technique, are retained and decorated within the SiNWs array without undergoing a dissolution process, referred to as Native SiNWs. Remained Ag+ ions on the SiNWs are activated photocathodically and reduced to Ag0, resulting in a significantly enhanced performance as an electrocatalyst for hydrogen evolution reaction (HER). Hence, this photocathodic activation of Native SiNWs (PCA-Native SiNWs) eliminates the need for additional cocatalyst deposition for HER, utilizing the Ag ions employed in the SiNWs preparation process. This enhancement in HER activity is exclusively observed by photocathodic activation, not by cathodic activation without light irradiation, indicating the crucial role of photoelectrons in SiNWs under light irradiation for the activation. Additionally, the nanowire structure serves as an ideal platform for Ag nanoparticles, providing sufficient surface area, resulting in excellent dispersion and an increased number of active sites. Furthermore, PCA-Native SiNWs demonstrates outstanding electrochemical stability for over 60 h, with no significant reduction in current density or structural degradation in a neutral electrolyte. Several characterizations and electrochemical analyses have been conducted to elucidate the in-situ decoration of Ag nanoparticles on SiNWs and investigate the surface chemistry for the activation mechanism. This work introduces a new perspective on using Ag-decorated SiNWs directly as an electrocatalyst for effective hydrogen evolution in a neutral media.

Electrodeposition of Ni/Cu Bimetallic Conductive Metal-Organic Frameworks Electrocatalysts with Boosted Oxygen Reduction Activity for Zinc-Air Batteries.

Zinc-air batteries employing non-Pt cathodes hold significant promise for advancing cathodic oxygen reduction reaction (ORR). However, poor intrinsic electrical conductivity and aggregation tendency hinder the application of metal-organic frameworks (MOFs) as active ORR cathodes. Conductive MOFs possess various atomically dispersed metal centers and well-aligned inherent topologies, eliminating the additional carbonization processes for achieving high conductivity. Here, a novel room-temperature electrochemical cathodic electrodeposition method is introduced for fabricating uniform and continuous layered 2D bimetallic conductive MOF films cathodes without polymeric binders, employing the organic ligand 2,3,6,7,10,11-hexaiminotriphenylene (HITP) and varying the Ni/Cu ratio. The influence of metal centers on modulating the ORR performance is investigated by density functional theory (DFT), demonstrating the performance of bimetallic conductive MOFs can be effectively tuned by the unpaired 3d electrons and the Jahn-Teller effect in the doped Cu. The resulting bimetallic Ni2.1Cu0.9(HITP)2 exhibits superior ORR performance, boasting a high onset potential of 0.93V. Moreover, the assembled aqueous zinc-air battery demonstrates high specific capacity of 706.2mA h g-1, and exceptional long-term charge/discharge stability exceeding 1250 cycles.

Direct Sonochemical Leaching of Li, Co, Ni, and Mn from Mixed Li-Ion Batteries with Organic Acids

Metals such as nickel, cobalt, lithium, and manganese are widely used in lithium-ion batteries (LIBs) in electronic devices and electric vehicles. It is forecast that there will be a strong increase in the number of electronic devices and electric vehicles in the coming years. (1) Background: In this paper, the application of ultrasound waves on improving Li, Co, Mn, and Ni leaching efficiency from mixed active cathode materials from different types of LIBs is presented. (2) Methods: Environmentally friendly, low-concentrated (0.75 M) organic acids (oxalic acid, citric acid) and, additionally, sulfuric acid, were used in sonochemical and chemical leaching (stirring process) at a temperature of 60 °C. (3) Results: The results showed significantly higher leaching efficiency of metals with ultrasound-assisted treatment, especially when using organic acids. An average of 50% better leaching results were obtained for Li in oxalic acid (99.6%) and for Co (93.1%) in citric acid during sonochemical leaching. (4) Conclusions: Based on the theory of hydrogen peroxide formation during ultrasound wave transition in solutions, the role of H2O2 as one of the most effective reductants used to enhance cobalt, manganese, and nickel leaching from LIBs is indicated.

Highly Effective Electrolytes Toward High‐Performance Aluminum/Seawater Batteries

AbstractThe poor performance of metal/water batteries caused by self‐corrosion of anodes and low catalytic activity of cathodes has been a long‐standing challenge, greatly limiting their practical applications, in particular the underwater unmanned vehicle (UUV) application. We have fabricated an Al/seawater battery using simulated seawater with an appropriate pH and added with polyacrylic acid (PAA) as the electrolyte. This electrolyte simultaneously greatly retards self‐corrosion of the Al anode by in situ forming a PAA‐Al3+ complex film on it and increases the electrocatalytic activity toward the hydrogen evolution reaction by improving the electronic structure of Pt. When utilizing the multielement‐doped Al sheet as the anode and nickel foam supported loading‐amount‐optimized Pt/C catalyst as the cathode and adopting the developed new electrolyte, the obtained Al/H2O battery exhibits an energy density of 2271 Wh kg−1, which is the highest among those of all the reported batteries, and a power density of 20.87 mW cm−2, which outperforms all the reported metal/H2O batteries. This work not only develops a new type of high‐performance Al/H2O batteries for practical applications such as UUVs, but provides scientific insight into the design of superior electrolytes, which could be further extended for improving the performances of various metal batteries.

Rapid oxygen atom capture on perovskite surface boosting the activity and durability of cathode for solid oxide fuel cells

The content and distribution of surface oxygen vacancies are crucial for the oxygen reduction reaction (ORR) activity of solid oxide fuel cell (SOFC) cathodes. Therefore, a facile and rapid oxygen atom capture strategy is developed to modulate the surface oxygen vacancies of the cathode. By controlling the duration of NaBH4 solution reduction, precise modulation of the surface oxygen vacancies of NdBa0.5Sr0.5Co2O5+δ (NBSC) is achieved. Consequently, the processes of oxygen adsorption, dissociation, and diffusion on the surface of the NBSC cathode are enhanced. The research findings demonstrate that NBSC reduced for 10 min (RE-NBSC-10) exhibits optimal ORR catalytic activity and CO2 tolerance. At 800 °C, the Rp of RE-NBSC-10 decreases by 45 %, reaching 0.006 Ω‧cm2. Moreover, the maximum power density (MPD) of the RE-NBSC-10 cathode reaches 1.16 W cm−2, representing a 90.2 % improvement compared to NBSC. This research provides an efficient approach for the advancement of materials tailored for next-generation energy conversion devices.

Modeling of Fluidized Bed Molten Carbonate Direct Carbon Fuel Cell: Effect of Reverse Boudouard Reaction

Direct carbon fuel cells (DCFCs) are an alternative technology to coal-fired power plants for converting the chemical energy of abundant carbon-rich fuel into electrical energy. DCFCs have higher electrical efficiency and lower greenhouse emissions, which are easier to separate and capture. In the transition to renewable sources of energy, efficient and low-emission technologies need to be explored. Since DCFC technologies are in their early stages of development, modeling and simulation studies are needed to reduce costs and aid in experimental design. In this study, an electrochemical and transport model for a fluidized bed molten carbonate DCFC (FBMCDCFC) is developed. The performance of the fuel cell is evaluated through the polarization losses. This study expounds on recent developments in DCFCs by considering the effect of the reverse Boudouard reaction and the 2-electron oxidation of CO alongside the 4-electron oxidation of carbon at higher temperatures. The electrolyte used is a 62 : 38 mol % Li2CO3/K2CO3 eutectic mixture, while the fuel is activated carbon impregnated by HNO3. The results show that the greatest polarization losses for the FBMCDCFC are from anode activation overpotential and ohmic overpotential. The cathode activation and concentration overpotentials are relatively small. Increasing the reaction temperature results in a greater decrease in anode activation overpotential than ohmic overpotential, despite the increase in CO formation from the reverse Boudouard reaction. The peak power density of the FBMCDCFC is 434.437 W m-2 when operated at 923 K and a gas flow rate of 30 mL min-1. The peak power density of the FBMCDCFC is greater with higher temperatures, where the peak increases to 584.802 W m-2 when operated at 1023 K. The peak power density is greater with lower gas flow rates, where the peak increases to 458.175 W m-2 at a gas flow rate of 25 mL min-1. The mathematical model can aid in optimizing the performance of FBMCDCFCs, such as how increasing the operating temperature favorably increases anode reaction kinetics and reduces ohmic resistances in the cell. Future work will focus on improving the model correlations to close the gap between the results of modeling and actual experiments.Figure 1. a) Power curves at different temperatures, 823 K to 1323 K (30 mL min-1 flow rate, 1 atm total pressure); b) Power curves at different gas (O2 and CO2) flow rates (923 K, 1 atm total pressure) Figure 1

Efficient Ni-NC Gas Diffusion Electrodes for CO2 Electrolyzer with High Utilization Efficiencies and Single Pass Conversions Towards CO

The electrochemical CO2 reduction in membrane electrolyzer devices can become a key technology to close the anthropologic carbon cycle. For industrialisation of CO2 electrolyzers, however, performance shortcomings of today’s state-of-art electrolyzer designs and cathodes have to be addressed. Alkaline Membrane CO2 electrolyzers suffer from low utilization efficiency of CO2 due to an acid-base CO2 loss to carbonates, which limits the CO2 utilization efficiency and single pass conversion to 50% in AEM CO2-to-CO electrolyzer. Bipolar Membrane CO2 electrolyzers suffer from high cell voltage and lower Faradic efficiencies due to the acidic environment. All thoses designs suffer from layer flooding or salting events which limit the durability of the cells. New cell designs and new diagnostic tools are needed to predict, diagnose, and eliminate detrimental operating regimes of CO2 electrolyzers.In this work, we report on NiNC catalyst-based cathode GDEs for CO2 reduction to CO in a zero-gap membrane electrolyzer cell. We compare AEM and BPM cell designs. We propose the carbon crossover coefficient, CCC, as a new diagnostic analysis tool to monitor and understand through- or in-plane mass transport limitations in AEM and BPM cells. We also demonstrate how N2 bleeds can be used as diagnostic tools to recognize salting inside the electrolyzer cell.In our AEM studies, we show that sufficient CO2 access to the catalyst surface sites is important to achieve a high performance. Under near neutral conditions on the anode we report 85% FE towards CO at 300 mA cm-2 at 3.6 V with single pass conversion of 40% which is very close to the theoretical maximum. In addition, we can report high energy efficiency but only a utilization efficiency of around 50%.In our BPM studies, we show that NiNC GDEs are active and stable cathodes in zero-gap membrane electrolyzer. Protons raise the utilization efficiency as the carbonate will decompose into CO2 and water. To handle the changed electro osmotic water drag we replaced the ionomer with PTFE and could achieve 82% FE and 69% single pass conversion at 500 mA cm-2 with close to 100% CO2 utilization efficiency towards CO.We show that using a either an AEM or BPM electrolyzer design we can reach over 100h stable performance at 100 mA cm-2.Figure caption: CO2 singel pass conversion and lambda comparison of AEM and BPM CO2 reduction electrolyzer cells. Figure 1

Nanoparticles for Active and Sustainable Fuel Cell Cathodes

Depletion of fossil fuels and environmental pollution raised interest in new technologies for sustainable energy production, conversion, and storage, among which fuel cell technology is greatly studied, in both academia and industry. Proton exchange membrane fuel cells (PEMFCs) are reputed energy devices, due to their high conversion efficiency and low environmental pollution.1 Nowadays, Pt-based catalysts exhibit the best electrocatalytic activity towards oxygen reduction reaction (ORR), but enhancing their catalytic efficiency and reducing costs are essential for commercializing fuel cell technology.2 Our interest relies with the development of Pt-based nanoalloys2,4 via solution organometallic chemistry approach.3 This approach allows control over the composition, structure, and morphology of metal nanoparticles, and could lead to increased catalytic activity and long-term stability by revealing more active sites of the catalyst. Additionally, the ability to alloy with a range of metals for producing bimetallic compounds is one of the key advantages of this approach.In this communication, the synthesis of Pt-based nanoparticles and their characterization by state-of-the-art techniques such as ICP, EA, IR, TEM and HR-TEM will be described. The influence of the Pt complexes used as precursors and of the reaction conditions on the morphology of the Pt nanoparticles will be shown. The obtained nanostructures offer interesting starting materials to incorporate other metals, such as transition or rare earth metals, in order to have nanoalloys and study their performance in ORR in comparison to pure Pt catalysts.

Modeling Metal Nitrides for Interface Design in Lithium-Sulfur Batteries with GPUs and CPUs

As current batteries reach their limits, finding new battery materials is crucial. Lithium-sulfur batteries are a promising next-generation technology but face three major issues: low active material utilization, cathode pulverization, and limited polysulfide conversion leading to anode corrosion. Nano-deposition of metal nitride (MNx, M = Ti, V, Zr, etc.) layers on the graphene sulfur cathodes could significantly improve conductivity and cycling performance. Nevertheless, the large number of potential metal candidates requires preliminary and efficient computational screening using density-functional theory (DFT). This modeling framework can be used to calculate many properties of the coatings and screen out poor candidates. Firstly, the surface-adsorption ability of metal nitride candidates for lithium polysulfide intermediates involved in the electrochemical cycle (Li2S, Li2S2, Li2S4, Li2S6, Li2S8, S8) must be greater than the adsorption by dioxolane and dimethyl ether electrolytes (>~0.99eV). Secondly, the electronic properties before and after adsorption must feature significant density of states near the Fermi level, as a possible indicator of good electrical conductivity. Lastly, the free-energy profiles for the sulfur reduction reaction (SRR) over the remaining candidates will be estimated to better understand the catalytic properties of the metals. Particular attention will be paid to the Li2S2 reduction to Li2S, the potential limiting step. The top catalyst candidates should allow for an exergonic reaction. Finally, this application serves as a case study for our modeling platform, and the relative merits of standard for CPUs and GPUs in terms of computation time and accuracy will be discussed. Careful analysis of binding energy results, densities of states, and energy profiles for the various metal candidates provides valuable insights into the design of experimentally viable lithium-sulfur batteries, as well as advanced interface design in the broader field of battery research.

Sodium-Metal Battery Based on Reversible Oxide Chemistry at the Cathode

Sodium-metal batteries are considered as a promising energy storage alternative for currently available lithium-based batteries owing to their high gravimetric energy density and more specifically the natural abundance and the low price of Na metal that can lead to an inexpensive and low weight battery technology.In this study, we employ a Na-metal cell design that works based on reversible phase/composition change of sodium oxides (superoxide and peroxide) using a highly active cathode catalyst and an ether-based ionic-liquid electrolyte. The process involves in-situ production of sodium oxides in the controlled oxygen environment at the cathode. Subsequently, the cathode composed of sodium oxide compositions is assembled into a Na-metal architecture to do performance study and analysis. Our results indicated that the designed Na-metal battery demonstrates stable performance over 50 cycles with an overpotential of less than 100 mV and a coulombic efficiency exceeding 99%. Various electrochemical and physicochemical characterization techniques, including Raman spectroscopy, X-Ray diffraction analysis (XRD), X-ray photoelectron spectroscopy (XPS), Scanning electron microscopy (SEM), and Transmission Electron Microscopy (TEM), were employed to gain insight into cell chemistry and mixed ion-electron conduction mechanism. The findings underscore the significance of well-designed cell components in Na-O2 battery technologies, positioning them as a promising avenue in energy conversion and storage systems.

A highly active catalytic cathode La0.8Sr0.2Co0.7Ni0.3O3-δ for protonic ceramic fuel cells: experimental and computational insights

A highly active catalytic cathode La0.8Sr0.2Co0.7Ni0.3O3-δ for protonic ceramic fuel cells: experimental and computational insights