Venkataraman Thangadurai

• Doctor of Philosophy
• Professor at University of Calgary

Solid-state batteries with desirable advantages, including high-energy density, wide temperature tolerance, and fewer safety-concerns, have been considered as a promising energy storage technology to replace organic liquid electrolyte-dominated Li-ion batteries. Solid-state electrolytes (SSEs) as the most critical component in solid-state batteries...

Ubiquitous low-cost sodium ore is abundant and increasingly of interest for sodium-based battery research for grid-scale energy storage systems. The conventional organic liquid electrolytes in currently used sodium-based batteries endure inflammability, thermal instability, and risk of safety issues. The recent trend in developing solid-state-Li ba...

The world’s energy system is still dominated by fossil fuels. While there is a rapid reduction in the cost of renewable energy and the environmental costs of continued carbon dioxide emissions from fossil fuel recovery and use are well understood, current economic, infrastructure and political constraints sustain the fossil fuel enterprise as a dom...

A solid-state lithium-sulfur battery (SSLSB) exhibits much higher theoretical energy density compared with current intercalation electrode-based lithium-ion batteries (LiBs) and possesses excellent safety originated from the less flammable electrolyte. However, a small sulfur loading and limited utilization of active material hamper its practical a...

Analysed current trends in development of garnet-type structured Li 7 La 3 Zr 2 O 12 -based oxides as solid electrolytes for next-generation all-solid-state lithium batteries.

The infiltration technique is a cost-effective method to develop nanostructured electrodes that can accelerate sluggish oxygen reduction reaction (ORR) and enhance the electrochemical performance of solid oxide fuel cells (SOFCs) at intermediate temperatures (600–800 °C). For metal-supported SOFCs, identifying a highly efficient ORR catalyst is an...

Ceramic solid electrolytes are promising candidates for advanced solid-state batteries (SSBs) owing to their good ionic conductivity, wide electrochemical stability window, excellent thermal stability and enhanced safety compared to organic liquid electrolytes. In this study, we developed a series of sodium samarium silicates via a conventional sol...

In pursuing advanced clean energy storage technologies, all-solid-state Li metal batteries (ASSMBs) emerge as promising alternatives to conventional organic liquid electrolyte-based batteries due to their reduced flammability risks, increased energy densities, extended lifespan, and design flexibility. Here, we estimate lithium requirements per uni...

Solid oxide fuel cells (SOFCs) are recognized as a clean energy source that, unlike internal combustion engines, produces no CO2 during operation when H2 is used as a fuel. They use a highly efficient chemical-to-electrical energy conversion process to convert oxygen and hydrogen into electricity and water. They can provide smaller-scale power for...

Li metal batteries with garnet‐type solid electrolytes have the potential to increase specific energy and power densities of current Li‐ion batteries. Li metal batteries have been hampered by the poor wettability of solid electrolyte with elemental lithium. Here, to resolve the solid garnet electrolyte/Li interface issue, a scalable, cost‐effective...

Sodium-ion batteries (SIBs) represent a promising alternative to commercially prevalent Lithium-ion batteries (LIBs), primarily attributed to the economic feasibility and widespread availability of sodium resources. Solid-State Sodium Batteries (SSSBs) have garnered significant attention owing to their capacity to mitigate safety risks associated w...

Renewable energy sources are intermittent and thus require provision to store the energy when available using energy storage devices. These energy storage devices should be safe, efficient, and have a long life cycle for use in grid-scale energy storage systems. Lead-acid, Li-ion, and Redox Flow Batteries (RFBs) are examples of such energy storage...

Development and application of large‐scale energy storage systems are surging due to the increasing proportion of intermittent renewable energy sources in the global energy mix. Redox flow batteries are prime candidates for large‐scale energy storage due to their modular design and scalability, flexible operation, and ability to decouple energy and...

Garnet‐type Li7La3Zr2O12 electrolytes have garnered significant attention as promising solid‐state electrolyte candidates in all‐solid‐state lithium batteries (ASSLBs). However, its susceptibility to forming Li2CO3 upon atmospheric exposure leads to performance degradation, limiting its application. This study introduces a co‐doping strategy of Mg...

Sodium-ion hybrid capacitors (Na-HCs) often experience limited rate capabilities due to the inherent challenges of hard carbon anodes, such as sloped discharge profiles and poor kinetics. Despite this, the effectiveness of hard carbon for sodium plating opens opportunities beyond its conventional use. Leveraging this property, we explore hard carbo...

Recent advancements in wearable, flexible, and portable electronics have stimulated a swift increase in demand for compatible energy storage devices with promising performance. Supercapacitors offer the potential to satisfy the demands for complicated design and integrated functionality due to their highly adaptable manufacturing process. This chap...

Flexible, scalable, and low‐cost energy storage solutions are required for the widespread use of renewable energy and the mitigation of climate change. State‐of‐the‐art lithium‐ion batteries provide high specific energy density; however, designing a safe and cost‐effective grid‐scale lithium‐ion battery is still a major challenge. Redox flow batter...

Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3 onto various substrates without any thickness limitation, in this study, using density functional theory (DFT), we assessed the structural stability of a group of two-dimensional perovskite-type materials which we call perovskenes. Specifically, we analyzed the...

With the ever-growing energy storage demands for electrical grids, vanadium redox flow batteries, a stellar candidate, require continuous cost, cyclability, and energy density improvement. Vanadium redox flow batteries tend to lose vanadium from electrolyte solutions due to the precipitation of V2O5 during charging, resulting in a significant loss...

Perovskite-type metal oxides with a nominal chemical formula of Nd 1-x Ba x Co 0.8 Fe 0.2 O 3-δ (NBCF) (0 ≤ x ≤ 0.7) were prepared by solid-state synthesis method at 1300 °C in air. Powder X-ray diffraction showed that the x = 0.25 member is a single-phase perovskite-type Nd 0.75 Ba 0.25 Co 0.8 Fe 0.2 O 3-δ in the Pnma space group and all other mem...

In the 21st century, proton exchange membrane fuel cells (PEMFCs) represent a promising source of power generation due to their high efficiency compared with coal combustion engines and eco-friendly design. Proton exchange membranes (PEMs), being the critical component of PEMFCs, determine their overall performance. Perfluorosulfonic acid (PFSA) ba...

Perovskite-type metal oxides with a nominal chemical formula of Nd 1-x Ba x Co 0.8 Fe 0.2 O 3-δ (NBCF) (0 ≤ x ≤ 0.7) were prepared by solid-state synthesis method at 1300 °C in air. All members were found to be multiphase. 4-probe DC chronopotentiometry measurements were performed on the sintered sample pellets. The x = 0.4 member reaches a maximum...

All‐solid‐state lithium batteries (ASSLBs) are prepared using garnet‐type solid electrolytes by quick liquid phase sintering (Q‐LPS) without applying high pressure during the sintering. The cathode layers are quickly sintered with a heating rate of 50–100 K min⁻¹ and a dwell time of 10 min. The battery performance is dramatically improved by simult...

Finding the optimum material with improved properties for a given application is challenging because data acquisition in materials science and chemistry is time consuming and expensive. Therefore, dealing with small datasets is a reality in chemistry, whether the data are obtained from synthesis or computational experiments. In this work, we propos...

The shuttle effects by lithium polysulfides (LiPSs) and the sluggish reaction kinetics are crucial obstacles in the commercialization of Li−S batteries. Hence, effectively trapping and promoting the conversion of LiPSs is of prime importance. However, the fundamental kinetics of the electrocatalytic charging and discharging of Li−S batteries have n...

Garnet Type Solid Electrolytes In article number 2203897, Venkataraman Thangadurai and co‐workers report the use of an AlCl3 Lewis acid and fluoroethylene carbonate dual additive based non‐aqueous liquid electrolyte stabilizing garnet solid‐liquid electrolyte interphase, towards improved durability and high critical current density for hybrid solid...

Perovskite-type Nd0.75Ba0.25Co0.8Fe0.2O3-δ (NBCF25) was prepared via solid-state synthesis method at 1300 °C in air. Powder X-ray diffraction showed the formation of a single-phase orthorhombic phase in the Pnma space group. It showed minor reactivity with Sr and Mg-co-doped lanthanum gallate (LSGM) when sintered with 30 wt.% LSGM at 1050 °C. 4-pro...

All solid‐state sodium batteries (ASSSBs) are considered a promising alternative to lithium‐ion batteries due to increased safety in employing solid‐state components and the widespread availability and low cost of sodium. As one of the indispensable components in the battery system, organic liquid electrolytes are the currently used electrolytes du...

The hybrid solid‐liquid electrolyte concept is one of the best approaches for counteracting the interface problems between solid electrolytes and Li anodes/cathodes. However, a solid‐liquid electrolyte layer forming at the interfaces degrades battery capacity and power during a longer cycle due to highly reactive chemical and electrochemical reacti...

Sodium gadolinium silicate solid electrolyte showed an outstanding sodium plating/stripping performance for 1000 cycles that proves excellent interfacial contact between the sodium anode and solid electrolyte.

These days, Li-S battery has been arisen as one of the key energy storage technologies due to its high theoretical energy density compared to conventional lithium and sodium ion-based batteries. The present Li-S batteries suffer due to Li dendrite formation and capacity decay due to polysulfide dissolution effect, due to organic electrolytes used i...

These days, Li metal anode-based battery has been arisen as one of the key energy storage technologies due to its high theoretical energy density compared to conventional lithium and sodium ion-based batteries. The present Li-S batteries suffer due to Li dendrite formation and capacity decay due to polysulfide dissolution effect, because of organic...

All solid-state Li batteries are foreseen as the future state of battery technology due to their safety, high energy density, and high potential window as compared to the present organic liquid electrolyte batteries. Li-ion conducting garnet-type electrolytes have received considerable research interests due to their compatibility with Li metal ano...

The increasing demand to decarbonize the power grid is driving the development of low cost, sustainable and stable energy storage media. Redox flow batteries (RFB) have always been a strong candidate owing to their easy scalability, long cycle life and versatility. Modular design of RFB’s allows better control on energy and power density and many c...

Development of solid inorganic lithium (Li) ion conducting materials for the use as solid electrolytes is indispensable for the realization of next-generation all-solid-state Li batteries with high safety and reliability. Among various oxide-based solid electrolyte materials, a garnet-type oxide with the formula of Li 7 La 3 Zr 2 O 12 (LLZO) has at...

As the world works to move away from traditional energy sources, effective efficient energy storage devices have become a key factor for success. The emergence of unconventional electrochemical energy storage devices, including hybrid batteries, hybrid redox flow cells and bacterial batteries, is part of the solution. These alternative electrochemi...

Improving the energy and power densities of sodium-ion batteries is a prime challenge to establish this energy storage technology to be on par with state-of-the-art lithium-ion batteries. The energy density of the sodium-ion batteries is limited due to the lower redox potential of their electrode materials compared to that of the corresponding Li a...

A hybrid Li-ion capacitor represents an emerging class of devices, which results from the coupling of high-energy-density battery-type electrode materials at one side and high-power EDLC electrode at other side. Here, we develop a simple and scalable method including ball-milling, followed by a heating process to synthesize MoS2/graphene composite...

Solid-state lithium-metal batteries (SS-LMBs) suffer from the very high resistance at the garnet electrolyte/cathode interface that hampers their commercialization. Herein, a carbonate-based liquid electrolyte (LE) is introduced at the interface of a Li6.5La2.9Ba0.1Zr1.4Ta0.6O12 (LLBZTO) garnet/LiNi0.6Mn0.2Co0.2O2 (NMC 622) cathode to lower the int...

Lithium–sulfur batteries are regarded as the imminent energy storage device for high energy density applications. However, at practical sulfur loadings >5 mg cm⁻², the cell suffers from severe capacity fade and durability. In the present work, a hybrid MoS2–WS2 heterodimensional structure is reported. The strain induced growth of transition metal d...

We dedicate this paper to Prof. John B. Goodenough's 100th birthday, who has made several seminal contributions to the modern electrochemical energy storage and conversion technologies that made significant social and economic impacts on humankind. This review paper reports two battery systems that he contributed in the early stage of solid-state i...

Solid-state sodium-ion batteries (ss-SIBs) are a promising alternative to commercially available lithium-ion batteries (LIBs) for next-generation energy storage applications. They have lower production costs and are safer than LIBs. Moreover, sodium is more abundant than lithium. The incorporation of solid polymer electrolytes (SPEs) into SIBs has...

The success of rechargeable lithium-ion batteries (LIBs) has brought evident convenience to human society, but state-of-the-art LIBs with a graphite anode are approaching their energy density limits. Li metal is considered the ultimate anode material due to its ultra-high theoretical specific capacity of 3860 mAh g ⁻¹ , which is more than 10 times...

Current lithium-ion batteries (LIBs) are approaching their energy density limits and thus may not keep up with the ever-increasing demand for higher specific energy density in today’s energy storage and power applications. Anode-free lithium metal batteries (AFLMBs) utilize the full theoretical capacity of Li metal anode (3860 mAh g ⁻¹ , ten times...

Solid-state sodium-ion batteries (ss-SIBs) are a promising alternative to commercially available lithium-ion batteries for next-generation energy storage applications due to the abundance and cost-effectiveness of sodium over lithium. Herein, using a facile solution casting process, a high sodium-ion conductive, filler-less composite solid polymer...

Widespread commercialization of high‐energy‐density lithium–sulfur (Li–S) batteries is difficult due to the lithium polysulfide, Li2Sn (n = 4, 6, 8), shuttle effect. Efficient adsorption/conversion of Li2Sn species on an electrocatalytic surface can suppress the shuttle effect. Modeling of the adsorption of Li2Sn species using density functional th...

Current lithium-ion batteries have been widely used in portable electronic devices, electric vehicles, and peak power demand. However, the organic liquid electrolytes used in the lithium-ion battery are flammable and not stable in contact with elemental lithium and at a higher voltage. To eliminate the safety and instability issues, solid-state (ce...

A new strategy is presented to immobilize the lithium polysulfides (LiPSs) and promote charge transfer kinetics at the sulfur electrode interface of lithium-sulfur (Li–S) batteries. In this work, biomass-derived porous carbonized pine (p-Cp), abundantly available in Canada, is used as the carbon host for S electrode in the Li–S batteries. A multifu...

As a highly efficient clean power generation technology, intermediate temperature (600-800 °C) solid oxide fuel cells (IT-SOFCs) have gained much interest due to their rapid start-up and shut-down capability, longer life-time and lower cost compared to the conventional SOFCs. However, the sluggish oxygen reduction reaction (ORR) at the cathode at l...

Electrochemical synthesis of hydrogen peroxide (H2O2) via a two‐electron (2e–) oxygen reduction reaction (ORR) has emerged as a sustainable synthesis route compared to the anthraquinone oxidation synthesis process. Ba0.5Sr0.5Fe(1‐x)CuxO3‐δ perovskite is a particularly interesting electrocatalyst for ORR applications owing to its doping flexibility....

The goal of the current work was to identify an air-side-optimized contact material for La0.3Ca0.7Fe0.7Cr0.3O3−δ (LCFCr) electrodes and a Crofer22APU interconnect for use in reversible solid oxide fuel cells (RSOFCs). LaNi0.6Co0.4−xFexO3 (x = 0–0.3) perovskite-type oxides were investigated in this work. The partial substitution of Co by Fe decrease...

The developed nano-engineered NSPC membranes exhibit high flexibility, good electrochemical stability, high thermal endurance, and high mechanical strength, making them a promising choice for solid-state lithium batteries.

This chapter aims to provide a systematic overview of the current state of the research in the field of solid-state electrolytes for all-solid-state Li batteries. The desired functional properties and ion transport mechanism of solid-state electrolytes are explained, followed by a detailed survey on the existing understanding of the metal oxides, s...

Among the alkaline earth-based perovskite oxides, the Ba-based perovskites have superior chemical stability and tunable electrical/catalytic property via chemical substitution/doping. One of the best-known examples is Ba3Ca1.18Nb1.82O8.73 as ceramic proton...

Rechargeable Li batteries are promising candidates for next-generation energy storage devices due to their high energy density. Electrolyte compositions profoundly impact their electrochemical performance. The carbonate-based electrolytes employed in conventional Li-ion batteries (LIBs) are highly corrosive to elemental Li. Glyme-based electrolytes...

Perovskite-type structured BaMg0.33Nb0.67O3 (BMN) and Co-doped BMNCs, BaMg0.33Nb0.67-xCoxO3-δ (x = 0.12, 0.17, 0.24, and 0.34), were prepared by the conventional solid-state method at 1350 °C in air. The role of Co-substitution on BMNCs was critical to achieve high chemical stability at elevated temperature since it helped make the material denser...

Fundamental understanding of mass transport in solids as a function of temperature is crucial to applications in various all-solid-state ionic devices, including fuel cells, sensors, and batteries. Commonly, electrical properties have been investigated at various temperatures and the activation energy computed from the slope of the Arrhenius plot....

Quinary and senary non-stoichiometric double perovskites such as Ba2Ca0.66Nb1.34-xFexO6-δ (BCNF) have been utilized for gas sensing, solid oxide fuel cells and thermochemical CO2 reduction. Herein, we examined their potential as narrow bandgap semiconductors for use in solar energy harvesting. A cobalt co-doped BCNF, Ba2Ca0.66Nb0.68Fe0.33Co0.33O6-δ...

A conventional solid-state sintering method was used to prepare double perovskite structured compounds BCN (Ba2Ca0.67Nb1.33O6), BCNCo (Ba2Ca0.67Nb1.33-xCoxO6-δ) and BCNCoFe (Ba2Ca0.67Nb0.67Co0.66-yFeyO6-δ), which exhibit significant chemical stability in nitrogen, air, and 2 % CO2 (balanced by nitrogen). SEM images show that the Co dopant causes a...

Here, we demonstrate that altering the cell configuration can increase the compression level inside a coin cell, resulting in superior charge and discharge cycle performance. A normal anode-free coin cell’s capacity drops to zero within 20 cycles, while the more compressed cell retains 150 mAh g ⁻¹ at the 20th cycle, which is 87.3% of the first cyc...

The economic feasibility of electrocatalytic carbon dioxide reduction reaction (CO 2 RR) relies on the development of highly selective and efficient catalysts operating at a high current density. Herein, we explore a ligand engineering strategy involving the use of metal-organic frameworks (MOFs) and combining the desirable features of homogeneous...

Correction for ‘An auxiliary electrode mediated membrane-free redox electrochemical cell for energy storage’ by Senthil Velan Venkatesan et al. , Sustainable Energy Fuels , 2020, 4 , 2149–2152, DOI: 10.1039/c9se00734b.

In this study, we investigated the effect of postannealing on the properties of a garnet-type Ta-doped Li6.55La3Zr1.55Ta0.45O12 (Ta-LLZO) ceramic solid electrolyte degraded by lithium (Li) dendrite penetration during electrochemical Li plating and stripping testing in a Li/Ta-LLZO/Li symmetric cell. After the electrochemical testing in the symmetri...

Bivalent cations (M = Ni2+, Co2+, Mg2+) with different doping contents (x = 0.1, 0.2, 0.3, 0.4, 0.5) were incorporated for vanadium in the Na3+xV2-xMx(PO4)3 (NVP), yielded enhanced rate performance and capacity retention. Successful doping of these cations in the NVP structure was confirmed by powder X-ray diffraction (PXRD), vibrational FT-IR spec...

Garnet-type solid Li ion conductor Li7La3Zr2O12 (LLZO) has received considerable attention due to its high total (bulk + grain boundary) ionic conductivity at room temperature and its chemical stability with Li metal. To improve the ionic conductivity of LLZO, the hetrovalent doping at Zr-site and Al-doping at Li site was done for the optimization...

Chemical stability of garnet-type lithium ion conductors is one of the critical issues in their application in all-solid-state batteries. Here, we conducted quantitative analysis of impurity layers on the garnet-type solid electrolytes, Li6.5La3-xAE x Zr1.5-xTa0.5+xO12 (x = 0 and 0.1; AE = Ca, Sr, and Ba), by means of X-ray photoelectron spectrosco...

In this study, effect of Ca-doping on electrical and electrochemical properties of garnet structure Y3-xCaxFe5O12-δ (x = 0, 0.05, 0.1, 0.3, 0.5 and 0.7) was investigated. Cubic-phase (Ia-3d) garnet was prepared through sol-gel method and final sintered at 1100 °C for 2 h in air. Highest oxygen non-stoichiometry (δ = 0.19) was found in x = 0.3 membe...

Renewable energy sources are forecasted to supply half of the global energy demand in the future. Development of improved and cost-effective energy storage methods are in high demand due to the intermittency and locally distributed nature of renewable energy sources [1]. Redox flow battery (RFB) is a candidate technology for large-scale energy stor...