Conductivity Of Electrolyte Research Articles

Asymmetric ionogel electrolyte with an ultrathin metal–organic framework layer for lithium dendrite inhibition in solid-state lithium-metal batteries

Solid-state electrolytes (SSEs) are used to prevent internal short circuits caused by the growth of lithium dendrites in solid-state lithium-metal batteries (SSLMBs). Ionogel electrolytes are new polymeric SSEs with outstanding processability, excellent flexibility, and superior ionic conductivity. Lithium-ion transport in ionogel electrolytes depends on ionic liquid (IL) content; however, increasing the IL content improves ionic conductivity but sharply decreases mechanical properties, thus limiting the ability to resist lithium dendrites. Thus, ionogel electrolytes must strike a balance between ionic conductivity and mechanical properties. Herein, we adopt a new strategy to suppress the growth of lithium dendrites by in situ polymerizing an ultrathin metal–organic framework (MOF) layer (9.8 μm) onto a highly ionic conductive ionogel electrolyte. The ionogel electrolyte provides an asymmetric SSE (ASSE) with a remarkable ionic conductivity of 4.8 × 10−4 S cm−1 (30 °C), whereas the ultrathin MOF layer regulates uniform dissolution/deposition of lithium and inhibits lithium dendrite growth, thereby increasing critical current density of the ASSE to 0.65 mA cm−2. An SSLMB assembled with the ASSE and LiFePO4 exhibits excellent performance and cycling stability, maintaining a specific capacity of 125.4 mAh g−1 after 500 cycles at 0.3C.

ARGET-ATRP-Mediated Grafting of Bifunctional Polymers onto Silica Nanoparticles Fillers for Boosting the Performance of High-Capacity All-Solid-State Lithium-Sulfur Batteries with Polymer Solid Electrolytes.

The shuttle effect in lithium-sulfur batteries, which leads to rapid capacity decay, can be effectively suppressed by solid polymer electrolytes. However, the lithium-ion conductivity of polyethylene oxide-based solid electrolytes is relatively low, resulting in low reversible capacity and poor cycling stability of the batteries. In this study, we employed the activator generated through electron transfer atom transfer radical polymerization to graft modify the surface of silica nanoparticles with a bifunctional monomer, 2-acrylamide-2-methylpropanesulfonate, which possesses sulfonic acid groups with low dissociation energy for facilitating Li+ migration and transfer, as well as amide groups capable of forming hydrogen bonds with polyethylene oxide chains. Subsequently, the modified nanoparticles were blended with polyethylene oxide to prepare a solid polymer electrolyte with low crystallinity and high ion conductivity. The resulting electrolyte demonstrated excellent and stable electrochemical performance, with a discharge-specific capacity maintained at 875.2 mAh g-1 after 200 cycles.

Revealing the effect of double bond-modified Li6.75La3Zr1.75Ta0.25O12 on the Li-ion conduction of composite solid electrolytes

Lithium metal batteries with polyethylene oxide (PEO) electrolytes have shown great potential to be one of the next-generation energy candidates. As the branch family of PEO electrolytes, poly(ethylene glycol) acrylates (PEGAs) attract more attention owing to their better electrochemical properties than that of PEO electrolytes. Introducing double bond-modified Li6.75La3Zr1.75Ta0.25O12 fillers (KH@LLZTO) has been a popular method to improve the electrochemical properties of PEGAs electrolytes due to the homogeneous dispersion of LLZTO. However, in this work, an inverse phenomenon is discovered. The electrochemical properties of PEGAs electrolytes get worse when introducing KH@LLZTO. By exploring the Li+ transport mechanism, the reason for the inverse phenomenon is revealed. More importantly, the design principle of PEGAs electrolytes with fast ionic conductor fillers is presented. Double bond-modified LLZTO can decrease the electrochemical properties of PEGAs electrolytes instead when there are low-molecular weight monomers that can participate in the PEGAs polymer network and interact with Li+, while the double bond-modified LLZTO can improve the electrochemical properties of PEGAs electrolytes when there are not aforementioned low-molecular weight monomers. This work provides a new understanding for componential design and optimization of PEGAs electrolytes with fast ionic conductors, hoping to promote the practical application of PEGAs electrolytes.

Ruthenium doping of NASICON electrolyte augments the performance of solid-state sodium-ion batteries

Recently remarkably high ionic conductivities (up to 5.5 x 10-3 Ω-1cm−1) at 25 °C have been achieved in sodium superionic conducting (NASICON) solid-state electrolytes via aliovalent cation doping. Doping in NASICON leverages the synergic effects of bottleneck opening (lattice expansion) and correlated migration (higher carrier concentration). However, there is no report published that isolates the effect of correlated migration induced by heterovalent doping without the influence of structural/bottleneck changes. Therefore, here we report for the first time the substitution of trivalent Ru3+ cation into the Zr4+ site to enhance the ionic conductivity of the NASICON electrolyte. Even though Ru3+ has a smaller ionic radius than Zr4+ and leads to bottleneck shrinkage, high ionic conductivity is achieved on doping Ru as compared to undoped NZSP. Using first-principles calculations, we show that even though the bottleneck for Na+ migration shrinks, the diffusion barriers are nearly the same owing to the weaker Na-framework interaction. The doped electrolyte showed an ionic conductivity of 2.1 x 10-3 Ω-1cm−1, an ionic transference number of ∼ 98.9 %, and exhibited stable sodium plating/stripping at 0.5 mA-cm−2 for 100 h with an overpotential of 20 mV owing to the fused microstructure. The assembled all-solid-state battery with Ru-doped electrolyte exhibited an outstanding initial capacity of 87 mAh-g−1 at 0.3C as compared to 70 mAh-g−1 with undoped electrolyte. Compared to the pristine sample, which had capacity retention of 60 % after 100 cycles, the cell containing Ru-doped electrolyte demonstrated stable cycling with an 87 % capacity retention without external pressure.

The interface modification with polyethyleneimine enhances both ionic conductivity and interfacial compatibility of composite solid electrolyte

The composite solid electrolyte (CSE), polyethylene oxide (PEO)-Li6.4La3Zr1.4Ta0.6O12 (LLZTO), is deemed a promising candidate for all-solid-state batteries. Nevertheless, due to the poor interfacial compatibility between LLZTO nanoparticles and PEO, achieving a homogeneous dispersion of LLZTO nanoparticles within PEO is not readily attainable. The aggregation of LLZTO within PEO leads to a decline in the ionic conductivity of the CSE and poor interface stability with the electrode, ultimately resulting in deteriorated battery cyclic performance. In this work, the interface between LLZTO and PEO is designed and comprehensively investigated. Initially, dopamine self-polymerization is employed to form a uniform coating layer on the surface of LLZTO nanoparticles. Subsequently, by utilizing the amino groups present in polyethyleneimine (PEI), which can react with the phenolic hydroxyl groups of dopamine and the ether linkages in PEO, PEI serves as a bridging agent, enhancing the interfacial compatibility between LLZTO and PEO. Here it is shown that, the ionic conductivity of the LLZTO-PEO CSE containing 40 wt% modified LLZTO increases from 6.14✕10−5 S cm−1 to 1.89✕10−4 S cm−1. Furthermore, this CSE exhibits improved thermal stability, an enlarged electrochemical window of 4.8 V, a lithium-ion transference number of 0.45, and excellent interface stability with the lithium anode. The assembled LiFePO4 | 40 wt% LLZTO@PDA@PEI-PEO CSE | Li all-solid-state battery demonstrates an initial discharge specific capacity of 151.8 mA h g−1 at 0.2 C, with a capacity retention of 85.8% after 200 cycles. This work provides a novel strategy for interface-modified polymer- inorganic composite solid electrolytes, which will advance the development of high-energy-density all-solid-state lithium batteries.

Phase-field simulation of magnesium-metal anode interface growth in different electrolytes during electrodeposition

Various types of Mg electrolytes have emerged with the deepening and development of research on Rechargeable Magnesium-Metal Batteries. In order to assess the potential of these electrolytes to inhibit the growth of Mg dendrites, we apply a Mg-electrodeposition phase-field model with surface energy anisotropy to simulate the interface growth processes of Mg-metal anodes in different electrolytes during electrodeposition. The results show that the conductivity and Mg-ion diffusivity of the Mg electrolyte are key factors affecting the interface growth, with the diffusivity having a particularly significant effect. In the designed 1.0 M MgX/THF electrolyte with an applied overpotential of −0.30 V, by profoundly analyzing the fluctuation of the interface contour, we find that when the diffusivity reaches 1.4 × 10−10 m2/s, the Mg-metal anode interface can achieve stable growth.

Changes in performance and thermal stability of Ni0.8Co0.1Al0.1/graphite batteries with excessive water

AbstractDuring the production process of lithium‐ion batteries, there exists a scenario of excessive water inside the battery due to poor water control in the factory environment. In addition, the battery housing may be damaged by corrosion, external vibration etc., which would cause water to enter the battery. To the best of the authors’ knowledge, there is little literature to reveal the influencing mechanism related to the above issue. The effects of excessive water on battery performance and safety were discussed. The results show that when the battery absorbs excessive water, the capacity decreases and the self‐discharging rate increases rapidly. The self‐heating temperature of the battery shows an increasing trend. The thermal runaway temperature decreases significantly with the time from self‐heating to thermal runaway dramatically shortened. The thermal stability of the battery deteriorates throughout the reaction process. This is mainly due to the mechanisms by which the water absorbed in the battery reacts with the electrolyte and the electrode material, resulting in the decrease of the electrolyte conductivity and the corrosion of the electrode material, as well as the thickening of the Solid Electrolyte Interface film and the accumulation of impurities. The findings are of positive significance in demonstrating the quantitative relationship between excessive water and the performance and safety of batteries. Also, it can add to the understanding of the complex scenarios of battery spontaneous failure, which is vital for solving battery self‐thermal runaways.

Ion Transport in Polymer Electrolytes: Building New Bridges between Experiment and Molecular Simulation.

ConspectusPolymer electrolytes constitute a promising type of material for solid-state batteries. However, one of the bottlenecks for their practical implementation lies in the transport properties, often including restricted Li+ self-diffusion and conductivity and low cationic transference numbers. This calls for a molecular understanding of ion transport in polymer electrolytes in which molecular dynamics (MD) simulation can provide both new physical insights and quantitative predictions. Although efforts have been made in this area and qualitative pictures have emerged, direct and quantitative comparisons between experiment and simulation remain challenging because of the lack of a unified theoretical framework to connect them.In our work, we show that by computing the glass transition temperature (Tg) of the model system and using the normalized inverse temperature 1000/(T - Tg + 50), the Li+ self-diffusion coefficient can be compared quantitatively between MD simulations and experiments. This allows us to disentangle the effects of Tg and the polymer dielectric environment on ion conduction in polymer electrolytes, giving rise to the identification of an optimal solvating environment for fast ion conduction.Unlike Li+ self-diffusion coefficients and ionic conductivity, the transference number, which describes the fraction of current carried by Li+ ions, depends on the boundary conditions or the reference frame (RF). This creates a non-negligible gap when comparing experiment and simulation because the fluxes in the experimental measurements and in the linear response theory used in MD simulation are defined in different RFs. We show that by employing the Onsager theory of ion transport and applying a proper RF transformation, a much better agreement between experiment and simulation can be achieved for the PEO-LiTFSI system. This further allows us to derive the theoretical expression for the Bruce-Vincent transference number in terms of the Onsager coefficients and make a direct comparison to experiments. Since the Bruce-Vincent method is widely used to extract transference numbers from experimental data, this opens the door to calibrating MD simulations via reproducing the Bruce-Vincent transference number and using MD simulations to predict the true transference number.In addition, we also address several open questions here such as the time-scale effects on the ion-pairing phenomenon, the consistency check between different types of experiments, the need for more accurate force fields used in MD simulations, and the extension to multicomponent systems. Overall, this Account focuses on building new bridges between experiment and simulation for quantitative comparison, warnings of pitfalls when comparing apples and oranges, and clarifying misconceptions. From a physical chemistry point of view, it connects to concentrated solution theory and provides a unified theoretical framework that can maximize the power of MD simulations. Therefore, this Account will be useful for the electrochemical energy storage community at large and set examples of how to approach experiments from theory and simulation (and vice versa).

Tuning the Electrolyte and Interphasial Chemistry for All-Climate Sodium-ion Batteries.

Sodium-ion batteries (SIBs) present a promising avenue for next-generation grid-scale energy storage. However, realizing all-climate SIBs operating across a wide temperature range remains a challenge due to the poor electrolyte conductivity and instable electrode interphases at extreme temperatures. Here, we propose a comprehensively balanced electrolyte by pairing carbonates with a low-freezing-point and low-polarity ethyl propionate solvent which enhances ion diffusion and Na+-desolvation kinetics at sub-zero temperatures. Furthermore, the electrolyte leverages a combinatorial borate- and nitrile-based additive strategy to facilitate uniform and inorganic-rich electrode interphases, ensuring excellent rate performance and cycle stability over a wide temperature range from -45 °C to 60 °C. Notably, the Na||sodium vanadyl phosphate cell delivers a remarkable capacity of 105 mAh g-1 with a high rate of 2 C at -25 °C. In addition, the cells exhibit excellent cycling stability over a wide temperature range, maintaining a high capacity retention of 84.7 % over 3,000 cycles at 60 °C and of 95.1 % at -25 °C over 500 cycles. The full cell also exhibits impressive cycling performance over a wide temperature range. This study highlights the critical role of electrolyte and interphase engineering for enabling SIBs that function optimally under diverse and extreme climatic environments.

Tuning the Electrolyte and Interphasial Chemistry for All‐Climate Sodium‐ion Batteries

AbstractSodium‐ion batteries (SIBs) present a promising avenue for next‐generation grid‐scale energy storage. However, realizing all‐climate SIBs operating across a wide temperature range remains a challenge due to the poor electrolyte conductivity and instable electrode interphases at extreme temperatures. Here, we propose a comprehensively balanced electrolyte by pairing carbonates with a low‐freezing‐point and low‐polarity ethyl propionate solvent which enhances ion diffusion and Na+‐desolvation kinetics at sub‐zero temperatures. Furthermore, the electrolyte leverages a combinatorial borate‐ and nitrile‐based additive strategy to facilitate uniform and inorganic‐rich electrode interphases, ensuring excellent rate performance and cycle stability over a wide temperature range from −45 °C to 60 °C. Notably, the Na||sodium vanadyl phosphate cell delivers a remarkable capacity of 105 mAh g−1 with a high rate of 2 C at −25 °C. In addition, the cells exhibit excellent cycling stability over a wide temperature range, maintaining a high capacity retention of 84.7 % over 3,000 cycles at 60 °C and of 95.1 % at −25 °C over 500 cycles. The full cell also exhibits impressive cycling performance over a wide temperature range. This study highlights the critical role of electrolyte and interphase engineering for enabling SIBs that function optimally under diverse and extreme climatic environments.

GO based nanocomposite hydrogel enabled high performance wearable all-solid supercapacitor based on hierarchical structure electrodes derived from ZIF-67

The flexible and wearable supercapacitors have attracted wide interest because of their widespread application in smart electronic devices with rapid charging and discharging. As an important part of supercapacitor, the electrode materials with a hollow structure, especially those with hierarchical structures that provide an array of continuous hollow cages, are considered promising. Because of its porous shell which is rich in redox reaction sites for supercapacitors. In this work, we fabricated a ZIF-67 derived hollow Co3O4 growth on the surface of 1D NiCo2O4 to assemble into a beaded structure. In this case, NiCo precursor acted as a structure-directing agent to grow a ZIF-67, a promising electroactive material of electrochemical capacitors to provide capacitance after calcination. Combined with the grapheneoxide (GO) based high conductivity hydrogel as the solid electrolyte, the capacitance of the flexible supercapacitor exhibited a high specific capacitance of 90F g−1 at 0.5 A/g, and it was sturdy and durable. There was no significant loss of capacitance while suffering from bending and pressing. The outstanding electrochemical properties of the all-solid supercapacitor can be attributed to the unique nanostructure of the electrode that created more reactive active sites, increased the diffusion pathway for electrolyte ions, along with the high conductivity of the hydrogel electrolyte.

Improved ionic conductivity and Li7P3S11 solid electrolyte based all-solid state batteries for practical applications

Improved ionic conductivity and Li7P3S11 solid electrolyte based all-solid state batteries for practical applications

Carboxylic bacterial cellulose fiber-based hydrogel electrolyte with imidazole-type ionic liquid for dendrite-free zinc metal batteries

Aqueous zinc metal batteries are regarded as the most promising energy storage system due to their advantages of high safety, low cost, and high theoretical capacity. However, the growth of dendrites and the occurrence of side reactions hinder the development of zinc metal batteries. Despite previous attempts to design advanced hydrogel electrolytes, achieving high mechanical performance and ionic conductivity of hydrogel electrolytes has remained challenging. In this work, a hydrogel electrolyte with an ionic crosslinked network is prepared by carboxylic bacterial cellulose fiber and imidazole-type ionic liquid, following by a covalent network of polyacrylamide. The hydrogel electrolyte possesses a superior ionic conductivity of 43.76 mS cm−1, leading to a Zn2+ migration number of 0.45, and high mechanical performance with an elastic modulus of 3.48 GPa and an elongation at breaking of 38.36%. More importantly, under the anion-coordination effect of the carboxyl group in bacterial cellulose and [BF4]− in imidazole-type ionic liquid, the solvation sheath of hydrated Zn2+ ions and the nucleation overpotential of Zn plating are regulated. The results of cycled testing show that the growth of zinc dendrites is effectively inhibited and the generation of irreversible by-products is reduced. With the carboxylic bacterial cellulose-based hydrogel electrolyte, the Zn||Zn symmetric batteries offer good cyclability as well as Zn||Ti batteries.

Insight into the effect of strain on Li-ion diffusivity and conductivity in Li3OCl anti-perovskite solid-state electrolyte: A perspective from AIMD simulations

Utilizing first-principle calculations, this study elucidated the underlying mechanism of elastic strains affecting the Li-ion diffusivity and conductivity in Li3OCl anti-perovskite solid-state electrolyte. Strain was shown to modulate the Li-ion vibrational amplitude, attempt frequency and adjacent site jumps, as revealed by ab initio molecular dynamics (AIMD) simulation post-processing. Additionally, analysis of lattice dynamics and phonon behavior under various strain conditions demonstrated that tensile strains soften the lattice and lower the phonon band center frequency, thereby diminishing the energy barriers impeding ion transport. Further, we have systematically investigated strain-induced distortions of the coordination environment via continuous symmetry measures (CSM), assessing the variations at initial and saddle sites along the Li-ion migration routes. And the study of bonding variability under strain provided a deeper understanding of strain-induced conducting behavior. These results underscore insights into the fundamental mechanisms governing ionic transport in Li3OCl anti-perovskite under elastic strain, highlighting the potential of strain engineering as a promising avenue for optimizing the performance of solid-state electrolytes in energy storage applications.

Transport properties of ethylene glycol functionalized membranes exposed to nonaqueous electrolytes

Non-aqueous redox flow batteries (RFBs) are a promising technology to meet growing demand for grid-scale energy storage. Membrane separators, designed specifically for use with organic solvents, are necessary to advance non-aqueous RFBs. Herein, we report the development of a series of poly(phenylene oxide) (PPO) membranes functionalized with poly(ethylene glycol) (PEG) side chains to investigate the influence of PEG side chain length and degree of PEGylation on membrane transport properties. Increasing the degree of PEGylation generally led to increases in electrolyte uptake, hydroxy TEMPO permeability, and ionic conductivity likely caused by an increase in overall PEG content, as opposed to specific interactions caused by changing the degree of PEGylation. For membranes with similar PEG content, increasing the length of the PEG side chain resulted in decreases in electrolyte uptake, permeability, and conductivity possibly due to differences in the solvation behavior of the PEG chains with different lengths.

A parametric study of crystal structure, phase stability, and conductivity of the novel phosphate-based composite electrolyte

A parametric study of crystal structure, phase stability, and conductivity of the novel phosphate-based composite electrolyte

In Situ Forming Na─Sn Alloy/Na2S Interface Layer for Ultrastable Solid State Sodium Batteries

AbstractThe poor interfacial compatibility between sodium superionic conductor (NASICON) electrolyte and metallic sodium anode will lead to severe dendrite penetration, impeding the application of NASICON electrolytes for solid state sodium batteries. Herein, a homogeneous SnS2 coating layer is sputtered on the surface of Na3.4Zn0.1Zr1.9Si2.2P0.8O12 electrolyte to in situ construct a kinetically stable Na─Sn alloy/Na2S interlayer, possessing superior Na affinity, low diffusion barrier, and electronic insulating character to suppress dendrite growth, which is confirmed by experiments and density‐functional theory calculations. Benefiting from the Na─Sn alloy/Na2S interphase, the critical current density of Na3.4Zn0.1Zr1.9Si2.2P0.8O12 increases from 2.4 to 9.4 mA cm−2. In addition, the obtained Na3V2(PO4)3/Na3.4Zn0.1Zr1.9Si2.2P0.8O12@SnS2/Na solid state batteries exhibit a high initial reversible discharge capacity of 115.1 mAh g−1 at 0.1 °C with an initial Coulombic efficiency of 93.6%, and a capacity retention rate of 88.1% after 1000 cycles at 1 C.

Zwitterionic Polymer Ionogel Electrolytes Supported by Coulombic Cross-Links: Impacts of Alkali Metal Cation Identity.

Zwitterionic (ZI) polymers enable the formation of noncovalent cross-links within ionic liquid electrolytes (ILEs) to create nonflammable, mechanically robust, and highly conductive ionogel electrolytes. In this study, ZI homopolymer poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] scaffolds are synthesized in situ within lithium and/or sodium salt-based ILEs to construct a series of ionogels that contain between 3 and 15 wt % poly(MPC). Room-temperature ionic conductivity values of these ionogels are found to vary between approximately 1.3 and 2.2 mS cm-1. For sodium only and 1:1 lithium/sodium equimolar mixed salt ionogels containing 6 wt % poly(MPC), the ionic conductivity is found to improve by 14% compared to the neat ILE due to the presence of the ZI scaffold. Moreover, comparing the elastic modulus values of lithium- versus sodium-containing ionogels revealed a difference of up to 1 order of magnitude [10.6 vs 111 kPa, respectively, for 3 wt % poly(MPC)]. Molecular dynamics simulations of ionogel precursor solutions corroborate the experimental results by demonstrating differences in the lithium/ZI monomer and sodium/ZI monomer cluster size distributions formed, which is hypothesized to influence the scaffold network cross-link density obtained upon photopolymerization. This work provides insights into why ZI polymer-supported ionogel properties that are relevant for the development of safer electrolytes for lithium-ion and sodium-ion batteries depend upon the chemical identity of the alkali metal cation.

In Situ Phase-Transformation Forming a Bicontinuous (Ni, Co, Ti, and Al)-Oxide/Li2CO3 Interpenetrating Network Electrolyte for Solid Oxide Fuel Cells.

Designing heterogeneous electrolytes with superior interface charge transfer is promising for low-temperature solid oxide fuel cells (LT-SOFCs). However, a rational construction with optimal interfaces to maximize ionic conduction remains a challenge. Here an in situ phase-transformation strategy is demonstrated to prepare a highly conductive heterogeneous electrolyte. A pristine LiNiO2-TiO2 nanocomposite precursor undergoes chemical reactions and phase-transformation upon heating and feeding H2, destroying the original phases, and forming new species, including an amorphous Li2CO3 scaffold within a (Ni, Co, Al, and Ti)-oxide (NCAT) matrix. It creates an intertwining and continuous network inside the electrolyte with plentiful interfaces. The in situ formed NCAT/Li2CO3 heterogeneous electrolyte displays superior ionic conductivity and impressive fuel cell performance. This work emphasizes the potential of rational heterogeneous structure design and interface engineering for LT-SOFC electrolyte through an in situ phase-transform approach. The generated interfaces enhance ion transport, presenting an opportunity for further optimizing electrolyte candidates, and lowering the operating temperatures of SOFCs.

Multicomponent doping realized superior triple-conducting within cobalt-free Ruddlesden-Popper-type perovskite for Proton-conducting fuel cells cathode

Proton-conducting solid oxide fuel cells (H-SOFCs) are appealing for low-to-intermediate temperature operation due to their intrinsic lower activation energy and better ionic conductivity. Unfortunately, there are currently few acceptable and high-performing cathode materials available for H-SOFCs. Herein, we present a novel high performance multicomponent Ruddlesden-Popper (RP) type cathode Pr3Ni1.5Cu0.3Nb0.05Ta0.05Zr0.05Y0.05O7-δ (PNCNTZY) with superior triple conducting property. The multicomponent co-doping of Nb, Ta, Zr, and Y brings about the enhancement of configurational entropy and cocktail effect for improving H+/O2-/e- triple conductivity and oxygen vacancy concentration. Naturally, the ORR activity is improved by facilitated charge transfer and oxygen surface exchange, exhibiting reduced polarization resistance to just 0.24 Ω cm2 at 550 °C. When used as the cathode in H-SOFC single cells, excellent power production is demonstrated at 550 °C, with a peak power density of up to 0.84 W cm-2. Furthermore, the PNCNTZY sample shows adequate thermal compatibility with proton conductor electrolytes BaZr0.1Ce0.7Y0.1Yb0.1O3-δ (BZCYYb) and then appropriate endurance durability (0.8 A cm-2 at 550 °C for about 250 h) due to their match of thermal expansion coefficient (TEC) brought about by the Co-free and partial replacement of larger-size elements. This extremely promising Co-free RP perovskite cathode for H-SOFCs produced by this work might provide a new type candidate and novel strategy for the commercialization of H-SOFCs.