An Amphiphilic Molecule Induced Anion-Enrichment Interface for Next-Generation Lithium Metal Batteries.

The electrolyte engineering enables the fabrication of robust electrode/electrolyte interphase with excellent electrochemical stability for reliable lithium (Li) metal batteries (LMBs). Herein, an amphiphilic molecule nonafluoro-1-butanesulfonate (NFSA) is employed in electrolytes to realize anion-enrichment interfacial design. The functions of such an amphiphilic molecule in the electrolyte and anode/electrolyte interphases of LMBs are elucidated via theoretical and experimental analyses.

Phosphorous and Nitrogen Dual-Doped Carbon as a Highly Efficient Electrocatalyst for Sodium-Oxygen Batteries.

Sodium-oxygen batteries have been regarded as promising energy storage devices due to their low overpotential and high energy density. Its applications, however, still face formidable challenges due to the lack of understanding about the influence of electrocatalysts on the discharge products. Here, a phosphorous and nitrogen dual-doped carbon (PNDC) based cathode is synthesized to increase the electrocatalytic activity and to stabilize the NaO superoxide nanoparticle discharge products, leading to enhanced cycling stability when compared to the nitrogen-doped carbon (NDC).

2D MXene/MBene Superlattice with Narrow Bandgap as Superior Electrocatalyst for High-Performance Lithium-Oxygen Battery.

Lithium-oxygen (Li-O) battery with large theoretical energy density (≈3500 Wh kg) is one of the most promising energy storage and conversion systems. However, the slow kinetics of oxygen electrode reactions inhibit the practical application of Li-O battery. Thus, designing efficient electrocatalysts is crucial to improve battery performance.

Energy level regulation of anions hydrogen bond effects to construct a stable solid electrolyte interface for a high-stability lithium metal anode.

An intermolecular hydrogen bond between 2,5-dihydroxyterephthalic acid and the anions in the Li solvation shell is constructed to promote the formation of a LiF-rich SEI on a metallic Li electrode. Li metal batteries with improved cyclability (140 cycles under an N/P ratio of 4.9) and high capacity retention (90%) are eventually obtained.

Controllable Regulation of the Oxygen Redox Process in Lithium-Oxygen Batteries by High-Configuration-Entropy Spinel with an Asymmetric Octahedral Structure.

Designing bifunctional electrocatalysts to boost oxygen redox reactions is critical for high-performance lithium-oxygen batteries (LOBs). In this work, high-entropy spinel (CoMnNiFeCr)O (HEOS) is fabricated by modulating the internal configuration entropy of spinel and studied as the oxygen electrode catalyst in LOBs. Under the high-entropy atomic environment, the Co-O octahedron in spinel undergoes asymmetric deformation, and the reconfiguration of the electron structure around the Co sites leads to the upward shift of the d-orbital centers of the Co sites toward the Fermi level, which is conducive to the strong adsorption of redox intermediate LiO on the surface of the HEOS, ultimately forming a layer of a highly dispersed LiO thin film.

Structure and Charge Regulation Strategy Enabling Superior Cycling Stability of Ni-Rich Cathode Materials.

Ni-rich layered oxides LiNiCoMnO (NCMs, > 0.8) are the most promising cathode candidates for Li-ion batteries because of their superior specific capacity and cost affordability. Unfortunately, NCMs suffer from a series of formidable challenges such as structural instability and incompatibility with commonly used electrolytes, which seriously hamper their practical applications on a large scale.

Adjusting Li Solvation Structures via Dipole-Dipole Interaction to Construct Inorganic-Rich Interphase for High-Performance Li Metal Batteries.

Practical applications of lithium metal batteries are limited by unstable solid electrolyte interphase (SEI) and uncontrollable dendrite Li deposition. Regulating the solvation structure of Li via modifying electrolyte components enables optimizing the structure of the SEI and realizing dendrite-free Li deposition. In this work, it is found that the ionic-dipole interactions between the electron-deficient B atoms in lithium oxalyldifluoro borate (LiDFOB) and the O atoms in the DME solvent molecule can weaken the interaction between the DME molecule and Li, accelerating the desolvation of Li.

Bimetallic MXene with tailored vanadium d-band as highly efficient electrocatalyst for reversible lithium-oxygen battery.

Lithium-oxygen (Li-O) battery possesses high theoretical energy density of ∼ 3500 Wh kg, yet the sluggish kinetics of oxygen redox reactions hinder its practical application. Herein, TiVC bimetallic MXene solid solution is prepared as the efficient electrocatalyst for Li-O battery. The results of experiment and theoretical calculations reveal that through the formation of Ti-C-V bond in TiVC, electrons transfer from V site to Ti site enhances electron delocalization of V sites, which causes the upshift of d band center of V site and strengthens the adsorption of intermediate products (LiO) on TiVC electrode surface.

Prediction of a planar BP monolayer with inherent metallicity and its potential as an anode material for Na and K-ion batteries: a first-principles study.

Borophene, the lightest two-dimensional material, exhibits exceptional storage capacity as an anode material for sodium-ion batteries (NIBs) and potassium-ion batteries (PIBs). However, the pronounced surface activity gives rise to strong interfacial bonding between borophene and the metal substrate it grows on. Incorporation of heterogeneous atoms capable of forming strong bonds with boron to increase borophene stability while preserving its intrinsic metallic conductivity and high theoretical capacity remains a great challenge.

Adjusting the 3d Orbital Occupation of Ti in Ti C MXene via Nitrogen Doping to Boost Oxygen Electrode Reactions in Li-O Battery.

Rationally designing efficient catalysts is the key to promote the kinetics of oxygen electrode reactions in lithium-oxygen (Li-O ) battery. Herein, nitrogen-doped Ti C MXene prepared via hydrothermal method (N-Ti C (H)) is studied as the efficient Li-O battery catalyst. The nitrogen doping increases the disorder degree of N-Ti C (H) and provides abundant active sites, which is conducive to the uniform formation and decomposition of discharge product Li O .

Surface-Preferred Crystal Plane Growth Enabled by Underpotential Deposited Monolayer toward Dendrite-Free Zinc Anode.

Aqueous Zn batteries with ideal energy density and absolute safety are deemed the most promising candidates for next-generation energy storage systems. Nevertheless, stubborn dendrite formation and notorious parasitic reactions on the Zn metal anode have significantly compromised the Coulombic efficiency (CE) and cycling stability, severely impeding the Zn metal batteries from being deployed in the proposed applications. Herein, instead of random growth of Zn dendrites, a guided preferential growth of planar Zn layers is accomplished via atomic-scale matching of the surface lattice between the hexagonal close-packed (hcp) Zn(002) and face-centered cubic (fcc) Cu(100) crystal planes, as well as underpotential deposition (UPD)-enabled zincophilicity.

A multifunctional protective layer with biomimetic ionic channel suppressing dendrite and side reactions on zinc metal anodes.

A multifunctional graphitic carbon nitride (GCN) protective layer with bionic ion channels and high stability is prepared to inhibit dendrite growth and side reactions on zinc (Zn) metal anodes. The high electronegativity of the nitrogen-containing organic groups (NOGs) in the GCN layer can effectively promote the dissociation of solvated Zn and its rapid transportation in bionic ion channels via a hopping mechanism. In addition, this GCN layer exhibits excellent mechanical strength to suppress the growth of Zn dendrites and the volume expansion of Zn metal anodes during the plating process.

Interfacial Electron Redistribution of Hydrangea-like NiO@Ni P Heterogeneous Microspheres with Dual-Phase Synergy for High-Performance Lithium-Oxygen Battery.

Lithium-oxygen batteries (LOBs) with ultra-high theoretical energy density (≈3500 Wh kg ) are considered as the most promising energy storage systems. However, the sluggish kinetics during the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) can induce large voltage hysteresis, inferior roundtrip efficiency and unsatisfactory cyclic stability. Herein, hydrangea-like NiO@Ni P heterogeneous microspheres are elaborately designed as high-efficiency oxygen electrodes for LOBs.

Synergy of cobalt vacancies and iron doping in cobalt selenide to promote oxygen electrode reactions in lithium-oxygen batteries.

Electronic structural engineering plays a key role in the design of high-efficiency catalysts. Here, to achieve optimal electronic states, introduction of exotic Fe dopant and Co vacancy into CoSe nanosheet (denoted as Fe-CoSe-V) is presented. The obtained Fe-CoSe-V demonstrates excellent catalytic activity as compared to CoSe.

Boosted Li transference number enabled interfacial engineering for dendrite-free lithium metal anodes.

Adverse dendritic growth destabilizes Li metal anodes (LMAs), dramatically limiting the commercial applications of Li metal batteries (LMBs). Herein, ZIF-67 with unsaturated coordinative metal sites is used to construct a protective coating to immobilize anions, which is capable of increasing the Li transference number () to mitigate the electrolyte concentration gradient in the vicinity of LMAs. In addition, the ZIF-67-based layer provides highly ordered ionic diffusion pathways, thus enabling dendrite-free Li deposition.

Rationalizing Surface Electronic Configuration of Ni-Fe LDO by Introducing Cationic Nickel Vacancies as Highly Efficient Electrocatalysts for Lithium-Oxygen Batteries.

Cationic defect engineering is an effective strategy to optimize the electronic structure of active sites and boost the oxygen electrode reactions in lithium-oxygen batteries (LOBs). Herein, Ni-Fe layered double oxides enriched with cationic nickel vacancies (Ni-Fe LDO-V ) are first designed and studied as the electrocatalysts for LOBs. Based on the density functional theory calculation, the existence of nickel vacancy in Ni-Fe LDO-V significantly improves its intrinsic affinity toward intermediates, thereby fundamentally optimizing the formation and decomposition pathway of Li O .

Synergistic Effect of Microstructure Engineering and Local Crystal Structure Tuning to Improve the Cycling Stability of Ni-Rich Cathodes.

Ultrahigh Ni-rich layered oxides have been regarded as one of the most promising cathode candidates. However, cycling instability induced by interfacial reactions and irreversible H2-H3 lattice distortion is yet to be demonstrated by an effective strategy that could construct a stable grain interface and microstructure. Here, Ni-rich cathode LiNiCoMnO is modified by B and Ti to realize the synchronous regulation of a microstructure and the oxygen framework robustness.

Adjusting the d-band center of metallic sites in NiFe-based Bimetal-organic frameworks via tensile strain to achieve High-performance oxygen electrode catalysts for Lithium-oxygen batteries.

Developing effective electrocatalyst and fundamentally understanding the corresponding working mechanism are both urgently desired to overcome the current challenges facing lithium-oxygen batteries (LOBs). Herein, a series of NiFe-based bimetal-organic frameworks (NiFe-MOFs) with certain internal tensile strain are fabricated via a simple organic linker scission strategy, and served as cathode catalysts for LOBs. The introduced tensile strain broadens the inherent interatomic distances, leading to an upshifted d-band center of metallic sites and thus the enhancement of the adsorption strength of catalysts surface towards intermediates, which is contributed to rationally regulate the crystallinity of discharge product LiO.

Two-Dimensional Boron-Rich Monolayer BN as High Capacity for Lithium-Ion Batteries: A First-Principles Study.

Owing to lightweight, abundant reserves, low cost, and nontoxicity, B-based two-dimensional (2D) materials, e.g., borophene, exhibit great potential as new anode materials with higher energy density for Li-ion batteries (LIBs).

Adjusting the Covalency of Metal-Oxygen Bonds in LaCoO by Sr and Fe Cation Codoping to Achieve Highly Efficient Electrocatalysts for Aprotic Lithium-Oxygen Batteries.

Developing high-efficiency dual-functional catalysts to promote oxygen electrode reactions is critical for achieving high-performance aprotic lithium-oxygen (Li-O) batteries. Herein, Sr and Fe cation-codoped LaCoO perovskite (LaSrCoFeO, LSCFO) porous nanoparticles are fabricated as promising electrocatalysts for Li-O cells. The results demonstrate that the LSCFO-based Li-O batteries exhibit an extremely low overpotential of 0.

Surface atomic modulation of CoP bifunctional catalyst for high performance Li-O battery enabled by high-index (211) facets.

The rational design of the surface structure and morphology characteristics of the catalyst at atomic level are the key to improve the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) in lithium-oxygen (Li-O) battery. Here a series of cobalt phosphide (CoP) electrocatalysts with a variety of index facets are successfully prepared including concave polyhedrons CoP exposing with (211) crystal planes (CoP CPHs) spherical nanoparticles CoP exposed with (011) crystal planes and polyhedron particles CoP exposing with (011) and (111) crystal planes. The results show that CoP CPHs based Li-O battery presents a large discharge capacity of 33743 mA h g at current density of 50 mA g and a remarkable long cycle life of up to 950 h.

Rationalizing the Effect of Oxygen Vacancy on Oxygen Electrocatalysis in Li-O Battery.

Albeit the effectiveness of surface oxygen vacancy in improving oxygen redox reactions in Li-O battery, the underpinning reason behind this improvement remains ambiguous. Herein, the concentration of oxygen vacancy in spinel NiCo O is first regulated via magnetron sputtering and its relationship with catalytic activity is comprehensively studied in Li-O battery based on experiment and density functional theory (DFT) calculation. The positive effect posed by oxygen vacancy originates from the up shifted antibond orbital relative to Fermi level (E ), which provides extra electronic state around E , eventually enhancing oxygen adsorption and charge transfer during oxygen redox reactions.