Micro-Structure Engineering in Pd-InO Catalysts and Mechanism Studies for CO Hydrogenation to Methanol.

Significant interest has emerged for the application of Pd-InO catalysts as high-performance catalysts for CO hydrogenation to CHOH. However, precise active site control in these catalysts and understanding their reaction mechanisms remain major challenges. In this investigation, a series of Pd-InO catalysts were synthesized, revealing three distinct types of active sites: In-O, Pd-O(H)-In, and PdIn.

Catalytic role of in-situ formed C-N species for enhanced LiCO decomposition.

Sluggish kinetics of the CO reduction/evolution reactions lead to the accumulation of LiCO residuals and thus possible catalyst deactivation, which hinders the long-term cycling stability of Li-CO batteries. Apart from catalyst design, constructing a fluorinated solid-electrolyte interphase is a conventional strategy to minimize parasitic reactions and prolong cycle life. However, the catalytic effects of solid-electrolyte interphase components have been overlooked and remain unclear.

Structural Distortion in the Wadsley-Roth Niobium Molybdenum Oxide Phase Triggering Extraordinarily Stable Battery Performance.

Wadsley-Roth niobium oxide phases have attracted extensive research interest recently as promising battery anodes. We have synthesized the niobium-molybdenum oxide shear phase (Nb, Mo) O with superior electrochemical Li-ion storage performance, including an ultralong cycling lifespan of at least 15000 cycles. During electrochemical cycling, a reversible single-phase solid-solution reaction with lithiated intermediate solid solutions is demonstrated using in situ X-ray diffraction, with the valence and short-range structural changes of the electrode probed by in situ Nb and Mo K-edge X-ray absorption spectroscopy.

Revisiting the Role of Discharge Products in Li-CO Batteries.

Rechargeable lithium-carbon dioxide (Li-CO ) batteries are promising devices for CO recycling and energy storage. However, thermodynamically stable and electrically insulating discharge products (DPs) (e.g.

Solvent control of water O-H bonds for highly reversible zinc ion batteries.

Aqueous Zn-ion batteries have attracted increasing research interest; however, the development of these batteries has been hindered by several challenges, including dendrite growth, Zn corrosion, cathode material degradation, limited temperature adaptability and electrochemical stability window, which are associated with water activity and the solvation structure of electrolytes. Here we report that water activity is suppressed by increasing the electron density of the water protons through interactions with highly polar dimethylacetamide and trimethyl phosphate molecules. Meanwhile, the Zn corrosion in the hybrid electrolyte is mitigated, and the electrochemical stability window and the operating temperature of the electrolyte are extended.

Stabilizing Cobalt-free Li-rich Layered Oxide Cathodes through Oxygen Lattice Regulation by Two-phase Ru Doping.

The application of Li-rich layered oxides is hindered by their dramatic capacity and voltage decay on cycling. This work comprehensively studies the mechanistic behaviour of cobalt-free Li Ni Mn O and demonstrates the positive impact of two-phase Ru doping. A mechanistic transition from the monoclinic to the hexagonal behaviour is found for the structural evolution of Li Ni Mn O and the improvement mechanism of Ru doping is understood using the combination of in operando and post-mortem synchrotron analyses.

Introducing 4s-2p Orbital Hybridization to Stabilize Spinel Oxide Cathodes for Lithium-Ion Batteries.

Oxides composed of an oxygen framework and interstitial cations are promising cathode materials for lithium-ion batteries. However, the instability of the oxygen framework under harsh operating conditions results in fast battery capacity decay, due to the weak orbital interactions between cations and oxygen (mainly 3d-2p interaction). Here, a robust and endurable oxygen framework is created by introducing strong 4s-2p orbital hybridization into the structure using LiNi Mn O oxide as an example.

Crystallographic-Site-Specific Structural Engineering Enables Extraordinary Electrochemical Performance of High-Voltage LiNi Mn O Spinel Cathodes for Lithium-Ion Batteries.

The development of reliable and safe high-energy-density lithium-ion batteries is hindered by the structural instability of cathode materials during cycling, arising as a result of detrimental phase transformations occurring at high operating voltages alongside the loss of active materials induced by transition metal dissolution. Originating from the fundamental structure/function relation of battery materials, the authors purposefully perform crystallographic-site-specific structural engineering on electrode material structure, using the high-voltage LiNi Mn O (LNMO) cathode as a representative, which directly addresses the root source of structural instability of the Fd m structure. By employing Sb as a dopant to modify the specific issue-involved 16c and 16d sites simultaneously, the authors successfully transform the detrimental two-phase reaction occurring at high-voltage into a preferential solid-solution reaction and significantly suppress the loss of Mn from the LNMO structure.

Phase Compatible NiFeO Coating Tunes Oxygen Redox in Li-Rich Layered Oxide.

Li-rich layered oxides have attracted intense attention for lithium-ion batteries, as provide substantial capacity from transition metal cation redox simultaneous with reversible oxygen-anion redox. However, unregulated irreversible oxygen-anion redox leads to critical issues such as voltage fade and oxygen release. Here, we report a feasible NiFeO (NFO) surface-coating strategy to turn the nonbonding coordination of surface oxygen into metal-oxygen decoordination.

A Long Cycle-Life High-Voltage Spinel Lithium-Ion Battery Electrode Achieved by Site-Selective Doping.

Spinel LiNi Mn O (LNMO) is a promising cathode candidate for the next-generation high energy-density lithium-ion batteries (LIBs). Unfortunately, the application of LNMO is hindered by its poor cycle stability. Now, site-selectively doped LNMO electrode is prepared with exceptional durability.

Coupling Topological Insulator SnSb Te Nanodots with Highly Doped Graphene for High-Rate Energy Storage.

Topological insulators have spurred worldwide interest, but their advantageous properties have scarcely been explored in terms of electrochemical energy storage, and their high-rate capability and long-term cycling stability still remain a significant challenge to harvest. p-Type topological insulator SnSb Te nanodots anchoring on few-layered graphene (SnSb Te /G) are synthesized as a stable anode for high-rate lithium-ion batteries and potassium-ion batteries through a ball-milling method. These SnSb Te /G composite electrodes show ultralong cycle lifespan (478 mAh g at 1 A g after 1000 cycles) and excellent rate capability (remaining 373 mAh g even at 10 A g ) in Li-ion storage owing to the rapid ion transport accelerated by the PN heterojunction, virtual electron highways provided by the conductive topological surface state, and extraordinary pseudocapacitive contribution, whose excellent phase reversibility is confirmed by synchrotron in situ X-ray powder diffraction.

Understanding Rechargeable Battery Function Using In Operando Neutron Powder Diffraction.

The performance of rechargeable batteries is influenced by the structural and phase changes of components during cycling. Neutron powder diffraction (NPD) provides unique and useful information concerning the structure-function relation of battery components and can be used to study the changes to component phase and structure during battery cycling, known as in operando measurement studies. The development and use of NPD for in operando measurements of batteries is summarized along with detailed experimental approaches that impact the insights gained by these.

Heterocarbides Reinforced Electrochemical Energy Storage.

The feasibility of transition metal carbides (TMCs) as promising high-rate electrodes is still hindered by low specific capacity and sluggish charge transfer kinetics. Improving charge transport kinetics motivates research toward directions that would rely on heterostructures. In particular, heterocomposing with carbon-rich TMCs is highly promising for enhancing Li storage.

Multiple Anionic Transition-Metal Oxycarbide for Better Lithium Storage and Facilitated Multielectron Reactions.

As an important class of multielectron reaction materials, the applications of transition-metal oxides (TMOs) are impeded by volume expansion and poor electrochemical activity. To address these intrinsic limitations, the renewal of TMOs inspires research on incorporating an advanced interface layer with multiple anionic characteristics, which may add functionality to support properties inaccessible to a single-anion TMO electrode. Herein, a transition-metal oxycarbide (TMOC, M = Mo) with more than one anionic species was prepared as an interface layer on a corresponding oxide.

FeO-Decorated Porous Graphene Interlayer for High-Performance Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries are seriously restrained by the shuttling effect of intermediary products and their further reduction on the anode surface. Considerable researches have been devoted to overcoming these issues by introducing carbon-based materials as the sulfur host or interlayer in the Li-S systems. Herein, we constructed a multifunctional interlayer on a separator by inserting FeO nanoparticles (NPs) in a porous graphene (PG) film to immobilize polysulfides effectively.

Suppressing Self-Discharge and Shuttle Effect of Lithium-Sulfur Batteries with V O -Decorated Carbon Nanofiber Interlayer.

V O decorated carbon nanofibers (CNFs) are prepared and used as a multifunctional interlayer for a lithium-sulfur (Li-S) battery. V O anchored on CNFs can not only suppress the shuttle effect of polysulfide by the strong adsorption and redox reaction, but also work as a high-potential dam to restrain the self-discharge behavior in the battery. As a result, Li-S batteries with a high capacity and long cycling life can be stored and rested for a long time without obvious capacity fading.

Breathable and Wearable Energy Storage Based on Highly Flexible Paper Electrodes.

Breathable and wearable energy storage is achieved based on an innovative design solution. Carbon nanotube/MnO -decorated air-laid paper electrodes, with outstanding flexibility and good electrochemical performances, are prepared. They are then assembled into solid-state supercapacitors.

Ultrafine TiO2 Decorated Carbon Nanofibers as Multifunctional Interlayer for High-Performance Lithium-Sulfur Battery.

Although lithium-sulfur (Li-S) batteries deliver high specific energy densities, lots of intrinsic and fatal obstacles still restrict their practical application. Electrospun carbon nanofibers (CNFs) decorated with ultrafine TiO2 nanoparticles (CNF-T) were prepared and used as a multifunctional interlayer to suppress the volume expansion and shuttle effect of Li-S battery. With this strategy, the CNF network with abundant space and superior conductivity can accommodate and recycle the dissolved polysulfides for the bare sulfur cathode.