Valence Electron: A Descriptor of Spinel Sulfides for Sulfur Reduction Catalysis.

Catalysts are essential for achieving high-performance lithium-sulfur batteries. The precise design and regulation of catalytic sites to strengthen their efficiency and robustness remains challenging. In this study, spinel sulfides and catalyst design principles through element doping are investigated.

Deciphering Water Oxidation Catalysts: The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity Promotion.

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction. The surface reconstruction has been widely observed in perovskite catalysts, and the reconstruction degree has been often correlated with the activity enhancement. Here, a systematic study on the roles of Fe substitution in activation of perovskite LaNiO is reported.

Dynamic Active Sites in Electrocatalysis.

In-depth understanding of the real-time behaviors of active sites during electrocatalysis is essential for the advancement of sustainable energy conversion. Recently, the concept of dynamic active sites has been recognized as a potent approach for creating self-adaptive electrocatalysts that can address a variety of electrocatalytic reactions, outperforming traditional electrocatalysts with static active sites. Nonetheless, the comprehension of the underlying principles that guide the engineering of dynamic active sites is presently insufficient.

Recycled Tandem Catalysts Promising Ultralow Overpotential Li-CO Batteries.

Lithium-carbon dioxide (Li-CO ) batteries are regarded as a prospective technology to relieve the pressure of greenhouse emissions but are confronted with sluggish CO redox kinetics and low energy efficiency. Developing highly efficient and low-cost catalysts to boost bidirectional activities is craved but remains a huge challenge. Herein, derived from the spent lithium-ion batteries, a tandem catalyst is subtly synthesized and significantly accelerates the CO reduction and evolution reactions (CO RR and CO ER) kinetics with an in-built electric field (BEF).

Essential role of lattice oxygen in methanol electrochemical refinery toward formate.

Developing technologies based on the concept of methanol electrochemical refinery (e-refinery) is promising for carbon-neutral chemical manufacturing. However, a lack of mechanism understanding and material properties that control the methanol e-refinery catalytic performances hinders the discovery of efficient catalysts. Here, using O isotope-labeled catalysts, we find that the oxygen atoms in formate generated during the methanol e-refinery reaction can originate from the catalysts' lattice oxygen and the O-2p-band center levels can serve as an effective descriptor to predict the catalytic performance of the catalysts, namely, the formate production rates and Faradaic efficiencies.

Acidic enol electrooxidation-coupled hydrogen production with ampere-level current density.

Hydrogen production coupled with biomass upgrading is vital for future sustainable energy developments. However, most biomass electrooxidation reactions suffer from high working voltage and low current density, which substantially hinder large-scale industrial applications. Herein, we report an acidic hydrogen production system that combined anodic ascorbic acid electrooxidation with cathodic hydrogen evolution.

Multi-Domain versus Single-Domain: A Magnetic Field is Not a Must for Promoting Spin-Polarized Water Oxidation.

The reaction kinetics of spin-polarized oxygen evolution reaction (OER) can be enhanced by ferromagnetic (FM) catalysts under an external magnetic field. However, applying a magnetic field necessitates additional energy consumption and creates design difficulties for OER. Herein, we demonstrate that a single-domain FM catalyst without external magnetic fields exhibits a similar OER increment to its magnetized multi-domain one.

Navigating surface reconstruction of spinel oxides for electrochemical water oxidation.

Understanding and mastering the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity. Herein, we demonstrate that surface reconstruction of spinel oxides originates from the metal-oxygen covalency polarity in the M-O-M backbone. A stronger M-O covalency relative to M-O covalency is found beneficial for a more thorough reconstruction towards oxyhydroxides.

Reconstruction of Thiospinel to Active Sites and Spin Channels for Water Oxidation.

Water electrolysis is a promising technique for carbon neutral hydrogen production. A great challenge remains at developing robust and low-cost anode catalysts. Many pre-catalysts are found to undergo surface reconstruction to give high intrinsic activity in the oxygen evolution reaction (OER).

Enhanced oxygen evolution over dual corner-shared cobalt tetrahedra.

Developing efficient catalysts is of paramount importance to oxygen evolution, a sluggish anodic reaction that provides essential electrons and protons for various electrochemical processes, such as hydrogen generation. Here, we report that the oxygen evolution reaction (OER) can be efficiently catalyzed by cobalt tetrahedra, which are stabilized over the surface of a Swedenborgite-type YBCoO material. We reveal that the surface of YBaCoO possesses strong resilience towards structural amorphization during OER, which originates from its distinctive structural evolution toward electrochemical oxidation.

The effect of the hydroxyl group position on the electrochemical reactivity and product selectivity of butanediol electro-oxidation.

This article presents a study on the effect of the hydroxyl group position on the electro-oxidation of butanediols, including 1,2-butanediol, 2,3-butanediol, 1,3-butanediol, and 1,4-butanediol. The effect of the hydroxyl group position in butanediols on their electro-oxidation reactivities is investigated by cyclic voltammetry, linear sweep voltammetry, chronopotentiometry and chronoamperometry in 1.0 M KOH.

Lattice site-dependent metal leaching in perovskites toward a honeycomb-like water oxidation catalyst.

Metal leaching during water oxidation has been typically observed in conjunction with surface reconstruction on perovskite oxide catalysts, but the role of metal leaching at each geometric site has not been distinguished. Here, we manipulate the occurrence and process of surface reconstruction in two model ABO perovskites, i.e.

Spin pinning effect to reconstructed oxyhydroxide layer on ferromagnetic oxides for enhanced water oxidation.

Producing hydrogen by water electrolysis suffers from the kinetic barriers in the oxygen evolution reaction (OER) that limits the overall efficiency. With spin-dependent kinetics in OER, to manipulate the spin ordering of ferromagnetic OER catalysts (e.g.

Spin-polarized oxygen evolution reaction under magnetic field.

The oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons' transfer and the generation of triplet state O from singlet state species (OH or HO). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear.

Engineering High-Spin State Cobalt Cations in Spinel Zinc Cobalt Oxide for Spin Channel Propagation and Active Site Enhancement in Water Oxidation.

Spinel zinc cobalt oxide (ZnCo O ) is not considered as a superior catalyst for the electrochemical oxygen evolution reaction (OER), which is the bottleneck reaction in water-electrolysis. Herein, taking advantage of density functional theory (DFT) calculations, we find that the existence of low-spin (LS) state cobalt cations hinders the OER activity of spinel zinc cobalt oxide, as the t e configuration gives rise to purely localized electronic structure and exhibits poor binding affinity to the key reaction intermediate. Increasing the spin state of cobalt cations in spinel ZnCo O is found to propagate a spin channel to promote spin-selected charge transport during OER and generate better active sites for intermediates adsorption.

Anodic Oxidation Enabled Cation Leaching for Promoting Surface Reconstruction in Water Oxidation.

A rational design for oxygen evolution reaction (OER) catalysts is pivotal to the overall efficiency of water electrolysis. Much work has been devoted to understanding cation leaching and surface reconstruction of very active electrocatalysts, but little on intentionally promoting the surface in a controlled fashion. We now report controllable anodic leaching of Cr in CoCr O by activating the pristine material at high potential, which enables the transformation of inactive spinel CoCr O into a highly active catalyst.

Spin-Related Electron Transfer and Orbital Interactions in Oxygen Electrocatalysis.

Oxygen evolution and reduction reactions play a critical role in determining the efficiency of the water cycling (H O ⇔ H + O ), in which the hydrogen serves as the energy carrier. That calls for a comprehensive understanding of oxygen electrocatalysis for efficient catalyst design. Current opinions on oxygen electrocatalysis have been focused on the thermodynamics of the reactant/intermediate adsorption on the catalysts.

Constructing an Adaptive Heterojunction as a Highly Active Catalyst for the Oxygen Evolution Reaction.

Electrochemical water splitting is of prime importance to green energy technology. Particularly, the reaction at the anode side, namely the oxygen evolution reaction (OER), requires a high overpotential associated with OO bond formation, which dominates the energy-efficiency of the whole process. Activating the anionic redox chemistry of oxygen in metal oxides, which involves the formation of superoxo/peroxo-like (O ) , commonly occurs in most highly active catalysts during the OER process.

Impact Factors of Empathy in Mainland Chinese Youth.

Empathy was investigated in 592 Mainland Chinese youth using the Interpersonal Reactivity Index. Participants' empathy-related information covering demographic traits, emotional wellness, as well as academic and social problems were recorded. Results of Classification and Regression Tree (CART) analysis showed that emotional empathy, cognitive empathy, and empathy-related personal distress was impacted by inherited traits (e.

Surface Composition Dependent Ligand Effect in Tuning the Activity of Nickel-Copper Bimetallic Electrocatalysts toward Hydrogen Evolution in Alkaline.

Exploring efficient and low-cost electrocatalysts for hydrogen evolution reaction (HER) in alkaline media is critical for developing anion exchange membrane electrolyzers. The key to a rational catalyst design is understanding the descriptors that govern the alkaline HER activity. Unfortunately, the principles that govern the alkaline HER performance remain unclear and are still under debate.

Electrochemical Oxidation of Nitrogen towards Direct Nitrate Production on Spinel Oxides.

Nitrates are widely used as fertilizer and oxidizing agents. Commercial nitrate production from nitrogen involves high-temperature-high-pressure multi-step processes. Therefore, an alternative nitrate production method under ambient environment is of importance.

Antiferromagnetic Inverse Spinel Oxide LiCoVO with Spin-Polarized Channels for Water Oxidation.

Exploring highly efficient catalysts for the oxygen evolution reaction (OER) is essential for water electrolysis. Cost-effective transition-metal oxides with reasonable activity are raising attention. Recently, OER reactants' and products' differing spin configurations have been thought to cause slow reaction kinetics.

Significance of Engineering the Octahedral Units to Promote the Oxygen Evolution Reaction of Spinel Oxides.

The clean energy carrier, hydrogen, if efficiently produced by water electrolysis using renewable energy input, would revolutionize the energy landscape. It is the sluggish oxygen evolution reaction (OER) at the anode of water electrolyzer that limits the overall efficiency. The large spinel oxide family is widely studied due to their low cost and promising OER activity.

Shifting Oxygen Charge Towards Octahedral Metal: A Way to Promote Water Oxidation on Cobalt Spinel Oxides.

Cobalt spinel oxides are a class of promising transition metal (TM) oxides for catalyzing oxygen evolution reaction (OER). Their catalytic activity depends on the electronic structure. In a spinel oxide lattice, each oxygen anion is shared amongst its four nearest transition metal cations, of which one is located within the tetrahedral interstices and the remaining three cations are in the octahedral interstices.