The advancement of all-solid-state lithium metal batteries requires breakthroughs in solid-state electrolytes (SSEs) for the suppression of lithium dendrite growth at high current densities and high capacities (>3 mAh cm) and innovation of SSEs in terms of crystal structure, ionic conductivity and rigidness. Here we report a superionic conducting, highly lithium-compatible and air-stable vacancy-rich β-LiN SSE. This vacancy-rich β-LiN SSE shows a high ionic conductivity of 2.
View Article and Find Full Text PDFEutectic electrolytes hold promise for aqueous zinc metal batteries in sustainable energy storage chemistries, yet improvement from perspective of molecule configurational engineering are ambiguous. Herein, we propose design strategy of increasing asymmetric molecular geometry in organic ligands to regulate frustrated coordination and disordered structure for eutectic electrolytes toward enhanced zinc metal batteries. The introduced asymmetry in eutectic component gives rise to relatively weak coordination strength and configurational disorder interaction among cation-anion-ligand, leading to suppressed local aggregation, steady eutectic phase and improved Zn diffusion kinetics.
View Article and Find Full Text PDFCoal ashes in Canada have gained attention as a potential source for recovering rare earth elements (REE) from industrial waste. However, the complex chemical properties of coal ashes have made it difficult to determine the desirability, feasibility, and viability of REE recovery. To address this issue, this study systematically investigated distribution and structural information, speciation and chemical-binding state, and purity and extraction capacity of REE in multiple Canadian coal ashes (i.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2024
The electrochemical CO reduction reaction (ECR) is a promising pathway to producing valuable chemicals and fuels. Despite extensive studies reported, improving CO adsorption for local CO enrichment or water dissociation to generate sufficient H* is still not enough to achieve industrial-relevant current densities. Herein, we report a "two-in-one" catalyst, defective Bi nanosheets modified by CrO (Bi-CrO), to simultaneously promote CO adsorption and water dissociation, thereby enhancing the activity and selectivity of ECR to formate.
View Article and Find Full Text PDFEnhancing active states on the catalyst surface by modulating the adsorption-desorption properties of reactant species is crucial to optimizing the electrocatalytic activity of transition metal-based nanostructured materials. In this work, an efficient optimization strategy is proposed by co-modulating the dual anions (C and S) in NiC/NiS, the heterostructured electrocatalyst, which is prepared via a simple hot-injection method. The presence of NiC/NiS heterojunctions accelerates the charge carrier transfer and promotes the generation of active sites, enabling the heterostructured electrocatalyst to achieve current densities of 10/100 mA cm at 1.
View Article and Find Full Text PDFUpgrading excess CO toward the electrosynthesis of formic acid is of significant research and commercial interest. However, simultaneously achieving high selectivity and industrially relevant current densities of CO-to-formate conversion remains a grand challenge for practical implementations. Here, an electrically conductive zeolite support is strategically designed by implanting Sn ions into the skeleton structure of a zeolite Y, which impregnates ultrasmall InSn alloy nanoclusters into the supercages of the tailored 12-ring framework.
View Article and Find Full Text PDFNanocrystalline (nc) metals are generally strong yet thermally unstable, rendering them difficult to process and unsuitable for use, particularly at elevated temperatures. Nc multicomponent and high-entropy alloys (HEAs) are found to offer enhanced thermal stability but only in a few empirically discovered systems out of a vast compositional space. In response, this work develops a combinatorial strategy to accelerate the discovery of nc-(TiZrHf)(NbTa) alloy library with distinct thermal stability, in terms of phases and grain sizes.
View Article and Find Full Text PDFEffective removal of chemically toxic selenium oxoanions at high-capacity and trace levels from contaminated water remains a challenge in current scientific pursuits. Here, we report the functionalization of the MgAl layered double hydroxide with molybdenum-oxysulfide (MoOS) anion, referred to as LDH-MoOS, and its potential to sequester SeO and SeO from aqueous solution. LDH-MoOS nanosheets were synthesized by an ion exchange method in solution.
View Article and Find Full Text PDFThe accurate characterisation of centreline segregation requires precise measurements of composition variations over large length scales (10 ) across the centreline of the cast product, while having high resolution, sufficient to quantify the significant composition variations between dendrites due to microsegregation at very small length scales (10 ). This study investigates the potential of a novel microscopy technique, named Synchrotron Micro X-ray Flurorescence (SMXRF), to generate large-scale high-resolution segregation maps from a steel sample taken from a thin slab caster. Two methods, Point Analysis and Regression Analysis, are proposed for SMXRF data calibration.
View Article and Find Full Text PDFChalcogel represents a unique class of meso- to macroporous nanomaterials that offer applications in energy and environmental pursuits. Here, the synthesis of an ion-exchangeable amorphous chalcogel using a nominal composition of KCoMoS (KCMS) at room temperature is reported. Synchrotron X-ray pair distribution function (PDF), X-ray absorption near-edge structure (XANES), and extended X-ray absorption fine structure (EXAFS) reveal a plausible local structure of KCMS gel consisting of Mo and Mo clusters in the vicinity of di/polysulfides which are covalently linked by Co ions.
View Article and Find Full Text PDFCatalyst supports play an essential role in catalytic reactions, hinting at pronounced metal-support effects. Zeolites are a propitious support in heterogeneous catalysts, while their use in the electrocatalytic CO reduction reaction has been limited as yet because of their electrically insulating nature and serious competing hydrogen evolution reaction (HER). Enlightened by theoretical prediction, herein, we implant zinc ions into the structural skeleton of a zeolite Y to strategically tailor a favorable electrocatalytic platform with remarkably enhanced electronic conduction and strong HER inhibition capability, which incorporates ultrafine cadmium oxide nanoclusters as guest species into the supercages of the tailored 12-ring window framework.
View Article and Find Full Text PDFSci Total Environ
March 2024
The Three Gorges Reservoir area is recognized by its vast size, dense population, bustling economic and social activities along its banks, and by the significant volume of waterway traffic. These factors make it with a high risk of water pollution accidents, posing a serious threat to water environmental safety. Therefore, it is imperative to conduct a water environmental safety assessment in this region to ensure the safety of the water environment.
View Article and Find Full Text PDFConstructing the efficacious and applicable bi-functional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction (OER) are critical to the development of electrochemically-driven technologies for efficient hydrogen production and avoid CO emission. Herein, the hetero-nanocrystals between monodispersed Pt (~ 2 nm) and NiS (~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H generation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2024
Rechargeable zinc-based batteries are finding their niche in energy storage applications where cost, safety, scalability matter, yet they are plagued by rapid performance degradation due to the lack of suitable electrolytes to stabilize Zn anode. Herein, we report a competitive coordination structure to form unique quaternary hydrated eutectic electrolyte with ligand-cation-anion cluster. Unraveled by experiment and calculation results, the competing component can enter initial primary coordination shell of Zn ion, partially substituting Lewis basic eutectic ligands and reinforcing cation-anion interaction.
View Article and Find Full Text PDFIn order to mitigate the hazards of water pollution in drinking water source areas (DWSAs), developing applicable models and proposing effective solutions is of paramount significance. The study developed the Heshangshan Drinking Water Source Area (HDWSA) Hydrodynamic Model, integrating Geographic Information System (GIS) into a two-dimensional hydrodynamic water quality model using FORTRAN. TECPLOT360 software (Software Tools for Numerical Simulation with Visualization) visualized contamination transportation and diffusion.
View Article and Find Full Text PDFDeveloping commercially viable electrocatalyst lies at the research hotspot of rechargeable Zn-air batteries, but it is still challenging to meet the requirements of energy efficiency and durability in realistic applications. Strategic material design is critical to addressing its drawbacks in terms of sluggish kinetics of oxygen reactions and limited battery lifespan. Herein, a "raisin-bread" architecture is designed for a hybrid catalyst constituting cobalt nitride as the core nanoparticle with thin oxidized coverings, which is further deposited within porous carbon aerogel.
View Article and Find Full Text PDFThe electrosynthesis of multi-carbon chemicals from excess carbon dioxide (CO) is an area of great interest for research and commercial applications. However, improving both the yield of CO-to-ethanol conversion and the stability of the catalyst at the same time is proving to be a challenging issue. Here it is proposed to stabilize active Cu(I) and In dual sites with sulfur defects through an electro-driven intercalation strategy, which leads to the delocalization of electron density that enhances orbital hybridizations between the Cu-C and In-H bonds.
View Article and Find Full Text PDFResolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metal-sulfur batteries. Motivated by a theoretical prediction, herein, we strategically propose nitrogen-vacancy tantalum nitride (TaN) impregnated inside the interconnected nanopores of nitrogen-decorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in room-temperature sodium-sulfur batteries. Through a pore-constriction mechanism, the nitrogen vacancies are controllably constructed during the nucleation of TaN.
View Article and Find Full Text PDFAll-solid-state lithium metal batteries can address crucial challenges regarding insufficient battery cycling life and energy density. The demonstration of long-cycling dendrite-free all-solid-state lithium metal batteries requires precise tailoring of lithium-ion transport of solid-state electrolytes (SSEs). In this work, a proof of concept is reported for precise tailoring of lithium-ion transport of a halide SSE, LiInCl, including intragranular (within grains) but also intergranular (between grains) lithium-ion transport.
View Article and Find Full Text PDFAttaining substantial areal capacity (>3 mAh/cm) and extended cycle longevity in all-solid-state lithium metal batteries necessitates the implementation of solid-state electrolytes (SSEs) capable of withstanding elevated critical current densities and capacities. In this study, we report a high-performing vacancy-rich LiNCl SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high-areal capacity, long-lasting all-solid-state lithium metal batteries. The LiNCl facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies.
View Article and Find Full Text PDFThe mono-dispersed cubic siegenite CuNi S ultra-fine (≈5 nm) nanocrystals are fabricated through crystallization engineering under hot injection. The strong hydroxylation on mostly exposed CuNi S (220) surface leads to the formation of multi-valence (Cu , Cu , Ni , Ni ) species with unsaturated hybridization and coordination micro-environments, which can induce rich redox reactions to optimize interfacial kinetics for the adsorbed reaction intermediates. The as-synthesized CuNi S nanocrystals with ultra-small particle size and the characteristics of being highly dispersed can increase specific surface area and hydroxylated active sites, which considerably contribute to the improvement of photocatalytic activities.
View Article and Find Full Text PDFSolid electrolyte is vital to ensure all-solid-state batteries with improved safety, long cyclability, and feasibility at different temperatures. Herein, we report a new family of amorphous solid electrolytes, xLiO-MCl (M = Ta or Hf, 0.8 ≤ x ≤ 2, y = 5 or 4).
View Article and Find Full Text PDFSubstrate-supported catalysts with atomically dispersed metal centers are promising for driving the carbon dioxide reduction reaction (CORR) to produce value-added chemicals; however, regulating the size of exposed catalysts and optimizing their coordination chemistry remain challenging. In this study, we have devised a simple and versatile high-energy pulsed laser method for the enrichment of a Bi "single atom" (SA) with a controlled first coordination sphere on a time scale of nanoseconds. We identify the mechanistic bifurcation routes over a Bi SA that selectively produce either formate or syngas when bound to C or N atoms, respectively.
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