Precise modulation of the electronic structure in transition metals, particularly the d-band center position and spin state, remains a critical challenge to expediting hydrogen evolution reaction (HER) kinetics. Herein, we report a NiPt/Ni-heterostructured catalyst enabling simultaneous optimization of the d-band electronic structure and spin state of Ni through regulation of the NiPt and Ni bridge sites. Combining operando spectroscopy, X-ray absorption spectroscopy, density functional theory, and ab initio molecular dynamics simulations, we establish that the coordination environment and spin states of Ni at the bridge sites were effectively modulated by altering the Pt content, achieving a transition of Ni centers from the low-spin to high-spin state, and optimized intermediate adsorption/desorption behaviors.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2025
Sodium (Na) storage in hard carbon (HC) is a fundamental electrochemical process for sodium-ion batteries, where adsorption energy critically influences charge/discharge rates and storage capacity. Accurate prediction of this energy is essential for designing of high-performance HC. Traditional quantum mechanical simulations often neglect charge effects from electrochemical potentials, leading to inaccurate adsorption energies and discrepancies with experiments.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2025
The issues related to corrosion, dendrite growth, and hydrogen evolution reaction (HER) of the Zn anode in aqueous environments have significantly obstructed the practical implementation of aqueous zinc ion batteries (AZIBs). Herein, the strategy of synergistically regulating the content of active water molecules located within the inner Helmholtz plane (IHP) by anions and cations is used to address the above-mentioned water-related issues of zinc metal anodes via using the 1-Ethyl-3-methylimidazolium tetrafluoroborate ionic liquid (IL) as an highly effective electrolyte additive. Theoretical computations and empirical outcomes show that the IL indirectly regulates IHP by tailoring solvation structure of Zn via anions and adsorbing cations on the surface of the zinc anode, directly and effectively reducing the content of chemically active HO molecules in IHP and thus significantly inhibiting the adverse reactions related to active HO molecules.
View Article and Find Full Text PDFSodium-ion batteries (SIBs) emerge as a sustainable and cost-effective alternative to lithium-ion batteries due to the abundant and widely distributed nature of sodium resources. Hard carbon anodes, characterized by their pseudo-graphitic layered structures and nanoporosity, are key to achieving high-performance SIBs. However, the commercialization of hard carbon is hindered by significant challenges in precursor design, carbonization optimization, and sustainability.
View Article and Find Full Text PDFJ Colloid Interface Sci
October 2025
Biomass-derived hard carbon materials stand out in the research of anode materials for sodium-ion batteries (SIBs) due to their low cost, high performance, and broad range of raw materials. However, the low carbonization yields of biomass-derived hard carbons and the waste produced during industrial production processes contribute to the high production cost of these hard carbons. Furthermore, it is essential to discuss the use of various electrolytes aimed at enhancing the ion storage capacity within SIBs.
View Article and Find Full Text PDFEnergy materials are essential for addressing global energy challenges, and their design, recycling, and performance optimization are critical for sustainable development. To efficiently rise to this occasion, advanced technology should be explored to address these challenges. This review focuses on the potential of ultrafast thermal engineering as an innovative approach to the design and recycling of energy materials and systematically examines ultrahigh temperature shock's origins, mechanisms, and developmental progress, clarifying fundamental differences between the Joule heating and carbothermal shock modes.
View Article and Find Full Text PDFChem Soc Rev
May 2025
Compared with the costly and toxic LiCoO cathode in lithium-ion batteries (LIBs), nickel-based layered oxide (NLO) cathode materials exhibit the advantages of high capacity, natural abundance, environment-friendliness, and low cost, displaying tremendous application potentials in power batteries for automobiles and aircrafts. This review comprehensively introduces the challenges faced by NLO cathode materials in all alkali-ion batteries (AIBs) in their material synthesis, cation mixing, particle cracking, phase changes, cation dissolution of Mn, and oxygen loss Various strategies, including heteroatom doping, surface coating, and concentration gradient, are applied to tackle these problems by developing layered LiNiMO (M: metal; 0 < < 1) and LiNiCoMnO ( + + = 1) materials. The successful commercial application of NLO cathode materials in LIBs has further driven their developments in sodium/potassium-ion batteries the synthesis of (Na/K)NiMO.
View Article and Find Full Text PDFLow-cost Fe-based Prussian blue analogues often suffer from capacity degradation, resulting in continuous energy loss, impeding commercialization for practical sodium-ion batteries. The underlying cause of capacity decrease remains mysterious. Herein, we show that irreversible phase transitions, structural degradation, deactivation of surface redox centres, and dissolution of transition metal ions in Prussian blue analogues accumulate continuously during cycling.
View Article and Find Full Text PDFSingle-atom catalysts (SACs) have become the forefront and hotspot in energy storage and conversion research, inheriting the advantages of both homogeneous and heterogeneous catalysts. In particular, carbon-supported SACs (CS-SACs) are excellent candidates for many energy storage and conversion applications, due to their maximum atomic efficiency, unique electronic and coordination structures, and beneficial synergistic effects between active catalytic sites and carbon substrates. In this review, we briefly review the atomic-level regulation strategies for optimizing CS-SACs for energy storage and conversion, including coordination structure control, nonmetallic elemental doping, axial coordination design, and polymetallic active site construction.
View Article and Find Full Text PDFThe rapid catalytic conversion toward polysulfides is considered to be an advantageous approach to boost the reaction kinetics and inhibit the shuttle effect in lithium-sulfur (Li─S) batteries. However, the prediction of high catalytic activity Li─S catalysts has become challenging given the carelessness in the relationship between important electronic characteristics of catalysts and catalytic activity. Herein, the relationships between the D-band regulation of catalysts with reaction kinetics toward polysulfides are described.
View Article and Find Full Text PDFBiomass holds significant potential for large-scale synthesis of hard carbon (HC), and HC is seen as the most promising anode material for sodium-ion batteries (SIBs). However, designing a HC anode with a rich pore structure, moderate graphitization and synthesis through a simple process using a cost-effective precursor to advance SIBs has long been a formidable challenge. This is primarily because high temperatures necessary for pore regulation invariably lead to excessive graphitization.
View Article and Find Full Text PDFWaste gourd shells enriched with ash-forming elements are selected as raw materials in this paper, discovering that the K and Ca compounds in the precursor not only exhibit the ability of self-forming pores, but also demonstrate catalytic graphitization of the hard carbon during the pyrolysis procedure.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2024
Currently, inhomogeneous distribution of Zn on the surface of the Zn anode is still the essential reason for dendrite formation and unsatisfactory stability of zinc ion batteries. Given the merits of strong interaction between Sn and Zn, as well as a low nucleation barrier during Zn deposition, the combination of metallic Sn with carbon material is expected to improve the deposition of zinc ions and inhibit the growth of zinc dendrites by guiding the homogeneous plating/stripping of zinc on the electrode surface. In this article, zincophilic Sn nanoparticles with low nucleation barriers and strong interaction with Zn were embedded into 3D N-doped carbon nanofibers using a simple electrostatic spinning technique.
View Article and Find Full Text PDFPotassium-ion batteries (PIBs) are considered potential candidates for large-scale energy storage systems due to the abundant resources of potassium. Among various reported anode materials, bismuth anodes with the advantages of high theoretical specific capacity, low cost, and nontoxicity have attracted widespread attention. However, bismuth anodes experience significant volume changes during the charge/discharge process, leading to unsatisfactory cycling stability and rate performance.
View Article and Find Full Text PDFThe development of cost-efficient, long-lifespan, and all-climate sodium-ion batteries is of great importance for advancing large-scale energy storage but is plagued by the lack of suitable cathode materials. Here, we report low-cost Na-rich Mn-based Prussian blue analogues with superior rate capability and ultralong cycling stability over 10,000 cycles via structural optimization with electrochemically inert Ni atoms. Their thermal stability, all-climate properties, and potential in full cells are investigated in detail.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Anion-reinforced solvation structure favors the formation of inorganic-rich robust electrode-electrolyte interface, which endows fast ion transport and high strength modulus to enable improved electrochemical performance. However, such a unique solvation structure inevitably injures the ionic conductivity of electrolytes and limits the fast-charging performance. Herein, a trade-off in tuning anion-reinforced solvation structure and high ionic conductivity is realized by the entropy-assisted hybrid ester-ether electrolyte.
View Article and Find Full Text PDFHard carbon (HC) is one of the most promising anode materials for sodium-ion batteries (SIBs) due to its cost-effectiveness and low-voltage plateau capacity. Heteroatom doping is considered as an effective strategy to improve the sodium storage capacity of HC. However, most of the previous heteroatom doping strategies are performed at a relatively low temperature, which could not be utilized to raise the low-voltage plateau capacity.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2024
Given the merits of abundant resource, low cost and high electrochemical activity, hard carbons have been regarded as one of the most commercializable anode material for sodium-ion batteries (SIBs). However, poor rate capability is one of the main obstacles that severely hinder its further development. In addition, the relationships between preparation method, material structure and electrochemical performance have not been clearly elaborated.
View Article and Find Full Text PDFBecause of its abundant resources, low cost and high reversible specific capacity, hard carbon (HC) is considered as the most likely commercial anode material for sodium-ion batteries (SIBs). Therefore, reasonable design and effective strategies to regulate the structure of HCs play a crucial role in promoting the development of SIBs. Herein, the progress in the preparation approaches for HC anode materials is systematically overviewed, with a special focus on the comparison between traditional fabrication methods and advanced strategies emerged in recent years in terms of their influence on performance, including preparation efficiency, initial coulombic efficiency (ICE), specific capacity and rate capability.
View Article and Find Full Text PDFIntrinsically safe sodium-ion batteries are considered as a promising candidate for large-scale energy storage systems. However, the high flammability of conventional electrolytes may pose serious safety threats and even explosions. Herein, a strategy of constructing a deep eutectic electrolyte is proposed to boost the safety and electrochemical performance of succinonitrile (SN)-based electrolyte.
View Article and Find Full Text PDFSodium metal batteries have attracted increasing interest recently, but suffer from severe dendrite growth caused by uneven Na plating/stripping behavior, which may result in the piercing of the membrane, with short circuiting and even cause explosions. Herein, a conductive and sodiophilic Ag coating layer is introduced to regulate Na deposition behaviors for highly reversible sodium metal batteries. Ag coated Zn foil with enhanced sodiophilicity, rapid Na transfer kinetics and superior electronic conductivity guarantee the homogenized Na ion and electric field distribution.
View Article and Find Full Text PDFAmmonium vanadates, featuring an N─H···O hydrogen bond network structure between NH and V─O layers, have become popular cathode materials for aqueous zinc-ion batteries (AZIBs). Their appeal lies in their multi-electron transfer, high specific capacity, and facile synthesis. However, a major drawback arises as Zn ions tend to form bonds with electronegative oxygen atoms between V─O layers during cycling, leading to irreversible structural collapse.
View Article and Find Full Text PDFTrimetallic nanowires (NWs) have drawn much attention in efficient alcohol oxidation reaction (AOR) due to their unique features, including high atomic utilization efficiency and fast electron transfer ability. However, a universal strategy to synthesize Pd-based trimetallic NWs with high catalytic performance is still lacking. Herein, we develop a universal method for facile synthesis of PdBiM (M = Pt, Ru, Ir, Co, Cu) NWs with excellent AOR activities.
View Article and Find Full Text PDFLarge reserves, high capacity, and low cost are the core competitiveness of disordered carbon materials as excellent anode materials for sodium-ion batteries (SIBs). And the existence and improper treatment of a large number of organic solid wastes will aggravate the burden on the environment, therefore, it is significant to transform wastes into carbon-based materials for sustainable energy utilization. Herein, a kind of hard carbon materials are reported with waste biomass-foam as the precursor, which can improve the sodium storage performance through pre-oxidation strategy.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2024
The stable three-dimensional framework and high operating voltage of sodium superionic conductor (NASICON)-type NaV(PO) has the potential to work with long cycle life and high-rate performance; however, it suffers from the poor intrinsic electronic conductivity and low energy density. Herein, Ga is introduced into NaV(PO) to activate the V/V redox couple at a high potential of 4.0 V for enhancing energy density of the materials (NaVGa(PO)).
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