The neutral oxygen catalysis is an electrochemical reaction of the utmost importance in energy generation, storage application, and chemical synthesis. However, the restricted availability of protons poses a challenge to achieving kinetically favorable oxygen catalytic reactions. Here, we alter the interfacial water orientation by adjusting the Brønsted acidity at the catalyst surface, to break the proton transfer limitation of neutral oxygen electrocatalysis.
View Article and Find Full Text PDFLiAlTi (PO) (LATP) is a promising NASICON-type solid electrolyte for all-solid-state lithium-ion batteries (ASSLIBs) owing to its high ionic conductivity, low cost, and stability in ambient atmosphere. However, the electrochemical stability of LATP suffers upon contact with lithium metals, resulting in a reduction of Ti to Ti in its structure. This limitation necessitates interface modification processes, hindering its use in lithium-ion batteries.
View Article and Find Full Text PDFThe catalyst-electrolyte interface plays a crucial role in proton exchange membrane water electrolysis (PEMWE). However, optimizing the interfacial hydrogen bonding to enhance both catalytic activity and stability remains a significant challenge. Here, a novel catalyst design strategy is proposed based on the hard-soft acid-base principle, employing hard Lewis acids (LAs = ZrO, TiO, HfO) to mediate the reconfiguration of interfacial hydrogen bonding, thereby enhancing the acidic oxygen evolution reaction (OER) performance of RuO.
View Article and Find Full Text PDFMetal-organic frameworks (MOFs) have been considered as promising hosts for immobilizing ultrafine metal nanoparticles (MNPs) due to their high surface area and porosity. However, electrochemical applications of such emerging composites are severely limited by the poor electrical conductivity and large size of the MOFs. Herein, we report the general synthesis of incorporating various MNPs into a conjugated MOF ultrathin nanosheet (Cu-TCPP UNS) matrix, which not only prevents agglomeration and restricts the growth of MNPs but also benefits the exposure of active sites and the transport of electrons.
View Article and Find Full Text PDFRechargeable zinc-air batteries (ZABs) are viewed as a promising solution for electric vehicles due to their potential to provide a clean, cost-effective, and sustainable energy storage system for the next generation. Nevertheless, sluggish kinetics of the oxygen evolution reaction (OER), the oxygen reduction reaction (ORR) at the air electrode, and low power density are significant challenges that hinder the practical application of ZABs. The key to resolving the development of ZABs is developing an affordable, efficient, and stable catalyst with bifunctional catalytic.
View Article and Find Full Text PDFPhase engineering is an effective strategy for modulating the electronic structure and electron transfer mobility of cobalt selenide (CoSe) with remarkable sodium storage. Nevertheless, it remains challenging to improve fast-charging and cycling performance. Herein, a heterointerface coupling induces phase transformation from cubic CoSe to orthorhombic CoSe accompanied by the formation of MoSe to construct a CoSe/MoSe heterostructure decorated with N-doped carbon layer on a 3D graphene foam (CoSe/MoSe@NC/GF).
View Article and Find Full Text PDFRealizing an efficient turnover frequency in the acidic oxygen evolution reaction by modifying the reaction configuration is crucial in designing high-performance single-atom catalysts. Here, we report a "single atom-double site" concept, which involves an activatable inert manganese atom redox chemistry in a single-atom Ru-Mn dual-site platform with tunnel Ni ions as the trigger. In contrast to conventional single-atom catalysts, the proposed configuration allows direct intramolecular oxygen coupling driven by the Ni ions intercalation effect, bypassing the secondary deprotonation step instead of the kinetically sluggish adsorbate evolution mechanism.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Investigating the formation and transformation mechanisms of spiral-concave crystals holds significant potential for advancing innovative material design and comprehension. We examined the kinetics-controlled nucleation and growth mechanisms of Prussian Blue crystals with spiral concave structures, and constructed a detailed crystal growth phase diagram. The spiral-concave hexacyanoferrate (SC-HCF) crystals, characterized by high-density surface steps and a low stress-strain architecture, exhibit enhanced activity due to their facile interaction with reactants.
View Article and Find Full Text PDFThe efficacy and structural evolution of Mo-doped titania nanoparticles (MTNPs) as advanced photocatalysts for degrading methyl blue (MB) are investigated by X-ray absorption spectroscopy (XAS). The 3 wt % MTNP, characterized by uniform size and anatase structure, exhibits higher efficiency. The spectral analyses unveiled structural variations in the TiO octahedral structure and revealed an active site of the distorted square pyramidal structure symmetry (C).
View Article and Find Full Text PDFThe poor durability of Ru-based catalysts limits the practical application in proton exchange membrane water electrolysis (PEMWE). Here, we report that the asymmetric active units in RuMO (M = Sb, In, and Sn) binary solid solution oxides are constructed by introducing acid-resistant p-block metal sites, breaking the activity and stability limitations of RuO in acidic oxygen evolution reaction (OER). Constructing highly asymmetric Ru-O-Sb units with a strong electron delocalization effect significantly shortens the spatial distance between Ru and Sb sites, improving the bonding strength of the overall structure.
View Article and Find Full Text PDFSub-nanoclusters with ultra-small particle sizes are particularly significant to create advanced energy storage materials. Herein, Sn sub-nanoclusters encapsulated in nitrogen-doped multichannel carbon matrix (denoted as Sn-SCs@MCNF) are designed by a facile and controllable route as flexible anode for high-performance potassium ion batteries (PIBs). The uniformly dispersed Sn sub-nanoclusters in multichannel carbon matrix can be precisely identified, which ensure us to clarify the size influence on the electrochemical performance.
View Article and Find Full Text PDFPrussian blue analogue (PBA)/metal-organic frameworks (MOFs) are multifunctional precursors for the synthesis of metal/metal compounds, carbon, and their derived composites (P/MDCs) in chemical, medical, energy, and other applications. P/MDCs combine the advantages of both the high specific surface area of PBA/MOF and the electronic conductivity of metal compound/carbon. Although the calcination under different atmospheres has been extensively studied, the transformation mechanism of PBA/MOF under hydrothermal conditions remains unclear.
View Article and Find Full Text PDFDemetalation caused by the electrochemical dissolution of metallic Fe atoms is a major challenge for the practical application of Fe─N─C catalysts. Herein, an efficient single metallic Mn active site is constructed to improve the strength of the Fe─N bond, inhibiting the demetalation effect of Fe─N─C. Mn acts as an electron donor inducing more delocalized electrons to reduce the oxidation state of Fe by increasing the electron density, thereby enhancing the Fe─N bond and inhibiting the electrochemical dissolution of Fe.
View Article and Find Full Text PDFJ Colloid Interface Sci
September 2024
Lithium cobalt phosphate (LiCoPO) has great potential to be developed as a cathode material for lithium-ion batteries (LIBs) due to its structural stability and higher voltage platform with a high theoretical energy density. However, the relatively low diffusion of lithium ions still needs to be improved. In this work, Fe and Zn co-doped LiCoPO: LiCoFeZnPO/C is utilized to enhance the battery performance of LiCoPO.
View Article and Find Full Text PDFModulating the microenvironment of single-atom catalysts (SACs) is critical to optimizing catalytic activity. Herein, we innovatively propose a strategy to improve the local reaction environment of Ru single atoms by precisely switching the crystallinity of the support from high crystalline and low crystalline, which significantly improves the hydrogen evolution reaction (HER) activity. The Ru single-atom catalyst anchored on low-crystalline nickel hydroxide (Ru-LC-Ni(OH) ) reconstructs the distribution balance of the interfacial ions due to the activation effect of metal dangling bonds on the support.
View Article and Find Full Text PDFNeutral oxygen evolution reaction (OER) with unique reactive environments exhibits extremely slow reaction kinetics, posing significant challenges in the design of catalysts. Herein, a built-in electric field between the tungstate (Ni-FeWO ) with adjustable work function and Lewis acid WO is elaborately constructed to regulate asymmetric interfacial electron distribution, which promotes electron accumulation of Fe sites in the tungstate. This decelerates the rapid dissolution of Fe under the OER potentials, thereby retaining the active hydroxyl oxide with the optimized OER reaction pathway.
View Article and Find Full Text PDFDesigning stable single-atom electrocatalysts with lower energy barriers is urgent for the acidic oxygen evolution reaction. In particular, the atomic catalysts are highly dependent on the kinetically sluggish acid-base mechanism, limiting the reaction paths of intermediates. Herein, we successfully manipulate the steric localization of Ru single atoms at the CoO surface to improve acidic oxygen evolution by precise control of the anchor sites.
View Article and Find Full Text PDFDesigning novel single-atom catalysts (SACs) supports to modulate the electronic structure is crucial to optimize the catalytic activity, but rather challenging. Herein, a general strategy is proposed to utilize the metalloid properties of supports to trap and stabilize single-atoms with low-valence states. A series of single-atoms supported on the surface of tungsten carbide (M-WC , M=Ru, Ir, Pd) are rationally developed through a facile pyrolysis method.
View Article and Find Full Text PDFMolybdenum selenium (MoSe ) has tremendous potential in potassium-ion batteries (PIBs) due to its large interlayer distance, favorable bandgap, and high theoretical specific capacity. However, the poor conductivity and large K insertion/extraction in MoSe inevitably leads to sluggish reaction kinetics and poor structural stability. Herein, Coinduced engineering is employed to illuminate high-conductivity electron pathway and mobile ion diffusion of MoSe nanosheets anchored on reduced graphene oxide substrate (Co-MoSe /rGO).
View Article and Find Full Text PDFDual-carbon engineering combines the advantages of graphite and hard carbon, thereby optimizing the potassium storage performance of carbon materials. However, dual-carbon engineering faces challenges balancing specific capacity, capability, and stability. In this study, we present a coordination engineering of Zn-N moieties on dual-carbon through additional P doping, which effectively modulates the symmetric charge distribution around the Zn center.
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