Rational engineering of the surfaces of heterogeneous catalysts (especially the surfaces of supported metals) can endow intriguing catalytic functionalities for electrochemical reactions. However, it often requires complicated steps, and even if it does not, breaking the trade-off between activity and stability is quite challenging. Herein, we present a strategy for reconstructing supported catalysts via in situ growth of metallic nanolayers from the perovskite oxide support.
View Article and Find Full Text PDFTwo-dimensional (2D) semiconductors, particularly transition metal dichalcogenides (TMDs), are promising for advanced electronics beyond silicon. Traditionally, TMDs are epitaxially grown on crystalline substrates by chemical vapour deposition. However, this approach requires post-growth transfer to target substrates, which makes controlling thickness and scalability difficult.
View Article and Find Full Text PDFThe dry battery electrode (DBE) process offers significant advantages over conventional wet-coating methods for electrode fabrication. Unlike traditional processes that rely on toxic solvents such as N-methyl-2-pyrrolidone (NMP), the DBE technique uses solvent-free methods, reducing environmental impact and production costs while enhancing compatibility and performance. However, polytetrafluoroethylene (PTFE), the only binder currently used for large-scale DBE fabrication (binder fibrillation), faces potential regulatory restrictions under Polyfluoroalkyl Substances (PFAS) guidelines and limits Li-ion conductivity, elastomeric properties, and particle adhesion.
View Article and Find Full Text PDFDesigning an electrocatalyst that simultaneously satisfies high catalytic activity and surface stability is essential for realizing high-performance lithium-sulfur (Li||S) batteries. Here, we propose an advanced electrocatalyst by constructing a thin protective catalytic layer (PCL) on the surface of metal nanoparticle catalysts. This few atomic layer thicknesses of the PCL composed of pyridinic N embedded graphitic carbon allows electrons to transfer from a metal nanoparticle to pyridinic N, resulting in an optimized p-orbital level of pyridinic N of PCL favorable for highly active conversion reaction of lithium sulfide.
View Article and Find Full Text PDFSupported nanoparticles incorporating catalytically attractive nonmetal elements have gained significant attention as a promising strategy for enhancing catalytic activity in various industrial applications. This study presents an innovative one-pot synthesis method for fabricating hybrid catalysts, which simultaneously modifies surface properties through the precipitation of nanoparticles with the concurrent incorporation of nonmetal elements. The underlying concept is to synchronize the temperature required for particle formation with that of nonmetal incorporation by adjusting the oxygen chemical potential of the host oxide.
View Article and Find Full Text PDFThe development of accurate methods for determining how alloy surfaces spontaneously restructure under reactive and corrosive environments is a key, long-standing, grand challenge in materials science. Using machine learning-accelerated density functional theory and rare-event methods, in conjunction with environmental transmission electron microscopy (ETEM), we examine the interplay between surface reconstructions and preferential segregation tendencies of CuNi(100) surfaces under oxidation conditions. Our modeling approach predicts that oxygen-induced Ni segregation in CuNi alloys favors Cu(100)-O c(2 × 2) reconstruction and destabilizes the Cu(100)-O (2√2 × √2)45° missing row reconstruction (MRR).
View Article and Find Full Text PDFForming defect sites on catalyst supports and immobilizing precious metal atoms at these sites offers an efficient approach for preparing single-atom catalysts. In this study, we employed an Fe-Ce oxide solid solution (FC), which has surface oxygen that reduces more readily than that of ceria, to anchor Rh single atoms (Rh). When utilized in the selective catalytic reduction of NO with CO (CO-SCR), Rh/FC reduced at 500 °C-characterized by less oxidic Rh state induced by an oxygen-deficient coordination-exhibited superior activity and durability compared to Rh/ceria and Rh/FC reduced at 300 °C.
View Article and Find Full Text PDFWater is pursued as an electrolyte solvent for its non-flammable nature compared to traditional organic solvents, yet its narrow electrochemical stability window (ESW) limits its performance. Solvation chemistry design is widely adopted as the key to suppress the reactivity of water, thereby expanding the ESW. In this study, an acetamide-based ternary eutectic electrolyte achieved an ESW ranging from 1.
View Article and Find Full Text PDFThe chemical conversion of CO into value-added products is the key technology to realize a carbon-neutral society. One representative example of such conversion is the reverse water-gas shift reaction, which produces CO from CO. However, the activity is insufficient at ambient pressure and lower temperatures (<600 °C), making it a highly energy-intensive and impractical process.
View Article and Find Full Text PDFThe octahedral symmetry in ionic crystals can play a critical role in atomic nucleation and migration during solid-solid phase transformation. Similarly, octahedron distortion, which is characterized by Goldschmidt tolerance factor, strongly influences the exsolution kinetics in the perovskite lattice framework during high-temperature annealing. However, a fundamental study on manipulating the exsolution process by octahedron distortion is still lacking.
View Article and Find Full Text PDFChlorine has been supplied by the chlor-alkali process that deploys dimensionally stable anodes (DSAs) for the electrochemical chlorine evolution reaction (ClER). The paramount bottlenecks have been ascribed to an intensive usage of precious elements and inevitable competition with the oxygen evolution reaction. Herein, a unique case of Ru-O active motifs anchored on Magnéli TiO (Ru-TiO) via a straightforward wet impregnation and mild annealing is reported.
View Article and Find Full Text PDFNumerous systematic methods have been developed to search for the global minimum of the potential energy surface, which corresponds to the optimal atomic structure. However, the majority of them still demand a substantial computing load due to the relaxation process that is embedded as an inner step inside the algorithm. Here, we propose a hybrid approach that combines Bayesian optimization (BO) and a local search that circumvents the relaxation step and efficiently finds the optimum structure, particularly in supported metal systems.
View Article and Find Full Text PDFThe 1T phase of MoS exhibits much higher electrocatalytic activity and better stability than the 2H phase. However, the harsh conditions of 1T phase synthesis remain a significant challenge for various extensions and applications of MoS. In this work, a simple hydrothermal-based synthesis method for the phase transition of MoS is being developed.
View Article and Find Full Text PDFA key issue in lithium-ion batteries is understanding the solid electrolyte interphase (SEI) resulting from a reductive reaction on the anode/electrolyte interface. The presence of the SEI layer affects the transport behavior of the ions and electrons between the anode and electrolyte. Despite the influence on interfacial properties, the formation and evolution mechanism of the SEI layer are unclear owing to their complexity and dynamic nature.
View Article and Find Full Text PDFSingle-atom nanozymes (SAzymes) constitute a promising category of enzyme-mimicking materials with outstanding catalytic performance. The performance of SAzymes improves through modification of the coordination environments around the metal center. However, the catalytic turnover rates of SAzymes, which are key measures of the effectiveness of active site modifications, remain lower than those of natural enzymes, especially in peroxidase-reactions.
View Article and Find Full Text PDFMetal nanoparticle-organic interfaces are common but remain elusive for controlling reactions due to the complex interactions of randomly formed ligand-layers. This paper presents an approach for enhancing the selectivity of catalytic reactions by constructing a skin-like few-nanometre ultrathin crystalline porous covalent organic overlayer on a plasmonic nanoparticle surface. This organic overlayer features a highly ordered layout of pore openings that facilitates molecule entry without any surface poisoning effects and simultaneously endows favourable electronic effects to control molecular adsorption-desorption.
View Article and Find Full Text PDFStrong circularly polarized excitation opens up the possibility to generate and control effective magnetic fields in solid state systems, e.g., via the optical inverse Faraday effect or the phonon inverse Faraday effect.
View Article and Find Full Text PDFObjectives: Focused ultrasound (FUS) therapy has emerged as a promising noninvasive solution for tumor ablation. Accurate monitoring and guidance of ultrasound energy is crucial for effective FUS treatment. Although ultrasound (US) imaging is a well-suited modality for FUS monitoring, US-guided FUS (USgFUS) faces challenges in achieving precise monitoring, leading to unpredictable ablation shapes and a lack of quantitative monitoring.
View Article and Find Full Text PDFAdvanced energy-storage devices are indispensable for expanding electric mobility applications. While anion intercalation-type redox chemistry in graphite cathodes has opened the path to high-energy-density batteries, surpassing the limited energy density of conventional lithium-ion batteries , a significant challenge remains: the large volume expansion of graphite upon anion intercalation. In this study, a novel polymeric binder and cohesive graphite cathode design for dual-ion batteries (DIBs) is presented, which exhibits remarkable stability even under high voltage conditions (>5 V).
View Article and Find Full Text PDFThe performance of nanocrystal (NC) catalysts could be maximized by introducing rationally designed heterointerfaces formed by the facet- and spatio-specific modification with other materials of desired size and thickness. However, such heterointerfaces are limited in scope and synthetically challenging. Herein, we applied a wet chemistry method to tunably deposit Pd and Ni on the available surfaces of porous 2D-Pt nanodendrites (NDs).
View Article and Find Full Text PDFNanoparticle (NP) exsolution from perovskite-based oxides matrix upon reduction has emerged as an ideal platform for designing highly active catalysts for energy and environmental applications. However, the mechanism of how the material characteristics impacts the activity is still ambiguous. In this work, taking PrSrCoFeNbO thin film as the model system, we demonstrate the critical impact of the exsolution process on the local surface electronic structure.
View Article and Find Full Text PDFTwo essential characteristics that are required for hybrid electrocatalysts to exhibit higher oxygen and hydrogen evolution reaction (OER and HER, respectively) activity are a favorable electronic configuration and a sufficient density of active sites at the interface between the two materials within the hybrid. In the present study, a hybrid electrocatalyst is introduced with a novel architecture consisting of coral-like iron nitride (Fe N) arrays and tungsten nitride (W N ) nanosheets that satisfies these requirements. The resulting W N /Fe N catalyst achieves high OER activity (268.
View Article and Find Full Text PDFPseudo-capacitive negative electrodes remain a major bottleneck in the development of supercapacitor devices with high energy density because the electric double-layer capacitance of the negative electrodes does not match the pseudocapacitance of the corresponding positive electrodes. In the present study, a strategically improved Ni-Co-Mo sulfide is demonstrated to be a promising candidate for high energy density supercapattery devices due to its sustained pseudocapacitive charge storage mechanism. The pseudocapacitive behavior is enhanced when operating under a high current through the addition of a classical Schottky junction next to the electrode-electrolyte interface using atomic layer deposition.
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