Strengthened d-p orbital hybridization and hydrogen diffusion in a hollow N-doped porous carbon/Ru cluster catalyst system for hydrogen evolution reactions.

Developing advanced catalysts with rapid hydrogen evolution reaction (HER) kinetics in alkaline media is vital for hydrogen production. Through the d-p orbital hybridization effect, the electronic structure and H* adsorption can be optimized on metal species. Herein, a N-doped hollow carbon (H-NPC)-supported Ru cluster (c-Ru@H-NPC) catalyst was constructed carbonization of well-defined hollow metal-organic frameworks, followed by etching and anchoring of Ru clusters.

Ultrafast Synthesis of Nanoscale Metal Borides for Efficient Hydrogen Evolution.

Nanoscale metal borides, with exceptional physicochemical properties, have been attracted widespread attention. However, traditional synthesis methods of metal borides often lead to surface coking and large particle sizes. Herein, we have employed a flash Joule heating (FJH) technique to enable the ultrafast synthesis of metal boride nanomaterials.

Twin-distortion modulated ultra-low coordination PtRuNi-O catalyst for enhanced hydrogen production from chemical wastewater.

The development of efficient and robust catalysts for hydrogen evolution reaction is crucial for advancing the hydrogen economy. In this study, we demonstrate that ultra-low coordinated hollow PtRuNi-O nanocages exhibit superior catalytic activity and stability across varied conditions, notably surpassing commercial Pt/C catalysts. Notably, the PtRuNi-O catalysts achieve current densities of 10 mA cm at only 19.

Dynamic Micelle-Hydrogels for 3D-Architected Transition Metal Sulfides.

Additive manufacturing of transition metal sulfides (TMS) enables the creation of complex 3D structures, significantly expanding their applications. However, preparing 3D-structured TMS remains challenging due to difficulties in developing suitable inks. In this study, a supramolecular micelle hydrogel as the ink to fabricate 3D-structured TMS is utilized.

Dual active site-mediated Ir single-atom-doped RuO catalysts for highly efficient and stable water splitting.

The electronic structure modulation through heterogeneous single-atom doping is an effective strategy to improve electrocatalysis performance of catalysts. Here, Ir single-atom doped RuO (Ir/RuO) is constructed by substituting Ru sites with mono-disperse Ir atoms in RuO crystals. The Ir/RuO-850 catalyst shows excellent activity for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline media, with overpotentials of only 37 and 234 mV respectively, at a current density of 10 mA cm, lower than that of commercial Pt/C (39 mV-HER) and RuO (295 mV-OER).

Hydrogen Evolution Reactivity of Pentagonal Carbon Rings and p-d Orbital Hybridization Effect with Ru.

Topological defects are inevitable existence in carbon-based frameworks, but their intrinsic electrocatalytic activity and mechanism remain under-explored. Herein, the hydrogen evolution reaction (HER) of pentagonal carbon-rings is probed by constructing pentagonal ring-rich carbon (PRC), with optimized electronic structures and higher HER activity relative to common hexagonal carbon (HC). Furthermore, to improve the reactivity, we couple Ru clusters with PRC (Ru@PRC) through p-d orbital hybridization between C and Ru atoms, which drives a shortcut transfer of electrons from Ru clusters to pentagonal rings.

Molten Salt-Assisted Synthesis of Catalysts for Energy Conversion.

A breakthrough in manufacturing procedures often enables people to obtain the desired functional materials. For the field of energy conversion, designing and constructing catalysts with high cost-effectiveness is urgently needed for commercial requirements. Herein, the molten salt-assisted synthesis (MSAS) strategy is emphasized, which combines the advantages of traditional solid and liquid phase synthesis of catalysts.

Hollow Structure Derived Phosphide Nanosheets for Water Oxidation.

Avoiding the stacking of active sites in catalyst structural design is a promising route for realizing active oxygen evolution reaction (OER). Herein, using a CoFe Prussian blue analoge cube with hollow structure (C-CoFe PBA) as a derived support, a highly effective NiP-FeP-CoP catalyst with a larger specific surface area is reported. Benefiting from the abundant active sites and fast charge transfer capability of the phosphide nanosheets, the NiP-FeP-CoP catalyst in 1 m KOH requires only overpotentials of 248 and 277 mV to reach current density of 10 and 50 mA cm and outperforms the commercial catalyst RuO and most reported non-noble metal OER catalysts.

Entropy-increased LiMnO-based positive electrodes for fast-charging lithium metal batteries.

Fast-charging, non-aqueous lithium-based batteries are desired for practical applications. In this regard, LiMnO is considered an appealing positive electrode active material because of its favourable ionic diffusivity due to the presence of three-dimensional Li-ion diffusion channels. However, LiMnO exhibits inadequate rate capabilities and rapid structural degradation at high currents.

Non-Noble-Metal-Based Electrocatalysts for Acidic Oxygen Evolution Reaction: Recent Progress, Challenges, and Perspectives.

The oxygen evolution reaction (OER) plays a pivotal role in diverse renewable energy storage and conversion technologies, including water electrolysis, electrochemical CO reduction, nitrogen fixation, and metal-air batteries. Among various water electrolysis techniques, proton exchange membrane (PEM)-based water electrolysis devices offer numerous advantages, including high current densities, exceptional chemical stability, excellent proton conductivity, and high-purity H. Nevertheless, the prohibitive cost associated with Ir/Ru-based OER electrocatalysts poses a significant barrier to the broad-scale application of PEM-based water splitting.

Boron-Induced Interstitial Effects Drive Water Oxidation on Ordered Ir-B Compounds.

Interstitial filling of light atoms strongly affects the electronic structure and adsorption properties of the parent catalyst due to ligand and ensemble effects. Different from the conventional doping and surface modification, constructing ordered intermetallic structures is more promising to overcome the dissolution and reconstruction of active sites through strong interactions generated by atomic periodic arrangement, achieving joint improvement in catalytic activity and stability. However, for tightly arranged metal lattices, such as iridium (Ir), obtaining ordered filling atoms and further unveiling their interstitial effects are still limited by highly activated processes.

Sharply expanding single-atomically dispersed Fe-N active sites through bidirectional coordination for oxygen reduction.

For Fe-NC systems, high-density Fe-N sites are the basis for high-efficiency oxygen reduction reaction (ORR), and P doping can further lower the reaction energy barrier, especially in the form of metal-P bonding. However, limited to the irregular agglomeration of metal atoms at high temperatures, Fe-P bonds and high-density Fe-N cannot be guaranteed simultaneously. Here, to escape the random and violent agglomeration of Fe species during high-temperature carbonization, triphenylphosphine and 2-methylimidazole with a strong metal coordination capability are introduced together to confine Fe growth.

Hybrid supercapacitors using metal-organic framework derived nickel-sulfur compounds.

Hypothesis: Metal-organic frameworks (MOFs) are highly suitable precursors for supercapacitor electrode materials owing to their high porosity and stable backbone structures that offer several advantages for redox reactions and rapid ion transport.

Experiments: In this study, a carbon-coated NiS composite (NiS@C-5) was prepared via sulfuration at 500 ℃ using a spherical Ni-MOF as the sacrificial template.

Finding: The stable carbon skeleton derived from Ni-MOF and positive structure-activity relationship due to the multinuclear NiS components resulted in a specific capacity of 278.

Symmetry-Broken Ru Nanoparticles with Parasitic Ru-Co Dual-Single Atoms Overcome the Volmer Step of Alkaline Hydrogen Oxidation.

Efficient dual-single-atom catalysts are crucial for enhancing atomic efficiency and promoting the commercialization of fuel cells, but addressing the sluggish kinetics of hydrogen oxidation reaction (HOR) in alkaline media and the facile dual-single-atom site generation remains formidable challenges. Here, we break the local symmetry of ultra-small ruthenium (Ru) nanoparticles by embedding cobalt (Co) single atoms, which results in the release of Ru single atoms from Ru nanoparticles on reduced graphene oxide (Co Ru /rGO). In situ operando spectroscopy and theoretical calculations reveal that the oxygen-affine Co atom disrupts the symmetry of ultra-small Ru nanoparticles, resulting in parasitic Ru and Co dual-single-atom within Ru nanoparticles.

Constructing Symmetry-Mismatched RuFeO Heterointerface-Supported Ru Clusters for Efficient Hydrogen Evolution and Oxidation Reactions.

Ru-related catalysts have shown excellent performance for the hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR); however, a deep understanding of Ru-active sites on a nanoscale heterogeneous support for hydrogen catalysis is still lacking. Herein, a click chemistry strategy is proposed to design Ru cluster-decorated nanometer RuFeO heterointerfaces (Ru/RuFeO) as highly effective bifunctional hydrogen catalysts. It is found that introducing Ru into nanometric FeO species breaks the symmetry configuration and optimizes the active site in Ru/RuFeO for HER and HOR.

Correlating Single-Atomic Ruthenium Interdistance with Long-Range Interaction Boosts Hydrogen Evolution Reaction Kinetics.

Correlated single-atom catalysts (c-SACs) with tailored intersite metal-metal interactions are superior to conventional catalysts with isolated metal sites. However, precise quantification of the single-atomic interdistance (SAD) in c-SACs is not yet achieved, which is essential for a crucial understanding and remarkable improvement of the correlated metal-site-governed catalytic reaction kinetics. Here, three Ru c-SACs are fabricated with precise SAD using a planar organometallic molecular design and π-π molecule-carbon nanotube confinement.

Ru Cluster Incorporated NiMoO(P) Nanosheet Arrays as High-Efficient Bifunctional Catalyst for Wind/Solar-To-Hydrogen Generation Systems.

Developing cost-efficient bifunctional water splitting catalysts is crucial for sustainable hydrogen energy applications. Herein, ruthenium (Ru)-incorporated and phosphorus (P)-doped nickel molybdate (Ru-NiMoO(P) ) nanosheet array catalysts are synthesized. Due to the synergy of Ru clusters and NiMoO(P) by the modulated electronic structure and the rich active sites, impressively, Ru-NiMoO(P) exhibits superior OER (194 mV @ 50 mA cm ) and HER (24 mV @ 10 mA cm ) activity in alkaline media, far exceeding that of commercial Pt/C and RuO catalysts.

Ge-Regulated Ordered Phase in Pseudosphere-Structured LiNiMnO Spinel Effectively Inhibits Mn Dissolution.

Due to the higher energy density, high thermal stability, and low cost, LiNiMnO (LNMO) spinel, with a large voltage operating window, has been one of the most promising cathode materials for lithium-ion batteries (LIBs). However, the interfacial reaction between the cathode and electrolyte and the two-phase reaction within the bulk of LNMO would destroy the original structure and lead to capacity deterioration, posing a significant challenge. Therefore, the way to suppress the transition-metal (TM) dissolution in LNMO has attracted much attention.

Tuning Active Metal Atomic Spacing by Filling of Light Atoms and Resulting Reversed Hydrogen Adsorption-Distance Relationship for Efficient Catalysis.

Precisely tuning the spacing of the active centers on the atomic scale is of great significance to improve the catalytic activity and deepen the understanding of the catalytic mechanism, but still remains a challenge. Here, we develop a strategy to dilute catalytically active metal interatomic spacing (d) with light atoms and discover the unusual adsorption patterns. For example, by elevating the content of boron as interstitial atoms, the atomic spacing of osmium (d) gradually increases from 2.

Monomicelle-Directed Engineering of Strained Carbon Nanoribbons as Oxygen Reduction Catalyst.

To date, precisely tailoring local active sites of well-defined earth-abundant metal-free carbon-based electrocatalysts for attractive electrocatalytic oxygen reduction reaction (ORR), remains challenging. Herein, the authors successfully introduce a strain effect on active C-C bonds adjacent to edged graphitic nitrogen (N), which raises appropriate spin-polarization and charge density of carbon active sites and kinetically favor the facilitation of O adsorption and the activation of O-containing intermediates. Thus, the constructed metal-free carbon nanoribbons (CNRs-C) with high-curved edges exhibit outstanding ORR activity with half-wave potentials of 0.

Fe-Regulated Amorphous-Crystal Ni(Fe)P Nanosheets Coupled with Ru Powerfully Drive Seawater Splitting at Large Current Density.

Water electrolysis is an ideal method for industrial green hydrogen production. However, due to increasing scarcity of freshwater, it is inevitable to develop advanced catalysts for electrolyzing seawater especially at large current density. This work reports a unique Ru nanocrystal coupled amorphous-crystal Ni(Fe)P nanosheet bifunctional catalyst (Ru-Ni(Fe)P /NF), caused by partial substitution of Fe to Ni atoms in Ni(Fe)P , and explores its electrocatalytic mechanism by density functional theory (DFT) calculations.