Optimal design of Ru-Sn oxide catalysts for enhanced oxygen evolution reaction using the cluster-plus-glue-atom model.

Using the cluster-plus-glue-atom model, we optimized Ru-Sn oxide catalysts for the oxygen evolution reaction (OER). Optimal performance is achieved when all glue-atom sites are occupied by Sn (, Ru : Sn = 1 : 2), thereby maximizing both OER activity and stability. This work provides novel insights and a rapid strategy for designing efficient, stable Ru-based catalysts.

Ultralow Content of Chromium Species in Zeolite for Efficient Catalytic Propane Dehydrogenation.

Supported chromia catalysts have been commercially used in propane dehydrogenation, which relies on Cr loading at weight fractions of up to 20 wt %. This leads to problems in managing spent catalysts with a high content of toxic chromium species. These catalysts also rapidly deactivate within 10-15 min, requiring frequent regeneration in each cycle.

Unconventional phase metal heteronanostructures with tunable exposed interface for efficient tandem nitrate electroreduction to ammonia.

Tandem catalysis is an effective approach to achieve highly selective and high-rate multi-electron/proton transfer reactions, such as nitrate electroreduction, which are important for various physicochemical and biological processes. However, present tandem catalysts suffer from uncontrollable interface, limited crystal phase, and complex synthesis protocols. Here, we report facile seed-mediated synthesis of unconventional phase 4H/fcc Au-Cu heterostructures with a unique beaded-bracelet nanostructure (BBN).

Unveiling Long-Range Wavelike Alternately Competitive and Cooperative Bond Coupling Modes in Single-Atom Catalysis.

Supports can critically influence or even dominate the chemical state, adsorption property, and catalytic performance of single-atom catalysts (SACs), but the fundamental physicochemical principles driving adsorbate-M-ligand-support bond interactions have not been fully understood yet. Here, we reveal the orbital-level interaction modes underlying the long-range bond couplings in SACs by using single-atom Ru (Ru) supported on rutile-type oxides (TiO, SnO, and MnO) in CO adsorption and oxidation as a model system. Our results show that Ru-support binding strength and catalytic activity for CO oxidation increase in the following order: Ru/TiO < Ru/SnO < Ru/MnO, while CO-Ru adsorption strength oppositely decreases as Ru/TiO > Ru/SnO > Ru/MnO.

Core/Shell-Structured Carbon Support Boosting Fuel Cell Durability.

To enhance the lifetime of proton exchange membrane fuel cells, developing highly durable platinum-based cathode catalysts is essential. While two degradation pathways for the cathode catalyst-carbon corrosion and electrocatalyst (platinum nanoparticles) coarsening-have been identified, current approaches to enhance its durability are limited to addressing individual degradation pathways. Herein, the study develops a core/shell-structured carbon support that is designed to afford cathode catalysts capable of simultaneously inhibiting carbon corrosion and electrocatalyst coarsening.

Cooperative mechanisms of oxide ion conduction in tellurites with secondary bond interactions and Grotthuss-like processes.

Oxide-ion conducting materials are gaining considerable attention in various applications ranging from oxide fuel cells to oxygen permeation membranes. The oxide ion migration mechanisms are the basis for designing oxide-ion conducting materials. Here, enlightened by proton diffusion in hydrogen-bond networks, we report the coordination polyhedra cooperative mechanism with similar Grotthuss process of oxide ion migration in tellurites.

Regulating the Intralayer Cation Disorder in Layered Lithium-Rich Cathodes to Improve Cycle Performance.

The Li/Mn ordered structure of lithium-rich (LR) cathodes leads to the heterogeneous LiMnO and LiTMO components, readily triggering structural degeneration and performance degradation in long-term cycling. However, the lack of guiding principles for promoting cation disorder within the transition metal (TM) layers has posed a persistent challenge in designing homogeneous layered LR cathodes. Herein, the (Li + Mn) content in the TM layer as a criterion for the design of cation-disordered layered LR cathodes is proposed.

Active Learning Guided Discovery of High Entropy Oxides Featuring High H-production.

High entropy oxides (HEOs) represent a class of solid solutions comprising multiple elements, offering significant scientific potential. Due to the enormous combination types of elements, the design of HEOs with desirable properties within high-dimensional composition spaces has traditionally relied heavily on knowledge and intuition. In this study, we present an active learning (AL) strategy tailored to efficiently explore the vast compositional space of HEOs.

Oriented Crystal Polarization Tuning Bulk Charge and Single-Site Chemical State for Exceptional Hydrogen Photo-Production.

Rapid bulk charge recombination and mediocre surface catalytic sites harshly restrict the photocatalytic activities. Herein, the aforementioned concerns are well addressed by coupling macroscopic spontaneous polarization and atomic-site engineering of CdS single-crystal nanorods for superb H photo-production. The oriented growth of CdS nanorods along the polar axis, vectorially superimposing substantial polar units with orderly arrangement, renders a strong polarization electric field (20.

Selective Activation of Lattice Oxygen Site Through Coordination Engineering to Boost the Activity and Stability of Oxygen Evolution Reaction.

Although Ru-based materials are among the outstanding catalysts for the oxygen evolution reaction (OER), the instability issue still haunts them and impedes the widespread application. The instability of Ru-based OER catalysts is generally ascribed to the formation of soluble species through the over-oxidation of Ru and structural decomposition caused by involvement of lattice oxygen. Herein, an effective strategy of selectively activating the lattice oxygen around Ru site is proposed to improve the OER activity and stability.

Site-Selective Growth of fcc-2H-fcc Copper on Unconventional Phase Metal Nanomaterials for Highly Efficient Tandem CO Electroreduction.

Copper (Cu) nanomaterials are a unique kind of electrocatalysts for high-value multi-carbon production in carbon dioxide reduction reaction (CORR), which holds enormous potential in attaining carbon neutrality. However, phase engineering of Cu nanomaterials remains challenging, especially for the construction of unconventional phase Cu-based asymmetric heteronanostructures. Here the site-selective growth of Cu on unusual phase gold (Au) nanorods, obtaining three kinds of heterophase fcc-2H-fcc Au-Cu heteronanostructures is reported.

Surface-Integrating Oxygen Vacancy and CuO Nanodots Enabling Synergistic Electric Field and Dual Catalytic Sites Boosting CO Photoreduction.

High carrier separation efficiency and rapid surface catalytic reaction are crucial for enhancing catalytic CO photoreduction reaction. Herein, integrated surface decoration strategy with oxygen vacancies (Ov) and anchoring CuO (1 < x < 2) nanodots below 10 nm is realized on BiMoO for promoting CO photoreduction performance. The charge interaction between Ov and anchored CuO enables the formation of enhanced internal electric field, which provides a strong driving force for accelerating the separation of photocharge carriers on the surface of BiMoO (η ≈71%).

Enhancing Surface Strain of Intermetallic Fuel Cell Catalysts by Composition-Induced Phase Transition.

The lattice parameter of platinum-based intermetallic compounds (IMCs), which correlates with the intrinsic activity of the oxygen reduction reaction (ORR), can be modulated by crystal phase engineering. However, the controlled preparation of IMCs with unconventional crystal structures remains highly challenging. Here, we demonstrate the synthesis of carbon-supported PtCu-based IMC catalysts with an unconventional L1 structure by a composition-regulated strategy.

Controlled Synthesis of Unconventional Phase Alloy Nanobranches for Highly Selective Electrocatalytic Nitrite Reduction to Ammonia.

The controlled synthesis of metal nanomaterials with unconventional phases is of significant importance to develop high-performance catalysts for various applications. However, it remains challenging to modulate the atomic arrangements of metal nanomaterials, especially the alloy nanostructures that involve different metals with distinct redox potentials. Here we report the general one-pot synthesis of IrNi, IrRhNi and IrFeNi alloy nanobranches with unconventional hexagonal close-packed (hcp) phase.

Coordination Environment Engineering of Metal Centers in Coordination Polymers for Selective Carbon Dioxide Electroreduction toward Multicarbon Products.

Electrocatalytic carbon dioxide reduction reaction (CORR) toward value-added chemicals/fuels has offered a sustainable strategy to achieve a carbon-neutral energy cycle. However, it remains a great challenge to controllably and precisely regulate the coordination environment of active sites in catalysts for efficient generation of targeted products, especially the multicarbon (C) products. Herein we report the coordination environment engineering of metal centers in coordination polymers for efficient electroreduction of CO to C products under neutral conditions.

Artificial neural network for deciphering the structural transformation of condensed ZnO by extended x-ray absorption fine structure spectroscopy.

Pressure-induced structural phase transitions play a pivotal role in unlocking novel material functionalities and facilitating innovations in materials science. Nonetheless, unveiling the mechanisms of densification, which relies heavily on precise and comprehensive structural analysis, remains a challenge. Herein, we investigated the archetypal4 →1 phase transition pathway in ZnO by combining x-ray absorption fine structure (XAFS) spectroscopy with machine learning.

Atomic coordination environment engineering of bimetallic alloy nanostructures for efficient ammonia electrosynthesis from nitrate.

Electrochemical nitrate reduction reaction (NORR) to ammonia has been regarded as a promising strategy to balance the global nitrogen cycle. However, it still suffers from poor Faradaic efficiency (FE) and limited yield rate for ammonia production on heterogeneous electrocatalysts, especially in neutral solutions. Herein, we report one-pot synthesis of ultrathin nanosheet-assembled RuFe nanoflowers with low-coordinated Ru sites to enhance NORR performances in neutral electrolyte.

A Stable and Energy-Dense Polysulfide/Permanganate Flow Battery.

Redox flow batteries (RFBs) as promising technologies for energy storage have attracted burgeoning efforts and have achieved many advances in the past decades. However, for practical applications, the exploration of high-performance RFB systems is still of significance. In this work, inspired by the high solubility and low cost of both polysulfides and permanganates, the S/Mn RFBs with S/S and MnO/MnO as negative and positive redox pairs are demonstrated.

Strong metal oxide-support interaction in MoO/N-doped MCNTs heterostructure for boosting lithium storage performance.

The low-rate capability and fast capacity decaying of the molybdenum dioxide anode material have been a bottleneck for lithium-ion batteries (LIBs) due to low carrier transport, drastic volume expansion and inferior reversibility. Furthermore, the lithium-storage mechanism is still controversial at present. Herein, we fabricate a new kind of MoO nanoparticles with nitrogen-doped multiwalled carbon nanotubes (MoO/N-MCNTs) as anode for LIBs.

Toward Highly Selective Heteroatom Dopants in Hard Carbon with Superior Lithium Storage Performance.

Hard carbons (HCs) have gained much attention for next-generation high energy density lithium-ion battery (LIB) anode candidates. However, voltage hysteresis, low rate capability, and large initial irreversible capacity severely affect their booming application. Herein, a general strategy is reported to fabricate heterogeneous atom (N/S/P/Se)-doped HC anodes with superb rate capability and cyclic stability based on a three-dimensional (3D) framework and a hierarchical porous structure.

Water-Regulated Lead Halide Perovskites Precursor Solution: Perovskite Structure Making and Breaking.

Identifying the impact of water on iodoplumbate complexes in various solutions is essential for linking the coordination environment of the perovskite precursor to its final perovskite solar cell (PSC) properties. In this study, we propose a digital twin approach based on X-ray absorption fine structure and molecular dynamic simulation to investigate the structure evolution of iodoplumbate complexes in precursor solutions as a function of storage time under a constant humidity environment. A full picture about what water does in the perovskite formation process is brought out, and the "making and breaking" role of water molecules is uncovered to link the structure of iodoplumbate complexes to its final properties.

Robust and Wide Temperature-Range Zinc Metal Batteries with Unique Electrolyte and Substrate Design.

Rechargeable zinc metal batteries are promising for large-scale energy storage. However, their practical application is limited by harsh issues such as uncontrollable dendrite growth, low Coulombic efficiency, and poor temperature tolerance. Herein, a unique design strategy using γ-valerolactone-based electrolyte and nanocarbon-coated aluminum substrate was reported to solve the above problems.

Synergy-Compensation Effect of Ferroelectric Polarization and Cationic Vacancy Collaboratively Promoting CO Photoreduction.

Photocatalytic CO reduction is severely limited by the rapid recombination of photo-generated charges and insufficient reactive sites. Creating electric field and defects are effective strategies to inhibit charge recombination and enrich catalytic sites, respectively. Herein, a coupled strategy of ferroelectric poling and cationic vacancy is developed to achieve high-performance CO photoreduction on ferroelectric Bi MoO , and their interesting synergy-compensation relationship is first disclosed.