Recent progress of density functional theory studies on carbon-supported single-atom catalysts for energy storage and conversion.

Single-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.

investigation of hot electron transfer in CO plasmonic photocatalysis in the presence of hydroxyl adsorbate.

Photoreduction of carbon dioxide (CO) on plasmonic structures is of great interest in photocatalysis to aid selectivity. While species commonly found in reaction environments and associated intermediates can steer the reaction down different pathways by altering the potential energy landscape of the system, they are often not addressed when designing efficient plasmonic catalysts. Here, we perform an atomistic study of the effect of the hydroxyl group (OH) on CO activation and hot electron generation and transfer using first-principles calculations.

Electrocatalytic Urea Synthesis via N Dimerization and Universal Descriptor.

Electrocatalytic urea synthesis through N + CO coreduction and C-N coupling is a promising and sustainable alternative to harsh industrial processes. Despite considerable efforts, limited progress has been made due to the challenges of breaking inert N≡N bonds for C-N coupling, competing side reactions, and the absence of theoretical principles guiding catalyst design. In this study, we propose a mechanism for highly electrocatalytic urea synthesis using two adsorbed N molecules and CO as nitrogen and carbon sources, respectively.

High density electron doping in boron-doped twisted bilayer graphene: a ladder to extended flat-band.

Realizing Von Hove singularity (VHS) and extended flat bands of graphene near the Fermi level () is of great significance to explore many-body interactions, with a high tendency towards superconductivity. In this study, we report that the VHS of π* bands near can be realized by high-density lithium intercalation in p-type doped twisted bilayer graphene (tBLG). First, a method to predict the highest lithium intercalation in tBLG systems with arbitrary twist angle was established which proves that the interlayer twisting leads to the clustering of lithium ions in the AA-region but reduces the overall concentration.

Lithium intercalation in two-dimensional penta-NiN: insights from NiN/NiN homostructure and G/NiN heterostructure.

High-energy-density lithium-ion batteries (LIBs) are essential to meet the requirements of emerging technologies for advanced power storage and enhanced device performance. The next generation of LIBs will require high-capacity anode materials that move beyond the lithium intercalation chemistry of conventional graphite electrodes. The use of two-dimensional (2D) bilayer structures offers immediate advantages in the development of LIBs.

A high-energy-density NASICON-type NaVGa(PO) cathode with reversible V/V redox couple for sodium ion batteries.

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)).

Analytic description of nanowires II: morphing of regular cross sections for zincblende- and diamond-structures to match arbitrary shapes. Corrigendum.

Corrections to the article by König and Smith [Acta Cryst. (2022), B78, 643-664] are given.

Analytical description of nanowires III: regular cross sections for wurtzite structures.

Setting out from König & Smith [Acta Cryst. (2019), B75, 788-802; Acta Cryst. (2021), B77, 861], we present an analytic description of nominal wurtzite-structure nanowire (NWire) cross sections, focusing on the underlying geometric-crystallographic description and on the associated number theory.

Analytic description of nanowires II: morphing of regular cross sections for zincblende- and diamond-structures to match arbitrary shapes.

Setting out from our recent publication [König & Smith (2021). Acta Cryst. B77, 861], we extend our analytic description of the regular cross sections of zincblende- and diamond-structure nanowires (NWires) by introducing cross section morphing to arbitrary convex shapes featuring linear interfaces as encountered in experiment.

Modulating Pt-O-Pt atomic clusters with isolated cobalt atoms for enhanced hydrogen evolution catalysis.

Platinum is the most efficient catalyst for hydrogen evolution reaction in acidic conditions, but its widespread use has been impeded by scarcity and high cost. Herein, Pt atomic clusters (Pt ACs) containing Pt-O-Pt units were prepared using Co/N co-doped carbon (CoNC) as support. Pt ACs are anchored to single Co atoms on CoNC by forming strong interactions.

Electronic Regulation of Nickel Single Atoms by Confined Nickel Nanoparticles for Energy-Efficient CO Electroreduction.

Modulating the electronic structure of atomically dispersed active sites is promising to boost catalytic activity but is challenging to achieve. Here we show a cooperative Ni single-atom-on-nanoparticle catalyst (NiSA/NP) prepared via direct solid-state pyrolysis, where Ni nanoparticles donate electrons to Ni(i)-N-C sites via a network of carbon nanotubes, achieving a high CO current density of 346 mA cm at -0.5 V vs RHE in an alkaline flow cell.

Sulfur-Dopant-Promoted Electroreduction of CO over Coordinatively Unsaturated Ni-N Moieties.

Atomically dispersed nickel-nitrogen-carbon (Ni-N-C) moieties are promising for efficient electrochemical CO -to-CO conversion. To improve the intrinsic electrocatalytic activity, it is essential but challenging to steer the coordination environment of Ni centers for promoting the CO formation kinetics. Here, we introduce alien sulfur atoms to tune the local electronic density of unsaturated NiN species.

Intrinsic ORR Activity Enhancement of Pt Atomic Sites by Engineering the d-Band Center via Local Coordination Tuning.

A considerable amount of platinum (Pt) is required to ensure an adequate rate for the oxygen reduction reaction (ORR) in fuel cells and metal-air batteries. Thus, the implementation of atomic Pt catalysts holds promise for minimizing the Pt content. In this contribution, atomic Pt sites with nitrogen (N) and phosphorus (P) co-coordination on a carbon matrix (PtNPC) are conceptually predicted and experimentally developed to alter the d-band center of Pt, thereby promoting the intrinsic ORR activity.

Broadbill swordfish (Xiphias gladius) foraging and vertical movements in the north-west Atlantic.

The northern edge of Georges Bank is an important seasonal foraging habitat for swordfish (Xiphias gladius) in the North Atlantic, where aggregations support commercial pelagic longline and harpoon fisheries. Following a period of overfishing during the 1990s, the North Atlantic X. gladius stock underwent a period of recovery during the early 2000s and was considered rebuilt in 2009.

Template-Directed Rapid Synthesis of Pd-Based Ultrathin Porous Intermetallic Nanosheets for Efficient Oxygen Reduction.

Atomically ordered intermetallic nanoparticles exhibit improved catalytic activity and durability relative to random alloy counterparts. However, conventional methods with time-consuming and high-temperature syntheses only have rudimentary capability in controlling the structure of intermetallic nanoparticles, hindering advances of intermetallic nanocatalysts. We report a template-directed strategy for rapid synthesis of Pd-based (PdM, M=Pb, Sn and Cd) ultrathin porous intermetallic nanosheets (UPINs) with tunable sizes.

Isolated copper-tin atomic interfaces tuning electrocatalytic CO conversion.

Direct experimental observations of the interface structure can provide vital insights into heterogeneous catalysis. Examples of interface design based on single atom and surface science are, however, extremely rare. Here, we report Cu-Sn single-atom surface alloys, where isolated Sn sites with high surface densities (up to 8%) are anchored on the Cu host, for efficient electrocatalytic CO reduction.

Atomically Dispersed Indium Sites for Selective CO Electroreduction to Formic Acid.

An atomically dispersed structure is attractive for electrochemically converting carbon dioxide (CO) to fuels and feedstock due to its unique properties and activity. Most single-atom electrocatalysts are reported to reduce CO to carbon monoxide (CO). Herein, we develop atomically dispersed indium (In) on a nitrogen-doped carbon skeleton (In-N-C) as an efficient catalyst to produce formic acid/formate in aqueous media, reaching a turnover frequency as high as 26771 h at -0.

An Ultra-Long-Life Flexible Lithium-Sulfur Battery with Lithium Cloth Anode and Polysulfone-Functionalized Separator.

Flexible and high-performance batteries are urgently required for powering flexible/wearable electronics. Lithium-sulfur batteries with a very high energy density are a promising candidate for high-energy-density flexible power source. Here, we report flexible lithium-sulfur full cells consisting of ultrastable lithium cloth anodes, polysulfone-functionalized separators, and free-standing sulfur/graphene/boron nitride nanosheet cathodes.

Efficient Water Splitting Actualized through an Electrochemistry-Induced Hetero-Structured Antiperovskite/(Oxy)Hydroxide Hybrid.

Exploring active, stable, and low-cost bifunctional electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is crucial for water splitting technology associated with renewable energy storage in the form of hydrogen fuel. Here, a newly designed antiperovskite-based hybrid composed of a conductive InNNi core and amorphous InNi(oxy)hydroxide shell is first reported as promising OER/HER bifunctional electrocatalyst. Prepared by a facile electrochemical oxidation strategy, such unique hybrid (denoted as EO-InNNi ) exhibits excellent OER and HER activities in alkaline media, benefiting from the inherent high-efficiency HER catalytic nature of InNNi antiperovskite and the promoting role of OER-active InNi(oxy)hydroxide thin film, which is confirmed by theoretical simulations and in situ Raman studies.

Single-phase perovskite oxide with super-exchange induced atomic-scale synergistic active centers enables ultrafast hydrogen evolution.

The state-of-the-art active HER catalysts in acid media (e.g., Pt) generally lose considerable catalytic performance in alkaline media mainly due to the additional water dissociation step.

Design guidelines for transition metals as interstitial emitters in silicon nanocrystals to tune photoluminescence properties: zinc as biocompatible example.

Silicon nanocrystals (Si NCs) are attractive candidates for biomarkers in medical imaging. Building on recent work [McVey et al., J.

Analytical description of nanowires. I. Regular cross sections for zincblende and diamond structures.

Semiconductor nanowires (NWires) experience stress and charge transfer from their environment and impurity atoms. In response, the environment of a NWire experiences a NWire stress response which may lead to propagated strain and a change in the shape and size of the NWire cross section. Here, geometric number series are deduced for zincblende- (zb-) and diamond-structured NWires of diameter d to obtain the numbers of NWire atoms N(d[i]), bonds between NWire atoms N(d[i]) and interface bonds N(d[i]) for six high-symmetry zb NWires with the low-index faceting that occurs frequently in both bottom-up and top-down approaches of NWire processing.

Surface Reconstruction of Ultrathin Palladium Nanosheets during Electrocatalytic CO Reduction.

A surface reconstructing phenomenon is discovered on a defect-rich ultrathin Pd nanosheet catalyst for aqueous CO electroreduction. The pristine nanosheets with dominant (111) facet sites are transformed into crumpled sheet-like structures prevalent in electrocatalytically active (100) sites. The reconstruction increases the density of active sites and reduces the CO binding strength on Pd surfaces, remarkably promoting the CO reduction to CO.

Implanting Ni-O-VOx sites into Cu-doped Ni for low-overpotential alkaline hydrogen evolution.

Nickel-based catalysts are most commonly used in industrial alkaline water electrolysis. However, it remains a great challenge to address the sluggish reaction kinetics and severe deactivation problems of hydrogen evolution reaction (HER). Here, we show a Cu-doped Ni catalyst implanted with Ni-O-VOx sites (Ni(Cu)VOx) for alkaline HER.

Boosting Oxygen Evolution Reaction by Creating Both Metal Ion and Lattice-Oxygen Active Sites in a Complex Oxide.

Developing efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) is of paramount importance to many chemical and energy transformation technologies. The diversity and flexibility of metal oxides offer numerous degrees of freedom for enhancing catalytic activity by tailoring their physicochemical properties, but the active site of current metal oxides for OER is still limited to either metal ions or lattice oxygen. Here, a new complex oxide with unique hexagonal structure consisting of one honeycomb-like network, Ba Sr (Co Fe ) O (hex-BSCF), is reported, demonstrating ultrahigh OER activity because both the tetrahedral Co ions and the octahedral oxygen ions on the surface are active, as confirmed by combined X-ray absorption spectroscopy analysis and theoretical calculations.