Regulating Co-O covalency to manipulate mechanistic transformation for enhancing activity/durability in acidic water oxidation.

Developing earth-abundant electrocatalysts with high activity and durability for acidic oxygen evolution reaction is essential for H production, yet it remains greatly challenging. Here, guided by theoretical calculations, the challenge of overcoming the balance between catalytic activity and dynamic durability for acidic OER in CoO was effectively addressed the preferential substitution of Ru for the Co (T) site of CoO. characterization and DFT calculations show that the enhanced Co-O covalency after the introduction of Ru SAs facilitates the generation of OH* species and mitigates the unstable structure transformation direct O-O coupling.

Photothermal CO conversion to ethanol through photothermal heterojunction-nanosheet arrays.

Photothermal CO conversion to ethanol offers a sustainable solution for achieving net-zero carbon management. However, serious carrier recombination and high C-C coupling energy barrier cause poor performance in ethanol generation. Here, we report a Cu/CuSe-CuO heterojunction-nanosheet array, showcasing a good ethanol yield under visible-near-infrared light without external heating.

A General Synthesis of Nanostructured Conductive Metal-Organic Frameworks from Insulating MOF Precursors for Supercapacitors and Chemiresistive Sensors.

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) are emerging as a unique subclass of layer-stacked crystalline coordination polymers that simultaneously possess porous and conductive properties, and have broad application potential in energy and electronic devices. However, to make the best use of the intrinsic electronic properties and structural features of 2D c-MOFs, the controlled synthesis of hierarchically nanostructured 2D c-MOFs with high crystallinity and customized morphologies is essential, which remains a great challenge. Herein, we present a template strategy to synthesize a library of 2D c-MOFs with controlled morphologies and dimensions via insulating MOFs-to-c-MOFs transformations.

Role of the Metal Precursor in Preparing Dual-Atom Catalysts for the Oxygen Reduction Reaction.

Dual-atom catalysts (DACs) have arisen as a novel type of heterogeneous catalyst that extends from single-atom catalysts (SACs) by incorporating two kinds of metals. These materials have demonstrated enhanced performance when compared to SACs. The choice of metal precursors plays an important role in the synthesis of DACs.

Accessing parity-forbidden d-d transitions for photocatalytic CO reduction driven by infrared light.

A general approach to promote IR light-driven CO reduction within ultrathin Cu-based hydrotalcite-like hydroxy salts is presented. Associated band structures and optical properties of the Cu-based materials are first predicted by theory. Subsequently, Cu(SO)(OH) nanosheets were synthesized and are found to undergo cascaded electron transfer processes based on d-d orbital transitions under infrared light irradiation.

Exceptionally high charge mobility in phthalocyanine-based poly(benzimidazobenzophenanthroline)-ladder-type two-dimensional conjugated polymers.

Two-dimensional conjugated polymers (2DCPs), composed of multiple strands of linear conjugated polymers with extended in-plane π-conjugation, are emerging crystalline semiconducting polymers for organic (opto)electronics. They are represented by two-dimensional π-conjugated covalent organic frameworks, which typically suffer from poor π-conjugation and thus low charge carrier mobilities. Here we overcome this limitation by demonstrating two semiconducting phthalocyanine-based poly(benzimidazobenzophenanthroline)-ladder-type 2DCPs (2DCP-MPc, with M = Cu or Ni), which are constructed from octaaminophthalocyaninato metal(II) and naphthalenetetracarboxylic dianhydride by polycondensation under solvothermal conditions.

Three-Dimensional Sulfated Bacterial Cellulose/Gelatin Composite Scaffolds for Culturing Hepatocytes.

The liver is the hub of human metabolism and involves many diseases. To better work on the mechanism and treatment of liver diseases, it is of particular interest to design 3-dimensional scaffolds suitable for culturing hepatocytes in vitro to simulate their metabolic and regenerative abilities. In this study, sulfated bacterial cellulose (SBC) was prepared as the building block of cell scaffolds, motivated by the anionic nature and 3-dimensional structure of hepatic extracellular matrix, and its reaction condition for sulfate esterification was optimized by changing the reaction time.

Redox-Bipolar Polyimide Two-Dimensional Covalent Organic Framework Cathodes for Durable Aluminium Batteries.

Emerging rechargeable aluminium batteries (RABs) offer a sustainable option for next-generation energy storage technologies with low cost and exemplary safety. However, the development of RABs is restricted by the limited availability of high-performance cathode materials. Herein, we report two polyimide two-dimensional covalent organic frameworks (2D-COFs) cathodes with redox-bipolar capability in RAB.

Largely Pseudocapacitive Two-Dimensional Conjugated Metal-Organic Framework Anodes with Lowest Unoccupied Molecular Orbital Localized in Nickel-bis(dithiolene) Linkages.

Although two-dimensional conjugated metal-organic frameworks (2D -MOFs) provide an ideal platform for precise tailoring of capacitive electrode materials, high-capacitance 2D -MOFs for non-aqueous supercapacitors remain to be further explored. Herein, we report a novel phthalocyanine-based nickel-bis(dithiolene) (NiS)-linked 2D -MOF (denoted as Ni[CuPcS]) with outstanding pseudocapacitive properties in 1 M TEABF/acetonitrile. Each NiS linkage is disclosed to reversibly accommodate two electrons, conferring the Ni[CuPcS] electrode a two-step Faradic reaction with a record-high specific capacitance among the reported 2D -MOFs in non-aqueous electrolytes (312 F g) and remarkable cycling stability (93.

Boosting Oxygen Electrocatalytic Activity of Fe-N-C Catalysts by Phosphorus Incorporation.

Nitrogen-doped graphitic carbon materials hosting single-atom iron (Fe-N-C) are major non-precious metal catalysts for the oxygen reduction reaction (ORR). The nitrogen-coordinated Fe sites are described as the first coordination sphere. As opposed to the good performance in ORR, that in the oxygen evolution reaction (OER) is extremely poor due to the sluggish O-O coupling process, thus hampering the practical applications of rechargeable zinc (Zn)-air batteries.

Exploring the Effect of Selenidation Time on the Ni-Doped CuZnSn(S,Se) Solar Cell.

The CuNiZnSn(S,Se) (CNZTSSe) films were synthesized by sol-gel combined with selenidation treatment. To further enhance the crystal quality of the film, the selenidation conditions were optimized, and the effects of selenidation time on the properties of the CNZTSSe films and devices were systematically studied. The results show that the crystallinity of the films increased remarkably with the increase of selenidation time.

Pressure-Engineered TiCT MXene with Enhanced Conductivity and Accelerated Reaction Kinetics of Lithium Storage.

We studied the structure-function relationship of compressed TiCT MXene using high-pressure in situ synchrotron radiation, impedance spectroscopy, Hall effect measurements, and first-principles calculations. With increasing pressure, the conductivity of TiCT MXene increases along with its continued lattice shrinkage. A pressure range of 0.

Competitive Adsorption: Reducing the Poisoning Effect of Adsorbed Hydroxyl on Ru Single-Atom Site with SnO for Efficient Hydrogen Evolution.

Ruthenium (Ru) has been theoretically considered a viable alkaline hydrogen evolution reaction electrocatalyst due to its fast water dissociation kinetics. However, its strong affinity to the adsorbed hydroxyl (OH ) blocks the active sites, resulting in unsatisfactory performance during the practical HER process. Here, we first reported a competitive adsorption strategy for the construction of SnO nanoparticles doped with Ru single-atoms supported on carbon (Ru SAs-SnO /C) via atomic galvanic replacement.

Upgrading Organic Compounds through the Coupling of Electrooxidation with Hydrogen Evolution.

The electrocatalytic splitting of water is recognized to be the most sustainable and clean technology for the production of hydrogen (H ). Unfortunately, the efficiency is seriously restricted by the sluggish kinetics of the oxygen evolution reaction (OER) at the anode. In contrast to the OER, the electrooxidation of organic compounds (EOO) is more thermodynamically and kinetically favorable.

An Anode-Free Zn-Graphite Battery.

The anode-free battery concept is proposed to pursue the aspiration of energy-dense, rechargeable metal batteries, but this has not been achieved with dual-ion batteries. Herein, the first anode-free Zn-graphite battery enabled by efficient Zn plating-stripping onto a silver-coated Cu substrate is demonstrated. The silver coating guides uniform Zn deposition without dendrite formation or side reaction over a wide range of electrolyte concentrations, enabling the construction of anode-free Zn cells.

Identification of Distinct Inflammatory Programs and Biomarkers in Systemic Juvenile Idiopathic Arthritis and Related Lung Disease by Serum Proteome Analysis.

Objective: Recent observations in systemic juvenile idiopathic arthritis (JIA) suggest an increasing incidence of high-mortality interstitial lung disease often characterized by a variant of pulmonary alveolar proteinosis (PAP). Co-occurrence of macrophage activation syndrome (MAS) and PAP in systemic JIA suggests a shared pathology, but patients with lung disease associated with systemic JIA (designated SJIA-LD) also commonly experience features of drug reaction such as atypical rashes and eosinophilia. This study was undertaken to investigate immunopathology and identify biomarkers in systemic JIA, MAS, and SJIA-LD.

Two-Dimensional Conjugated Metal-Organic Frameworks for Electrocatalysis: Opportunities and Challenges.

A highly effective electrocatalyst is the central component of advanced electrochemical energy conversion. Recently, two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have emerged as a class of promising electrocatalysts because of their advantages including 2D layered structure with high in-plane conjugation, intrinsic electrical conductivity, permanent pores, large surface area, chemical stability, and structural diversity. In this Review, we summarize the recent advances of 2D c-MOF electrocatalysts for electrochemical energy conversion.

Active site engineering of single-atom carbonaceous electrocatalysts for the oxygen reduction reaction.

The electrocatalytic oxygen reduction reaction (ORR) is the vital process at the cathode of next-generation electrochemical storage and conversion technologies, such as metal-air batteries and fuel cells. Single-metal-atom and nitrogen co-doped carbonaceous electrocatalysts (M-N-C) have emerged as attractive alternatives to noble-metal platinum for catalyzing the kinetically sluggish ORR due to their high electrical conductivity, large surface area, and structural tunability at the atomic level, however, their application is limited by the low intrinsic activity of the metal-nitrogen coordination sites (M-N ) and inferior site density. In this Perspective, we summarize the recent progress and milestones relating to the active site engineering of single atom carbonous electrocatalysts for enhancing the ORR activity.

Boosting the Electrocatalytic Conversion of Nitrogen to Ammonia on Metal-Phthalocyanine-Based Two-Dimensional Conjugated Covalent Organic Frameworks.

The electrochemical N reduction reaction (NRR) under ambient conditions is attractive in replacing the current Haber-Bosch process toward sustainable ammonia production. Metal-heteroatom-doped carbon-rich materials have emerged as the most promising NRR electrocatalysts. However, simultaneously boosting their NRR activity and selectivity remains a grand challenge, while the principle for precisely tailoring the active sites has been elusive.

Dual-Redox-Sites Enable Two-Dimensional Conjugated Metal-Organic Frameworks with Large Pseudocapacitance and Wide Potential Window.

Advanced supercapacitor electrodes require the development of materials with dense redox sites embedded into conductive and porous skeletons. Two-dimensional (2D) conjugated metal-organic frameworks (-MOFs) are attractive supercapacitor electrode materials due to their high intrinsic electrical conductivities, large specific surface areas, and quasi-one-dimensional aligned pore arrays. However, the reported 2D -MOFs still suffer from unsatisfying specific capacitances and narrow potential windows because large and redox-inactive building blocks lead to low redox-site densities of 2D -MOFs.

Facile assembly of layer-interlocked graphene heterostructures as flexible electrodes for Li-ion batteries.

Flexible electrodes with robust mechanical properties and high electrochemical performance are of significance for the practical implementation of flexible batteries. Here we demonstrate a general and straightforward co-assembly approach to prepare flexible electrodes, where electrochemically exfoliated graphene (EG) is exploited as the film former/conducting matrix and different binary metal oxides (LiTiO, LiCoO, LiMnO, LiFePO) are incorporated. The resultant EG-metal oxide hybrids exhibit a unique layer-interlocked structure, where the metal oxide is conformably wrapped by the highly flexible graphene.