Single-atom catalysts are promising for electrocatalytic CO conversion but face challenges in controllable syntheses. Herein, a facile selenic acid etching-assisted strategy has been developed to fabricate a hybrid metal-semimetal dual single-atom catalyst for electrocatalytic CO reduction. This strategy enables the simultaneous generation of monodisperse active sites and hierarchical morphologies with hollow nanostructures.
View Article and Find Full Text PDFA facile and general strategy is developed herein for the construction of circularly polarized luminescence (CPL) materials with simultaneously high fluorescence quantum efficiency (Φ) and large luminescence dissymmetry factor (g). The self-assembly of fluorescent dye, disodium 4,4'-bis(2-sulfonatostyryl)biphenyl (CBS), with chiral diamines such as (R,R)/(S,S)-1,2-diaminocyclohexane (R/S-DACH) and R/S-1,2-diaminopropane (R/S-DAP), produces four chiral crystalline organic salt networks (COSNs). These as-synthesized organic salts emit strong blue-color CPL upon excitation, with both high Φ and g values of up to 79% and 0.
View Article and Find Full Text PDFConstructing local microenvironments is one of the important strategies to improve the electrocatalytic performances, such as in electrochemical CO reduction (ECR). However, effectively customizing these microenvironments remains a significant challenge. Herein, utilizing carbon nanotube (CNT) heterostructured semi-open Co-NO catalytic configurations (Co-salophen), we have demonstrated the role of the local microenvironment on promoting ECR through regulating the location of hydroxyl groups.
View Article and Find Full Text PDFIn the deep-ultraviolet (DUV) region, nonlinear optical (NLO) crystals must meet stringent requirements, including a large optical band gap and sufficient second harmonic generation (SHG) response. Typically, these criteria are fulfilled by borates, carbonates and nitrates containing π-conjugated groups. In contrast, sulfates and phosphates, with polarizabilities significantly smaller than those of π-conjugated groups, struggle to achieve similar performance.
View Article and Find Full Text PDFThe electrosynthesis of hydrogen peroxide (HO) from O or HO via the two-electron (2e) oxygen reduction (2e ORR) or water oxidation (2e WOR) reaction provides a green and sustainable alternative to the traditional anthraquinone process. Herein, a paired-electrosynthesis tactic is reported for concerted HO production at a high rate by coupling the 2e ORR and 2e WOR, in which the bifunctional oxygen-vacancy-enriched BiO nanorods (O-BiO-EO), obtained through electrochemically oxidative reconstruction of Bi-based metal-organic framework (Bi-MOF) nanorod precursor, are used as both efficient anodic and cathodic electrocatalysts, achieving concurrent HO production at both electrodes with high Faradaic efficiencies. Specifically, the coupled 2e ORR//2e WOR electrolysis system based on such distinctive oxygen-defect Bi catalyst displays excellent performance for the paired-electrosynthesis of HO, delivering a remarkable cell Faradaic efficiency of 154.
View Article and Find Full Text PDFThe coupling electrosynthesis involving CO upgrade conversion is of great significance for the sustainable development of the environment and energy but is challenging. Herein, we exquisitely constructed the self-supported bimetallic array superstructures from the Cu(OH) array architecture precursor, which can enable high-performance coupling electrosynthesis of formate and adipate at the anode and the cathode, respectively. Concretely, the faradaic efficiencies (FEs) of CO-to-formate and cyclohexanone-to-adipate conversion simultaneously exceed 90% at both electrodes with excellent stabilities.
View Article and Find Full Text PDFPurpose: The potential efficacy of metformin in breast cancer (BC) has been hotly discussed but never conclusive. This genetics-based study aimed to evaluate the relationships between metformin targets and BC risk.
Methods: Metformin targets from DrugBank and genome-wide association study (GWAS) data from IEU OpenGWAS and FinnGen were used to investigate the breast cancer (BC)-metformin causal link with various Mendelian Randomization (MR) methods (e.
With the continuous development of laser technology and the increasing demand for lasers of different frequencies in the infrared (IR) spectrum, research on infrared nonlinear optical (NLO) crystals has garnered growing attention. Currently, the three main commercially available types of borate materials each have their drawbacks, which limit their applications in various areas. Rare-earth (RE)-based chalcogenide compounds, characterized by the unique f-electron configuration, strong positive charges, and high coordination numbers of RE cations, often exhibit distinctive optical responses.
View Article and Find Full Text PDFOrdered pore engineering that embeds uniform pores with periodic alignment in electrocatalysts opens up a new avenue for achieving further performance promotion. Hierarchically ordered porous metal-organic frameworks (HOP-MOFs) possessing multilevel pores with ordered distribution are the promising precursors for the exploration of ordered porous electrocatalysts, while the scalable acquisition of HOP-MOFs with editable components and adjustable pore size regimes is critical. This review presents recent progress on hierarchically ordered pore engineering of MOF-based materials for enhanced electrocatalysis.
View Article and Find Full Text PDFNoncentrosymmetric (NCS) oxychalcogenides have attracted great attention in recent years due to their immense potential as candidates for IR nonlinear-optical (NLO) applications. Despite notable advancements in this field, the discovery of oxychalcogenides with three-dimensional (3D) framework structures remains a formidable challenge. In this study, we report the discovery of the first hexanary oxychalcogenide, BaInMnSiOS, exhibiting second-order NLO activity, using a high-temperature solid-phase method.
View Article and Find Full Text PDFThe rational design of an oxygen electrocatalyst with low cost and high activity is greatly desired for realization of the practical water-splitting industry. Herein, we put forward a rational method to construct nonprecious-metal catalysts with high activity by designing the microstructure and modulating the electronic state. Iron (Fe)-doped NiP hollow polyhedrons decorated with nitrogen-doped carbon (Fe-NiP/NC HPs) are prepared by a sequential metal-organic-framework-templated strategy.
View Article and Find Full Text PDFTransition metal-based single-atom catalysts (TM-SACs) are promising alternatives to Au- and Ag-based electrocatalysts for CO production through CO reduction reaction. However, developing TM-SACs with high activity and selectivity at low overpotentials is challenging. Herein, a novel Fe-based SAC with Si doping (Fe-N-C-Si) was prepared, which shows a record-high electrocatalytic performance toward the CO-to-CO conversion with exceptional current density (>350.
View Article and Find Full Text PDFJ Colloid Interface Sci
June 2023
Anodic oxidation assisted hydrogen production under mild conditions powered by renewable electricity represents a sustainable approach to energy conversion systems. Here, we fabricated a versatile and universal self-supported nanoarray platform that can be intelligently edited to achieve adaptive electrocatalysis for alcohol oxidation reactions and hydrogen evolution reaction (HER). The obtained self-supported nanoarray electrocatalysts exhibit excellent catalytic activity due to the integration of multiple merits of rich nanointerface-reconstruction and self-supported hierarchical structures.
View Article and Find Full Text PDFInorganic chalcogenides have been studied as the most promising infrared (IR) nonlinear optical (NLO) candidates for the past decades. However, it is proven difficult to discover high-performance materials that combine the often-incompatible properties of large energy gap (E ) and strong second harmonic generation (SHG) response (d ), especially for rare-earth chalcogenides. Herein, centrosymmetric Cs [Sb O ][Ge O ] is selected as a maternal structure and a new noncentrosymmetric rare-earth oxychalcogenide, namely, Nd [Ga O S ][Ge O ], is successfully designed and obtained by the module substitution strategy for the first time.
View Article and Find Full Text PDFThe acquisition of a non-centrosymmetric (NCS) structure and achieving a nice trade-off between a large energy gap ( > 3.5 eV) and a strong second-harmonic generation (SHG) response ( > 1.0 × benchmark AgGaS) are two formidable challenges in the design and development of infrared nonlinear optical (IR-NLO) candidates.
View Article and Find Full Text PDFOxychalcogenides have gained widespread attention as promising infrared nonlinear optical (IR-NLO) candidates. However, high-performance oxychalcogenides have rarely been reported in the ultraviolet (UV) region owing to the low energy gaps ( < 4.0 eV).
View Article and Find Full Text PDFChallenges remain in the development of novel multifunctional electrocatalysts and their industrial operation on low-electricity pair-electrocatalysis platforms for the carbon cycle. Herein, an enzyme-inspired single-molecular heterojunction electrocatalyst ((NH ) -NiPc/CNTs) with specific atomic nickel centers and amino-rich local microenvironments for industrial-level electrochemical CO reduction reaction (eCO RR) and further energy-saving integrated CO electrolysis is designed and developed. (NH ) -NiPc/CNTs exhibit unprecedented catalytic performance with industry-compatible current densities, ≈100% Faradaic efficiency and remarkable stability for CO -to-CO conversion, outperforming most reported catalysts.
View Article and Find Full Text PDFMultinary rare-earth chalcogenides with d-block transition metals have attracted considerable attention owing to their intriguing structural architectures and promising practical applications. In this work, three quaternary rare-earth sulfides, BaRECdS (RE = Sm, Gd, or Tb), have been obtained by the high-temperature solid-state method. These compounds are isostructural and belong to the noncentrosymmetric orthorhombic space group 2 (No.
View Article and Find Full Text PDFThe electrochemical carbon dioxide reduction reaction (CO RR) converting CO into value-added chemicals and fuels to realize carbon recycling is a solution to the problem of renewable energy shortage and environmental pollution. Among all the catalysts, the carbon-based single-atom catalysts (SACs) with isolated metal atoms immobilized on conductive carbon substrates have shown significant potential toward CO RR, which intrigues researchers to explore high-performance SACs for fuel and chemical production by CO RR. Especially, regulating the coordination structures of the metal centers and the microenvironments of the substrates in carbon-based SACs has emerged as an effective strategy for the tailoring of their CO RR catalytic performance.
View Article and Find Full Text PDFInfrared (IR) nonlinear optical (NLO) materials are the core devices to realize IR laser output, which are of vital importance in civilian and military fields. Non-centrosymmetric chalcogenide and pnictide compounds have already been widely accepted as favorable systems for IR-NLO materials. Compared to the extensively investigated IR-NLO chalcogenides during the past few decades, the research of non-centrosymmetric phosphides as IR-NLO materials is relatively scarce.
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