Electrochemical CO reduction (CORR) to carbon monoxide (CO) offers a sustainable pathway for carbon utilization, yet challenges remain in terms of improving selectivity and activity. Herein, we report a Ni/NC catalyst synthesized via a milling - pyrolysis method, in which Ni particles anchored on nitrogen-doped carbon (NC) are electrochemically activated under an Ar atmosphere, leading to their structural evolution into single-atom Ni sites. After activation in Ar atmosphere, the current density nearly doubles (from ≈30 to ≈60 mA cm), and concurrently, the Faradaic efficiency of CO stays at ∼90% with the potential set to -0.
View Article and Find Full Text PDFJ Am Chem Soc
September 2025
The inherent trade-off between activity and stability in platinum single-atom catalysts (SACs) poses a significant challenge for catalytic oxidation reactions. High-coordination Pt sites have good stability, but their overoxidation often passivates activity. In contrast, metastable low-coordination Pt structures typically display high activity but are prone to oxidation and aggregation under harsh conditions.
View Article and Find Full Text PDFThe conversion of cellulose to levulinic acid (LA) catalyzed by solid acid is of great significance for high-value utilization of cellulosic biomass, while conventional solid acid catalysts exhibit unsatisfactory activity and stability. Herein, a strategy of supramolecular network-mediated spatial confinement-electronic bridge framework was proposed to construct a biomass carbon-coated AlZr (CA-AZ@BC) solid acid catalyst with Brønsted and Lewis dual-acid sites for high-efficiency conversion of cellulose. Based on a self-assembly sodium lignosulfonate-citric acid-bimetal supramolecular network, the specific spatial confinement effect of the supramolecular framework ensured the dispersibility and stability of active sites in the CA-AZ@BC catalyst.
View Article and Find Full Text PDFMimicking the structure of natural enzymes can reproduce their similar high catalytic activity. Herein, Ru-Se dual single atomic sites on nitrogen-doped carbon catalysts (RuSe-N/C) are fabricated by an atomic capture strategy. Se atoms replace partial pyridinic N sites in RuSe-N/C, which results in undulating structure and high structural similarity to β-sheets in the protein.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2025
The imperative to minimize iridium usage in proton exchange membrane water electrolysis (PEMWE) process presents a pivotal challenge for hydrogen economy deployment, while inherent destabilization of iridium (Ir) active sites under corrosive operational conditions, originating from insufficient Ir bonding strength, remains a fundamental barrier. Here, we resolve this dilemma through heterointerface-engineered stabilization, where the strategically constructed Nb-TiO rutile/anatase heterophase homojunction stabilizes Ir sites with enhanced orbital overlap and intensified charge transfer. This atomic-scale anchoring mechanism, validated by operando characterization and theoretical calculations, strengthens Ir─O bonding and optimizes *OOH adsorption energetics, thereby enabling concurrent activity-stability improvements.
View Article and Find Full Text PDFAccurate diagnosis and severity estimation of gastrointestinal tract (GT) lesions are crucial for patient care and effective treatment plan decisions. Traditional methods for diagnosing lesions face challenges in accurately estimating severity due to requiring interpretable biomarkers, inter-observer variability, and overlapping lesions. Moreover, existing deep-learning models treat lesion classification and severity estimation as separate tasks, complicating diagnosis.
View Article and Find Full Text PDFIntroduction: Gallbladder and Biliary Tract Cancer (GBTC) accounts for a notable proportion of cancer cases worldwide. This study aims to assess the burden of GBTC among aged 55 years and older, enhancing our understanding of its trends and their relationship with Socio-Demographic Index (SDI) across regions and countries.
Methods: We used the data from the Global Burden of Disease study from 2010 to 2021 to analyze GBTC incidence, death numbers, disability-adjusted life years (DALYs) and their respective rates for individuals aged 55 years and older.
The high performance of Fe-based electrocatalyst for electrochemical nitrate reduction reaction to ammonia (eNO RR-to-NH) is currently constrained by low NH selectivity and insufficient stability under high current density. Hence, the incorporation of ruthenium single-atom into the CuFeO (Ru-CuFeO) with self-recycling property is developed. The Cu and Ru sites synergistically promote the water dissociation and facilitate the redeposition of in situ adsorbed Fe (Fe ) as α-FeOOH by self-reinforcing local alkalinity at the Ru-CuFeO surface, thereby achieving high activity and robust stability for eNO RR-to-NH process.
View Article and Find Full Text PDFMimicking the hierarchical structure as well as the asymmetric Fe-N sites in natural horseradish peroxidase (HRP) is of great importance in developing Fe/CN with high peroxidase-like (POD-like) activity. In this work, Fe/CN with an asymmetric FeN moiety and ordered porous structure (FeN/CN) is fabricated by an ammonia-assisted redispersion strategy, which shows high structural similarity with HRP. Therefore, FeN/CN shows an excellent catalytic efficiency (specific activity = 117.
View Article and Find Full Text PDFThe symmetry-breaking nature of Janus materials enables the design of multifunctional compounds with distinct properties that are inaccessible to traditional materials. However, the limited availability of intrinsically stable Janus materials hinders a complete understanding of their full potential. Here, the first millimeter-sized Janus material, RhSeCl, is successfully synthesized through the precisely controlled chemical vapor transport (CVT) method.
View Article and Find Full Text PDFFe-based photo-Fenton process is widely used to remove antibiotic in wastewater, however, the synthesis of efficient and stable catalysts to solve the problems of Fe/Fe ions cycling and iron sludge formation of FeS-based catalysts is challenging. Herein, a strategy combining mechanical activation and pyrolysis was proposed to construct a novel FeS/amorphous carbon nitride (2D/2D FeS/ACN) composite with a two-dimensional (2D) stacked structure, where the FeS and ACN connected by Fe-N bonds. The removal rates of oxytetracycline, tetracycline, and chlorotetracycline over 2D/2D FeS/ACN both surpassed 96.
View Article and Find Full Text PDFJ Steroid Biochem Mol Biol
September 2025
Cancer is a prominent disease that poses a significant threat to human health, and the exploration of highly efficient and low-toxicity anticancer drugs remains an active area of research. Leveraging the cell-penetrating and binding capabilities of steroids, along with the multifunctional pharmacological properties of selenocyano groups, novel compounds are being designed and synthesized with the aim of discovering highly efficient and minimally toxic anti-tumor drugs. In the present study, two selenocyano pharmacophores were incorporated into estradiol to synthesize a series of estradiol diselenocyanate derivatives with a 3-selenocyanoalkoxy-17-selenocyanoester structure.
View Article and Find Full Text PDFTwo-dimensional composites with a core-shell structure used as lubricant additives tend to experience separation and delamination of the core and shell materials under high loads, resulting in poor tribological performance. Herein, monodisperse and spherical cellulose acetate-laurate/calcium borate/cellulose acetate-laurate (CAL/CB/CAL) nanocapsules with three-dimensional network structure were prepared by high-pressure homogenization combined with solvent evaporation method. CAL/CB/CAL exhibited good dispersibility and long-term dispersion stability in polyalphaolefin (PAO) oil, and only slight stratification appeared after 21 d.
View Article and Find Full Text PDFThe integration of two entirely unrelated organic reactions into a novel reaction poses a formidable challenge. While diatomic catalysts (DACs) have exhibited promise as a framework for realizing this concept, the fusion of disparate organic reactions using DACs remains exceptionally uncommon. The reason for this is that there are often interactions between the two metal sites in DACs, which create new difficulties in catalyst design for already complex reaction systems.
View Article and Find Full Text PDFThe advancement of rechargeable zinc-air batteries significantly depends on bifunctional oxygen electrocatalysts to provide outstanding oxygen reduction/evolution reaction (ORR/OER) performance. However, it is still challenging to design electrocatalysts with excellent bifunctional activity and stability. Here, we adopt an ultrafast printing method to efficiently embed a triatom cobalt complex precursor onto graphene nanosheets to obtain a triatomic catalyst (Co-NG), exhibiting a durable and excellent bifunctional catalyst in the electrocatalytic ORR (E = 0.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2025
Electrochemical biomass conversion offers a sustainable route to diverse products, minimizing environmental impact. However, conventional 5-hydroxymethylfurfural electrooxidation (HMFOR) catalysts such as Ni(OH)₂ and NiS suffer from low conductivity, poor stability, and limited active sites. This work introduces a CoNiMnMoPd high entropy alloy (HEA) to address these limitations by simultaneously maintaining high conductivity, stability, and a high Ni oxidation state, enabling nucleophilic dehydrogenation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2025
The use of clean electric energy to activate inert compounds has garnered significant attention. Homogeneous redox mediators (RMs) in organic electrosynthesis are effective platforms for this purpose. However, understanding the RM's electronic structure under operational conditions, electron transport processes at the electrode surface, and substrate adsorption-desorption dynamics remains challenging.
View Article and Find Full Text PDFCarbon nitride, as a metal-free catalyst, is demonstrated to effectively catalyze toluene oxidation. The localized electrons surrounding nitrogen vacancies in CN are transferred to O, facilitating its adsorption and dissociation, thereby activating O, which in turn accelerates toluene oxidation.
View Article and Find Full Text PDFThe preparation of food-grade oxidized starch with eco-friendly ozone (O) as oxidant is limited by low mass transfer and reaction efficiency. This study proposed a porous spontaneously polarized ceramic-reinforced O micro-nano bubbles (PSPC-OMNB) technology to prepare oxidized cassava starch (PSPC-OMCS). Meanwhile, reaction uniformity, physicochemical properties, and formation mechanisms were emphasized for comprehensive investigation.
View Article and Find Full Text PDFAnion exchange membrane fuel cells (AEMFCs) are one of the ideal energy conversion devices. However, platinum (Pt), as the benchmark catalyst for the hydrogen oxidation reaction (HOR) of AEMFCs anodes, still faces issues of insufficient performance and susceptibility to CO poisoning. Here, we report the Joule heating-assisted synthesis of a small sized RuPt single-atom alloy catalyst loaded on nitrogen-doped carbon modified with single W atoms (s-RuPt@W/NC), in which the near-range single Ru atoms on the RuPt nanoparticles and the long-range single W atoms on the support simultaneously modulate the electronic structure of the active Pt-site, enhancing alkaline HOR performance of s-RuPt@W/NC.
View Article and Find Full Text PDFClin Transl Gastroenterol
March 2025
Introduction: Lugol chromoendoscopy (LCE) is valuable, cost-effective, and widely used in early esophageal cancer screening, yet it suffers from low compliance because of adverse events after LCE. In addition, the reflux of iodine during iodine staining in the upper esophagus brings the risk of bucking and aspiration. We introduced a new model called distance countdown (DC) aimed to reduce reflux during iodine staining in upper esophageal LCE.
View Article and Find Full Text PDFNumerous in situ characterization studies have focused on revealing the catalytic mechanisms of single-atom catalysts (SACs), providing a theoretical basis for their rational design. Although research is relatively limited, the stability of SACs under long-term operating conditions is equally important and a prerequisite for their real-world energy applications, such as fuel cells and water electrolyzers. Recently, there has been a rise in in situ characterization studies on the destabilization and regeneration of SACs; however, timely and comprehensive summaries that provide the catalysis community with valuable insights and research directions are still lacking.
View Article and Find Full Text PDFAdv Mater
January 2025
The design and synthesis of metal-organic frameworks (MOFs) with outstanding light-harvesting and photoexcitation for artificial photocatalytic CO reduction is an attractive but challenging task. In this work, a novel aggregation-induced emission (AIE)-active ligand, tetraphenylpyrazine (PTTBPC) is proposed and utilized for the first time to construct a Zr-MOF photocatalyst via coordination with stable Zr-oxo clusters. Zr-MOF is featured by a scu topology with a two-fold interpenetrated framework, wherein the PTTBPC ligands enable strong light-harvesting and photoexcitation, while the Zr-oxo clusters facilitate CO adsorption and activation, as well as offer potential sites for further metal modification.
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