To enhance the alkaline hydrogen evolution reaction (HER), it is crucial, yet challenging, to fundamentally understand and rationally modulate potential catalytic sites. In this study, we confirm that despite calculating a low water dissociation energy barrier and an appropriate H adsorption free energy (ΔG*H) at Ru-top sites, metallic Ru exhibits a relatively inferior activity for the alkaline HER. This is primarily because the Ru-top sites, which are potential H adsorption sites, are recessive catalytic sites, compared with the adjacent Ru-hollow sites that have a strong ΔG*H.
View Article and Find Full Text PDFLife on Earth relies on mechanisms to store heritable information and translate this information into cellular machinery required for biological activity. In all known life, storage, regulation, and translation are provided by DNA, RNA, and ribosomes. Life beyond Earth, even if ancestrally or chemically distinct from life may utilize similar structures: it has been proposed that charged linear polymers analogous to nucleic acids may be responsible for storage and regulation of genetic information in nonterran biochemical systems.
View Article and Find Full Text PDFThe rational design of multi-site electrocatalysts with three different functions for facile HO dissociation, H-H coupling, and rapid H release is desirable but difficult to achieve. This strategy can accelerate the sluggish kinetics of the hydrogen evolution reaction (HER) under alkaline conditions. To resolve this issue, a Mo/Ru-based catalyst with three different active sites (Ru/MoC/MoO) is rationally designed and its performance in alkaline HER is evaluated.
View Article and Find Full Text PDFExploring single-atom-catalysts for the acidic oxygen evolution reaction (OER) is of paramount importance for cost-effective hydrogen production via acidic water electrolyzers. However, the limited durability of most single-atom-catalysts and Ir/Ru-based oxides under harsh acidic OER conditions, primarily attributed to excessive lattice oxygen participation resulting in metal-leaching and structural collapse, hinders their practical application. Herein, an innovative strategy is developed to fabricate short-range Ir single-atom-ensembles (Ir) stabilized on the surface of Mn-substituted spinel CoO (Ir-CMO), which exhibits excellent mass activity and significantly improved durability (degradation-rate: ≈2 mV h), outperforming benchmark IrO (≈44 mV h) and conventional Ir on pristine-CoO for acidic OER.
View Article and Find Full Text PDFRu-based electrocatalysts hold great promise for developing affordable proton exchange membrane (PEM) electrolyzers. However, the harsh acidic oxidative environment of the acidic oxygen evolution reaction (OER) often causes undesirable overoxidation of Ru active sites and subsequent serious activity loss. Here, we present an ultrathin and conformal depletion layer attached to the Schottky heterojunction of core/shell RuCo/RuCoO that not only maximizes the availability of active sites but also improves its durability and intrinsic activity for acidic OER.
View Article and Find Full Text PDFRegulating the catalytic reaction pathway to essentially break the activity/stability trade-off that limits RuO and thus achieves exceptional stability and activity for the acidic oxygen evolution reaction (OER) is important yet challenging. Herein, we propose a novel strategy of incorporating atomically dispersed V species, including O-bridged V dimers and V single atoms, into RuO lattices to trigger direct O-O radical coupling to release O without the generation of *OOH intermediates. V-RuO showed high activity with a low overpotential of 227 mV at 10 mA cm and outstanding stability during a 1050 h test in acidic electrolyte.
View Article and Find Full Text PDFOperators of water distribution systems (WDSs) need continuous and timely information on pressures and flows to ensure smooth operation and respond quickly to unexpected events. While hydraulic models provide reasonable estimates of pressures and flows in WDSs, updating model predictions with real-time sensor data provides clearer insights into true system behavior and enables more effective real-time response. Despite the growing prevalence of distributed sensing within WDSs, standard hydraulic modeling software like EPANET do not support synchronous data assimilation.
View Article and Find Full Text PDFThe home robot-based child activity service aims to cultivate children's social emotions. A design theme was produced by interviewing child development experts and parents. The activity service is composed of 50 plays and 70 conversations.
View Article and Find Full Text PDFThe chlorine evolution reaction (CER) is a crucial anode reaction in the chlor-alkali industrial process. Precious metal-based dimensionally stable anodes (DSA) are commonly used as catalysts for CER but are constrained by their high cost and low selectivity. Herein, a Pt dual singe-atom catalyst (DSAC) dispersed on fluorine-doped carbon nanotubes (F-CNTs) is designed for an efficient and robust CER process.
View Article and Find Full Text PDFCurrently, conventional dimethoxymethane synthesis methods are environmentally unfriendly. Here, we report a photo-redox catalysis system to generate dimethoxymethane using a silver and tungsten co-modified blue titanium dioxide catalyst (Ag.W-BTO) by coupling CO reduction and CHOH oxidation under mild conditions.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2024
Regulating competitive reaction pathways to direct the selectivity of electrochemical CO reduction reaction toward a desired product is crucial but remains challenging. Herein, switching product from HCOOH to CO is achieved by incorporating Sb element into the CuS, in which the Cu-S ionic bond is coupled with S-Sb covalent bond through bridging S atoms that elongates the Cu-S bond from 2.24 Å to 2.
View Article and Find Full Text PDFElectrochemical CO reduction reaction (eCORR) over Cu-based catalysts is a promising approach for efficiently converting CO into value-added chemicals and alternative fuels. However, achieving controllable product selectivity from eCORR remains challenging because of the difficulty in controlling the oxidation states of Cu against robust structural reconstructions during the eCORR. Herein, we report a novel strategy for tuning the oxidation states of Cu species and achieving eCORR product selectivity by adjusting the Cu content in CuMgAl-layered double hydroxide (LDH)-based catalysts.
View Article and Find Full Text PDFLow-dimensional metal nanostructures have attracted considerable research attention, owing to their potential as catalysts. A controlled reductive phase transition of monolayer RuO nanosheets could provide an effective way to produce holey large-area 2D Ru nanosheets with tailored defect structures and metal coordination number. The locally optimized holey Ru metal nanosheet, with a metal coordination number of ∼10.
View Article and Find Full Text PDFThe design of high-entropy single-atom catalysts (HESAC) with 5.2 times higher entropy compared to single-atom catalysts (SAC) is proposed, by using four different metals (FeCoNiRu-HESAC) for oxygen reduction reaction (ORR). Fe active sites with intermetallic distances of 6.
View Article and Find Full Text PDFTo realize economically feasible electrochemical CO conversion, achieving a high partial current density for value-added products is particularly vital. However, acceleration of the hydrogen evolution reaction due to cathode flooding in a high-current-density region makes this challenging. Herein, we find that partially ligand-derived Ag nanoparticles (Ag-NPs) could prevent electrolyte flooding while maintaining catalytic activity for CO electroreduction.
View Article and Find Full Text PDFBackground: This study aimed to investigate the oncologic long-term safety of proximal gastrectomy for upper-third advanced gastric cancer (AGC) and Siewert type II esophagogastric junction (EGJ) cancer.
Methods: The study enrolled patients who underwent proximal gastrectomy (PG) or total gastrectomy (TG) with standard lymph node (LN) dissection for pathologically proven upper-third AGC and EGJ cancers between January 2007 and December 2018. Propensity score-matching with a 1:1 ratio was performed to reduce the influence of confounding variables such as age, sex, tumor size, T stage, N stage, and tumor-node-metastasis (TNM) stage.
Ruthenium oxide is currently considered as the promising alternative to Ir-based catalysts employed for proton exchange membrane water electrolyzers but still faces the bottlenecks of limited durability and slow kinetics. Herein, a 2D amorphous/crystalline heterophase ac-CrRuO substitutional solid solution with pervasive grain boundaries (GBs) is developed to accelerate the kinetics of acidic oxygen evolution reaction (OER) and extend the long-term stability simultaneously. The ac-CrRuO shows a super stability with a slow degradation rate and a remarkable mass activity of 455 A g at 1.
View Article and Find Full Text PDFAlthough great efforts on the delicate construction of a built-in electric field (BIEF) to modify the electronic properties of active sites have been conducted, the substantial impact of BIEF coupled with electrode potential on the electrochemical reactions has not been clearly investigated. Herein, we designed an alkaline hydrogen evolution reaction (HER) catalyst composed of heterogeneous Ru-CoP urchin arrays on carbon cloth (Ru-CoP/CC) with a strong BIEF with the guidance of density functional theory (DFT) calculations. Impressively, despite its unsatisfactory activity at 10 mA cm (overpotential of 44 mV), Ru-CoP/CC exhibited better activity (357 mV) than the benchmark Pt/C catalyst (505 mV) at 1 A cm .
View Article and Find Full Text PDFPurpose: Bariatric surgery is an increasingly common treatment for obesity and related comorbidities. This meta-analysis aimed to compare the outcomes of bariatric surgery and medical treatment (MT).
Materials And Methods: A systematic search of articles published from January 2013 to May 2023 identified 20 studies.