Acidic CO electroreduction reaction (CORR) garners significant attention as a promising approach for cutting carbon density, as it effectively mitigates CO loss by suppressing carbonate species formation. Unfortunately, achieving efficient multi-carbon products (C) production in acidic media remains challenging due to two main limitations: weak CO adsorption on Cu sites and competitive H* adsorption caused by the high concentration protons (H). To overcome these challenges, a cation-anion-modification strategy is proposed using an ionic liquid layer-1-Propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([PMIM][NTf])-on Cu surface.
View Article and Find Full Text PDFCatalytic hydrolysis is a sustainable method for the degradation of perfluorinated compounds (PFCs) but is challenged by the high reaction temperatures required to cleave strong C-F bonds. Herein, we developed an innovative C-F activation strategy by constructing synergistic Lewis and Brønsted acid pairs over atomically dispersed Zn-O-Al sites to promote C-F bond activation for decomposition of typical PFCs, CF. Density functional theory (DFT) calculations demonstrate tricoordinated Al (Al) sites and Zn-OH functional, respectively, as Lewis and Brønsted acid sites over Zn-O-Al, synergistically enhancing the adsorption and decomposition of CF.
View Article and Find Full Text PDFEnviron Sci Technol
February 2025
Thermocatalytic hydrolysis of perfluorocarbons (PFCs) is a promising way to reduce their emission and environmental hazards. However, hydrolysis of PFCs, such as CF, usually suffers from a drastic activity decline during the induction period, which seriously hinders its conversion performances and practical applications. In this work, we found that the carbonaceous (*COO) species account for the activity decline during the induction period, and their detoxification could promote PFC hydrolysis at low temperature.
View Article and Find Full Text PDFSingle-atom Fe-N-C catalysts have attracted significant attention in the NO reduction reaction (NORR). However, the origin of their selectivity in the NORR remains unclear, impeding further advancements in application. Herein, we investigate the potential-driven competitive mechanism for NH and NHOH production in the NORR over single-atom pyridinic-FeN and pyrrolic-FeN sites using constant-potential density functional theory calculations.
View Article and Find Full Text PDFPerfluorinated compounds (PFCs) are emerging environmental pollutants characterized by their extreme stability and resistance to degradation. Among them, tetrafluoromethane (CF) is the simplest and most abundant PFC in the atmosphere. However, the highest C─F bond energy and its highly symmetrical structure make it particularly challenging to decompose.
View Article and Find Full Text PDFCopper smelter dust, a typical hazardous waste that is abundant in valuable heavy metals, holds the potential to be regarded as a promising resource. This study introduces a new approach that integrates chlorination roasting and cascade condensation to efficiently recover heavy metals from copper smelter dust. The findings demonstrate the successful separation of heavy metals (Cu, Pb, and Zn) as chlorides at nearly 100% efficiency while also effectively converting trivalent arsenic (As(III)) into pentavalent arsenic (As(V)) and immobilizing it in the roasting residues, thereby reducing environmental risk.
View Article and Find Full Text PDFWith high current density, the intense near-electrode CO reduction reaction (CORR) will cause the concentration gradients of bicarbonate (HCO) and hydroxyl (OH) ions, which affect the selectivity of high-value C products of the CORR. In this work, we simulated the near-electrode concentration gradients of electrolyte species with different porous Cu-based CLs (catalyst layers) of GDE (gas diffusion electrode) by COMSOL Multiphysics. The higher porosity CL exhibits a better buffer ability of local alkalinity while ensuring a sufficient supply of H and local CO concentration.
View Article and Find Full Text PDFWhile the role of crystal facets is well known in traditional heterogeneous catalysis, this effect has not yet been thoroughly studied in plasmon-assisted catalysis, where attention has primarily focused on plasmon-derived mechanisms. Here, we investigate plasmon-assisted electrocatalytic CO reduction using different shapes of plasmonic Au nanoparticles - nanocube (NC), rhombic dodecahedron (RD), and octahedron (OC) - exposing {100}, {110}, and {111} facets, respectively. Upon plasmon excitation, Au OCs doubled CO Faradaic efficiency (FE) and tripled CO partial current density (j) compared to a dark condition, with NCs also improving under illumination.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2024
Histone methylation plays crucial roles in regulating chromatin structure and gene transcription in epigenetic modifications. Lysine-specific demethylase 1 (LSD1), the first identified histone demethylase, is universally overexpressed in various diseases. LSD1 dysregulation is closely associated with cancer, viral infections, and neurodegenerative diseases, etc.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
December 2023
Tetrafluoromethane (CF), the simplest perfluorocarbons, is a permanently potent greenhouse gas due to its powerful infrared radiation adsorption capacity. The highly symmetric and robust C-F bond structure makes its activation a great challenge. Herein, we presented an innovated approach that efficiently activates C-F bond utilizing protonated sulfate (-HSO) modified AlO@ZrO (S-AlO@ZrO) catalyst, resulting in highly efficient CF decomposition.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2024
Electroreduction of nitric oxide (NO) to NH (NORR) has gained extensive attention for the sake of low carbon emission and air pollutant treatment. Unfortunately, NORR is greatly hindered by its sluggish kinetics, especially under low concentrations of NO. Herein, we developed a chlorine (Cl) vacancy strategy to overcome this limitation over FeOCl nanosheets (FeOCl-V ).
View Article and Find Full Text PDFDuring the electrocatalytic CO reduction reaction, the faradaic efficiency of products seriously deviates from 100% due to the misjudgment of outlet flow, especially at industrial-level large current density. In this work, several modified equations and internal standard methods are recommended to calibrate the thermal mass flowmeter and establish benchmarks for CO reduction performance assessment.
View Article and Find Full Text PDFObjective: To explore the impact of link quality management on healthcare quality.
Methods: In 2021, The Fourth Hospital of Harbin Medical University followed various regulations and systems to manage the quality of hospital links. In 2022, the hospital upgraded and strengthened the quality management of hospital links.
Purpose: To inveatigate how effective LMWH was at preventing venous thromboembolism (VTE), major bleeding events, and minor bleeding events after simple knee arthroscopic surgery and anterior cruciate ligament reconstruction (ACLR).
Methods: We conducted a comprehensive search of PubMed, EMBASE, Cochrane Library, and the CNKI database for potentially eligible articles. The outcomes were evaluated in terms of odds ratio (OR) and the associated 95% confidence intervals (CIs).
Electrocatalytic CO reduction into value-added fuels and chemicals by renewable electric energy is one of the important strategies to address global energy shortage and carbon emission. Though the classical H-type electrolytic cell can quickly screen high-efficiency catalysts, the low current density and limited CO mass transfer process essentially impede its industrial applications. The electrolytic cells based on electrolyte flow system (flow cells) have shown great potential for industrial devices, due to higher current density, improved local CO concentration, and better mass transfer efficiency.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2023
Electrocatalytic CO reduction reaction (CO RR) to multi-carbon products (C ) in acidic electrolyte is one of the most advanced routes for tackling our current climate and energy crisis. However, the competing hydrogen evolution reaction (HER) and the poor selectivity towards the valuable C products are the major obstacles for the upscaling of these technologies. High local potassium ions (K ) concentration at the cathode's surface can inhibit proton-diffusion and accelerate the desirable carbon-carbon (C-C) coupling process.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2023
Tetrafluoromethane (CF ), the simplest perfluorocarbon (PFC), has the potential to exacerbate global warming. Catalytic hydrolysis is a viable method to degrade CF , but fluorine poisoning severely restricts both the catalytic performance and catalyst lifetime. In this study, Ga is introduced to effectively assists the defluorination of poisoned Al active sites, leading to highly efficient CF decomposition at 600 °C with a catalytic lifetime exceeding 1,000 hours.
View Article and Find Full Text PDFSingle-atom M-N (M=Fe, Co, Ni) catalysts exhibit high activity for CO reduction reaction (CO RR). However, the CO RR mechanism and the origin of activity at the single-atom sites remain unclear, which hinders the development of single-atom M-N catalysts. Here, using density functional theory calculations, we reveal intermediates-induced CO RR activity at the single-atom M-N sites.
View Article and Find Full Text PDFThe real active moiety of Fe-N-C single-atom catalysts (SACs) during the oxygen reduction reaction (ORR) depends on the applied potential. Here, we examine the ORR activity of various SAC active moieties (Fe-N, Fe-(OH)N, Fe-(O)N, and Fe-(OH)N) over a wide potential window ranging from -0.8 to 1.
View Article and Find Full Text PDFMain group single atom catalysts (SACs) are promising for CO electroreduction to CO by virtue of their ability in preventing the hydrogen evolution reaction and CO poisoning. Unfortunately, their delocalized orbitals reduce the CO activation to *COOH. Herein, an O doping strategy to localize electrons on p-orbitals through asymmetric coordination of Ca SAC sites (Ca-N O) is developed, thus enhancing the CO activation.
View Article and Find Full Text PDFACS Appl Mater Interfaces
March 2023
ZnS materials exhibit very negative potential of the conduction band, which is promising in photocatalytic reduction reactions. Unfortunately, previously reported ZnS materials for photocatalysis are mainly in the cubic phase, which produce high activity for H evolutions and low activity toward CO reductions. Herein, a hexagonal phase ZnS photocatalyst is fabricated for highly efficient CO reduction reactions.
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