Abstract ：

The dopant WO3 of the catalyst Pt-0.5P&W/TiO2 enhanced the SO2 resistance of the catalyst for CO oxidation in sintering waste gas, but it also had an impact on strong metal-support interactions (SMSI), which decreased the CO catalytic activity. Adding alkali metal Na to Pt-0.5P&W/TiO2 can effectively improve the CO catalytic performance. The Pt-O-Na bond replaced the Pt-O-Ti bond, allowing Na to act as an electron and structure promoter instead of TiO2 to contribute the electronic and synergistic effects in catalysis. XPS and EPR date indicated that the positively charged group centered on Pt adsorbed hydroxyl groups by electrostatic interaction, which coacted with Na to form Pt-Ox(OH)yNa. In situ infrared data indicated that Na promoted the electron density on the Pt surface leading to the disproportionation of CO on the Pt surface to produce inactive C*. The production of C* facilitated the adsorption and activation of O2 by blocking the single-layer adsorption of CO on Pt. The active oxygen species adsorbed on the catalyst surface increased the CO activity of the catalyst. In sulfur-containing flue gas conditions, SO2 reacted with Na around Pt to generate sodium sulfate, which enhanced the local acidity of the active site and the sulfur resistance of the catalyst.

Keyword ：

Active oxygen Sulfur resistance Interaction Alkali metal

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Abstract ：

Herein, a single-atom catalyst (SAC) featuring Fe-N-5 sites (FeNC) with optimized electronic structures was constructed and applied to activate peroxymonosulfate (PMS) for wastewater purification. The high-coordinated Fe-N-5 sites was obtained by creating a high-nitrogen gas environment around fully exposed Fe atomic sites on chitosan surface during pyrolysis. The FeNC/PMS system demonstrated excellent decontamination capability, superior anti-pH interference ability, while also exceptional durability in a continuous-flow catalytic filtration reactor. Experiments and density functional theory calculations unveiled that Fe-N-5 site was the active center. Meaningfully, neighboring carbonyl groups narrowed the gap between d-band center of Fe 3d and Fermi level, which increased the adsorption energy of PMS on Fe-N-5 sites, thus lowering the energy barrier for singlet oxygen generation. This study brings a vivid electronic structure optimization strategy for enhancing the catalytic activity of Fe SAC as well as guiding the selection of desirable catalysts for wastewater purification by Fenton-like chemistry.

Keyword ：

Electronic structure optimization High-coordinated M-N-x sites Density functional theory Fenton-like reaction Single-atom catalysts

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Abstract ：

Antibiotics pose significant risks to both the environment and human health. Herein, we develop a collaborative strategy for the enhanced removal of a typical antibiotic, Ciprofloxacin (CIP), by using a bamboo leaf -derived biochar/iron silicate composite (BL-FeSi) with the assistance of peroxymonosulfate (PMS). The rationale behind the design is the construction of composited material with synergistic adsorption -catalysis functions, based on covalent bonding networks of the biochar and specific Fe(III)/Fe(II) redox chemistry of iron silicate in PMS activation system. H 2 reduction of pristine BL-FeSi increases Fe(II) content and thus improves catalytic activity. Batch experiments demonstrate that the preferred BL-FeSi 400 (H 2 treatment at 400 degrees C) exhibits superior efficiency in activating PMS. The CIP removal efficiency is highly dependent on pH value of reaction solution. A remarkable 97% removal is achieved at pH = 5.5 (CIP: 60 mL, 20 mg/L; BL-FeSi 400 : 0.2 g/L, PMS: 0.2 g/L), and the pH increase to 11 results in 100% CIP removal. The BL-FeSi 400 shows robust resistance to inorganic ions (NO 3 - , SO 4 (2 -) , HCO 3 - , and H- 2 PO 4 (-) ), and the catalytic activity remains consistently high ( >82%) even after four consecutive cycles, making it highly promising for practical applications. It is found that both radical pathway (center dot OH and SO 4 center dot - ) and non - radical pathway ( O-1 ( 2) ) contribute to CIP degradation in the BL-FeSi 400 /PMS system, while the active center dot OH dominates the oxidization process. The coupling of adsorption and degradation holds great potentials for effective removal of more organic contaminants.

Keyword ：

Adsorption Advanced oxidation Biochar Iron silicate Ciprofloxacin

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In recent years, Iron-based materials(IBMs)/Periodate(PI) systems have gained attention in the treatment of water environments due to their excellent high oxidizing capacity, high stability, and strong resistance to environmental impacts. This work provides a synthetical overview of the current research status and progress of IBM/PI systems, and the vital role of Fe species is emphasized. The IBMs were categorized into three main groups by the different substances complexed with Fe: iron-carbon composites, iron-metal/nonmetallic composites, and iron with iron oxides. The possible catalytic influences of the aqueous species were explored. The mechanistic discussion was categorized into four groups, Fe0, Fe(II), Fe(IV), and Electron transfer pathway(ETP), depending on the valence of Fe at the beginning. Among them, Fe (II) is the most important valence state because it is an indispensable valence state before the formation of Fe(IV), and Fe(II) is also the valence state that can activate most kinds of active substances in PI. Interestingly, ETP-dominated PI activation systems tend to occur in ironcarbon complexes, and carbon materials may be necessary for triggering the ETP. In addition, the applicable state of IBMs/PI systems in water environments was explored from both the radical and non-radical perspectives. In the end, the deficiencies and improvements of the current IBMs/PI systems were summarized. Hoping that new inspirations can be provided for the subsequent IBMs/PI systems development.

Keyword ：

Periodate Iron-based materials Water environmental treatment Catalysis

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Abstract ：

Single-atom catalysts (SACs), as a thriving subfield of catalysis, have progressed tremendously. However, the contradiction between the isolated dispersion feature of metal sites and the high mass-specific activity of the catalyst inhibits the advances of the SACs. Herein, the Pt atoms are confined at the metallic Co phase edge in two-dimensional Co/Co(OH)(2) hierarchy structure (Pt-SA-Co@Co-Co(OH)(2)) by the defect inducted order electrode-position strategy. Both integrations of in-situ/ex-situ experimental characterizations and theoretical calculation reveal that such metal edge confined Pt atoms possess an enlarged atom exposure ratio, high stability, and the like-metal electronic state contributed by metal Co 3d, which enables the Pt atoms with more suitable affinity to simultaneously bind the multiple H atoms for durable H*-H-2 conversion and H-2 evolution. Moreover, the metallic PtSA-Co collaborated Co/Co(OH)(2) interfaces demonstrate a strong H2O dissociation capacity by the preference adsorption of H* on metallic Pt-SA-Co and OH*on Co/Co(OH)(2) interfaces. Combining a further enhancement of constructing the catalysts on an Ag nanowire network to form a seamlessly conductive nanostructure, the Pt-SA-Co@Co-Co(OH)(2) achieves a high mass activity with 5.92 A mg(-1) at the overpotential of 100 mV in alkaline condition, 37 times to that of the benchmark Pt/C catalyst and significantly outperforming the reported catalysts. While our work has focused on the hydrogen evolution reaction, this class of metal edge collaborated single-atom catalysts may be conducive to unlock the low mass-specific activity of atomically dispersed catalysts for various processes, such as oxygen evolution reactions (OER), CO2 reduction, and biomass conversion, etc.

Keyword ：

Hierarchy structure Multiple hydrogen conversion Metal edge Single-atom catalysts Confinement effect

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In various domains spanning materials synthesis, chemical catalysis, life sciences, and energy materials, in situ transmission electron microscopy (TEM) methods exert a profound influence. These methodologies enable the real-time observation and manipulation of gas-phase and liquid-phase reactions at the nanoscale, facilitating the exploration of pivotal reaction mechanisms. Fundamental research areas like crystal nucleation, growth, etching, and self-assembly have greatly benefited from these techniques. Additionally, their applications extend across diverse fields such as catalysis, batteries, bioimaging, and drug delivery kinetics. However, the intricate nature of 'soft matter' presents a challenge due to the unique molecular properties and dynamic behavior of these substances that remain insufficiently understood. Investigating soft matter within in situ liquid-phase TEM settings demands further exploration and advancement compared to other research domains. This research harnesses the potential of in situ liquid-phase TEM technology while integrating deep learning methodologies to comprehensively analyze the quantitative aspects of soft matter dynamics. This study centers on diverse phenomena, encompassing surfactant molecule nucleation, block copolymer behavior, confinement-driven self-assembly, and drying processes. Furthermore, deep learning techniques are employed to precisely analyze Ostwald ripening and digestive ripening dynamics. The outcomes of this study not only deepen the understanding of soft matter at its fundamental level but also serve as a pivotal foundation for developing innovative functional materials and cutting-edge devices.

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Exploration of multifunctional integrated catalysts is of great significance for photocatalysis toward practical application. Herein, a 1D confined nanoreactor with a heterogeneous core-shell structure is designed for synergies of efficient catalysis and temperature monitoring by custom encapsulation of Z-scheme heterojunction CuS quantum dots/BiVO4 (CuS QDs/BiVO4) and Y2O2S-Er, Yb. The dispersed active sites created by the QDs with high surface energy improve the mass transfer efficiency, and the efficient electron transport channels at the heterogeneous interface extend the carrier lifetime, which endows the nanoreactor with excellent catalytic performance. Meanwhile, real-time temperature monitoring is realized based on the thermally coupled levels H-2(11/2)/S-4(3/2)-> I-4(15/2) of Er3+ using fluorescence intensity ratio, which enables the monitorable photocatalysis. Furthermore, the nanoreactor with a multidimensional structure increases effective intermolecular collisions to facilitate the catalytic process by restricting the reaction within distinct enclosed spaces and circumvents potential unknown interaction effects. The design of multi-space nanoconfined reactors opens up a new avenue to modulate catalyst function, providing a unique perspective for photocatalytic applications in the mineralization of organic pollutants, hydrogen production, and nitrogen fixation.

Keyword ：

core-shell structure coaxial electrospinning multifunctional nanoreactor temperature sensing Z-scheme heterojunction

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Abstract ：

As a solid hazardous waste material, economical and environmental efficacy of spent adsorbent loaded by toxic heavy metals (HMs) are often neglected, which maybe bring serious secondary pollution. In this work, we report a green recycle route for spent HM-bearing calcium silicate hydrate (CSH) adsorbents to construct nanocrystalloaded functional materials. Typically, bimetallic CuNi catalyst (Cu-Ni@deCa-CSH) is obtained by CO2 weathering decalcification of the exhausted CSH adsorbed by Cu2+ and Ni2+, and subsequently reducing at 550 celcius for 6 h under 5 vol% H2/Ar. The universal precursor, HM loaded CSH spent adsorbents, could be ideal for implementing 'CO2 decalcification-H2 reduction' to obtain more metal or metal oxide nanoparticle loaded deCa-CSH samples (Cu-Fe@deCa-CSH, Cu-ZnO@deCa-CSH, Cu-CoO@deCa-CSH, Cu-CeO2@deCa-CSH, etc.), which can dramatically change the surface acidity of substrate owing to the phase transformation from basic CSH to inert silica (deCa-CSH), thus benefitting catalytic reactions. As a case study, the typical 100Cu-100Ni@deCa-CSH (The initial ion concentration is 100 mg/L) exhibits good catalytic activity and stability for p-nitrophenol (p-NP) hydrogenation into p-aminophenol (p-AP) with NaBH4 reducing agent. The conversion efficiency of 99.04% can be achieved within 18 min (initial p-NP: 60 mL, 20 mg/L, Catalyst: 20 mg, NaBH4: 40 mg, pH = 8). Ni addition facilitates electron transfer from Ni to Cu, and the resultant lower electron binding restraint in the heterostructure thus improves the conversion efficiency of p-NP. Important parameters (p-NP initial concentration, NaBH4 addition dosage, solution pH, etc.) are discussed extensively to understand how to prefer reaction conditions for p-NP hydrogenation. The developed surface chemistry strategy thus provides a realistic basis for the formation of functional materials via explore the potential value of solids post-use.

Keyword ：

Adsorbent Recycle Cu -Ni heterostructure Calcium silicate hydrate Catalysis

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Copper (Cu) is evidenced to be effective for constructing advanced catalysts. In particular, Cu2O is identified to be active for general catalytic reactions. However, conflicting results regarding the true structure-activity correlations between Cu2O-based active sites and efficiencies are usually reported. The structure of Cu2O undergoes dynamic evolution rather than remaining stable under working conditions, in which the actual reaction cannot proceed over the prefabricated Cu2O sites. Therefore, the dynamic construction of Cu2O active sites can be developed to promote catalytic efficiency and reveal the true structure-activity correlations. Herein, by introducing the redox pairs of Cu2+ and reducing sugar into a photocatalysis system, it is clarified that the Cu2O sub-nanoclusters (NCs), working as novel active sites, are on-site constructed on the substrate via a photoinduced pseudo-Fehling's route. The realistic interfacial charge separation and transformation capacities are remarkably promoted by the dynamic Cu2O NCs under the actual catalysis condition, which achieves a milestone efficiency for nitrate-to-ammonia photosynthesis, including the targets of production rate (1.98 +/- 0.04 mol g(Cu)(-1) h(-1)), conversion ratio (94.2 +/- 0.91 %), and selectivity (98.6 %+/- 0.55 %). The current work develops an effective strategy for integrating the active site construction into realistic reactions, providing new opportunities for Cu-based chemistry and catalysis sciences research.

Keyword ：

Nitrate Reduction Operando Identification Ammonia Photosynthesis Cu2O Dynamic Active Sites

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NiCuFe layered double oxide (LDO) catalysts were synthesized using co-precipitation, impregnation, and urea hydrothermal methods. The NH3-SCR activity of NiCuFe-LDO catalysts was investigated to determine the effect of different synthesis methods. All NiCuFe-LDO samples exhibited good catalytic performance at low temperatures, with the sample synthesized using the urea hydrothermal method (NiCuFe-LDO-3) being the most efficient catalyst. The NiCuFe-LDO-3 catalyst achieved over 80% NO conversion in the temperature range of 180(degrees)C to 280 C-degrees, with a peak of 95.13% at 240(degrees)C. The physicochemical properties of the samples were systematically characterized using XRD, SEM, BET, NH3-TPD, H-2-TPR, XPS, and in-situ DRIFTS. The results showed that the NiCuFe-LDO-3 sample had the best crystallinity, as demonstrated by XRD and SEM. BET analysis revealed that the NiCuFe-LDO-3 sample had the largest specific surface area. The NiCuFe-LDO-3 sample was found to have more acidic sites and a better redox capacity than the other samples, according to the H-2-TPR and NH3-TPD results. In-situ DRIFTS analysis showed that the catalyst operates through both E-R and L-H reaction mechanisms.

Keyword ：

NH3-SCR Urea Hydrothermal Heterogeneous catalysis LDO NiCuFeOx

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