New Journal of Chemistry最新文献

An effective strategy for enhancing photocatalytic hydrogen evolution reaction (HER) activity is the implementation of the hydrogen spillover effect. Herein, a Ru/TiO₂–GO (graphene oxide) catalyst was fabricated by means of simple hydrothermal and ultrasound-assisted techniques. By using the secondary hydrogen spillover process, which involves the transfer of active hydrogen species from Ru to TiO₂ and then further to GO, the hydrogen evolution activity of Ru/TiO₂–2GO reached 23.9 mmol g⁻¹ h⁻¹, which is 45.2 times and 3.85 times greater than that of TiO₂ (0.53 mmol g⁻¹ h⁻¹) and Ru/TiO₂ (6.2 mmol g⁻¹ h⁻¹), respectively. Controlled experiments and detailed characterization have revealed that the dispersion of GO on the support provides critical desorption sites for H*, thereby promoting the cleavage of Ti–H bonds. H* undergoes secondary spillover onto GO and desorbs to generate H₂, enhancing the photocatalytic HER activity. This study enhances the photocatalytic activity of water splitting for hydrogen production by employing a secondary hydrogen spillover strategy, thereby presenting a novel approach for the design of efficient hydrogen production catalysts.

The reduction of carbon dioxide (CO₂) using electrochemical methods is one of the ways to achieve carbon recycling, as the increase in carbon dioxide emissions causes environmental problems. Single-atom dispersed Ni-NC site catalysts have emerged as effective electrocatalysts for the reduction of CO₂ to CO. Using ZIF-8 as a carrier, we aim to design a high-performance single nickel-site catalyst by elucidating the structure evolution of NiN_x sites during thermal activation as well as other key external factors such as the carbon particle size and nickel content. The pyridine N active sites generated after calcination have higher activity and CO selectivity. The catalyst achieved up to 99.6% CO generation at −0.88 V vs. RHE, and is one of the best catalysts for the reduction of CO₂ to CO. This work demonstrates an effective method for designing efficient electrochemical CO₂ reduction catalysts by tuning the surface structure of single-atom anchored carriers.

The metal catalytic active centers in solid catalysts containing metal-based polymeric ionic liquids exist in an ionic state, significantly enhancing their catalytic efficiency. In this study, a desulfurization catalyst, vinyl-3-butylimidazolium manganese chloride ionic liquid, is synthesized through the polymerization of approximately six monomers. This desulfurization catalyst is combined with the oxidant potassium peroxymonosulfate (PMS) and the extractant acetonitrile (ACN) to remove dibenzothiophene (DBT) from octane. In a reaction involving 20 mg of the catalyst, 1 g of PMS, 1 g of ACN, and 6 g of simulated oil containing 600 ppm DBT at 20 °C, the DBT removal efficiency reaches 99%. Furthermore, after six cycles of use, the desulfurization rate remains as high as 90%. GC-MS analysis reveals that the desulfurization products are DBTO and DBTO₂. The oxidation mechanism primarily involves Mn²⁺ in the catalyst losing electrons to activate HSO₅⁻, generating sulfate radicals (˙SO₄⁻), which oxidize the sulfur atom in DBT. HSO₅⁻ also facilitates the cyclic transformation among Mn²⁺, Mn³⁺, and Mn⁴⁺. Based on the desulfurization mechanism, the reaction kinetics for this catalytic oxidative desulfurization process are established. This desulfurization process is a zero-order reaction, with a reaction rate constant between Mn²⁺ and HSO₅⁻ of 0.09173 ppm mg⁻¹ min⁻¹ g⁻¹, and the activation energy for catalytic desulfurization is 35.62 kJ mol⁻¹.

The most effective method of resolving the issue of inadequate conductivity and significant volume expansion of the converted sodium storage anode material is to hybridize/combine the electroactive material with a conductive carbon material to form a carbonaceous nanocomposite material. Herein, a one-step solvothermal method was employed to construct a cobalt diselenide@carbon nanotube (CoSe₂@CNTs) composite with a heterojunction structure. The incorporation of CNTs not only enhances the overall conductivity of the composite but also effectively mitigates the expansion of CoSe₂ during charging and discharging, providing structural support to the material. Moreover, the electronic coupling effect between the distinct elements at the interface between CoSe₂ and CNTs optimizes the electronic structure and charge distribution of the composite, establishing a built-in electric field within the composite and enhancing the rapid transport of sodium ions. X-ray photoelectron spectroscopy (XPS) tests and density functional theory (DFT) calculations further substantiate these findings. Among all the prepared samples, the optimized CoSe₂@CNTs-2 electrode demonstrates outstanding sodium storage properties, characterized by ultrahigh long-term cycling stability (345.8 mA h g⁻¹ at 2 A g⁻¹ after 1750 cycles). Finally, the Na₃V₂(PO₄)₃@C//CoSe₂@CNTs-2 full battery was investigated, retaining a reversible capacity of 164.2 mA h g⁻¹ after 100 cycles at 0.1 A g⁻¹. This finding provides important theoretical support for the optimization and design of conversion anode materials for sodium storage.

This perspective provides an overview of recent studies on the use of photocatalysis for hydrogen production, with a particular focus on water splitting. It examines the developments in this field that have been facilitated by artificial intelligence tools, especially machine learning algorithms. The photocatalytic generation of hydrogen has been the subject of extensive study in recent years, as the necessity for higher efficiency and hydrogen production rates represents a crucial step in the development of this technology for its mass deployment. The known difficulties of these systems pertain to the complexities associated with the photocatalysts, including the effect of reactants, the synthesis process, and their efficiency, particularly in harvesting sunlight. Moreover, the design of the reactor is a challenging undertaking, particularly in light of the dynamic behavior and the interaction between photons, solutions, photocatalysts, and co-catalysts that must be considered in the photocatalytic production of hydrogen. Research on this subject must consider the use of green materials and processes for synthesis, avoid extensive experimentation to reduce the carbon footprint, and seek efficient and less resource-intensive computational resources. To surmount the challenges inherent to the synthesis and development process, while simultaneously enabling the establishment of structure–performance relationships for knowledge acquisition, high-performing computational methods are key. This article concludes by potential avenues for improvement by highlighting strategies that have been successfully implemented in other related fields and could be beneficial for this field.

The exponential surge in energy demand, driven by technological progress and evolving lifestyles, has precipitated a critical juncture. Energy sourcing now spans the spectrum from conventional to renewable alternatives. The limitations of conventional sources, entwined with their contributions to ecological degradation, deforestation, and the amplification of global warming and climate change, have come to the forefront. In response, renewable energy sources have surged into prominence, capturing both industrial and scientific attention. This comprehensive review navigates through the labyrinth of technological hurdles, breakthroughs, and heightened efficiencies that characterize diverse solar cell (SC) paradigms. Importantly, this exploration encompasses SC materials grouped under II–VI, III–V, and perovskite categories. While these materials bear utility, their intrinsic carcinogenic nature raises alarms regarding potential ecological and health impacts. The imperative to cultivate ecologically mindful alternatives reverberates as a persistent motif, underscored by a dedicated focus on the maturation of environmentally friendly carbon-based SCs. In this study, a meticulous comparative investigation of pivotal performance indicators such as V_oc, I_sc, fill-factor, and efficiency is meticulously conducted. This assessment spans an expansive array of materials and substrates utilized within the realm of SCs. In a broader context, the ultimate aspiration of this paper is to untie the intricate interaction of factors that govern the trajectory of solar cell performance. By doing so, it serves as an illuminating guidepost, steering the course of inquiry and advancement in the domain of sustainable energy technologies.

The growing global energy demand, fuelled by urbanization and globalization, has highlighted nuclear energy as a key sustainable solution. However, managing radioactive waste, particularly iodine, remains a critical challenge for its long-term viability. Recent studies indicate that nitrogen-rich adsorbents exhibit a strong affinity for iodine due to forming charge-transfer complexes with I₂, enhancing interaction forces. In this context, an N-heteroatom engineering strategy was employed to synthesize a hybrid zirconium triethylenetetramine (ZrT) exchanger of the class of tetravalent metal acid (TMA) salts. To further improve its potential for large-scale industrial applications, ZrT was subsequently fabricated into a spherical ZrT@PVDF composite granule for iodine adsorption. Adsorption experiments revealed that ZrT and ZrT@PVDF exhibit outstanding iodine capture performance in vapor (1262.5 and 945.2 mg g⁻¹), including saturated I₂ (886 and 706 mg g⁻¹) and I₃⁻ (NaI/I₂) (920 and 746 mg g⁻¹) aqueous solution and organic phase (772 and 598 mg g⁻¹). However, the presence of single, double, and triple interfering ions had only a marginal impact on the iodine removal efficiency of both adsorbents. Spectroscopic, kinetic, and several isothermal studies demonstrate that iodine adsorption occurs through both physisorption and chemisorption mechanisms. The interaction between iodine and the nitrogen atoms of ZrT, leading to the formation of a stable charge-transfer complex, contributes to the high performance of the material in adsorption applications. Notably, ZrT@PVDF exhibited outstanding regeneration and reusability, retaining 87% of its initial adsorption capacity over five adsorption–desorption cycles, highlighting its potential for practical applications. This research presents an effective strategy for developing efficient iodine sorbents with tuneable morphologies, offering a promising solution to environmental challenges.

SiO₂–ZrO₂ hybrid polymeric network films incorporating silver nanoparticles (Ag NPs) with long-term stability were developed by a sol–gel spray coating technique under room temperature (RT) curing using tetraethyl orthosilicate (TEOS), (3-glycidyloxypropyl)trimethoxysilane (GLYMO), a diamine based curing agent, zirconium(IV) isopropoxide, trimethylsiloxy-terminated polydimethylsiloxane (PDMS) and silver nitrate. Formation of zirconium oxide (ZrO₂) in the Ag NPs embedded polymeric hybrid structure at RT plays a vital role in this robust hybrid matrix to keep Ag NPs stable over a period of 500 days under ambient conditions without significant degradation of absorbance intensity at 415 nm with retention of a strong brownish yellow color. Comprehensive characterization of the RT cured coated film with an Ag NP embedded hybrid matrix was conducted using UV-visible absorption spectroscopy, grazing incidence X-ray diffraction (GIXRD), attenuated total reflectance-Fourier transform infrared (ATR-FTIR), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and water contact angle (WCA) measurement. The physico-mechanical and weather resistance properties of the prepared zirconia embedded film were evaluated using pencil hardness, adhesion, chemical durability, humidity, thermal effect and UV resistance tests. Due to the long-term stability of Ag NPs in the RT cured hybrid polymeric matrix, it shows potential for antibacterial applications.

The global concern regarding environmental contamination caused by antimony (Sb) in water has become increasingly prominent, presenting a complex environmental challenge. To improve Sb adsorption efficiency, novel N-methylglucamine modified cellulose microspheres (Celp-g-GMA-NMG) offer a sustainable and effective solution for the simultaneous removal of Sb(III) and Sb(V) with promising application in actual mine inflow. Celp-g-GMA-NMG retain high adsorption efficiency for Sb(III) over a wide pH range. The prepared adsorbent exhibits a fast adsorption rate and high adsorption capacity of 217.61 mg g⁻¹ for Sb(III) and 49.11 mg g⁻¹ for Sb(V). The adsorption process confirms the Langmuir and pseudo-second-order kinetic model. In batch and dynamic experiments, Celp-g-GMA-NMG not only effectively removes Sb from actual mine inflow, but also simultaneously captures highly toxic arsenic. In addition, the Celp-g-GMA-NMG captured Sb(III) and Sb(V) by coordination and electrostatic interactions, respectively.

A series of water-soluble gold(I) complexes bearing phosphine ligands, [AuCl(L)] {where L = 1,3,5-triaza-7-phosphaadamantane, PTA (1); 3,7-diacetyl-1,3,7-triaza-5-phosphabicyclo[3.3.1]nonane, DAPTA (2); or 1,3,7-triaza-5-phosphabicyclo[3.3.1]nonane-3,7-diylbisphenylmethanone, DBPTA (3)} and [AuCl(L)]X {where L is either PTA-CH₂-C₆H₄-p-COOH and X = Br (4) or PTA-CH₂-C₆H₃-p-OH-m-CHO and X = Cl (5)}, were synthesized under mild conditions and characterized with multinuclear (¹H, ¹³C and ³¹P) nuclear magnetic resonance (NMR) spectroscopy, attenuated total reflection – Fourier transform infrared (ATR-FTIR) spectroscopy, matrix-assisted laser desorption/ionization – mass spectrometry (MALDI-MS) and elemental analysis. The catalytic activity of the complexes was evaluated in the peroxidative oxidation of cyclohexane to cyclohexanol and cyclohexanone. Homogeneous reactions were conducted in aqueous media, while heterogeneous reactions were performed after immobilizing the complexes on porous carbon supports, including activated carbon (AC), carbon nanotubes (CNT) and their oxidized derivatives (AC-ox, AC-ox-Na, CNT-ox and CNT-ox-Na). The results demonstrated a better catalytic performance, in terms of yields and selectivity, under heterogeneous conditions depending on the nature of the carbon support. Finally, complexes 1–5 showed remarkable cytotoxicity against a selection of ovarian, lung and colon cancer cell lines, with IC₅₀ values comparable to (or even better than) those of cisplatin. Interestingly, the most promising complexes exhibited good to excellent cytotoxicity against cancer cells while demonstrating substantial inactivity against normal ones.