J Colloid Interface Sci
June 2024
The floatable photocatalyst at N-water interface allows the adequate supply of N reactant and the utilization of photothermal energy for photocatalytic N fixation, however, the presence of non-volatile NO product poses a challenge to the stability as it easily covers the catalytic active sites. Herein, a floatable TiO/Bi/CC (Carbon cloth) photocatalyst was designed, in which the non-volatile NO can be transformed to the volatile NH via the newly synergistic relay photocatalysis pathway (N → NO → NH) between TiO (N → NO) and Bi (NO → NH). Attractively, the spontaneous NO → NO step occurs on Bi component to promote the relay pathway performing.
View Article and Find Full Text PDFSelective removal of Ca and Mg ions using the 001 × 7 resin and Fe and Al ions using the S957 resin is able to achieve the deep purification of the phosphoric acid-nitric acid solution, but the adsorption behaviors of Fe and Al ions are seriously suppressed by phosphoric acid. In order to understand the interaction mechanism of separation processes and the influence of phosphoric acid, we first studied the bonding form of Ca, Mg, Fe, and Al ions on 001 × 7 and S957 resins using FT-IR and XPS techniques; subsequently, quantum chemistry computation was carried out to further explore the bonding mechanism between the functional groups on resins and metal ions. FT-IR and XPS results reveal that for the adsorption process on the 001 × 7 resin, hydroxyls from sulfonic acid groups combine with Ca and Mg ions.
View Article and Find Full Text PDFThe Volmer step in alkaline hydrogen evolution reactions (HERs), which supplies H* to the following steps by cleaving H-O-H bonds, is considered the rate-determining step of the overall reaction. The Volmer step involves water dissociation and adsorbed hydroxyl (*OH) desorption; Ru-based catalysts display a compelling water dissociation process in an alkaline HER. Unfortunately, the strong affinity of Ru for *OH blocks the active sites, resulting in unsatisfactory performance during HER processes.
View Article and Find Full Text PDFIn the process of photocatalytic ammonia synthesis, efficient activation of nitrogen molecules constitutes a fundamental challenge. During the N activation, the close interdependence between the acceptance and donation of electron results in their mutual limitation, leading to high energy barrier for N activation and unsatisfactory photocatalytic performance. This work decoupled the electron acceptance and donation processes by constructing Fe-Bi dual active sites, resulting in enhancing N activation through the high electron trapping ability of Fe and strong electron donating ability of Bi.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2023
Hydrogen spillover effects will significantly improve the activity of photocatalytic hydrogen evolution reactions (HER), while their introduction and optimization require the construction of an excellent metal/support structure. In this study, we have synthesized Ru/TiO catalysts with controlled oxygen vacancy (OVs) concentrations using a simple one-pot solvothermal method. The results show that Ru/TiO with the optimal OVs concentration exhibits an unprecedentedly high H evolution rate of 13604 μmol·g·h, which was 45.
View Article and Find Full Text PDFThe electrochemical hydrogen evolution reaction (HER) in alkaline media provides an environmentally friendly industrial application approach to replace traditional fossil energy. The search for efficient, low-cost, and durable active electrocatalysts is central to the development of this area. Transition metal carbides (MXenes) have been emerging as a new family of two-dimensional (2D) materials that have great potential in the HER.
View Article and Find Full Text PDFPhotocatalysis CO reduction into high-value-added chemical feedstocks is desirable for simultaneously addressing the solar energy storage, CO excess and energy shortage issues. In this work, a kind of original S-scheme BiOBr-(001)/BiSiO/Bi (OSB) heterostructure photocatalyst with rich oxygen vacancies is in-situ synthesized, which significantly promotes the photocatalytic CO reduction performance. Interestingly, the lower formation energy of oxygen vacancy exhibits the easy feasibility on the BiOBr-(001) surface via the assistant of ultrasound.
View Article and Find Full Text PDFThe scaling relations between nitrogen adsorption and NH destabilization are key challenges to the widespread adoption of the photocatalytic synthesis of ammonia. In this work, a Fe-rich MIL-101(Fe) (MIL-101(Fe/Fe)) was synthesized using a one-step solvent thermal method with ethylene glycol (EG) as a reducing agent, which can break the scaling relationship by photoinduced Fe (high nitrogen adsorption ability) and Fe (high NH destabilization ability) cycling. XPS was used to detect the change in iron valence state in the MIL-101(Fe/Fe) material.
View Article and Find Full Text PDFIn this study, a set of BiOCl with controllable ratios of (001) and (110) facets was prepared by adjusting the content of diethylene glycol (DEG) during the preparation process. The degradation experiment of bisphenol A (BPA) shows that under simulated sunlight, when the ratio of (001) to (110) is 0.61, BiOCl (BOC-2) has the best degradation activity, which can degrade 96.
View Article and Find Full Text PDFRegulating electron density at the active site by electronic directional transport from special channels is an effective strategy to accelerate the reaction rate in photocatalytic water splitting. Here, a novel two dimensional/two dimensional (2D/2D) BiOBr/TiC heterojunction with special interfacial charge transfer channel was fabricated successfully via in-situ growth of BiOBr on the surface of ultrathin TiC by using a convenient hydrolysis method. The electrostatic attraction between Bi cations and electronegative TiC ensures the construction of 2D/2D heterojunction and a strong intimate interface contact between TiC and BiOBr, which establishes an electronic transport channel, and shortens the charge transport distance, assuring excellent bulk-to-surface and interfacial charge transfer abilities.
View Article and Find Full Text PDFCarbon dioxide (CO) activation by effective electrons has been regarded as the rather necessary first-step for a CO reduction reaction (CORR). In addition, the electron migration and photoreaction selectivity are closely associated with the dominant crystal surface of a catalyst. Therefore, it is very interesting and important to elucidate the electron transfer and charge density effects on the catalyst surface for the CORR.
View Article and Find Full Text PDFPerformance of single-atom catalysis largely depends on the interaction between the metal and the supporter. Herein, ethylene glycol (EG) was used as a molecular bridge connecting Palladium (Pd) and bismuth oxybromide (BiOBr) to form atomically dispersed Pd catalyst (Pd-EG-BiOBr) for photocatalytic nitrogen fixation under ambient conditions. Compared with 0.
View Article and Find Full Text PDFPhotocatalytic nitrogen fixation has been considered to be a safe, green, eco-friendly, and sustainable technology. However, photoinduced activation of inert dinitrogen is an important factor hindering the development of this technology. Herein, in-situ Fe doped flower-like BiOCl with highly active sites exposure was prepared by a solvent thermal method, which has excellent performance of N photofixation.
View Article and Find Full Text PDFPorous carbon spheres with high surface area and microporous structure were synthesized from alkyl phenols and formaldehyde suspension polymerization and steam activation. The effects of air oxidation and ammonia solution heat treatment on the pore structure and surface chemistry of the carbon spheres were studied for catalytic oxidation of CHSH. The structure property and surface chemistry of the obtained carbon spheres were characterized by N adsorption-desorption, FTIR, scanning electron microscopy, XRD, elemental analysis, X-ray photoelectron spectroscopy and Boehm titration, and then thermal analysis and gas chromatography-mass spectrometry were applied to investigate the catalytic oxidation product.
View Article and Find Full Text PDFBiOBr-based photocatalysts hold great promise in the application of organic wastewater treatment and air purification. However, the catalysis ability of photocatalyst is greatly limited by its poor reduction capacity and intrinsic high recombination rate of photo-generated charge carriers. In this work, a novel direct Z-scheme BiOBr/BiOBr photocatalyst is prepared via a facile hydrolysis route at room temperature, which exhibits highly enhanced performance for resorcinol degradation and NO removal than pure BiOBr and BiOBr.
View Article and Find Full Text PDFPhotocatalytic reduction of CO using solar energy to decrease CO emission is a promising clean renewable fuel production technology. Recently, Bi-based semiconductors with excellent photocatalytic activity and carbon-based carriers with large specific surface areas and strong CO adsorption capacity have attracted extensive attention. In this study, activated carbon spheres (ACSs) were obtained carbonization and steam activation of phenolic resin-based carbon spheres at 850 °C synthesized by suspension polymerization.
View Article and Find Full Text PDFThe introduction of oxygen vacancies (OVs) on the surface of photocatalysts has already been proven to be an effective way to extend the light response to visible light and trap charge carriers, thereby promoting the photocatalytic performance. In this study, h-BN/OV-BiOCl composites were prepared using hexagonal boron nitride (h-BN) to further improve the visible-light photocatalytic activity of oxygen-vacancy-enriched bismuth oxychloride (OV-BiOCl). The composition and morphology of these materials were investigated, and the photocatalytic performance experiments showed that the introduction of h-BN could significantly improve the visible-light photocatalytic activity of OV-BiOCl, which was 1.
View Article and Find Full Text PDFThe electron transfer process (ETP) of a photocatalyst plays a crucial role in clarifying its photoelectrochemical catalytic mechanism. BiOX (X = F, Cl, Br, I) (001) surfaces display excellent photocatalytic performance due to the high separation efficiency of photogenerated electron-hole (e--h+) pairs in their own efficient internal electric field (IEF). The oxygen vacancies (OVs) on the surfaces could cause a change in localized electronic states, then improve the photocatalytic activity of BiOX.
View Article and Find Full Text PDFRecently, bismuth oxychloride nanomaterials (BiOCls) are showing great promise in pollutant removal. Residues from these environmental remediations are potential hazardous materials. Unfortunately, human health risks of BiOCls are still unexplored widely.
View Article and Find Full Text PDFIn this study, a novel visible-light-driven Bi4O5Br2 photocatalyst was successfully synthesized via the structure reorganization of BiOBr at room temperature using NH3·H2O as a structure-controlling agent. The obtained Bi4O5Br2 exhibited outstanding visible light activity and stability compared to BiOBr and P25 for the degradation of resorcinol. The physicochemical properties of Bi4O5Br2 were analyzed and calculated by modern characterization techniques and density functional theory (DFT).
View Article and Find Full Text PDFA theoretical investigation on the esterification mechanism of free fatty acid (FFA) in waste cooking oils (WCOs) has been carried out using DMol(3) module based on the density functional theory (DFT). Three potential pathways of FFA esterification reaction are designed to achieve the formation of fatty acid methyl ester (FAME), and calculated results show that the energy barrier can be efficiently reduced from 88.597kcal/mol to 15.
View Article and Find Full Text PDFNano-sized bismuth oxybromide (BiOBr) particles are being considered for applications within the semiconductor industry. However, little is known about their potential impact on human health. In this study, we comparatively investigated the cytotoxicity of BiOBr and titanium dioxide (TiO2) nanoparticles (NPs) using human skin keratinocyte cell line (HaCaT) as a research model.
View Article and Find Full Text PDFAs an emerging nanomaterial, bismuth oxychloride (BiOCl) has attracted explosive interests in diverse areas. However, how it interfaces with biological systems, particularly its interaction with human cells and the resulting effects are completely unknown. In this paper, the cytotoxicity of BiOCl nanosheets (NSs) was investigated toward a human skin derived cell line (HaCaT).
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