基于高孔活性炭的无金属光催化剂。表征和光催化评价

IF 4.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2025-05-01 Epub Date: 2025-01-02 DOI:10.1016/j.jphotochem.2024.116247
John J. Alvear-Daza , Victoria Melin , Karina G. Irvicelli , Juan C. Murillo-Sierra , Antonela Canneva , Jorge A. Donadelli , Cristian H. Campos , Cecilia C. Torres , David Contreras , Alain Celzard , Vanessa Fierro , Luis R. Pizzio , Julián A. Rengifo-Herrera
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引用次数: 0

摘要

用H3PO4对葵花籽壳(SSS)进行化学活化,得到了含有碳中心环境持久性自由基(EPFRs)、醌类官能团等的高孔活性炭(ACSSSH3PO4),并具有轻微的石墨化程度。ACSSSH3PO4具有较高的双氯芬酸(DFC)和布洛芬(IBP)暗吸附量(1 h后约98%),在紫外和可见光照射下,采用定量和定性方法评价了ACSSSH3PO4作为无金属光催化剂的性能。然而,由于这两种污染物在固体上的高度吸附,监测光催化活性是不可能的。为此,我们开发了一种定量和定性的策略来评估高孔活性炭中污染物降解的存在。一方面,定性方法基于ATR-FTIR光谱,检测吸附在活性炭上的两种分子的红外波段,并评估其强度降低或在光照射5h后氧化副产物的新红外波段的出现。另一方面,定量方法是基于解吸程序,在光照射5小时后,从ACSSSH3PO4中去除DFC和IBP,并通过UHPLC测定其浓度。结果表明,在λ >下辐照5h;260 nm时,ACSSSH3PO4对吸附的DFC和IBP的降解率分别为62%和30%,而在可见光照射下,ACSSSH3PO4对污染物的降解率分别为42 - 29%和20%。因此,ACSSSH3PO4表现出显著的光诱导活性,可能是由于EPFRs、醌和石墨官能团。
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Metal-free photocatalyst based on highly porous activated carbon obtained from agro-industrial residues. Characterization and photocatalytic evaluation
The chemical activation of sunflower seed shells (SSS) with H3PO4 led to highly porous activated carbon (ACSSSH3PO4) containing carbon-centered environmentally persistent free radicals (EPFRs), quinone functional groups, among others, and a slight graphitization degree. With high diclofenac (DFC) and ibuprofen (IBP) dark adsorption capacity (∼98 % after 1 h), ACSSSH3PO4 was evaluated as a metal-free photocatalyst using quantitative and qualitative approaches under UV and visible light irradiation. However, due to the high adsorption of both pollutants onto the solid, monitoring photocatalytic activity was impossible. For this reason, a quantitative and qualitative strategy was developed to evaluate the existence of pollutant degradation in highly porous activated carbon. On the one hand, the qualitative approach was based on the use of ATR-FTIR spectroscopy, detecting IR bands of both molecules adsorbed on the activated carbon and evaluating their intensity reduction or the apparition of new IR bands assigned to oxidized byproducts after 5 h of light irradiation. On the other hand, the quantitative approach was based on a desorption procedure to remove DFC and IBP from the ACSSSH3PO4 after 5 h of light irradiation and quantifying their concentrations by UHPLC. Thus, it was found that under irradiation for 5 h at λ > 260 nm, ACSSSH3PO4 showed 62 and 30 % degradation for adsorbed DFC and IBP, respectively, while under visible irradiation, pollutants degradation was 42–29 % and 20 %. ACSSSH3PO4 thus demonstrated significant photoinduced activity, probably due to EPFRs, quinone, and graphitic functional groups.
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来源期刊
CiteScore
7.90
自引率
7.00%
发文量
580
审稿时长
48 days
期刊介绍: JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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