Enhanced super-ultra-deep photocatalytic oxidative desulfurization by titanium-activated metal-organic frameworks nanophotocataltyst

IF 4.1 3区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2024-09-30 DOI:10.1016/j.jphotochem.2024.116056

Mehdi Beshtar , Afsanehsadat Larimi , Ali Akbar Asgharinezhad

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Abstract

Addressing the escalating global demand for fossil fuels and the urgent environmental concerns associated with their use necessitates the development and implementation of efficient and cost-effective techniques for the removal of sulfur compounds. In this study, titanium-activated MIL-101(Fe) was utilized for the removal of organosulfur compounds through the photocatalytic oxidation desulfurization (PODS) process. The coexistence of active sites with titanium and iron resulted in an ultra-deep desulfurization. The impact of titanium loading was assessed, with TxML representing the ratio of Ti to Fe (x = 1, 1.5, and 2, respectively). Nanophotocatalysts were fabricated by solvothermal method. The physicochemical properties of the new materials were investigated by performing XRD, TEM, FT-IR, FESEM, EDX, UV–Vis DRS, PL, GC–MS, ESR, TGA, transient photocurrent, and nitrogen adsorption–desorption analyses. The effect of titanium loading on the structure, and performance of photocatalysts in the PODS reaction was investigated. The reaction parameters were optimized for maximum efficiency. Under optimal conditions of T2ML loading at 1.5 g/L, a volumetric solvent to fuel ratio (S/F) of 1, and a temperature of 50 ℃, T2ML shows the best performance by removing 100 % of dibenzothiophene.

Kinetic experiments revealed that the PODS reaction obeys a pseudo-first order equation, and activation energy is 47.08 kJ.mol⁻¹.

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钛活化金属有机框架纳米光催化材料增强的超超深光催化氧化脱硫能力

全球对化石燃料的需求不断攀升，而与使用化石燃料相关的环境问题又迫在眉睫，因此有必要开发并实施高效且经济的脱硫技术。本研究利用钛活化 MIL-101（Fe）通过光催化氧化脱硫（PODS）工艺去除有机硫化合物。钛和铁的活性位点共存导致了超深度脱硫。评估了钛负载的影响，TxML 代表钛与铁的比例（分别为 x = 1、1.5 和 2）。纳米光催化剂是通过溶热法制造的。通过 XRD、TEM、FT-IR、FESEM、EDX、UV-Vis DRS、PL、GC-MS、ESR、TGA、瞬态光电流和氮吸附-解吸分析，研究了新材料的理化性质。研究了钛负载对 PODS 反应中光催化剂结构和性能的影响。为了获得最高效率，对反应参数进行了优化。在 T2ML 的负载量为 1.5 g/L、溶剂与燃料的体积比（S/F）为 1 和温度为 50 ℃ 的最佳条件下，T2ML 的性能最佳，可去除 100% 的二苯并噻吩。

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来源期刊

Journal of Photochemistry and Photobiology A-chemistry 化学-物理化学

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.