Mechanistic insight into the synergistic effect of O2 and SO2 for improving removal of arsenic over Mn-modified Fe2O3-based sorbent

IF 2.1 4区化学 Q3 CHEMISTRY, PHYSICAL Surface Science Pub Date : 2024-09-16 DOI:10.1016/j.susc.2024.122614

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Abstract

Iron-based materials are promising sorbents for controlling arsenic emissions. However, the effects of SO₂, especially the synergistic mechanism of As₂O₃ adsorption under the combined effects of O₂ and SO₂, remain inadequately explored. This study investigated for the first time the impact of the newly formed surface resulting from the adsorption and dissociation of O₂ and SO₂ on the adsorption of As₂O₃. The results showed that Mn_3f and Fe_3f sites were the active sites for the adsorption of O₂ and SO₂, which competed with As₂O₃ and hindered its adsorption. Conversely, dissociation created more reactive sites, which promoted the process. Selectivity analysis revealed that As₂O₃ preferentially adsorbed on the dissociated surface, highlighting the dominance of the promotion effect. Finally, starting from the adsorption sequence of O₂ and SO₂, the impact of arsenic adsorption and oxidation was examined on sorbents created through the sequential adsorption of O₂ and SO₂. Regardless of the adsorption sequence, active O atoms with catalytic effects were exposed, supporting the enhanced removal of arsenic under the synergistic effect of O₂ and SO₂. Building upon this analysis, a theoretical framework for efficiently removing As₂O₃ from O₂ and SO₂ flue gases using Mn-modified Fe₂O₃-based materials was developed.

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从机理上深入了解氧气和二氧化硫在锰改性的 Fe2O3 基吸附剂上提高砷去除率的协同效应

铁基材料是一种很有前景的砷排放控制吸附剂。然而，对于二氧化硫的影响，尤其是二氧化硫和二氧化硫共同作用下 As2O3 的协同吸附机理，研究仍显不足。本研究首次探讨了 O2 和 SO2 吸附和解离后形成的新表面对 As2O3 吸附的影响。结果表明，Mn3f 和 Fe3f 位点是吸附 O2 和 SO2 的活性位点，它们与 As2O3 竞争，阻碍了 As2O3 的吸附。相反，解离产生了更多的活性位点，促进了吸附过程。选择性分析表明，As2O3 更倾向于吸附在解离的表面上，突出了促进效应的主导地位。最后，从 O2 和 SO2 的吸附顺序入手，研究了砷的吸附和氧化对通过 O2 和 SO2 的顺序吸附产生的吸附剂的影响。无论采用哪种吸附顺序，都会暴露出具有催化作用的活性 O 原子，从而支持在 O2 和 SO2 的协同作用下提高砷的去除率。在此分析的基础上，我们建立了一个理论框架，利用锰改性的 Fe2O3 基材料高效去除 O2 和 SO2 烟气中的 As2O3。

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来源期刊

Surface Science 化学-物理：凝聚态物理

CiteScore

3.30

自引率

5.30%

发文量

137

审稿时长

25 days

期刊介绍： Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.