中国环境科学2024,Vol.44Issue(12) :6628-6640.

Mn-Fe改性碳基磁性吸附剂去除Hg0性能及机制

The performance and mechanism of Hg0 removal by Mn-Fe modified magnetic carbon sorbent

张敬东 杨娇羽 揭翠 李鸿鹄 彭喜燕 安淼
中国环境科学2024,Vol.44Issue(12) :6628-6640.

Mn-Fe改性碳基磁性吸附剂去除Hg0性能及机制

The performance and mechanism of Hg0 removal by Mn-Fe modified magnetic carbon sorbent

张敬东 1杨娇羽 1揭翠 1李鸿鹄 1彭喜燕 1安淼1
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作者信息

  • 1. 中南财经政法大学,环境与健康研究中心,中南财经政法大学信息工程学院,湖北武汉 430073
  • 折叠

摘要

采用溶胶凝胶法制备了一系列Mn-Fe改性碳基磁性吸附剂(MnxFey/C),并评价了其对气态单质汞(Hg0)的脱除性能及抗SO2中毒性能.采用SEM、TEM、BET、XRD、H2-TPR、Raman、XPS等方法对吸附剂理化结构进行了分析,以此探讨了不同MnxFey/C吸附剂性能差异的内在原因.结果表明,在反应温度150℃,Hg0浓度250μg/m3条件下,Mn2Fe1/C的Hg0脱除性能最好,达到99.99%.适当含量Fe的加入会引起Mn-Fe间强相互作用,发生Mn3++Fe3+↔Mn4++Fe2+的氧化还原循环,促进Mn4+的生成,同时降低Mn-O-Mn的化学键强度,增加氧空位(Ov)、活性氧物种(Oα)浓度,从而增强Hg0的吸附脱除性能.此外,Mn2Fe1/C具有良好的抗SO2性能,在2000×10-6SO2浓度下其Hg0脱除率依然保持在80%以上.XPS表明Fe能保护大部分Mn活性位点免受SO2中毒,同时抑制了吸附剂表面硫酸盐的形成与沉积.Mn2Fe1/C可以通过磁分离从粉煤灰中分离出来,其经4次吸附再生循环后仍有95.69%的Hg0脱除效率,具备优越的再生能力,是一种具有应用前景的燃煤烟气汞吸附剂.

Abstract

In this study,a series of Mn-Fe modified carbon-based magnetic sorbents(MnxFey/C)were prepared by the sol-gel method and further evaluated for gaseous elemental mercury(Hg0)removal and anti-SO2 poisoning.SEM,TEM,BET,XRD,H2-TPR,Raman and XPS were employed to analyze the physicochemical structure of sorbents.According to the characterization results,the inherent reasons for the performance differences of MnxFey/C sorbents were clarified.The results indicated that Mn2Fe1/C achieved best Hg0 removal performance(99.99%)under 150℃ and 250μg/m3 Hg0.The addition of an appropriate amount of Fe could cause strong interaction between Mn and Fe.It led to an oxidation-reduction cycle of Mn3++Fe3+↔Mn4++Fe2+,thus promoting the generation of Mn4+and weakening the chemical bond strength of Mn-O-Mn.Resultantly,the concentration of oxygen vacancies(Ov)and reactive oxygen species(Oa)was increased,which facilitated Hg0 removal over Mn2Fe1/C.In addition,Mn2Fe1/C showed good resistance to SO2.Its Hg0removal efficiency remained above 80%at a concentration of 2000× 10-6 SO2.XPS showed that Fe could protect most of the Mn active sites from SO2 poisoning,thus inhibiting the formation and deposition of sulfate on the sorbent surface.Mn2Fe1/C could be separated from fly ash through magnetic separation.After four cycles of adsorption and regeneration,Mn2Fe1/C still exhibited a Hg0removal efficiency of 95.69%.It showed superior regeneration ability and might be a promising mercury sorbent for coal-fired flue gas.

关键词

氧空位/过渡金属/吸附剂/气态单质汞/SO2抗性

Key words

oxygen vacancy/transition metal/sorbent/gaseous elemental mercury/SO2 resistance

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出版年

2024
中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCSCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
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