<br>[Mo3S(S2)6]2–功能化层状双氢氧化物氧化固定气态汞,Chemistry of Materials

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[Mo3S(S2)6]2–功能化层状双氢氧化物氧化固定气态汞
Chemistry of Materials ( IF 7.2 ) Pub Date : 2024-05-28 , DOI: 10.1021/acs.chemmater.4c01098
Subrata Chandra Roy ₁ , Abu Asaduzzaman ₂ , Brooklynn May ₁ , Airin M. Beals ₁ , Xinqi Chen ₃ , Xianchun Zhu ₄ , Saiful M. Islam ₁

Affiliation

全球每年都会释放数千吨气态汞，促使世界卫生组织 (WHO) 在 2020 年将汞指定为构成严重健康风险的十大化学物质之一。因此，从环境中去除汞 ⁰ 势在必行。我们的研究引入了 [Mo ₃ S(S ₂ ) ₆ ] ^2– ≡ [Mo ₃ S < b6> ] ^2– -功能化层状双氢氧化物纳米颗粒（LDH–Mo ₃ S ₁₃ ），作为气态 Hg 的优异吸附剂< b10> 。该材料对气态元素 Hg ⁰ 具有 ∼2.33 × 10 ³ mg/g 的显着吸附能力。如此高的吸附能力使该材料成为迄今为止已知的铅非铂基汞 ⁰ 气体吸附剂。虽然 LDH 的 Mo ₃ S(S ₂ ) ₆ 物种的硫化物主要充当捕获气态 Hg 的活性位点，但它们的集成对于可及性至关重要气态 Hg ⁰ 到 LDH 片层之间的单个反应活性位点。 Hg ⁰ 蒸气与固体 LDH–Mo ₃ S ₁₃ 吸附剂之间的非均相反应能够将气态 Hg ⁰ 氧化为Hg ²⁺ ，并且 S ₂ ^2– 基团还原为 2S ^2– 产生氧化还原驱动的纳米晶 HgS 形成到固体吸附剂。密度泛函理论 (DFT) 计算进一步深入了解 Hg ⁰ 和 S 之间的相互作用，表明吸附能范围为 -8 至 -19 kJ/mol。此外，总反应焓计算为-4048 kJ/mol，表明HgS的自发形成。这项研究揭示了对 Hg ⁰ 蒸气和 Mo ₃ S(S ₂ ) ₆ 物质之间氧化还原驱动相互作用的原子理解以及LDH-Mo ₃ S ₁₃ 极高的汞吸附能力，凸显了金属硫化物功能化LDH在有效固定气态元素汞方面的潜力。

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Oxidative Immobilization of Gaseous Mercury by [Mo3S(S2)6]2–-Functionalized Layered Double Hydroxide

Every year, thousands of tons of gaseous mercury are released globally, prompting the World Health Organization (WHO) in 2020 to designate mercury as one of the top 10 chemicals posing severe health risks. Therefore, removal of Hg⁰ from the environment is imperative. Our study introduces [Mo₃S(S₂)₆]^2– ≡ [Mo₃S₁₃]^2–-functionalized layered double hydroxide nanoparticles, (LDH–Mo₃S₁₃), as an excellent sorbent for gaseous Hg⁰. This material achieved a remarkable sorption capacity of ∼2.33 × 10³ mg/g for gaseous elemental Hg⁰. Such an enormously high sorption capacity makes this material the lead non-platinum-based Hg⁰ gas sorbent known to date. Although sulfides of the Mo₃S(S₂)₆ species of LDH predominantly serve as active sites for capturing gaseous Hg, their integration is essential for the accessibility of gaseous Hg⁰ to the individual reactive active site between the LDH lamella. A heterogeneous reaction between the Hg⁰ vapor and the solid LDH–Mo₃S₁₃ sorbent enables the oxidation of gaseous Hg⁰ to Hg²⁺, and the reduction of the S₂^2– groups to 2S^2– yields redox-driven formation of the nanocrystalline HgS onto the solid sorbents. Density functional theory (DFT) calculations provide further insights into the interactions between Hg⁰ and S, indicating adsorption energy ranging from −8 to −19 kJ/mol. Moreover, the overall reaction enthalpy was calculated as −4048 kJ/mol, suggesting the spontaneous formation of HgS. This investigation unveils an atomistic understanding of the redox-driven interactions between Hg⁰ vapor and Mo₃S(S₂)₆ species as well as the remarkably high mercury sorption capacity of LDH–Mo₃S₁₃, highlighting the potential of metal sulfide-functionalized LDHs for the efficient immobilization of gaseous elemental mercury.

更新日期：2024-05-28

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