Regulation of the Sulfur Environment in Clusters to Construct a Mn–Sn2S6 Framework for Mercury Bonding,Environmental Science & Technology

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Regulation of the Sulfur Environment in Clusters to Construct a Mn–Sn2S6 Framework for Mercury Bonding
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2022-02-03 , DOI: 10.1021/acs.est.1c08529
Qinyuan Hong ₁ , Haomiao Xu ₁ , Jiaxing Li ₁ , Wenjun Huang ₁ , Zan Qu _{1,

2} , Naiqiang Yan _{1,

2}

Affiliation

The remarkable chemical activity of metal–sulfur clusters lies in their unique spatial configuration associated with the abundant unsaturated-coordination nature of sulfur sites. Yet, the manipulation of sulfur sites normally requires direct contact with other metal atoms, which inevitably changes the state of the coordinated sulfur. Herein, we facilely construct a Mn–Sn₂S₆ framework by regulating the sulfur environment of the [Sn₂S₆]^4– cluster with metal ions. Mn–Sn₂S₆ showed superior removal performance to gaseous elemental mercury (Hg⁰) at low temperatures (20–60 °C) and exhibited high resistance against SO₂. Moreover, Mn–Sn₂S₆ can completely remove liquid Hg²⁺ ions with low or high concentrations from acid wastewater. In addition, the adsorption capacities of Mn–Sn₂S₆ toward Hg⁰ and Hg²⁺ reached 21.05 and 413.3 mg/g, respectively. The results of physico-chemical characterizations revealed that compared with Cu²⁺, Co²⁺, and Fe²⁺, the moderate regulation of Mn²⁺ led to the special porous spherical structure of Mn–Sn₂S₆ with uniform element distribution, due to the difference of electrode potentials [E^θ(Mn²⁺/Mn) < E^θ(S/S^2–) < E^θ(Sn⁴⁺/Sn²⁺)]. The porous structure was beneficial to Hg⁰ and Hg²⁺ adsorption, and the presence of Mn⁴⁺/Mn³⁺ and S^1– promoted the oxidation of Hg⁰, resulting in stable HgS species. The constructed Mn–Sn₂S₆, thus, is a promising sorbent for both Hg⁰ ang Hg²⁺ removal and provides guidelines for cluster-based materials design and tuning.

中文翻译：

调节簇中的硫环境以构建用于汞键合的 Mn-Sn2S6 框架

金属-硫簇的显着化学活性在于其独特的空间构型与硫位点丰富的不饱和配位性质相关。然而，硫位点的操作通常需要与其他金属原子直接接触，这不可避免地会改变配位硫的状态。在此，我们通过用金属离子调节[Sn ₂ S ₆ ] ^4-簇的硫环境，轻松地构建了Mn-Sn ₂ S _6骨架。Mn-Sn ₂ S ₆在低温（20-60 °C）下表现出优于气态元素汞（Hg ^{0 ）的去除性能，并表现出对SO}_{2的高抗性}. 此外，Mn-Sn ₂ S ₆可以完全去除酸性废水中低浓度或高浓度的液态Hg ^2+离子。此外，Mn-Sn ₂ S ₆对Hg ⁰和Hg ²⁺的吸附量分别达到21.05和413.3 mg/g。物理化学表征结果表明，与Cu ²⁺、Co ²⁺和Fe ^{2+相比，Mn}²⁺的适度调控导致Mn-Sn ₂ S ₆具有特殊的多孔球形结构，元素分布均匀，由于电极电位的不同[E ^θ (Mn ²⁺ /Mn) < E ^θ (S/S ^2– ) < E ^θ (Sn ⁴⁺ /Sn ²⁺ )]。多孔结构有利于Hg ⁰和Hg ²⁺的吸附，Mn ⁴⁺ /Mn ³⁺和S ^1-的存在促进了Hg ⁰的氧化，产生了稳定的HgS物种。因此，构建的 Mn-Sn ₂ S ₆是一种有前途的吸附剂，可用于 Hg ⁰和Hg ²⁺的去除，并为基于簇的材料设计和调整提供指导。

更新日期：2022-02-03

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