In-situ low-temperature sulfur CVD on metal sulfides with SO2 to realize self-sustained adsorption of mercury

Qinyuan Hong, Haomiao Xu (), Xiaoming Sun, Jiaxing Li, Wenjun Huang, Zan Qu (), Lizhi Zhang and Naiqiang Yan ()
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Qinyuan Hong: Shanghai Jiao Tong University
Haomiao Xu: Shanghai Jiao Tong University
Xiaoming Sun: Shanghai Jiao Tong University
Jiaxing Li: Shanghai Jiao Tong University
Wenjun Huang: Shanghai Jiao Tong University
Zan Qu: Shanghai Jiao Tong University
Lizhi Zhang: Shanghai Jiao Tong University
Naiqiang Yan: Shanghai Jiao Tong University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Capturing gaseous mercury (Hg0) from sulfur dioxide (SO2)-containing flue gases remains a common yet persistently challenge. Here we introduce a low-temperature sulfur chemical vapor deposition (S-CVD) technique that effectively converts SO2, with intermittently introduced H2S, into deposited sulfur (Sd0) on metal sulfides (MS), facilitating self-sustained adsorption of Hg0. ZnS, as a representative MS model, undergoes a decrease in the coordination number of Zn–S from 3.9 to 3.5 after Sd0 deposition, accompanied by the generation of unsaturated-coordinated polysulfide species (Sn2–, named Sd*) with significantly enhanced Hg0 adsorption performance. Surprisingly, the adsorption product, HgS (ZnS@HgS), can serve as a fresh interface for the activation of Sd0 to Sd* through the S-CVD method, thereby achieving a self-sustained Hg0 adsorption capacity exceeding 300 mg g−1 without saturation limitations. Theoretical calculations substantiate the self-sustained adsorption mechanism that S8 ring on both ZnS and ZnS@HgS can be activated to chemical bond S4 chain, exhibiting a stronger Hg0 adsorption energy than pristine ones. Importantly, this S-CVD strategy is applicable to the in-situ activation of synthetic or natural MS containing chalcophile metal elements for Hg0 removal and also holds potential applications for various purposes requiring MS adsorbents.

Date: 2024
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DOI: 10.1038/s41467-024-47725-3

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