Xu Haomiao, Hong Qinyuan, Zhang Zhao-Yang, Cai Xiangling, Fan Yurui, Liu Zhisong, Huang Wenjun, Yan Naiqiang, Qu Zan, Zhang Lizhi
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory of Electrical Insulation and Thermal Aging, Key Laboratory of Thin Film and Microfabrication (Ministry of Education), Shanghai Jiao Tong University, Shanghai 200092, China.
Environ Sci Technol. 2023 Apr 4;57(13):5424-5432. doi: 10.1021/acs.est.2c09640. Epub 2023 Mar 20.
Flue gas mercury removal is mandatory for decreasing global mercury background concentration and ecosystem protection, but it severely suffers from the instability of traditional demercury products (, HgCl, HgO, HgS, and HgSe). Herein, we demonstrate a superstable HgSeCl compound, which offers a promising next-generation flue gas mercury removal strategy. Theoretical calculations revealed a superstable Hg bonding structure in HgSeCl, with the highest mercury dissociation energy (4.71 eV) among all known mercury compounds. Experiments demonstrate its unprecedentedly high thermal stability (>400 °C) and strong acid resistance (5% HSO). The HgSeCl compound could be produced via the reduction of SeO to nascent active Se by the flue gas component SO and the subsequent combination of Se with Hg and Cl ions or HgCl. During a laboratory-simulated experiment, this HgSeCl-based strategy achieves >96% removal efficiencies of both Hg and HgCl enabling nearly zero Hg re-emission. As expected, real mercury removal efficiency under Se-rich industrial flue gas conditions is much more efficient than Se-poor counterparts, confirming the feasibility of this HgSeCl-based strategy for practical applications. This study sheds light on the importance of stable demercury products in flue gas mercury treatment and also provides a highly efficient and safe flue gas demercury strategy.
为了降低全球汞背景浓度并保护生态系统,烟气脱汞是必不可少的,但传统脱汞产品(HgCl、HgO、HgS和HgSe)的不稳定性严重影响了其效果。在此,我们展示了一种超稳定的HgSeCl化合物,它为下一代烟气脱汞策略提供了希望。理论计算表明,HgSeCl中存在超稳定的汞键结构,在所有已知汞化合物中具有最高的汞离解能(4.71 eV)。实验证明了其前所未有的高热稳定性(>400°C)和强耐酸性(5% H₂SO₄)。HgSeCl化合物可通过烟气成分SO₂将SeO₂还原为新生活性Se,随后Se与Hg和Cl离子或HgCl结合而生成。在实验室模拟实验中,这种基于HgSeCl的策略对Hg和HgCl的去除效率均超过96%,几乎实现零汞再排放。正如预期的那样,在富硒工业烟气条件下的实际脱汞效率比贫硒情况要高得多,证实了这种基于HgSeCl的策略在实际应用中的可行性。这项研究揭示了稳定脱汞产品在烟气汞处理中的重要性,也提供了一种高效且安全的烟气脱汞策略。