Abatement of mercury emission from coal-fired power plants remains a serious task for public health and environmental societies. Selenium functionalized metal−organic framework MIL-101 (Se/MIL-101) was prepared for mercury removal from power plants. The Se/MIL-101 exhibited a remarkable mercury adsorption capacity of 148.19 mg•g −1 , which was about 154 to 705 times larger than that of commercial activated carbons exclusively applied for mercury removal from power plants. The initial mercury adsorption rate for Se/MIL-101 reached up to 44.8 μg•g −1 •min −1 , which was 89to 1659-fold higher than those of mercury sorbents reported in the literature. The Se/MIL-101 maintained an excellent mercury adsorption stability under simulated flue gas atmosphere containing SO 2 , NO, and H 2 O. Gaseous elemental mercury (Hg 0 ) converted on the Se/MIL-101 to stable and water-insoluble mercury selenide (HgSe), which guaranteed a minimum re-emission even sequestration of mercury. Moreover, the mercury-laden Se/MIL-101 could also immobilize mercury in gypsum and efficiently capture mercury ions from desulfurization effluent to an undetectable level (<0.0035 μg•L −1 ). With these advantages, Se/MIL-101 appears to be a promising material for efficient and permanent sequestration of mercury from power plants.
Mercury emission from industrial activities is a great threat to public health and ecosystems. Developing new strategies and materials to remove mercury still remains a serious task. Herein, selenide-decorated copper foam prepared by a heating-stirring method (Cu-hs) was used as a monolithic mercury adsorption material. The Cu-hs exhibited much better adsorption of elemental mercury (Hg 0 ) compared with the selenidedecorated cordierite honeycomb prepared by the same method (Cordierite-hs). Nearly 100% Hg 0 adsorption efficiency was obtained under a high gaseous hourly space velocity of 6.0 × 10 4 . Excellent Hg 0 adsorption capacity was obtained in a wide range of reaction temperatures from 40 to 120 °C, suggesting the good adaptability of Cu-hs in different operating conditions. The Cu-hs exhibited high selectivity for Hg 0 against H 2 O and SO 2 , which is advantageous for real applications in industrial flue gas. The Hg 0 adsorption capacity of Cu-hs reached 3743 g/m 3 , about 14 times higher than the 243 g/m 3 of Cordierite-hs. The excellent Hg 0 adsorption performance of Cu-hs was attributed to the high affinity of the selenium in Cu 2 Se for mercury, the homogeneous distribution of Cu 2 Se, and the superior fluid characteristics of the Cu foam substrate. The adsorption performance of the spent Cu-hs could be effectively recovered by HCl solution leaching and subsequent reselenization. The utilization of recyclable Cu-hs provides a cost-effective and environmentally friendly method for removing mercury from industrial flue gas.
A key challenge in elemental mercury (Hg 0 ) decontamination from flue gas lies in the design of a sorbent with abundant reactive adsorption sites that exhibit high affinity toward Hg 0 to simultaneously achieve rapid capture and large capacity. Herein, zeolitic imidazolate framework-8 (ZIF-8) supported copper selenide (CuSe) nanocomposites are synthesized by a newly designed two-step surfactant-assisted method. The as-prepared CuSe/ZIF-8 with CuSe to ZIF-8 mass ratio of 80% (0.8NC-ZIF) exhibits unparalleled performance toward Hg 0 adsorption with equilibrium capacity and average rate reaching 309.8 mg g −1 and 105.3 µg g −1 min −1 , respectively, surpassing all reported metal sulfides and traditional activated-carbon-based sorbents. The impressive performance of 0.8NC-ZIF for Hg 0 immobilization is primarily attributed to the adequate exposure of the Se-terminated sites with high affinity toward Hg 0 resulted from the layered structure of CuSe. The adsorbed mercury selenide exhibits even higher stability than the most stable natural mercury ore-that is, mercury sulfide-hence minimizing its environmental impact when the CuSe/ZIF-8 sorbent is dumped. This work provides a new mindset for future design of sorbents for efficient Hg 0 capture from industrial flue gas. The results also justify the candidature of CuSe/ZIF to be applicable for mercury pollution remediation in real-world conditions.
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