A new approach to mercury speciation in solids using a thermal desorption technique

Rumayor, Marta; López-Antón, M. Antonia; Dı́az-Somoano, Mercedes; Martı́nez-Tarazona, M. Rosa

doi:10.1016/j.fuel.2015.08.028

Cited by 68 publications

(40 citation statements)

References 25 publications

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“…It is generally considered that mercury can be presented in coal as sulfide and selenides, in forms associated with pyrite and marcasite (Ward et al 1999;Hower et al 2008;Kolker 2012), calcite and chlorite (Zhang et al 2002), selenio-galena (Dai et al 2006b(Dai et al , 2015, clausthalite (Hower and Robertson 2003), kleinite and cinnabar (Brownfield et al 2005), sphalerite (HgFeS 2 ) and getchellite (Dai et al 2006a). It can also organically bounded to organic matter (HgOM) (Rumayor et al 2015), or even as HgS and metallic mercury (Hg 0 ) (Finkelman 1994;Yudovich and Ketris 2005). It is clear that mercury is mostly associated with pyrite, especially late-stage (epigenetic) pyrite deposited from hydrothermal basinal fluids (Hower et al 2007;Diehl et al 2012;Kolker 2012).…”

Section: Introductionmentioning

confidence: 99%

The distribution and occurrence of mercury in Chinese coals

Bai

Wang

et al. 2017

Int J Coal Sci Technol

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Mercury is one of the most concerned hazardous elements in coals. 1018 coal samples of different coal-forming periods, coal-accumulating areas and coal ranks all over the country were collected to study the distributions of mercury in Chinese coals. The modes of occurrence of mercury were studied with float-sink experiments of 10 coals from different basins in China and correlation analyses were conducted between concentrations of mercury and maceral and sulfur contents, as well as the ash yield. The theoretic concentrations and affinities of mercury in vitrinite, inertinite, clay and pyrite were then calculated following the methods proposed by Solari. The weighted average concentration of mercury in Chinese coals is 0.154 lg/g, which is similar to that in the word coals in general. The mercury concentrations vary largely in the coals of different coal-forming period and coal-accumulating areas as geological settings play key roles in determining the geochemistry of mercury. The concentrations of mercury in coals from south and southwest China and those from North China of C 3 -P 1 are relatively higher while those from North China of J 1-2 and Northeast of J 3 -K 1 relatively lower. The general distribution trends of mercury are very similar to that of ash yield, sulfur contents in coals. Pyrite is the dominant carrier of mercury in most coals, especially in some high-sulfur coals with abundant epigenetic pyrite formed during diagenesis and metamorphism. Mercury has higher affinity to vitrinite than to inertinite in most coals, which accords with the geological origin of macerals and geochemistry of mercury.

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Section: Introductionmentioning

confidence: 99%

The distribution and occurrence of mercury in Chinese coals

Bai

Wang

et al. 2017

Int J Coal Sci Technol

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“…The second reaction corresponding to the temperature range from 436.15 K to 694.15 K, is the thermal desorption of Hg and HgCl 2 , and the mass loss is 13%. According to the former researches [30][31][32][33], the desorption temperature range of the mercury and mercury compounds is from 323.15 K to 613.15 K, while this temperature range is lower than that in this work, and the reaction temperature difference might be caused by different sample compositions and structures. In this work, the matrix of the spent catalysts is activated carbon.…”

Section: Pressure Difference Approximate Calculationmentioning

confidence: 53%

Desorption kinetic study of mercury species in spent mercury chloride catalyst from polyvinyl chloride production process

Liu

et al. 2019

Env Prog and Sustain Energy

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In order to improve the hazard‐free treatment and comprehensive utilization of the spent chloride mercury catalysts, reaction kinetics, and diffusion process of the thermal desorption of mercury were investigated. For reaction kinetics, activation energy of the reactions in the temperature range 436.15–694.15 K was calculated by five different model‐free methods, among which, FWO (105.47 kJ·mol−1) model‐free method with the best fitting precision was applied as the parameter to deduce the reaction models and describe the kinetic mechanism. It was confirmed that three diffusion models (D1, D2, D3) dominated at the beginning/middle of the reactions and one reaction order model (F2) dominated at the later part. According to the deduced mechanism, diffusion enhancing and reaction temperature enhancing strategies were introduced. For diffusion process of mercury volatiles, the laminar state of the protective gas was confirmed when the nitrogen flow rate is 100 L/h; based on the boundary simplifications, the thickness and the pressure difference of the boundary layer were calculated. According to the results of pressure difference, mercury diffusion process has two stages: Higher pressure diffusion stage and Residual mercury removal stage. Reaction kinetics and diffusion calculation give a better understanding of the mercury removal process and the parameters obtained in this work are useful to design the reactor. © 2019 American Institute of Chemical Engineers Environ Prog, 38:e13146, 2019

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“…Lopez‐Anton and Rumayor et al obtained the pyrolysis spectrum of pure mercury compounds using TPD . The decomposition signal of black HgS (metacinnabar) is mainly distributed at 170°C to 290°C, and a characteristic peak appears at 245°C ± 15°C; red HgS (cinnabar) has a decomposition range of 240°C to 350°C, and the mercury signal peak is at 310°C ± 15°C with a shoulder at approximately 340°C; HgO presents a peak at approximately 505°C, and the peak range is 430°C to 560°C; the mercury release signal of HgSO 4 occurs primarily in the range of 500°C to 600°C with a clearly defined peak at 540°C ± 15°C; the peak of organic mercury (Hg‐OM) is approximately 217°C, and the thermal decomposition range is about 150°C to 290°C.…”

Section: Resultsmentioning

confidence: 99%

“…Lopez-Anton and Rumayor et al obtained the pyrolysis spectrum of pure mercury compounds using TPD. 25,26 The decomposition signal of black HgS (metacinnabar) is mainly distributed at 170°C to 290°C, and a characteristic peak appears at 245°C ± 15°C; red HgS (cinnabar) has a decomposition range of 240°C to 350°C, and the mercury signal peak is at 310°C ± 15°C with a shoulder at approximately 340°C;…”

Section: Pyrite Samplesmentioning

confidence: 99%

Mercury forms and their transformation in pyrite under weathering

Cao

Qian

Liang

et al. 2020

Surface & Interface Analysis

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Pyrite is considered to be the major carrier of mercury in coal. Here, the chemical characteristics of two natural pyrite samples of different weathering degrees were characterized by time‐of‐flight secondary ion mass spectrometry (TOF‐SIMS). Thermal stability of Hg was also analyzed via temperature programmed desorption experiment (TPD). Characteristic ions such as S−, Fe+, FeS−, and FeS2− were detected on the surface of fresh pyrite. The release temperature of Hg ranged between 180°C and 300°C, and the characteristic peak of black HgS was recorded. In addition, abundant Fe2O3−, FeSO−, SO4−, and HSO4− were detected on the surface of weathered pyrite, and the release temperature of Hg therein was mainly distributed at 260°C to 380°C and 520°C to 600°C, corresponding to the characteristic peaks of red HgS and HgSO4, respectively. The results show that pyrite is acidified during weathering and that Hg forms in pyrite are transformed from the original state (HgS) to HgSO4.

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A new approach to mercury speciation in solids using a thermal desorption technique

Cited by 68 publications

References 25 publications

The distribution and occurrence of mercury in Chinese coals

The distribution and occurrence of mercury in Chinese coals

Desorption kinetic study of mercury species in spent mercury chloride catalyst from polyvinyl chloride production process

Mercury forms and their transformation in pyrite under weathering

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