Adsorption mechanism of elemental mercury (Hg0) on the surface of MnCl2 (1 1 0) studied by Density Functional Theory

Ji, Wenchao; Shen, Zhemin; Fan, Maohong; Su, Pingru; Tang, Qingli; Zou, Cong-yang

doi:10.1016/j.cej.2015.06.033

Cited by 25 publications

(12 citation statements)

References 37 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…It shows that the Hg 0 adsorption system has positive slope at all temperatures and that the equilibrium constant decreases with increasing temperature. The same trend was found in the previous investigations of Hg 0 adsorption on MnCl 2 (110), 56 Co 3 O 4 (110), 14 MnO 2 (001), 17 and CaO(001) 24 surfaces. The distinct slope during the Hg 0 adsorption process suggests that temperature has a significant effect on the equilibrium constant for Hg 0 adsorption.…”

Section: Energy and Fuelssupporting

confidence: 90%

Unveiling Adsorption Mechanisms of Elemental Mercury on Defective Boron Nitride Monolayer: A Computational Study

et al. 2018

Self Cite

View full text Add to dashboard Cite

The control of mercury in flue gas is challenging, especially that of elemental mercury (Hg0). Recently, many researchers have focused on various mercury removal technologies. Here, by performing density functional theory (DFT) calculations, we systematically studied the adsorption of Hg0 on several experimentally available hexagonal boron nitride (h-BN) nanosheets with no defects, nitrogen vacancies (VN), boron vacancies (VB), and both nitrogen and boron vacancies (VN+B) as well as their structures and electronic properties. Our calculation results show that the presence of VN, VB, and VN+B enhances the adsorption energies of Hg0 by 9, 45, and 214 kJ/mol, respectively. Moreover, a more negative potential at the VB and VN+B sites makes the h-BN-VB and h-BN-VN+B surfaces more reactive than those of h-BN and h-BN-VN. The partial density of states analysis reveals that the Hg atom interacts firmly with surface B or/and N atoms through orbital hybridization. The trend of the equilibrium constant implies that adsorption of Hg0 on the h-BN-VN+B surface is beneficial at low temperature. Our computational studies reveal that defective h-BN nanosheets with VB and VN+B have great potential to serve as novel sorbents for the efficient removal of mercury in flue gas.

show abstract

Section: Energy and Fuelssupporting

confidence: 90%

Unveiling Adsorption Mechanisms of Elemental Mercury on Defective Boron Nitride Monolayer: A Computational Study

et al. 2018

Self Cite

View full text Add to dashboard Cite

show abstract

“…To investigate exothermicity of adsorption processes and favorability of the spontaneous reaction as a function of temperature, the equilibrium constants ( eq K ) were calculated based on the thermodynamic data from frequency calculation [25,29]. The method has been applied to study the equilibrium constant of mercury adsorption on CaO [30] and CoCl 2 [31]surfaces. We used general relationships for statistical thermodynamic partition functions (translational, rotational, and vibrational partition functions) [32].…”

Section: Methodsmentioning

confidence: 99%

A DFT study of Hg0 adsorption on Co3O4 (1 1 0) surface

Shen

Tang

et al. 2016

Chemical Engineering Journal

Self Cite

View full text Add to dashboard Cite

Spin polarized density functional theory calculation combined with periodic slabs were employed to reveal the elemental mercury (Hg 0) adsorption mechanism on Co 3 O 4 (1 1 0) surface. The adsorption energies and possible adsorption sites were investigated. To understand the adsorption interaction more directly, the electronic structural changes of before and after adsorption were compared. The hybridization of orbitals was studied by the partial density of states (PDOS) analysis. In addition, the temperature effects toward equilibrium constants of Hg 0-Co 3 O 4 system were taken into consideration. The results manifested that the interaction between Hg 0 and Co 3 O 4 (1 1 0) surface is chemisorption with-74.037kJ/mol. Co 3+ sites, the highest oxidation state of Co atoms, are crucial in this process which can accept the electrons after Hg oxidation. The redundant electrons transfer to O and other Co atoms nearby. PDOS analysis indicates the hybridization of s orbitals (Hg 0) and p, d orbitals (Co atom). And d orbitals of Hg interacts with s, p orbitals of Co atom strongly. The trends of equilibrium constants suggest that Hg 0 adsorption on Co 3 O 4 (1 1 0) surface is favorable at low temperature.

show abstract

“…Generally, it can be considered chemisorption when the absolute value of negative adsorption energy exceeds 40 kJ/mol. 38,45 The formation energy of the surface S vacancy was calculated according to the following formula…”

Section: Computational Detailsmentioning

confidence: 99%

First-Principles Study of Hg⁰ Immobilization on a Defective Pyrite Surface

Deng

Yang

et al. 2023

Energy Fuels

View full text Add to dashboard Cite

The formation of defects over a crystal surface could significantly improve the elemental mercury (Hg 0 ) removal performance of pyrite (FeS 2 ). Herein, the role of surface defects in Hg 0 immobilization over FeS 2 (100) was investigated by adopting quantum chemistry. The contribution of surface defects to mercury immobilization over pyrite was mainly manifested in facilitating Hg 0 adsorption. Compared with a perfect pyrite surface, a defective pyrite surface exhibited a higher affinity to Hg 0 , whose adsorption energy was up to −53.03 kJ/mol. In addition, surface defects could induce the dissociation of HCl, a common component in coal combustion flue gas, which provided active chlorine (Cl*) for subsequent Hg 0 oxidation. The Langmuir−Hinshelwood mechanism is responsible for Hg 0 oxidation over the defective FeS 2 (100) surface. First, Hg 0 and HCl were simultaneously adsorbed over the defective surface, and the presence of defects could promote Hg 0 adsorption and HCl dissociation. Subsequently, adsorbed Hg 0 would combine with the adjacent active Cl* site, whose energy barrier was 92.60 kJ/mol. Eventually, HgCl could spontaneously react with another Cl* site to form a HgCl 2 molecule. Thus, the formation of a HgCl intermediate was the rate-determining step for Hg 0 oxidation over a defective pyrite surface. This work reveals the role of defects in Hg 0 immobilization over a pyrite surface, which provides a scientific basis for the design and modification of natural mineral sulfide sorbents.

show abstract

Adsorption mechanism of elemental mercury (Hg0) on the surface of MnCl2 (1 1 0) studied by Density Functional Theory

Cited by 25 publications

References 37 publications

Unveiling Adsorption Mechanisms of Elemental Mercury on Defective Boron Nitride Monolayer: A Computational Study

Unveiling Adsorption Mechanisms of Elemental Mercury on Defective Boron Nitride Monolayer: A Computational Study

A DFT study of Hg0 adsorption on Co3O4 (1 1 0) surface

First-Principles Study of Hg⁰ Immobilization on a Defective Pyrite Surface

Contact Info

Product

Resources

About

Adsorption mechanism of elemental mercury (Hg0) on the surface of MnCl2 (1 1 0) studied by Density Functional Theory

Cited by 25 publications

References 37 publications

Unveiling Adsorption Mechanisms of Elemental Mercury on Defective Boron Nitride Monolayer: A Computational Study

Unveiling Adsorption Mechanisms of Elemental Mercury on Defective Boron Nitride Monolayer: A Computational Study

A DFT study of Hg0 adsorption on Co3O4 (1 1 0) surface

First-Principles Study of Hg0 Immobilization on a Defective Pyrite Surface

Contact Info

Product

Resources

About

First-Principles Study of Hg⁰ Immobilization on a Defective Pyrite Surface