Study of the Molecular Structure and Elemental Mercury Adsorption Mechanism of Biomass Char

Based on a comprehensive study of the pyrolysis characteristics, pore structure, surface chemical functional groups, organic carbon framework structure, microcrystalline morphology and lattice characteristics of walnut shell biochar for mercury adsorption, the structural characteristics of biochar were analysed, and a model of the monomeric molecular structure of biochar was constructed. In addition, the density functional theory of quantum mechanics was introduced into the gas-solid adsorption reaction of elemental mercury with biochar. By quantitatively studying the adsorption energy, adsorption height, and Mulliken population number of the adsorption system, the adsorption mechanism of Hg0 by biochar was revealed to provide a theoretical basis for future mercury removal methods. The results showed that walnut shell biochar consisted mainly of C, H, O and N. Aromatic carbon was the main component of the biochar molecular structure, while aliphatic carbon was linked to aromatic structural units. The molecular structure model was mainly composed of aromatic structures, including one methyl, 4 hydroxyl and 8 carbonyl groups. The molecular formula was C55H37NO14, and the molecular weight was 935. The adsorption of Hg0 by biochar was mainly via chemical adsorption, and the adsorbed Hg0 could stably exist on the biochar surface. The Hg0 adsorption process on the biochar surface mainly depended on the charge of the adsorption site. An adsorption site with a negative charge and with a high number of charges facilitated the adsorption of elemental mercury on the biochar surface. Moreover, the charge of the ortho atom adjacent to the adsorption site had a substantial influence on the adsorption activity of the adsorption site.

[1]  Yue Yu,et al.  Low-carbon development path research on China’s power industry based on synergistic emission reduction between CO2 and air pollutants , 2020 .

[2]  Zhibin He,et al.  Separation of hemicellulose and cellulose from wood pulp using a γ-valerolactone (GVL)/water mixture , 2020 .

[3]  A. Messineo,et al.  On the suitability of thermogravimetric balances for the study of biomass pyrolysis , 2020 .

[4]  Yiming Sun,et al.  Gas-pressurized torrefaction of biomass wastes: The effect of varied pressure on pyrolysis kinetics and mechanism of torrefied biomass , 2020 .

[5]  Min Liu,et al.  Preparation and Characterization of Porous Microcrystalline Cellulose from Corncob , 2020, Industrial Crops and Products.

[6]  Xing Liu,et al.  Mechanism study of nitric oxide reduction by light gases from typical Chinese coals , 2020 .

[7]  M. Srivastava,et al.  Suitability of graphene monolayer as sensor for carcinogenic heavy metals in water: A DFT investigation , 2020 .

[8]  K. Mohanty,et al.  Kinetic analysis and pyrolysis behaviour of waste biomass towards its bioenergy potential. , 2020, Bioresource technology.

[9]  J. Ran,et al.  Insight into the effect of facet-dependent surface and oxygen vacancies of CeO2 for Hg removal: From theoretical and experimental studies. , 2020, Journal of hazardous materials.

[10]  Dawei Wu,et al.  Plasma-Modified N/O-Doped Porous Carbon for CO2 Capture: An Experimental and Theoretical Study , 2020 .

[11]  Jiang Wu,et al.  Experimental Study on the Influence of Surface Characteristics of Activated Carbon on Mercury Removal in Flue Gas , 2020 .

[12]  K. Zhao,et al.  Chemical Looping Gasification of Torrefied Biomass Using NiFe2O4 as an Oxygen Carrier for Syngas Production and Tar Removal , 2020 .

[13]  Yijun Zhao,et al.  Investigation of Heterogeneous NO Reduction by Biomass Char and Coal Char Blends in a Microfluidized Bed Reaction Analyzer , 2020 .

[14]  N. Yan,et al.  Atomically Dispersed Manganese on a Carbon-Based Material for the Capture of Gaseous Mercury: Mechanisms and Environmental Applications. , 2020, Environmental science & technology.

[15]  Zelong Zhang,et al.  Energetics of Interfacial Interactions of Hydrocarbon Fluids with Kerogen and Calcite Using Molecular Modeling , 2019, Energy & Fuels.

[16]  W. Pan,et al.  Preadsorbed SO3 Inhibits Oxygen Atom Activity for Mercury Adsorption on Cu/Mn Doped CeO2(110) Surface , 2020 .

[17]  Q. Yao,et al.  Molecular Simulation of the Adsorption Behaviors of CO2/CH4 in Curvature, Planar, and Mixture Models , 2020 .

[18]  Minghou Xu,et al.  Seawater-assisted synthesis of MnCe/zeolite-13X for removing elemental mercury from coal-fired flue gas , 2020 .

[19]  T. Dziok,et al.  Valorization Method for Hard Coal as Fuel for Nonindustrial Combustion Installations with Special Regard to Reduction of Mercury Content , 2020 .

[20]  Y. Duan,et al.  Influence of Different Sulfur Forms on Gas-Phase Mercury Removal by SO2-Impregnated Porous Carbons , 2020 .

[21]  Hailong Li,et al.  In Situ Decoration of Selenide on Copper Foam for the Efficient Immobilization of Gaseous Elemental Mercury. , 2020, Environmental science & technology.

[22]  H. Wong,et al.  Propane pyrolysis facilitated by phenyl radicals: A combined experimental and kinetic modeling study , 2019 .

[23]  B. Jiang,et al.  The tectonic stress–driving alteration and evolution of chemical structure for low- to medium-rank coals—by molecular simulation method , 2019, Arabian Journal of Geosciences.

[24]  Xiao-lei Qiao,et al.  Study of the Effect of Adsorption Temperature on Elemental Mercury Removal Performance of Iron-Based Modified Biochar , 2019, Energy & Fuels.

[25]  Xiaodong Li,et al.  Adsorption Characteristics of Polycyclic Aromatic Hydrocarbons by Biomass-Activated Carbon in Flue Gas , 2019, Energy & Fuels.

[26]  L. Chai,et al.  Catalytic Oxidation of Elemental Mercury in Coal-Combustion Flue Gas over the CuAlO2 Catalyst , 2019, Energy & Fuels.

[27]  Junying Zhang,et al.  Role of SO3 in Elemental Mercury Removal by Magnetic Biochar , 2019, Energy & Fuels.

[28]  Longlong Ma,et al.  Molecular Structure and Formation Mechanism of Hydrochar from Hydrothermal Carbonization of Carbohydrates , 2019, Energy & Fuels.

[29]  Sai Zhang,et al.  Enhanced photodegradation of toxic organic pollutants using dual-oxygen-doped porous g-C3N4: Mechanism exploration from both experimental and DFT studies , 2019, Applied Catalysis B: Environmental.

[30]  Hailong Li,et al.  Role of flue gas components in Hg0 oxidation over La0.8Ce0.2MnO3 perovskite catalyst in coal combustion flue gas , 2019, Chemical Engineering Journal.

[31]  Xuehai Fu,et al.  Research on the organic geochemical and mineral composition properties and its influence on pore structure of coal-measure shales in Yushe-Wuxiang Block, South Central Qinshui Basin, China , 2019, Journal of Petroleum Science and Engineering.

[32]  Hailong Li,et al.  Elemental Mercury Removal from Flue Gas over TiO2 Catalyst in an Internal-Illuminated Honeycomb Photoreactor , 2018, Industrial & Engineering Chemistry Research.

[33]  Yan Jin,et al.  Study on the Elemental Mercury Adsorption Characteristics and Mechanism of Iron-Based Modified Biochar Materials , 2018, Energy & Fuels.

[34]  Hailong Li,et al.  Simultaneous NO Reduction and Hg0 Oxidation over La0.8Ce0.2MnO3 Perovskite Catalysts at Low Temperature , 2018, Industrial & Engineering Chemistry Research.

[35]  Xiao-lei Qiao,et al.  Study on quenching hydration reaction kinetics and desulfurization characteristics of magnesium slag , 2018, Journal of Cleaner Production.

[36]  Xiao-lei Qiao,et al.  Study on the Effects of the Pyrolysis Atmosphere on the Elemental Mercury Adsorption Characteristics and Mechanism of Biomass Char , 2018, Energy & Fuels.

[37]  RajenderKumar Gupta,et al.  Mercury co-beneficial capture in air pollution control devices of coal-fired power plants , 2017 .

[38]  Minghou Xu,et al.  Elemental mercury oxidation over manganese-based perovskite-type catalyst at low temperature , 2016 .

[39]  Kefeng Yan,et al.  Adsorption of collectors on model surface of Wiser bituminous coal: A molecular dynamics simulation study , 2015 .

[40]  Minghou Xu,et al.  Effects of existing energy saving and air pollution control devices on mercury removal in coal-fired power plants , 2015 .

[41]  J. Wilcox,et al.  Uncertainty Analysis of the Mercury Oxidation over a Standard SCR Catalyst through a Lab-Scale Kinetic Study , 2015 .

[42]  P. Agrawal,et al.  Effect of Temperature, Pressure, and Residence Time on Pyrolysis of Pine in an Entrained Flow Reactor , 2014 .

[43]  J. Wilcox,et al.  Heterogeneous mercury oxidation on au(111) from first principles. , 2013, Environmental science & technology.

[44]  B. Trofimov,et al.  Structural studies of meso-CF3-3(5)-aryl(hetaryl)- and 3,5-diaryl(dihetaryl)-BODIPY dyes by 1H, 13C and 19F NMR spectroscopy and DFT calculations , 2013 .

[45]  M. Kaupp,et al.  Evaluation of a combination of local hybrid functionals with DFT-D3 corrections for the calculation of thermochemical and kinetic data. , 2011, The journal of physical chemistry. A.

[46]  C. Zheng,et al.  Theoretical Studies of Properties and Reactions Involving Mercury Species Present in Combustion Flue Gases , 2010 .

[47]  Jun-ichiro Hayashi,et al.  Characterization of the structural features of char from the pyrolysis of cane trash using Fourier transform-Raman spectroscopy , 2007 .

[48]  J. Wilcox,et al.  Evaluation of basis sets and theoretical methods for estimating rate constants of mercury oxidation reactions involving chlorine , 2004 .

[49]  J. Wilcox,et al.  Theoretically predicted rate constants for mercury oxidation by hydrogen chloride in coal combustion flue gases. , 2003, Environmental science & technology.

[50]  G. Pacchioni,et al.  Chemisorption and Reactivity of Methanol on MgO Thin Films , 2002 .

[51]  G. Pacchioni,et al.  Conversion of NO to N 2 O on MgO Thin Films , 2002 .

[52]  G. Pacchioni,et al.  NO monomers on MgO powders and thin films , 2002 .