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Elemental mercury (Hg^(0)) removal from coal syngas using magnetic tea-biochar: Experimental and theoretical insights

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Journal of Environmental Sciences 2022年第12期34卷 150-161页

作者： Adnan Raza Altaf Yusuf GAdewuyi Haipeng Teng Gang Liu Fazeel Abid School of Chemical Engineering Northwest University Xi’an 710069China Chemical Biological and Bio Engineering DepartmentNorth Carolina Agricultural and Technical State UniversityGreensboroNC 27411USA State Key Laboratory of Clean Coal-based Energy China Huaneng Group Clean Energy Research Institute Co.Ltd.Changping DistrictBeijing 102209China Department of Information System Dr Hassan Murad School of ManagementUniversity of Management and TechnologyLahore 54770Pakistan

mercury is ranked 3^(rd)as a global pollutant because of its long persistence in the environment. Approximately 65% of its anthropogenic emission (Hg^(0)) to the atmosphere is from coal-thermal power plants. Thus, the Hg^(0)emission control from coal-thermal power plants is inevitable. Therefore, multiple sorbent materials were synthesized using a one-step pyrolysis method to capture the Hg^(0)from simulated coal syngas. Results showed, the Hg^(0)removal performance of the sorbents increased by the citric acid/ultrasonic application.T5CUF_(0.3)demonstrated the highest Hg^(0)capturing performance with an adsorption capacity of 106.81 μg/g within 60 min at 200 °C under complex simulated syngas mixture (20% CO,20% H_(2), 10 ppm V HCl, 6% H_(2)O, and 400 ppm V H_(2)S). The Hg^(0)removal mechanism was proposed, revealing that the chemisorption governs the Hg^(0)removal process. Besides, the active Hg^(0)removal performance is attributed to the high dispersion of valence Fe_(3)O_(4)and lattice oxygen (α) contents over the T5CUF_(0.3)surface. In addition, the temperature programmed desorption (TPD) and XPS analysis confirmed that H_(2)S/HCl gases generate active sites over the sorbent surface, facilitating high Hg^(0)adsorption from syngas. This work represented a facile and practical pathway for utilizing cheap and eco-friendly tea waste to control the Hg^(0)emission.

关键词： mercury removal Waste management Citric acid Ultrasound Coal gasification TPD analysis

mercury removal performance over a Ce-doped V-W/TiO_(2) catalyst in an internally illuminated honeycomb photoreactor

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Science China(Technological Sciences) 2021年第11期64卷 2441-2452页

作者： GAO Tian ZHANG YiLi QIU YaQin XIONG Zhuo YANG JianPing ZHAO YongChun ZHANG JunYing State Key Laboratory of Coal Combustion Huazhong University of Science and TechnologyWuhan 430074China School of Optical and Electronic Information Huazhong University of Science and TechnologyWuhan 430074China School of Energy Science and Engineering Central South UniversityChangsha 410083China

A new type of internally illuminated honeycomb photoreactor was designed. The honeycomb catalyst prepared by using Cedoped TiO2 with 1%–2% vanadium and tungsten was employed for mercury removal from simulated industrial flue gas. The adsorption kinetics in the reaction process were studied. The results showed that the internally illuminated honeycomb photoreactor had good mercury removal performance. When the temperature was 25℃ and the ultraviolet(UV) light intensity reached 80 μW/cm2, the mercury removal efficiency reached 92.5%. The mercury removal efficiency increased significantly with the doping ratio of Ce. XPS analysis showed that the oxidation state of Ce changed from 4 to 3 in the mercury removal reaction and produced lattice oxygen, which acts as an oxidant. O2 can promote mercury removal by honeycomb catalysts;SO2 and HCl also had positive effects, while NO had an inhibitory effect on mercury removal. Kinetic research in the reaction process showed that the quasi-first-order dynamic model had good fitting results, and the correlation coefficients of the fitting results for multiple sets of experimental data were more than 0.999.

关键词： mercury removal Ce-doped V-W/TiO2 catalyst internally illuminated honeycomb photoreactor flue gas

mercury removal from aqueous solution using petal-like MoS_(2) nanosheets

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Frontiers of Environmental Science & Engineering 2021年第1期15卷 213-222页

作者： Ragini Pirarath Palani Shivashanmugam Asad Syed Abdallah MElgorban Sambandam Anandan Muthupandian Ashokkumar Department of Chemistry National Institute of TechnologyTiruchirappalli-620015India Department of Chemical Engineering National Institute of TechnologyTiruchirappalli-620015India Department of Botany and Microbiology College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia School of Chemistry University of MelbourneMelbourneVic-3010Australia

Recently,different nanomaterial-based adsorbents have received greater attention for the removal of environmental pollutants,specifically heavy metals from aqueous media.In this work,we synthesized few-layered MoS2 nanosheets via a surfactant-assisted hydrothermal method and utilized them as an efficient adsorbent for the removal of mercury from aqueous media.The synthesized MoS2 nanosheets showed petal-like morphology as confirmed by scanning electron microscope and high-resolution transmission electron microscopic analysis.The average thickness of the nanosheets is found to be about 57 nm.Possessing high stability and negative zeta potential makes this material suitable for efficient adsorption of mercury from aqueous media.The adsorption efficiency of the adsorbent was investigated as a function of pH,contact time and adsorbent dose.The kinetics of adsorption and reusability potential of the adsorbent were also performed.A pseudo-second-order kinetics for mercury adsorption was observed.As prepared MoS_(2) nanosheets showed 93%mercury removal efficiency,whereas regenerated adsorbent showed 91%and 79%removal efficiency in the respective 2^(nd) and 3^(rd) cycles.The adsorption capacity of the adsorbent was found to be 289 mg/g at room temperature.

关键词： Anionic surfactant 2D material MoS_(2)nanosheets mercury removal Adsorption capacity

Evaluation of mercury speciation and removal through air pollution control devices of a 190 MW boiler

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Journal of Environmental Sciences 2010年第2期22卷 277-282页

作者： Chengli Wu Yan Cao Zhongbing Dong Chinmin Cheng Hanxu Li Weiping Pan School of Chemical Engineering Anhui University of Science and Technology Huainan 232001 China Institute for Combustion Science and Environmental Technology Western Kentucky University Bowling Green Kentucky 42101 USA

Air pollution control devices （APCDs） are installed at coal-fired power plants for air pollutant regulation. Selective catalytic reduction （SCR） and wet flue gas desulftLrization （FGD） systems have the co-benefits of air pollutant and mercury removal. Configuration and operational conditions of APCDs and mercury speciation affect mercury removal efficiently at coal-fired utilities. The Ontario Hydro Method （OHM） recommended by the U.S. Environmental Protection Agency （EPA） was used to determine mercury speciation simultaneously at five sampling locations through SCR-ESP-FGD at a 190 MW unit. Chlorine in coal had been suggested as a factor affecting the mercury speciation in flue gas; and low-chlorine coal was purported to produce less oxidized mercury （Hg^2＋） and more elemental mercury （Hg^0） at the SCR inlet compared to higher chlorine coal. SCR could oxidize elemental mercury into oxidized mercury when SCR was in service, and oxidation efficiency reached 71.0%. Therefore, oxidized mercury removal efficiency was enhanced through a wet FGD system. In the non-ozone season, about 89.5%-96.8% of oxidized mercury was controlled, but only 54.9%-68.8% of the total mercury was captured through wet FGD. Oxidized mercury removal efficiency was 95.9%-98.0%, and there was a big difference in the total mercury removal efficiencies from 78.0% to 90.2% in the ozone season. mercury mass balance was evaluated to validate reliability of OHM testing data, and the ratio of mercury input in the coal to mercury output at the stack was from 0.84 to 1.08.

关键词： mercury speciation mercury removal air pollution control device field testing

Elemental mercury removal from coal gas by CeMnTi sorbents and their regeneration performance

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2021年第3期22卷 222-234页

作者： Hui CAO Jin-song ZHOUn Qi-xin ZHOU Xin-yu XU Cong XIE State Key Laboratory of Clean Energy Utilization Zhejiang UniversityHangzhou 310027China

Ce and Mn modified TiO_(2) sorbents(CeMnTi) were prepared by a co-precipitation method,and their ability to remove elemental mercury from coal gas in a fixed bed reactor was studied.Based on results of Brunauer-Emmett-Teller(BET),X-ray diffraction(XRD),scanning electron microscope(SEM),and X-ray photoelectron spectroscopy(XPS) studies,the modification mechanisms of the CeMnTi sorbents are discussed.Mn doping improved the specific surface area and dispersion of cerium oxides on the sorbent surface,while Ce doping increased the proportion of Mn^(4+)in manganese oxides by a synergetic effect between manganese oxides and cerium oxides.The effects of the active component,temperature,and coal gas components on the mercury removal performance of the sorbents were investigated.The results showed that the CeMnTi sorbents exhibited high mercury removal efficiency.Ce_(0.2)Mn_(0.1)Ti adsorbed 91.55% elemental mercury from coal gas at 160℃.H2 S and O2 significantly improved the ability of sorbents to remove mercury.Part of the H2_(S) formed stable sulfates or sulfites through a series of oxidation reaction chains on the sorbent surface.HCl also improved the mercury removal performance,but reduced the promotion effect of H2_(S) for mercury removal when coexisting with H2_(S).CO and H2 had a minor inhibitory effect on mercury adsorption.The recycling performance of the sorbents was investigated by thermal regeneration.The thermal decomposition of the used sorbents indicated that mercury compounds were present mainly in the form of HgO and HgS,and higher temperature was beneficial for regeneration.The formation of sulfates and sulfites in the presence of H2_(S) led to a decrease in mercury removal efficiency.

关键词： CeMnTi Synergistic effect Gas components mercury removal Thermal regeneration

mercury removal and recovery by immobilized Bacillus megaterium MB1

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Frontiers of Chemical Science and Engineering 2012年第2期6卷 192-197页

作者： Meifang CHIEN Ryo NAKAHATA Tetsuya ONO Keisuke MIYAUCHI Ginro ENDO Faculty of Engineering Tohoku-Gakuin University Miyagi 985-8537 Japan

From several mercury removing microorgan- isms, we selected Bacillus megaterium MB 1, which is non- pathogenic, broad-spectrum mercury resistant, mercuric ion reducing, heat tolerant, and spore-forming, as a useful bacterium for bioremediation of mercury pollution. In this study, mercury removal performance of the immobilized B. megaterium MB1 was investigated to develop safe, efficient and stable catalytic bio-agent for mercury bioremediation. The results showed that the alginate gel immobilized B. megaterium MB 1 cells efficiently removed 80% of mercury from the solution containing 10mg/L mercuric chloride within 24 h. These cells still had high activity of mercury removal even after mercuric ion loading was repeated for nine times. The analysis of mercury contents of the alginate beads with and without immobilized B. megaterium MB1 suggested that a large portion of reduced metallic mercury was trapped in the gel beads. It was concluded that the alginate gel immobilized B. megaterium MB 1 cells have potential to remove and recover mercury from mercury-containing water.

关键词： mercury removal immobilized bacteria alginate gel bioremediation

removal OF mercury FROM WATER USING POLYPYRROLE AND ITS COMPOSITES

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Chinese Journal of Polymer Science 2007年第4期25卷 393-397页

作者： Hossein Eisazadeh Faculty of Chemical Engineering University of MazandaranP.O.Box 484BabolIran

One of the suitable methods for removing heavy metals from water is by using surface adsorption process. In this paper, the preparation of polypyrrole and its composites as adsorbents are discussed and the capability of separating mercury from water is investigated. The results indicated that the polypyrrole and its composites are able to remove mercury from aqueous media. Furthermore the adsorption percentage is related to the surface morphology, type of additives and its concentration.

关键词： Polypyrrole and its composites mercury removal Additives Surface morphology.

removal of mercury(Hg(Ⅱ)) from Seaweed Extracts by Electrodialysis and Process Optimization Using Response Surface Methodology

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Journal of Ocean University of China 2020年第1期19卷 135-142页

作者： SUN Jiuyi SU Xin LIU Zhen LIU Junlan MA Zhun SUN Yongchao GAO Xueli GAO Jun College of Chemical and Environmental Engineering Shandong University of Science and TechnologyQingdao 266590China Key Laboratory of Marine Chemistry Theory and Technology Ministry of EducationCollege of Chemistry and Chemical EngineeringOcean University of ChinaQingdao 266100China

In this work,response surface methodology(RSM)was employed to model and optimize electrodialysis process for mercury(Hg(II))removal from seaweed extracts.Box-Behnken design(BBD)was utilized to evaluate the effects and the interaction of influential variables such as operating voltage,influent flow rate,initial concentration of Hg(II)on the removal rate of Hg(II).The developed regression model for removal rate response was validated by analysis of variance,and presented a good agreement of the experimental data with the quadratic equation with high value coefficient of determination value(R2=0.9913,RAdj 2=0.9678).The optimum operating parameters were determined as 7.17V operating voltage,72.54L h−1 influent flow rate and 5.04mgL−1 initial concentration of mercury.Hg(II)removal rate of 76.45%was acquired under the optimum conditions,which showed good agreement with model-predicted(75.81%)result.The results revealed that electrodialysis can be considered as a promising strategy for removal of Hg(II)from seaweed extracts.

关键词： electrodialysis seaweed extracts mercury removal response surface methodology Box-Behnken design

Graphene oxide based carbon composite as adsorbent for Hg removal:Preparation, characterization, kinetics and isotherm studies

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Chinese Journal of Chemical Engineering 2017年第9期25卷 1170-1175页

作者： Tayebeh Esfandiyari Navid Nasirizadeh Mohammad Dehghani Mohammad Hassan Ehrampoosh Department of Environmental Health Engineering Shaheed Sadoughi University of Medical Sciences Young Researchers and Elite Club Yazd Branch Islamic Azad University

The presence of Hg in the aqueous media is known to cause severe health issues in both humans and animals.Many technologies and especially adsorbents have been applied for its removal. In this study, a graphene oxide–carbon composite(GO–CC) as a new adsorbent was prepared by sol gel procedure and characterized using field emission scanning electron microscopy, BET and EDX. The effects of different variables including solution p H, contact time, adsorbent dose and GO ratio in adsorbent matrix on the removal capacity of Hg were studied. The isotherm data correlated well with the Langmuir isotherm model. Further analysis recommended that the Hg^(2+) adsorption process is governed by the intra-particle and external mass transfer, in which the film diffusion was the rate restrictive step. The presented composite has maximum absorption capacity, q_(max) of 68.8 mg·g^(-1), which is comparable with carbon based adsorbent reported in the previous publications.

关键词： Adsorbent mercury removal Sol gel Carbon composite