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Source attribution for mercury deposition with an updated atmospheric mercury emission inventory in the

Jiajun Liu, Long Wang, Yun Zhu, Che-Jen Lin, Carey Jang, Shuxiao Wang, Jia Xing, Bin Yu, Hui Xu, Yuzhou Pan

《环境科学与工程前沿（英文）》 2019年第13卷第1期 doi: 10.1007/s11783-019-1087-6

摘要：

Estimated anthropogenic Hg emission was 11.9 tons in Pearl River Delta for 2014.

Quantifying contributions of emission sources helps to provide control strategies.

More attentions should be paid to Hg deposition around the large point sources.

Power plant, industrial source and waste incinerator were priorities for control.

A coordinated regional Hg emission control was important for controlling pollution.

关键词： Emission inventory Mercury deposition Pearl River Delta (PRD) Source attribution Control strategy

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Mercury enrichment in

Chunhao Dai, Pufeng Qin, Zhangwei Wang, Jian Chen, Xianshan Zhang, Si Luo

《环境科学与工程前沿（英文）》 2017年第11卷第1期 doi: 10.1007/s11783-017-0892-z

摘要： Mercury enrichment in response to elevated atmospheric mercury concentrations in the organs of rape ( ) was investigated. Elevated soil mercury content had significant impact on mercury accumulation in rape stems, roots, seeds and seed coats. Leaf mercury in the leaves was mostly affected by atmospheric input while the stems were mostly affected by soil concentrations. Mercury in the aboveground plant tissue mainly derived from atmospheric absorption, and atmospheric mercury absorption in leaves was higher than that in the stems. Mercury enrichment in response to elevated atmospheric mercury concentrations in the organs of rape ( ) was investigated using an open top chamber fumigation experiment and a soil mercury enriched cultivation experiment. Results indicate that the mercury concentration in leaves and stems showed a significant variation under different concentrations of mercury in atmospheric and soil experiments while the concentration of mercury in roots, seeds and seed coats showed no significant variation under different atmospheric mercury concentrations. Using the function relation established by the experiment, results for atmospheric mercury sources in rape field biomass showed that atmospheric sources accounted for at least 81.81% of mercury in rape leaves and 32.29% of mercury in the stems. Therefore, mercury in the aboveground biomass predominantly derives from the absorption of atmospheric mercury.

关键词： Open top chamber Gaseous elemental mercury (GEM) Soil Mercury Brassica napus

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Mercury removal from flue gas using nitrate as an electron acceptor in a membrane biofilm reactor

《环境科学与工程前沿（英文）》 2022年第16卷第2期 doi: 10.1007/s11783-021-1454-y

摘要：

Membrane bioreactor achieved mercury removal using nitrate as an electron acceptor.

关键词： Mercury removal Oxygen Ferrous sulfide Transformation of mercury Microbial community

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Progress on cleaner production of vinyl chloride monomers over non-mercury catalysts

Jinli ZHANG, Nan LIU, Wei LI, Bin DAI

《化学科学与工程前沿（英文）》 2011年第5卷第4期页码 514-520 doi: 10.1007/s11705-011-1114-z

摘要： Polyvinyl chloride (PVC) has become the third most used plastic after polyethylene and polypropylene and the worldwide demand continues to increase. Polyvinyl chloride is produced by polymerization of the vinyl chloride monomer (VCM), which is manufactured industrially via the dehydrochlorination of dichloroethane or the hydrochlorination of acetylene. Currently PVC production through the acetylene hydrochlorination method accounts for about 70% of the total PVC production capacity in China. However, the industrial production of VCM utilizes a mercuric chloride catalyst to promote the reaction of acetylene and hydrogen chloride. During the hydrochlorination, the highly toxic mercuric chloride tends to sublime, resulting in the deactivation of the catalyst and also in severe environmental pollution problems. Hence, for China, it is necessary to explore environmental friendly non-mercury catalysts for acetylene hydrochlorination as well as high efficiency novel reactors, with the aim of sustainable PVC production via the acetylene-based method. This paper presents a review of non-mercury heterogeneous and homogeneous catalysts as well as reactor designs, and recommends future work for developing cleaner processes to produce VCM over non-mercury catalysts with high activity and long stability.

关键词： polyvinyl chloride vinyl chloride monomer acetylene hydrochlorination non-mercury catalysts green chemical process

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A review of atmospheric mercury emissions, pollution and control in China

Shuxiao WANG,Lei ZHANG,Long WANG,Qingru WU,Fengyang WANG,Jiming HAO

《环境科学与工程前沿（英文）》 2014年第8卷第5期页码 631-649 doi: 10.1007/s11783-014-0673-x

摘要： Mercury, as a global pollutant, has significant impacts on the environment and human health. The current state of atmospheric mercury emissions, pollution and control in China is comprehensively reviewed in this paper. With about 500–800 t of anthropogenic mercury emissions, China contributes 25%–40% to the global mercury emissions. The dominant mercury emission sources in China are coal combustion, non-ferrous metal smelting, cement production and iron and steel production. The mercury emissions from natural sources in China are equivalent to the anthropogenic mercury emissions. The atmospheric mercury concentration in China is about 2–10 times the background level of North Hemisphere. The mercury deposition fluxes in remote areas in China are usually in the range of 10–50 μg∙m ∙yr . To reduce mercury emissions, legislations have been enacted for power plants, non-ferrous metal smelters and waste incinerators. Currently mercury contented in the flue gas is mainly removed through existing air pollution control devices for sulfur dioxide, nitrogen oxides, and particles. Dedicated mercury control technologies are required in the future to further mitigate the mercury emissions in China.

关键词： atmospheric mercury emissions pollution control China

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New insights into mercury removal mechanism on CeO

Ling Li, Yu He, Xia Lu

《环境科学与工程前沿（英文）》 2018年第12卷第2期 doi: 10.1007/s11783-018-1007-1

摘要： First-principles calculations were performed to investigate the mechanism of Hg adsorption and oxidation on CeO (111). Surface oxygen activated by the reduction of Ce to Ce was vital to Hg adsorption and oxidation processes. Hg was fully oxidized by the surface lattice oxygen on CeO (111), without using any other oxidizing agents. HCl could dissociate and react with the Hg adatom on CeO (111) to form adsorbed Hg–Cl or Cl–Hg–Cl groups, which promoted the desorption of oxidized Hg and prevented CeO catalyst deactivation. In contrast, O–H and H–O–H groups formed during HCl adsorption consumed the active surface oxygen and prohibited Hg oxidation. The consumed surface oxygen was replenished by adding O into the flue gas. We proposed that oxidized Hg desorption and maintenance of sufficient active surface oxygen were the rate-determining steps of Hg removal on CeO -based catalysts. We believe that our thorough understanding and new insights into the mechanism of the Hg removal process will help provide guidelines for developing novel CeO -based catalysts and enhance the Hg removal efficiency.

关键词： Elemental mercury removal Surface adsorption Ceria First-principles calculations

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Removal of elemental mercury by KI-impregnated clay

Boxiong SHEN,Jianhong CHEN,Ji CAI

《环境科学与工程前沿（英文）》 2016年第10卷第2期页码 236-243 doi: 10.1007/s11783-014-0765-7

摘要： This study described the use of clay impregnated by KI in gas phase elemental mercury (Hg ) removal in flue gas. The effects of KI loading, temperature, O , SO and H O on Hg removal were investigated using a fixed bed reactor. The Hg removal efficiency of KI-clay with 3% KI loading could maintain at a high level (approximately 80 %) after 3 h. The KI-clay demonstrated to be a potential adsorbent for Hg removal when compared with activated carbon based adsorbent. O was found to be an important factor in improving the Hg removal. O was demonstrated to assist the transfer of KI to I on the surface of KI-clay, which could react with Hg directly. NO and SO could slightly improve Hg removal, while H O inhibited it greatly. The results indicated that after adsorption, most of the mercury escaped from the surface again. Some of the mercury may have been oxidized as it left the surface. The results demonstrated that the chemical reaction primarily occurred between KI and mercury on the surface of the KI-clay.

关键词： clay elemental mercury removal efficiency potassium iodide mechanism

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Biosorption of mercury and lead by aqueous

Pratibha SANJENBAM, Kumar SAURAV, Krishnan KANNABIRAN

《化学科学与工程前沿（英文）》 2012年第6卷第2期页码 198-202 doi: 10.1007/s11705-012-1285-2

摘要： Toxic heavy metals are increasingly accumulating in the environment worldwide and are considered to be life threatening contaminants. The biosorption of mercury and lead by marine actinomycetes isolated from marine sediment collected from the Bay of Bengal coast of Puducherry, India, was evaluated. The maximum tolerance concentration (MTC) of sp. was determined by a well diffusion method and a broth dilution method. The effects of the initial metal ion concentration, the pH and the biomass dosage on the biosorption of mercury and lead ions were investigated. The MTC of the isolate to metals was 200 mg·L for mercury and 1800 mg·L for lead. At neutral pH, the isolate had a maximum biosorption of metal ions of 200 mg·L and 150 mg·L for mercury and lead respectively. Fourier transform infrared (FTIR) absorption spectra showed the chemical interactions between the functional groups in the biomass such as hydroxyl (-OH), amine (-NH ), carboxyl (-COOH) and the metal ions. The isolate was further characterized by molecular taxonomy and identified as a member of the genus Based on the phenotypic and phylogenetic analysis, the strain was classified as a new species of the genus and designated as VITSVK9 sp. (HM137310). A blast search of the 16S rDNA sequence of the strain showed the most similarity (95%) with sp. A515 Ydz-FQ (EU384279). Based on the results, it can be concluded that this marine could be used as a biosorbent for the removal of heavy metal ions from aqueous environments.

关键词： mercury lead biosorption maximum tolerance concentration Streptomyces VITSVK9 sp.

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Mercury removal and recovery by immobilized

Meifang CHIEN, Ryo NAKAHATA, Tetsuya ONO, Keisuke MIYAUCHI, Ginro ENDO

《化学科学与工程前沿（英文）》 2012年第6卷第2期页码 192-197 doi: 10.1007/s11705-012-1284-3

摘要： From several mercury removing microorganisms, we selected MB1, 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 MB1 was investigated to develop safe, efficient and stable catalytic bio-agent for mercury bioremediation. The results showed that the alginate gel immobilized MB1 cells efficiently removed 80% of mercury from the solution containing 10 mg/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 MB1 suggested that a large portion of reduced metallic mercury was trapped in the gel beads. It was concluded that the alginate gel immobilized MB1 cells have potential to remove and recover mercury from mercury-containing water.

关键词： mercury removal immobilized bacteria alginate gel bioremediation

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Scaling up of cluster beam deposition technology for catalysis application

《化学科学与工程前沿（英文）》 2021年第15卷第6期页码 1360-1379 doi: 10.1007/s11705-021-2101-7

摘要： Many research works have demonstrated that the combination of atomically precise cluster deposition and theoretical calculations is able to address fundamental aspects of size-effects, cluster-support interactions, and reaction mechanisms of cluster materials. Although the wet chemistry method has been widely used to synthesize nanoparticles, the gas-phase synthesis and size-selected strategy was the only method to prepare supported metal clusters with precise numbers of atoms for a long time. However, the low throughput of the physical synthesis method has severely constrained its wider adoption for catalysis applications. In this review, we introduce the latest progress on three types of cluster source which have the most promising potential for scale-up, including sputtering gas aggregation source, pulsed microplasma cluster source, and matrix assembly cluster source. While the sputtering gas aggregation source is leading ahead with a production rate of ~20 mg·h^–1, the pulsed microplasma source has the smallest physical dimensions which makes it possible to compact multiple such devices into a small volume for multiplied production rate. The matrix assembly source has the shortest development history, but already show an impressive deposition rate of ~10 mg·h^–1. At the end of the review, the possible routes for further throughput scale-up are envisaged.

关键词： nanoparticle cluster cluster beam deposition magnetron sputtering heterogeneous catalysis

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Removal of elemental mercury with Mn/Mo/Ru/Al

Yongfu GUO, Naiqiang YAN, Ping LIU, Shijian YANG, Juan WANG, Zan QU

《环境科学与工程前沿（英文）》 2013年第7卷第3期页码 464-473 doi: 10.1007/s11783-012-0430-y

摘要： In this work, a catalytic membrane using Mn/Mo/Ru/Al O as the catalyst was employed to remove elemental mercury (Hg ) from flue gas at low temperature. Compared with traditional catalytic oxidation (TCO) mode, Mn/Al O membrane catalytic system had much higher removal efficiency of Hg . After the incorporation of Mo and Ru, the production of Cl from the Deacon reaction and the retainability for oxidants over Mn/Al O membrane were greatly enhanced. As a result, the oxidization of Hg over Mn/Al O membrane was obviously promoted due to incorporation of Mo and Ru. In the presence of 8 ppmv HCl, the removal efficiency of Hg by Mn/Mo/Ru/Al O membrane reached 95% at 423 K. The influence of NO and SO on Hg removal were insignificant even if 200 ppmv NO and 1000 ppmv SO were used. Moreover, compared with the TCO mode, the Mn/Mo/Ru/Al O membrane catalytic system could remarkably reduce the demanded amount of oxidants for Hg removal. Therefore, the Mn/Mo/Ru/Al O membrane catalytic system may be a promising technology for the control of Hg emission.

关键词： flue gas elemental mercury membrane catalysis transition metal

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A density functional theory study of the adsorption of Hg and HgCl2 on a CaO(001) surface

GUO Xin, ZHENG Chuguang, LU Nanxia

《能源前沿（英文）》 2007年第1卷第1期页码 101-104 doi: 10.1007/s11708-007-0011-0

摘要： The adsorption of mercury and mercury chloride on a CaO(001) surface was investigated by the density functional theory (DFT) by using CaO cluster embedded in an electrostatic field represented by 178 point charges at the crystal CaO lattice positions. For the mercury molecular axis normal to the surface, the mercury can only coordinate to the O anion and has a very weak binding energy of 19.649 kJ/mol. When the mercury chloride molecular axis is vertical to the surface, the Cl atom coordinates to the Ca cation and has a binding energy of 23.699 kJ/mol. When the mercury chloride molecular axis is parallel to the surface, the Hg atom coordinates to the O anion and has a binding energy of 87.829 kJ/mol, which means that the parallel geometry is more stable than the vertical one. The present calculations show that CaO injection could substantially reduce gaseous mercury chloride, but have no apparent effect on the mercury, which is compatible with the available experimental results. This research will provide valuable information for optimizing and selecting a sorbent for the trace element in flue gas.

关键词： mercury chloride mercury molecular surface cluster electrostatic

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Effect of carbon deposition over carbonaceous catalysts on CH

Yongfa ZHANG, Meng ZHANG, Guojie ZHANG, Huirong ZHANG

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 481-485 doi: 10.1007/s11705-010-0523-8

摘要： An investigation was made using a continuous fixed bed reactor to understand the influence of carbon deposition obtained under different conditions on CH -CO reforming. Thermogravimetry (TG) and X-ray diffraction (XRD) were employed to study the characteristics of carbon deposition. It was found that the carbonaceous catalyst is an efficient catalyst in methane decomposition and CH -CO reforming. The trend of methane decomposition at lower temperatures is similar to that at higher temperatures. The methane conversion is high during the initial of stage of the reaction, and then decays to a relatively fixed value after about 30 min. With temperature increase, the methane decomposition rate increases quickly. The reaction temperature has significant influence on methane decomposition, whereas the carbon deposition does not affect methane decomposition significantly. Different types of carbon deposition were formed at different methane decomposition reaction temperatures. The carbon deposition Type I generated at 900°C has a minor effect on CH -CO reforming and it easily reacts with carbon dioxide, but the carbon deposition Type II generated at 1000°C and 1100°C clearly inhibits CH -CO reforming and it is difficult to react with carbon dioxide. The results of XRD showed that some graphite structures were found in carbon deposition Type II.

关键词： carbon deposition carbonaceous catalyst CH₄-CO₂ reforming

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Mercury emission and adsorption characteristics of fly ash in PC and CFB boilers

Li JIA, Baoguo FAN, Xianrong ZHENG, Xiaolei QIAO, Yuxing YAO, Rui ZHAO, Jinrong GUO, Yan JIN

《能源前沿（英文）》 2021年第15卷第1期页码 112-123 doi: 10.1007/s11708-020-0682-3

摘要： The mercury emission was obtained by measuring the mercury contents in flue gas and solid samples in pulverized coal (PC) and circulating fluidized bed (CFB) utility boilers. The relationship was obtained between the mercury emission and adsorption characteristics of fly ash. The parameters included unburned carbon content, particle size, and pore structure of fly ash. The results showed that the majority of mercury released to the atmosphere with the flue gas in PC boiler, while the mercury was enriched in fly ash and captured by the precipitator in CFB boiler. The coal factor was proposed to characterize the impact of coal property on mercury emissions in this paper. As the coal factor increased, the mercury emission to the atmosphere decreased. It was also found that the mercury content of fly ash in the CFB boiler was ten times higher than that in the PC boiler. As the unburned carbon content increased, the mercury adsorbed increased. The capacity of adsorbing mercury by fly ash was directly related to the particle size. The particle size corresponding to the highest content of mercury, which was about 560 ng/g, appeared in the range from 77.5 to 106 µm. The content of mesoporous (4–6 nm) of the fly ash in the particle size of 77.5–106 µm was the highest, which was beneficial to adsorbing the mercury. The specific surface area played a more significant role than specific pore volume in the mercury adsorption process.

关键词： mercury combustion modes coal property fly ash particle size

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Influence mechanism of dynamic and static liquid bridge forces on particle deposition behaviors in solar

Xueqing LIU, Xiaodong ZHAO, Luyi LU, Jianlan LI

《能源前沿（英文）》 2021年第15卷第2期页码 499-512 doi: 10.1007/s11708-021-0742-3

摘要： Solar energy is one of the most promising forms of renewable energy for solving the energy crisis and environmental problems. Dust deposition on photovoltaic mirrors has a serious negative impact on the photoelectric conversion efficiency of solar power stations. In this paper, the influence mechanism of the dynamic and static liquid bridge forces on particle deposition behaviors on solar photovoltaic mirrors is investigated. In addition, the expression and physical meaning of the particle critical separation velocity are proposed. The research results show that the static liquid bridge force can be the primary deposition force causing dust particles to adhere to photovoltaic mirrors. However, the dynamic liquid bridge force can act as a resistance force for the particle motion process and even make dust particles roll along and finally stay on the mirror. The contact force is the primary separation force that causes dust particles to flow away from the mirror. Whether dust particles adhere to the mirror depends on the relative size of the deposition and separating forces. The particle critical separation velocity describes the relative size of the collision-rebound effect and mirror adhesion effect and is expressed in Eq. (16). These research findings can provide theoretical guidance for mirror cleaning methods in the operation process of photovoltaic mirrors.

关键词： dust deposition discrete element method (DEM) photovoltaic mirrors solar energy