The present paper covers the 199 Hg NMR chemical shifts of 24 substituted diphenylmercurials and phenyl(2-benzothiazolylthio)mercurials. There is a good linear relationship between the chemical shift and the Hammett c...The present paper covers the 199 Hg NMR chemical shifts of 24 substituted diphenylmercurials and phenyl(2-benzothiazolylthio)mercurials. There is a good linear relationship between the chemical shift and the Hammett constant of the substituents for both series of compounds, and electron donating substituents cause the chemical shift towards downfield.展开更多
Algae play a significant role in regulating the biogeochemical cycle of mercury(Hg),particularly its highly toxicform,methylmercury(MeHg),within wetlands and lakes.However,despite their widespread presence in paddyfield...Algae play a significant role in regulating the biogeochemical cycle of mercury(Hg),particularly its highly toxicform,methylmercury(MeHg),within wetlands and lakes.However,despite their widespread presence in paddyfields,their specific effects on MeHg dynamics are not yet fully understood.This study investigated the algae-mediated distribution and accumulation of MeHg in Hg-contaminated paddyfields,utilizingfield investigationand microcosm experiment.The results indicated that algae demonstrated a multi-source uptake pattern and hada high capacity to accumulate both total Hg(926±1.69 ng/g)and MeHg(83.6±1.12 ng/g).This accumulationwas predominantly characterized by inorganic Hg species,accounting for 88.4%.Algal capsular extracellularpolymeric substance(EPS)exhibited higher levels of labile organic fractions,such as cysteine(0.59±0.01μg/g),and increased MeHg concentration(84.2±4.51 ng/kg),which contrasted with the levels found in colloidal EPS(0.06±0.01 ng/g and 15.0±1.61 ng/kg).Meanwhile,a significant correlation(P<0.05)was observed betweenthiol-containing cysteine and MeHg concentrations in algal EPS.Algal incubation further revealed the formationof mineral-EPS-algae aggregates on algal surfaces,accompanied by the colonization of Hg-methylating bacteria.Therefore,the surface of algae may form a favorable matrix for microbial Hg methylation and the accumulationof MeHg.Thesefindings emphasize the crucial roles of algae in regulating MeHg dynamics within algae-watersystem in Hg-contaminated paddyfields.展开更多
Mercury removal from coal combustion flue gas remains a significant challenge for environmental protection due to the lack of cost-effective sorbents.In this study,a series of red mud(RM)-based sorbents impregnated wi...Mercury removal from coal combustion flue gas remains a significant challenge for environmental protection due to the lack of cost-effective sorbents.In this study,a series of red mud(RM)-based sorbents impregnated with sodium halides(NaBr and NaI)are presented to capture elemental mercury(Hg^(0))from flue gas.The modified RM underwent comprehensive characterization,including analysis of its textural qualities,crystal structure,chemical composition,and thermal properties.The results indicate that the halide impregnation substantially impacts the surface area and pore size of the RM.Hg^(0) removal performance was evaluated on a fixed-bed reactor in simulated flue gas(consisting of N_(2),O_(2),CO_(2),NO and SO_(2),etc.)on a modified RM.At an optimal adsorption temperature of 160℃,NaI-modified sorbent(RMI5)offers a removal efficiency of 98%in a mixture of gas,including O_(2),NO and HCl.Furthermore,pseudo-second-order model fitting results demonstrate the chemisorption mechanism for the adsorption of Hg^(0) in kinetic investigations.展开更多
This study used steel slag,fly ash,and metakaolin as raw materials(SFM materials)to create silica-alumina-based geopolymers that can solidify Hg^(2+)when activated with sodiumbased water glass.The experiments began wi...This study used steel slag,fly ash,and metakaolin as raw materials(SFM materials)to create silica-alumina-based geopolymers that can solidify Hg^(2+)when activated with sodiumbased water glass.The experiments began with a triangular lattice point mixing design experiment,and the results were fitted,analyzed,and predicted.The optimum SFM material mass ratio was found to be 70%steel slag,25%fly ash,and 5%metakaolin.The optimum modulus of the activator was identified by comparing the unconfined compressive strength and solidifying impact on Hg^(2+)of geosynthetics with different modulus.The SFM geopolymer was then applied in the form of potting to cure the granulated mercury tailings.The inclusion of 50%SFM material generated a geosynthetic that reduced mercury transport to the surface soil by roughly 90%.The mercury concentration of herbaceous plant samples was also reduced by 78%.It indicates that the SFM material can effectively attenuate the migration transformation of mercury.Finally,characterization methods such as XPS and FTIR were used to investigate the mechanism of Hg^(2+)solidification by geopolymers generated by SFM materials.The possible solidification mechanisms were proposed as alkaline environment-induced mercury precipitation,chemical bonding s,surface adsorption of Hg^(2+)and its precipitates by the geopolymer,and physical encapsulation.展开更多
Since scarce knowledge of soil mercury(Hg)concentrations and risks in the vulnerable Xinjiang,topsoils(0-15 cm)from its typical landscapes were extensively sampled.Topsoil total mercury(THg)concentrations varied broad...Since scarce knowledge of soil mercury(Hg)concentrations and risks in the vulnerable Xinjiang,topsoils(0-15 cm)from its typical landscapes were extensively sampled.Topsoil total mercury(THg)concentrations varied broadly between 0.9 and 35.3 ng/g,of which16.8%exceeded the background value of soil Hg for Xinjiang.Topsoil THg concentrations across various landscapes exhibited a declining order:farmland(11.7±6.0 ng/g)>grassland(10.5±8.5 ng/g)>woodland(10.2±8.2 ng/g)>desert(7.0±5.8 ng/g).The average topsoil THg concentration was higher in northwestern Xinjiang(11.3±7.2 ng/g)than that in southeastern Xinjiang(6.3±6.1 ng/g).Relatively high topsoil THg concentrations were observed near the cities with intensive human activities,followed by a gradual decline to the surroundings.The concentrations of topsoil THg were strongly correlated with the contents of total organic carbon(TOC),clay,silty,and sandy,and the distance from each sampling site to its nearest city,suggesting that the variation of topsoil Hg was significantly influenced by TOC content,soil granularity,and anthropogenic Hg emissions.Silty and TOC were the principal affecting factors,explaining 48.7%and 7.9%of the THg variation,respectively.The contamination and potential ecological risk evaluations revealed that topsoils in regions with dense populations were polluted with Hg and contained higher potential ecological risks.The health risk evaluations indicated that exposure risks of topsoil Hg were higher for children than those for adults.Fortunately,topsoil Hg posed acceptable risks to human health.展开更多
Objective: We describe patients with MCS, the evolution of the Quick Environmental Exposure and Sensitivity Inventory (QEESI) score with a special focus on people whose fillings were removed. Methods: We have conducte...Objective: We describe patients with MCS, the evolution of the Quick Environmental Exposure and Sensitivity Inventory (QEESI) score with a special focus on people whose fillings were removed. Methods: We have conducted a retrospective longitudinal cohort study in patients diagnosed with MCS and attended in the outpatient Internal Medicine department of the University Hospital of San Juan de Alicante, from January 1, 2008 to January 1, 2021. Sociodemographic, clinical, QEESI and treatment-related variables were collected. We performed descriptive and inferential analyses. Mixed linear models were used to analyze the QEESI. Calculations were carried out with an α error of 5%. Results: Thirty-three patients were included (72.7% women, mean age 56.2). MCS was mainly triggered by mercury (N = 20) and food intolerance (N = 22). The mean interval from symptoms onset was 120 months (SD 81.6). 114 QEESIs were analyzed: 82 (N = 17 without amalgams) and 32 (N = 16 with amalgams). In patients without amalgams, severity scores increased across all subscales except the masking index (vs. with amalgams). Mean scores for the group without amalgams (vs. with amalgams) were: chemical intolerance, 62.8 points (vs. 63.4 and 46.7);other intolerances, 52.7 points (vs. 62.8 and 50.3);symptom severity, 63.2 (vs. 76.7 and 63.3);masking index, 3.9 (vs. 3.2 and 2.8);and life impacts, 63.1 (vs. 58.4 and 49.8). Conclusion: The profile of patient with MCS is a middle-aged woman who is a frequent user of healthcare services, presents a long diagnostic delay and has borne a great personal, work and socioeconomic impact. The QEESI is useful for the clinical follow-up of patients, including the optimal treatment response in the case of amalgams. Clinical Significance: People affected by Multiple Chemical Sensitivity deserve the attention, understanding and help of health professionals and family members, to face an invisible illness for those who do not suffer from it. Support is needed and doctors must raise awareness, and make an effort to understand and address this pathology. We suggest that protocolized amalgam extraction in accredited and prepared centers can reduce symptoms and improve quality of life, generating clinical, personal, family, occupational, social and occupational benefits.展开更多
Mercury(Hg),especially methylmercury(MeHg),accumulation in rice grain due to rice paddy possessing conditions conducive to Hg methylation has led to human Hg exposure through consumption of rice-based daily meals.In a...Mercury(Hg),especially methylmercury(MeHg),accumulation in rice grain due to rice paddy possessing conditions conducive to Hg methylation has led to human Hg exposure through consumption of rice-based daily meals.In addition to being a food staple,rice is widely used as a raw material to produce a vast variety of processed food products.Little is known about Hg levels in snacking rice-food products and potential Hg exposure from consumption of them,besides previous studies on infant rice cereals.Aiming to provide complementary information for a more complete assessment on Hg exposure risk originated from Hgcontaining rice,this study determined total Hg(THg)and MeHg levels in 195 rice-containing and rice-free processed food products covering all major types of snack foods marketed in China and the estimated daily intake(EDI)of dietary Hg from the consumption of these foods.The results clearly showed THg and MeHg contents in rice-containing foods were significantly higher than rice-free products,suggesting the transfer of Hg and MeHg from the rice to the end products,even after manufacturing processes.Moreover,significant positive correlations were observed between THg,MeHg,or MeHg/THg ratio and rice content for samples containing multiple grains as ingredients,further indicating the deciding role of rice for Hg levels in the end food products.Although the EDI of THg and MeHg via ricebased food products were relatively low compared to the reference dose,it should be considered these snacking food products would contribute additive Hg intake outside of the daily regular meals.展开更多
The prevalence of autism and attention deficit/hyperactivity disorders is increasing worldwide.Recent studies suggest the excessive intake of ultra-processed food plays a role in the inheritance of these disorders via...The prevalence of autism and attention deficit/hyperactivity disorders is increasing worldwide.Recent studies suggest the excessive intake of ultra-processed food plays a role in the inheritance of these disorders via heavy metal exposures and nutritional deficits that impact the expression of genes.In the case of the metallothionein(MT)gene,biomarker studies show dietary zinc(Zn)deficits impact MT protein levels in children with autism and are associated with the bioaccumulation of lead and/or mercury in children exhibiting autism/attention deficit/hyperactivity disorders symptomology.The impact of dietary changes on lead and mercury exposures and MT gene behavior could be determined using a randomized test and control group design.Pregnant women serving in the testgroup would participate in a nutritional epigenetics education intervention/course designed to reduce ultra-processed food intake and heavy metal levels in blood while increasing whole food intake and MT and Zn levels.Changes in maternal diet would be measured using data derived from an online diet survey administered to the test and control groups pre-post intervention.Changes in maternal lead,mercury,Zn,and MT levels would be measured via blood sample analyses prior to the intervention and after childbirth via cord blood analyses to determine infant risk factors.展开更多
The high-pressure mercury intrusion (HPMI) experiment is widely used to assess the pore architecture oftight sandstone reservoirs. However, the conventional analysis of the high- pressure mercury intrusionhas always f...The high-pressure mercury intrusion (HPMI) experiment is widely used to assess the pore architecture oftight sandstone reservoirs. However, the conventional analysis of the high- pressure mercury intrusionhas always focused on the mercury injection curves themselves, neglecting the important geologicalinformation conveyed by the mercury ejection curves. This paper quantitatively describes the fractalcharacteristics of ejection curves by using four fractal models, i.e.,. Menger model, Thermodynamicmodel, Sierpinski model, and multi- fractal model. In comparison with mercury injection curves, weexplore the fractal significance of mercury ejection curves and define the applicability of different fractalmodels in characterizing pore architectures. Investigated tight sandstone samples can be divided intofour types (Types A, B, C and D) based on porosity, permeability, and mercury removal efficiency. Type Dsamples are unique in that they have higher permeability (>0.6 mD) but lower mercury removal effi-ciency (<35%). Fractal studies of the mercury injection curve show that it mainly reflects the pore throatcharacteristics, while the mercury ejection curve serves to reveal the pore features, and porosity andpermeability correlate well with the fractal dimension of the injection curve, while mercury removalefficiency correlates only with the Ds' value of the ejection curve. The studies on the mercury ejectioncurves also reveal that the small pores and micropores of the Type C and Type D samples are moredeveloped, with varying pore architecture. The fractal dimension Ds' value of Type D samples is greaterthan that of Type C samples, and the dissolution of Type D samples is more intense than that of Type Csamples, which further indicates that the Type D samples are smaller in pore size, rougher in surface, andwith greater difficulty for the hydrocarbon to enter, resulting in their reservoir capacity probably lessthan that of Type C samples. In this regard, the important information characterized by the mercuryejection curve should be considered in evaluating the tight sandstone reservoirs. Finally, the Menger andThermodynamic models prove to be more suitable for describing the total pore architecture, while theSierpinski model is better for characterizing the variability of the interconnected pores.展开更多
Carbon-supported mercury catalysts are extensivelyemployed in calcium carbide-based polyvinyl chloride(PVC)industries,but the usage of mercury-based catalysts can pose an environmental threat due to the release of mer...Carbon-supported mercury catalysts are extensivelyemployed in calcium carbide-based polyvinyl chloride(PVC)industries,but the usage of mercury-based catalysts can pose an environmental threat due to the release of mercury into the surrounding area during the operation period.In this study,a highly active and stable mercury-based catalyst was developed,utilizing the nitrogen atom of the support as the anchor site to enhance the interaction between active sites(HgCl_(2))and the carbon support(N-AC).Thermal loss rate testing and thermogravimetric analysis results demonstrate that,compared to commercial activated carbon,N-doped carbon can effectively increase the heat stability of HgCl_(2).The obtained mercury-based catalysts(HgCl_(2)/N-AC)exhibit significant catalytic performance,achieving 2.5 times the C2H2 conversion of conventional HgCl_(2)/AC catalysts.Experimental analysis combined with theoretical calculations reveals that,contrary to the Eley-Rideal(ER)mechanism of HgCl_(2)/AC,the HgCl_(2)/N-AC catalyst follows the Langmuir-Hinshelwood(LH)adsorption mechanism.The nitrogen sites and HgCl_(2) on the catalyst enhance the adsorption capabilities of the HCl and C2H2,thereby improving the catalytic performance.Based on the modification of the active center by these solid ligands,the loading amount of HgCl_(2) on the catalyst can be further reduced from the current 6.5%to 3%.Considering the absence of successful industrial applications for mercury-free catalysts,and based on the current annual consumption of commercial mercury chloride catalysts in the PVC industry,the widespread adoption of this technology could annually reduce the usage of chlorine mercury by 500 tons,making a notable contribution to mercury compliance,reduction,and emissions control in China.It also serves as a bridge between mercury-free and low-mercury catalysts.Moreover,this solid ligand technology can assist in the application research of mercury-free catalysts.展开更多
The pore structure of rocks significantly influences the porosity and permeability of reservoirs and the migration ability of oil and gas,and being the key task on the development of volcanic gas reservoirs.Nine volca...The pore structure of rocks significantly influences the porosity and permeability of reservoirs and the migration ability of oil and gas,and being the key task on the development of volcanic gas reservoirs.Nine volcanic rock samples from the Yingcheng Formation and Huoshiling Formation in the Longfengshan area of the Changling Fault Depression in the Songliao Basin were selected for this study.The pore structures of the volcanic rocks in the study area were investigated using high-pressure mercury injection,X-ray diffraction combined with fractal theory.The relationships between the fractal dimension and physical properties characteristics,pore structure parameters,and mineral content were analyzed to provide guidance for the development of volcanic rock gas reservoirs.The results show that the reservoir can be divided into 3 types(I,II,and III)based on the shape of the capillary pressure curve,and the physical properties deteriorate successively.Different types of reservoirs exhibit different fractal characteristics.For typesⅠ,ⅡandⅢ,the average total fractal dimensions were 2.3418,2.6850,and 2.9203,respectively.The larger the fractal dimension,the stronger the heterogeneity of reservoir.A small number of macro-pores primarily contributed to permeability.The fractal dimension was negatively correlated with porosity and permeability.The fractal dimension of the rock was strongly correlated with quartz and feldspar contents,and the mineral composition and content are closely related to the pore evolution of the reservoir,which are the internal factors affecting the fractal dimension of volcanic rock.展开更多
In this study,a string of Cr-Mnco-modified activated coke catalysts(XCryMn1-y/AC)were prepared to investigate toluene and Hg^(0) removal performance.Multifarious characterizations including XRD,TEM,SEM,in situ DRIFTS,...In this study,a string of Cr-Mnco-modified activated coke catalysts(XCryMn1-y/AC)were prepared to investigate toluene and Hg^(0) removal performance.Multifarious characterizations including XRD,TEM,SEM,in situ DRIFTS,BET,XPS and H_(2)-TPR showed that 4%Cr0.5Mn0.5/AC had excellent physicochemical properties and exhibited the best toluene and Hg^(0) removal efficiency at 200℃.By varying the experimental gas components and conditions,it was found that too large weight hourly space velocity would reduce the removal efficiency of toluene and Hg^(0).Although O_(2) promoted the abatement of toluene and Hg^(0),the inhibitory role of H_(2)O and SO_(2) offset the promoting effect of O_(2) to some extent.Toluene significantly inhibited Hg^(0) removal,resulting from that toluene was present at concentrations orders of magnitude greater than mercury’s or the catalyst was more prone to adsorb toluene,while Hg^(0) almost exerted non-existent influence on toluene elimination.The mechanistic analysis showed that the forms of toluene and Hg^(0) removal included both adsorption and oxidation,where the high-valent metal cations and oxygen vacancy clusters promoted the redox cycle of Cr^(3+)+Mn^(3+)/Mn^(4+)+Cr^(6+)+Mn^(2+),which facilitated the conversion and replenishment of reactive oxygen species in the oxidation process,and even the CrMn_(1.5)O_(4) spinel structure could provide a larger catalytic interface,thus enhancing the adsorption/oxidation of toluene and Hg^(0).Therefore,its excellent physicochemical properties make it a costeffective potential industrial catalyst with outstanding synergistic toluene and Hg^(0) removal performance and preeminent resistance to H_(2)O and SO_(2).展开更多
Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense...Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.展开更多
Metal-organic frameworks(MOFs)attract broad interests in mercury(Hg)ion adsorption field,while unreasonable distribution of active groups commonly restricts their utilization efficiency.In this work,we constructed a n...Metal-organic frameworks(MOFs)attract broad interests in mercury(Hg)ion adsorption field,while unreasonable distribution of active groups commonly restricts their utilization efficiency.In this work,we constructed a new MOF(TYUST-6)with dense thiol-rich traps in the 1D pore wall.This accessible channel and rational distribution of thiols allow the smooth diffusion of Hg ions and thereby result in a high Langmuir adsorption capacity of 1347.6 mg/g,almost reaching the theoretical maximum(1444.3 mg/g).Adsorption equilibrium needs 10 and 30 min at the initial concentrations of 10 and 100 mg/L,respectively.Common co-existing ions and solution pH show almost negligible interferences on the adsorption,and adsorbent regeneration can be well achieved.Combining experimental characterizations and theoretical calculations,the thiol groups in the pore wall are proved to be the dominant interaction sites.Thus,this work reports a novel high-capacity adsorbent for Hg^(2+),and proposes a feasible guideline for designing effective adsorbents.展开更多
The connectivity of shale pores and the occurrence of movable oil in shales have long been the focus of research.In this study,samples from wells BX7 and BYY2 in the Eq3^4-10 cyclothem of Qianjiang Formation in the Qi...The connectivity of shale pores and the occurrence of movable oil in shales have long been the focus of research.In this study,samples from wells BX7 and BYY2 in the Eq3^4-10 cyclothem of Qianjiang Formation in the Qianjiang depression,were analyzed.A double mercury injection method was used to distinguish between invalid and effective connected pores.The pore characteristics for occurrence of retained hydrocarbons and movable shale oil were identified by comparing pore changes in low temperature nitrogen adsorption and high pressure mercury injection experiments before and after extraction and the change in the mercury injection amounts in the pores between two separate mercury injections.The results show that less than 50%of the total connected pores in the Eq34-10 cyclothem samples are effective.The development of effective connected pores affects the mobility of shale oil but varies with different lithofacies.The main factor limiting shale oil mobility in Well BX7 is the presence of pores with throat sizes less than 15 nm.In Well BYY2,residual mercury in injection testing of lamellar dolomitic mudstone facies was mainly concentrated in pores with throats of 10-200 nm,and in bulk argillaceous dolomite facies,it was mainly concentrated at 60-300 nm.The throats of hydrocarbon-retaining pores can be 5 nm or even smaller,but pores with movable shale oil in the well were found to have throat sizes greater than 40 nm.Excluding the influence of differences in wettability,the movability of shale oil is mainly affected by differences in lithofacies,the degree of pore deformation caused by diagenesis,the complexity of pore structures,and the connectivity of pore throats.Dissolution and reprecipitation of halite also inhibit the mobility of shale oil.展开更多
Totally 24 arbor tree species and 6 shrub species were measured on their absorption capacities to heavy metal Pb, Cd, Cr, and Hg by collecting and analyzing the leaves of trees along different streets in Harbin city i...Totally 24 arbor tree species and 6 shrub species were measured on their absorption capacities to heavy metal Pb, Cd, Cr, and Hg by collecting and analyzing the leaves of trees along different streets in Harbin city in Sept. to Oct. of 2003. The results showed that all the measured species had certain absorbency to the pollutants (Pb, Cd, Cr and Hg), but there existed significant difference in absorption capacity for different species to different pollutants. The measured tree species were classified into three categories by their absorption quantum of heavy metal pollutants. Among the species measured,Betula platyphylla, Ulmus pumila var.pendula, andPrunus persicaf.rubro-plena had high capacity in absorbing Pb;Populus xiahei, P. nigra var.Italica, P. alba x P. berolinensis andSalix matsudana had had high capacity in absorbing Cd;Phellodendron amurense, Syringa oblata, Salix matsudana, Pinus tabulaeformis var.mukdensis, Picea koraiensis, Prunus persica f.rubro-plena, P. triloba andAcer negundo, etc. had high capacity in absorption of Cr;Prunus triloba, Quercus mongolica, Salix matsudana, Sambucus williamsii, Pyrus ussuuriensis andSpiraea fritschiana were good at absorption of Hg. This study might offer scientific foundation for selection of urban afforestation species in different polluted conditions caused by heavy metals. Keywords Greening tree species - Heavy metal - Pollutants - Plumbum - Cadmium - Chromium - Mercury - Absorptivity CLC number S731.2 - X501 Document code A Foundation item: This study is financially supported by the Special Programme for Agriculture under Ministry of Chinese Science and Technology (No. 2002BA516A15-01).Biography: MU Li-qiang (1966-), female, Associate professor in Northeast Forestry University, Harbin 150040, P. R. China.Responsible editor: Zhu Hong展开更多
文摘The present paper covers the 199 Hg NMR chemical shifts of 24 substituted diphenylmercurials and phenyl(2-benzothiazolylthio)mercurials. There is a good linear relationship between the chemical shift and the Hammett constant of the substituents for both series of compounds, and electron donating substituents cause the chemical shift towards downfield.
基金supported by the Natural Science Foundation of China(Nos.22166009,42477268 and 42267032)the High-Level Talent Training Program in Guizhou Province(No.GCC[2023]045)the Post-funded Project of National Key Research and Development Program of China and the Natural Science Foundation of Chongqing(No.CSTB2022NSCQ-MSX0563).
文摘Algae play a significant role in regulating the biogeochemical cycle of mercury(Hg),particularly its highly toxicform,methylmercury(MeHg),within wetlands and lakes.However,despite their widespread presence in paddyfields,their specific effects on MeHg dynamics are not yet fully understood.This study investigated the algae-mediated distribution and accumulation of MeHg in Hg-contaminated paddyfields,utilizingfield investigationand microcosm experiment.The results indicated that algae demonstrated a multi-source uptake pattern and hada high capacity to accumulate both total Hg(926±1.69 ng/g)and MeHg(83.6±1.12 ng/g).This accumulationwas predominantly characterized by inorganic Hg species,accounting for 88.4%.Algal capsular extracellularpolymeric substance(EPS)exhibited higher levels of labile organic fractions,such as cysteine(0.59±0.01μg/g),and increased MeHg concentration(84.2±4.51 ng/kg),which contrasted with the levels found in colloidal EPS(0.06±0.01 ng/g and 15.0±1.61 ng/kg).Meanwhile,a significant correlation(P<0.05)was observed betweenthiol-containing cysteine and MeHg concentrations in algal EPS.Algal incubation further revealed the formationof mineral-EPS-algae aggregates on algal surfaces,accompanied by the colonization of Hg-methylating bacteria.Therefore,the surface of algae may form a favorable matrix for microbial Hg methylation and the accumulationof MeHg.Thesefindings emphasize the crucial roles of algae in regulating MeHg dynamics within algae-watersystem in Hg-contaminated paddyfields.
基金supported by the National Natural Science Foundation of China(22278066,21776039)the National Key R&D Program of China(2023YFB4103001)The Fundamental Research Funds for the Central Universities(DUT2021TB03).
文摘Mercury removal from coal combustion flue gas remains a significant challenge for environmental protection due to the lack of cost-effective sorbents.In this study,a series of red mud(RM)-based sorbents impregnated with sodium halides(NaBr and NaI)are presented to capture elemental mercury(Hg^(0))from flue gas.The modified RM underwent comprehensive characterization,including analysis of its textural qualities,crystal structure,chemical composition,and thermal properties.The results indicate that the halide impregnation substantially impacts the surface area and pore size of the RM.Hg^(0) removal performance was evaluated on a fixed-bed reactor in simulated flue gas(consisting of N_(2),O_(2),CO_(2),NO and SO_(2),etc.)on a modified RM.At an optimal adsorption temperature of 160℃,NaI-modified sorbent(RMI5)offers a removal efficiency of 98%in a mixture of gas,including O_(2),NO and HCl.Furthermore,pseudo-second-order model fitting results demonstrate the chemisorption mechanism for the adsorption of Hg^(0) in kinetic investigations.
基金supported by the National Key R&D Projects of China(No.2018YFC1801706-01)the National Natural Science Foundation of China(No.22162007)+2 种基金the Science and Technology Supporting Project of Guizhou Province(No.[2021]480,[2023]379)the Wengfu(Group)Co.,Ltd.Technology Development Project(No.WH-220787(YF))the Project from Guizhou Institute of Innovation and Development of Dual-carbon and New Energy Technologies(No.DCRE-2023-05)。
文摘This study used steel slag,fly ash,and metakaolin as raw materials(SFM materials)to create silica-alumina-based geopolymers that can solidify Hg^(2+)when activated with sodiumbased water glass.The experiments began with a triangular lattice point mixing design experiment,and the results were fitted,analyzed,and predicted.The optimum SFM material mass ratio was found to be 70%steel slag,25%fly ash,and 5%metakaolin.The optimum modulus of the activator was identified by comparing the unconfined compressive strength and solidifying impact on Hg^(2+)of geosynthetics with different modulus.The SFM geopolymer was then applied in the form of potting to cure the granulated mercury tailings.The inclusion of 50%SFM material generated a geosynthetic that reduced mercury transport to the surface soil by roughly 90%.The mercury concentration of herbaceous plant samples was also reduced by 78%.It indicates that the SFM material can effectively attenuate the migration transformation of mercury.Finally,characterization methods such as XPS and FTIR were used to investigate the mechanism of Hg^(2+)solidification by geopolymers generated by SFM materials.The possible solidification mechanisms were proposed as alkaline environment-induced mercury precipitation,chemical bonding s,surface adsorption of Hg^(2+)and its precipitates by the geopolymer,and physical encapsulation.
基金supported by the Second Tibetan Plateau Scientific Expedition and Research Program(STEP)(No.2019QZKK0605)the National Natural Science Foundation of China(No.42201161)the Startup Foundation for Introducing Talent of NUIST(No.2022r024)。
文摘Since scarce knowledge of soil mercury(Hg)concentrations and risks in the vulnerable Xinjiang,topsoils(0-15 cm)from its typical landscapes were extensively sampled.Topsoil total mercury(THg)concentrations varied broadly between 0.9 and 35.3 ng/g,of which16.8%exceeded the background value of soil Hg for Xinjiang.Topsoil THg concentrations across various landscapes exhibited a declining order:farmland(11.7±6.0 ng/g)>grassland(10.5±8.5 ng/g)>woodland(10.2±8.2 ng/g)>desert(7.0±5.8 ng/g).The average topsoil THg concentration was higher in northwestern Xinjiang(11.3±7.2 ng/g)than that in southeastern Xinjiang(6.3±6.1 ng/g).Relatively high topsoil THg concentrations were observed near the cities with intensive human activities,followed by a gradual decline to the surroundings.The concentrations of topsoil THg were strongly correlated with the contents of total organic carbon(TOC),clay,silty,and sandy,and the distance from each sampling site to its nearest city,suggesting that the variation of topsoil Hg was significantly influenced by TOC content,soil granularity,and anthropogenic Hg emissions.Silty and TOC were the principal affecting factors,explaining 48.7%and 7.9%of the THg variation,respectively.The contamination and potential ecological risk evaluations revealed that topsoils in regions with dense populations were polluted with Hg and contained higher potential ecological risks.The health risk evaluations indicated that exposure risks of topsoil Hg were higher for children than those for adults.Fortunately,topsoil Hg posed acceptable risks to human health.
文摘Objective: We describe patients with MCS, the evolution of the Quick Environmental Exposure and Sensitivity Inventory (QEESI) score with a special focus on people whose fillings were removed. Methods: We have conducted a retrospective longitudinal cohort study in patients diagnosed with MCS and attended in the outpatient Internal Medicine department of the University Hospital of San Juan de Alicante, from January 1, 2008 to January 1, 2021. Sociodemographic, clinical, QEESI and treatment-related variables were collected. We performed descriptive and inferential analyses. Mixed linear models were used to analyze the QEESI. Calculations were carried out with an α error of 5%. Results: Thirty-three patients were included (72.7% women, mean age 56.2). MCS was mainly triggered by mercury (N = 20) and food intolerance (N = 22). The mean interval from symptoms onset was 120 months (SD 81.6). 114 QEESIs were analyzed: 82 (N = 17 without amalgams) and 32 (N = 16 with amalgams). In patients without amalgams, severity scores increased across all subscales except the masking index (vs. with amalgams). Mean scores for the group without amalgams (vs. with amalgams) were: chemical intolerance, 62.8 points (vs. 63.4 and 46.7);other intolerances, 52.7 points (vs. 62.8 and 50.3);symptom severity, 63.2 (vs. 76.7 and 63.3);masking index, 3.9 (vs. 3.2 and 2.8);and life impacts, 63.1 (vs. 58.4 and 49.8). Conclusion: The profile of patient with MCS is a middle-aged woman who is a frequent user of healthcare services, presents a long diagnostic delay and has borne a great personal, work and socioeconomic impact. The QEESI is useful for the clinical follow-up of patients, including the optimal treatment response in the case of amalgams. Clinical Significance: People affected by Multiple Chemical Sensitivity deserve the attention, understanding and help of health professionals and family members, to face an invisible illness for those who do not suffer from it. Support is needed and doctors must raise awareness, and make an effort to understand and address this pathology. We suggest that protocolized amalgam extraction in accredited and prepared centers can reduce symptoms and improve quality of life, generating clinical, personal, family, occupational, social and occupational benefits.
基金supported by the Shandong Provincial Natural Science Foundation (No.ZR2022QB242)the National Natural Science Foundation of China (No.22306111 and 22306108)+1 种基金the Shandong Provincial Natural Science Foundation (No.ZR2020ZD20)the Chinese Postdoctoral Science Foundation (No.2023M732059).
文摘Mercury(Hg),especially methylmercury(MeHg),accumulation in rice grain due to rice paddy possessing conditions conducive to Hg methylation has led to human Hg exposure through consumption of rice-based daily meals.In addition to being a food staple,rice is widely used as a raw material to produce a vast variety of processed food products.Little is known about Hg levels in snacking rice-food products and potential Hg exposure from consumption of them,besides previous studies on infant rice cereals.Aiming to provide complementary information for a more complete assessment on Hg exposure risk originated from Hgcontaining rice,this study determined total Hg(THg)and MeHg levels in 195 rice-containing and rice-free processed food products covering all major types of snack foods marketed in China and the estimated daily intake(EDI)of dietary Hg from the consumption of these foods.The results clearly showed THg and MeHg contents in rice-containing foods were significantly higher than rice-free products,suggesting the transfer of Hg and MeHg from the rice to the end products,even after manufacturing processes.Moreover,significant positive correlations were observed between THg,MeHg,or MeHg/THg ratio and rice content for samples containing multiple grains as ingredients,further indicating the deciding role of rice for Hg levels in the end food products.Although the EDI of THg and MeHg via ricebased food products were relatively low compared to the reference dose,it should be considered these snacking food products would contribute additive Hg intake outside of the daily regular meals.
文摘The prevalence of autism and attention deficit/hyperactivity disorders is increasing worldwide.Recent studies suggest the excessive intake of ultra-processed food plays a role in the inheritance of these disorders via heavy metal exposures and nutritional deficits that impact the expression of genes.In the case of the metallothionein(MT)gene,biomarker studies show dietary zinc(Zn)deficits impact MT protein levels in children with autism and are associated with the bioaccumulation of lead and/or mercury in children exhibiting autism/attention deficit/hyperactivity disorders symptomology.The impact of dietary changes on lead and mercury exposures and MT gene behavior could be determined using a randomized test and control group design.Pregnant women serving in the testgroup would participate in a nutritional epigenetics education intervention/course designed to reduce ultra-processed food intake and heavy metal levels in blood while increasing whole food intake and MT and Zn levels.Changes in maternal diet would be measured using data derived from an online diet survey administered to the test and control groups pre-post intervention.Changes in maternal lead,mercury,Zn,and MT levels would be measured via blood sample analyses prior to the intervention and after childbirth via cord blood analyses to determine infant risk factors.
基金The research project was co-funded by the National Natural Science Foundation of China(No.42072172,No.41772120)Shandong Province Natural Science Fund for Distinguished Young Scholars(No.JQ201311)the Graduate Scientific and Technological Innovation Project Financially Supported by Shandong University of Science and Technology(No.SDKDYC190313).
文摘The high-pressure mercury intrusion (HPMI) experiment is widely used to assess the pore architecture oftight sandstone reservoirs. However, the conventional analysis of the high- pressure mercury intrusionhas always focused on the mercury injection curves themselves, neglecting the important geologicalinformation conveyed by the mercury ejection curves. This paper quantitatively describes the fractalcharacteristics of ejection curves by using four fractal models, i.e.,. Menger model, Thermodynamicmodel, Sierpinski model, and multi- fractal model. In comparison with mercury injection curves, weexplore the fractal significance of mercury ejection curves and define the applicability of different fractalmodels in characterizing pore architectures. Investigated tight sandstone samples can be divided intofour types (Types A, B, C and D) based on porosity, permeability, and mercury removal efficiency. Type Dsamples are unique in that they have higher permeability (>0.6 mD) but lower mercury removal effi-ciency (<35%). Fractal studies of the mercury injection curve show that it mainly reflects the pore throatcharacteristics, while the mercury ejection curve serves to reveal the pore features, and porosity andpermeability correlate well with the fractal dimension of the injection curve, while mercury removalefficiency correlates only with the Ds' value of the ejection curve. The studies on the mercury ejectioncurves also reveal that the small pores and micropores of the Type C and Type D samples are moredeveloped, with varying pore architecture. The fractal dimension Ds' value of Type D samples is greaterthan that of Type C samples, and the dissolution of Type D samples is more intense than that of Type Csamples, which further indicates that the Type D samples are smaller in pore size, rougher in surface, andwith greater difficulty for the hydrocarbon to enter, resulting in their reservoir capacity probably lessthan that of Type C samples. In this regard, the important information characterized by the mercuryejection curve should be considered in evaluating the tight sandstone reservoirs. Finally, the Menger andThermodynamic models prove to be more suitable for describing the total pore architecture, while theSierpinski model is better for characterizing the variability of the interconnected pores.
基金supported by the National Key Research and Development Program of China(2024YFC3907904).
文摘Carbon-supported mercury catalysts are extensivelyemployed in calcium carbide-based polyvinyl chloride(PVC)industries,but the usage of mercury-based catalysts can pose an environmental threat due to the release of mercury into the surrounding area during the operation period.In this study,a highly active and stable mercury-based catalyst was developed,utilizing the nitrogen atom of the support as the anchor site to enhance the interaction between active sites(HgCl_(2))and the carbon support(N-AC).Thermal loss rate testing and thermogravimetric analysis results demonstrate that,compared to commercial activated carbon,N-doped carbon can effectively increase the heat stability of HgCl_(2).The obtained mercury-based catalysts(HgCl_(2)/N-AC)exhibit significant catalytic performance,achieving 2.5 times the C2H2 conversion of conventional HgCl_(2)/AC catalysts.Experimental analysis combined with theoretical calculations reveals that,contrary to the Eley-Rideal(ER)mechanism of HgCl_(2)/AC,the HgCl_(2)/N-AC catalyst follows the Langmuir-Hinshelwood(LH)adsorption mechanism.The nitrogen sites and HgCl_(2) on the catalyst enhance the adsorption capabilities of the HCl and C2H2,thereby improving the catalytic performance.Based on the modification of the active center by these solid ligands,the loading amount of HgCl_(2) on the catalyst can be further reduced from the current 6.5%to 3%.Considering the absence of successful industrial applications for mercury-free catalysts,and based on the current annual consumption of commercial mercury chloride catalysts in the PVC industry,the widespread adoption of this technology could annually reduce the usage of chlorine mercury by 500 tons,making a notable contribution to mercury compliance,reduction,and emissions control in China.It also serves as a bridge between mercury-free and low-mercury catalysts.Moreover,this solid ligand technology can assist in the application research of mercury-free catalysts.
基金Supported by Key Scientific and Technological Projects of Sinopec(No.P21104-2).
文摘The pore structure of rocks significantly influences the porosity and permeability of reservoirs and the migration ability of oil and gas,and being the key task on the development of volcanic gas reservoirs.Nine volcanic rock samples from the Yingcheng Formation and Huoshiling Formation in the Longfengshan area of the Changling Fault Depression in the Songliao Basin were selected for this study.The pore structures of the volcanic rocks in the study area were investigated using high-pressure mercury injection,X-ray diffraction combined with fractal theory.The relationships between the fractal dimension and physical properties characteristics,pore structure parameters,and mineral content were analyzed to provide guidance for the development of volcanic rock gas reservoirs.The results show that the reservoir can be divided into 3 types(I,II,and III)based on the shape of the capillary pressure curve,and the physical properties deteriorate successively.Different types of reservoirs exhibit different fractal characteristics.For typesⅠ,ⅡandⅢ,the average total fractal dimensions were 2.3418,2.6850,and 2.9203,respectively.The larger the fractal dimension,the stronger the heterogeneity of reservoir.A small number of macro-pores primarily contributed to permeability.The fractal dimension was negatively correlated with porosity and permeability.The fractal dimension of the rock was strongly correlated with quartz and feldspar contents,and the mineral composition and content are closely related to the pore evolution of the reservoir,which are the internal factors affecting the fractal dimension of volcanic rock.
基金supported by the Scientific Research Project of Hunan Provincial Department of Education (No.22B0458)the National Natural Science Foundation of China (No.52270102).
文摘In this study,a string of Cr-Mnco-modified activated coke catalysts(XCryMn1-y/AC)were prepared to investigate toluene and Hg^(0) removal performance.Multifarious characterizations including XRD,TEM,SEM,in situ DRIFTS,BET,XPS and H_(2)-TPR showed that 4%Cr0.5Mn0.5/AC had excellent physicochemical properties and exhibited the best toluene and Hg^(0) removal efficiency at 200℃.By varying the experimental gas components and conditions,it was found that too large weight hourly space velocity would reduce the removal efficiency of toluene and Hg^(0).Although O_(2) promoted the abatement of toluene and Hg^(0),the inhibitory role of H_(2)O and SO_(2) offset the promoting effect of O_(2) to some extent.Toluene significantly inhibited Hg^(0) removal,resulting from that toluene was present at concentrations orders of magnitude greater than mercury’s or the catalyst was more prone to adsorb toluene,while Hg^(0) almost exerted non-existent influence on toluene elimination.The mechanistic analysis showed that the forms of toluene and Hg^(0) removal included both adsorption and oxidation,where the high-valent metal cations and oxygen vacancy clusters promoted the redox cycle of Cr^(3+)+Mn^(3+)/Mn^(4+)+Cr^(6+)+Mn^(2+),which facilitated the conversion and replenishment of reactive oxygen species in the oxidation process,and even the CrMn_(1.5)O_(4) spinel structure could provide a larger catalytic interface,thus enhancing the adsorption/oxidation of toluene and Hg^(0).Therefore,its excellent physicochemical properties make it a costeffective potential industrial catalyst with outstanding synergistic toluene and Hg^(0) removal performance and preeminent resistance to H_(2)O and SO_(2).
基金supported by the Basic Research Business Fund Grant Program for University of Science and Technology Beijing (No.06500227)the Fundamental Research Funds for the Central Universities (No.FRF-TP-22-091A1).
文摘Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.
基金supported by the National Natural Science Foundation of China(No.22208230)Fundamental Research Program of Shanxi Province(No.202103021223281)。
文摘Metal-organic frameworks(MOFs)attract broad interests in mercury(Hg)ion adsorption field,while unreasonable distribution of active groups commonly restricts their utilization efficiency.In this work,we constructed a new MOF(TYUST-6)with dense thiol-rich traps in the 1D pore wall.This accessible channel and rational distribution of thiols allow the smooth diffusion of Hg ions and thereby result in a high Langmuir adsorption capacity of 1347.6 mg/g,almost reaching the theoretical maximum(1444.3 mg/g).Adsorption equilibrium needs 10 and 30 min at the initial concentrations of 10 and 100 mg/L,respectively.Common co-existing ions and solution pH show almost negligible interferences on the adsorption,and adsorbent regeneration can be well achieved.Combining experimental characterizations and theoretical calculations,the thiol groups in the pore wall are proved to be the dominant interaction sites.Thus,this work reports a novel high-capacity adsorbent for Hg^(2+),and proposes a feasible guideline for designing effective adsorbents.
基金supported by the National Natural Science Foundation of China(No.U19B6003)。
文摘The connectivity of shale pores and the occurrence of movable oil in shales have long been the focus of research.In this study,samples from wells BX7 and BYY2 in the Eq3^4-10 cyclothem of Qianjiang Formation in the Qianjiang depression,were analyzed.A double mercury injection method was used to distinguish between invalid and effective connected pores.The pore characteristics for occurrence of retained hydrocarbons and movable shale oil were identified by comparing pore changes in low temperature nitrogen adsorption and high pressure mercury injection experiments before and after extraction and the change in the mercury injection amounts in the pores between two separate mercury injections.The results show that less than 50%of the total connected pores in the Eq34-10 cyclothem samples are effective.The development of effective connected pores affects the mobility of shale oil but varies with different lithofacies.The main factor limiting shale oil mobility in Well BX7 is the presence of pores with throat sizes less than 15 nm.In Well BYY2,residual mercury in injection testing of lamellar dolomitic mudstone facies was mainly concentrated in pores with throats of 10-200 nm,and in bulk argillaceous dolomite facies,it was mainly concentrated at 60-300 nm.The throats of hydrocarbon-retaining pores can be 5 nm or even smaller,but pores with movable shale oil in the well were found to have throat sizes greater than 40 nm.Excluding the influence of differences in wettability,the movability of shale oil is mainly affected by differences in lithofacies,the degree of pore deformation caused by diagenesis,the complexity of pore structures,and the connectivity of pore throats.Dissolution and reprecipitation of halite also inhibit the mobility of shale oil.
基金Financially supported by the Special Pro-gramme for Agriculture under Ministry of Chinese Science and Technology (No. 2002BA516A15-01).
文摘Totally 24 arbor tree species and 6 shrub species were measured on their absorption capacities to heavy metal Pb, Cd, Cr, and Hg by collecting and analyzing the leaves of trees along different streets in Harbin city in Sept. to Oct. of 2003. The results showed that all the measured species had certain absorbency to the pollutants (Pb, Cd, Cr and Hg), but there existed significant difference in absorption capacity for different species to different pollutants. The measured tree species were classified into three categories by their absorption quantum of heavy metal pollutants. Among the species measured,Betula platyphylla, Ulmus pumila var.pendula, andPrunus persicaf.rubro-plena had high capacity in absorbing Pb;Populus xiahei, P. nigra var.Italica, P. alba x P. berolinensis andSalix matsudana had had high capacity in absorbing Cd;Phellodendron amurense, Syringa oblata, Salix matsudana, Pinus tabulaeformis var.mukdensis, Picea koraiensis, Prunus persica f.rubro-plena, P. triloba andAcer negundo, etc. had high capacity in absorption of Cr;Prunus triloba, Quercus mongolica, Salix matsudana, Sambucus williamsii, Pyrus ussuuriensis andSpiraea fritschiana were good at absorption of Hg. This study might offer scientific foundation for selection of urban afforestation species in different polluted conditions caused by heavy metals. Keywords Greening tree species - Heavy metal - Pollutants - Plumbum - Cadmium - Chromium - Mercury - Absorptivity CLC number S731.2 - X501 Document code A Foundation item: This study is financially supported by the Special Programme for Agriculture under Ministry of Chinese Science and Technology (No. 2002BA516A15-01).Biography: MU Li-qiang (1966-), female, Associate professor in Northeast Forestry University, Harbin 150040, P. R. China.Responsible editor: Zhu Hong
