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Comprehensive study on the spatial distribution of heavy metals and their environmental risks in high-sulfur coal gangue dumps in China

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Journal of Environmental Sciences 2024年第2期136卷 486-497页

作者： Yingbo Dong Huan Lu Hai Lin School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China beijing key laboratory on resource-oriented treatment of industrial pollutants Beijing 100083China

The accumulation of coal gangue(CG)from coal mining is an important source of heavy metals(HMs)in soil.Its spatial distribution and environment risk assessment are extremely important for the management and remediation of HMs.Eighty soil samples were collected from the high-sulfur CG site in northern China and analyzed for six HMs.The results showed that the soil was heavily contaminated by Mn,Cr and Ni based on the Nemerow index,and posed seriously ecological risk depended on the geo-accumulation index,potential ecological risk index and risk assessment code.The semi-variogram model and ordinary kriging interpolation accurately portrayed the spatial distribution of HMs.Fe,Mn,and Cr were distributed by band diffusion,Ni was distributed by core,the distribution of Cu had obvious patchiness and Zn was more uniform.The spatial autocorrelation indicated that all HMs had strong spatial heterogeneity.The BCR sequential extraction was employed to qualify the geochemical fractions of HMs.The data indicated that Fe and Cr were dominated by residual fraction;Cu,Ni and Zn were dominated by reducible and oxidizable fractions;Mn was dominated by reducible and acid-extractable(25.38%-44.67%)fractions.Pearson correlation analysis showed that pH was the main control factor affecting the non-residue fractions of HMs.Therefore,acid production from high sulfur CG reduced soil pH by 2-3,which indirectly promoted the activity of HMs.Finally,the conceptual model of HMs contamination at the CG site was proposed,which can be useful for the development of ecological remediation strategies.

关键词： High-sulfur coal gangue Soil contamination Heavy metals Spatial distribution Geochemical fractions Risk assessment

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Research progress on metal-organic framework compounds(MOFs)in electrocatalysis

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Journal of Environmental Sciences 2024年第7期141卷 261-276页

作者： Yutong Guo Shunzheng Zhao Xiaolong Tang Honghong Yi Department of Environmental Science and Engineering School of Energy and Environmental EngineeringUniversity of Science and Technology BeijingBeijing 100083China beijing key laboratory of resource-oriented treatment of industrial pollutants Beijing 100083China

Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attractive prospects in the research area of modern materials electrocatalysis.However,unsatisfactory catalytic activity and poor electronic conductivity are the main challenges facing MOFs.This review focuses on MOF-based materials used in electrocatalysis,based on the types of catalytic reactions that have used MOF-based materials in recent years along with their applications,and also looks at some new electrocatalytic materials and their future development prospects.

关键词： Metal-organic frame compounds Electrocatalysis Oxidation-reduction Nitrogen fixation to synthesize ammonia Carbon dioxide reduction

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A combined evaluation of the characteristics and antibiotic resistance induction potential of antibiotic wastewater during the treatment process

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Journal of Environmental Sciences 2024年第4期138卷 626-636页

作者： Sun Miao Yanyan Zhang Cong Men Yiou Mao Jiane Zuo State key Joint laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China School of Energy and Environmental Engineering Beijing Key Laboratory of Resource-Oriented Treatment of Industrial PollutantsUniversity of Science and Technology BeijingBeijing 100083China High School Affiliated to Renmin University of China Beijing 100080China Tsinghua Shenzhen International Graduate School Shenzhen 518055China

Antibiotic wastewater contains a variety of pollutant stressors that can induce and promote antibiotic resistance(AR)when released into the environment.Although these substances are mostly in concentrations lower than those known to induce AR individually,it is possible that antibiotic wastewater discharge might still promote the AR transmission risk via additive or synergistic effects.However,the comprehensive effect of antibiotic wastewater on AR development has rarely been evaluated,and its treatment efficiency remains unknown.Here,samples were collected from different stages of a cephalosporin production wastewater treatment plant,and the potential AR induction effect of their chemical mixtures was explored through the exposure of the antibiotic-sensitive Escherichia coli K12 strain.Incubation with raw cephalosporin production wastewater significantly promoted mutation rates(3.6×10^(3)-9.3×10^(3)-fold)and minimum inhibition concentrations(6.0-6.7-fold)of E.coli against ampicillin and chloramphenicol.This may be attributed to the inhibition effect and oxidative stress of cephalosporin wastewater on E.coli.The AR induction effect of cephalosporin wastewater decreased after the coagulation sedimentation treatment and was completely removed after the full treatment process.A Pearson correlation analysis revealed that the reduction in the AR induction effect had a strong positive correlation with the removal of organics and biological toxicity.This indicates that the antibiotic wastewater treatment had a collaborative processing effect of conventional pollutants,toxicity,and the AR induction effect.This study illustrates the potential AR transmission risk of antibiotic wastewater and highlights the need for its adequate treatment.

关键词： Antibiotic wastewater treatment plant Antibiotic resistance Antibiotic resistance induction effect Correlation analysis Biological toxicity

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Degradation of o-dichlorobenzene by DBD-NTP co-modified titanium gel catalyst

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Journal of Environmental Sciences 2024年第9期143卷 71-84页

作者： Wenbo Zhang Yi Xing Wei Su Jiaqing Wang Haoqi Jia Yongkang Cui Jing Chen Hui Zhang School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China beijing key laboratory of resource-oriented treatment of industrial pollutants University of Science and Technology BeijingBeijing 100083China Guangdong Province Engineering laboratory for Air Pollution Control Guangzhou 510530China College of Environmental and resource Sciences Shanxi UniversityTaiyuan 030006China Sinosteel Maanshan Mine Research Institute Co.Ltd. Anhui 243071China

In order to study the degradation process of dioxins in industrial flue gas,the decomposition of o-dichlorobenzene(o-DCB)in a DBD plasma catalytic reactor was investigated.The results showed that an NTP-catalyzed system,especially using the Cu Mn Ti Oxcatalyst,had better o-DCB degradation performance compared to plasma alone.The combination of the Cu Mn Ti Oxcatalyst with NTP can achieve a degradation efficiency of up to 97.2%for o-DCB;the selectivity of CO and CO_(2)and the carbon balance were 40%,45%,and 85%,respectively.The dielectric constant and electrical property results indicated that the surface discharge capacity of the catalysts played a major role in the degradation of o-DCB,and a higher dielectric constant could suppress the plasma expansion and enhance the duration of the plasma discharge per discharge cycle.According to the O1s XPS and O_(2)-TPD results,the conversion of CO to CO_(2)follows the M-v-K mechanism;thus,the active species on the catalyst surface play an important role.Moreover,the Cu Mn Ti Oxand NTP mixed system exhibited excellent stability,which is probably because Cu doping improved the lifetime of the catalyst.This work can provide an experimental and theoretical basis for research in the degradation of o-DCB by plasma catalyst systems.

关键词： o-dichlorobenzene(o-DCB) Non-thermal plasma catalysis Ozone concentration

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Bioleaching of vanadium from stone coal vanadium ore by Bacillus mucilaginosus:Influencing factors and mechanism

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International Journal of Minerals,Metallurgy and Materials 2024年第8期31卷 1828-1838页

作者： Yingbo Dong Jinyu Zan Hai Lin School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China beijing key laboratory on resource-oriented treatment of industrial pollutants Beijing 100083China

Vanadium and its derivatives are used in various industries,including steel,metallurgy,pharmaceuticals,and aerospace engineering.Although China has massive reserves of stone coal resources,these resources have low grades.Therefore,the effective extraction and recovery of metallic vanadium from stone coal is an important way to realize the efficient resource utilization of stone coal vanadium ore.Herein,Bacillus mucilaginosus was selected as the leaching strain.The vanadium leaching rate reached 35.5%after 20 d of bioleaching under optimal operating conditions.The cumulative vanadium leaching rate in the contact group reached 35.5%,which was higher than that in the noncontact group(9.3%).The metabolites of B.mucilaginosus,such as oxalic,tartaric,citric,and malic acids,dominated in bioleaching,accounting for 73.8%of the vanadium leaching rate.Interestingly,during leaching,the presence of stone coal stimulated the expression of carbonic anhydrase in bacterial cells,and enzyme activity increased by 1.335-1.905 U.Enzyme activity positively promoted the production of metabolite organic acids,and total organic acid content increased by 39.31 mg·L^(-1),resulting in a reduction of 2.51 in the pH of the leaching system with stone coal.This effect favored the leaching of vanadium from stone coal.Atomic force microscopy illustrated that bacterial leaching exacerbated corrosion on the surface of stone coal beyond 10 nm.Our study provides a clear and promising strategy for exploring the bioleaching mechanism from the perspective of microbial enzyme activity and metabolites.

关键词： Bacillus mucilaginosus stone coal vanadium ore bioleaching carbonic anhydrase organic acids

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Low-temperature NH_(3)-SCR performance of a novel Chlorella@Mn composite denitrification catalyst

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Journal of Environmental Sciences 2024年第3期137卷 271-286页

作者： Hengheng Liu Fengyu Gao Songjin Ko Ning Luo Xiaolong Tang Erhong Duan Honghong Yi Yuansong Zhou School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China beijing key laboratory of resource-oriented treatment of industrial pollutants Beijing 100083China School of Environmental Science and Engineering University of Science and Technology HebeiHebei 050018China Department of Chemistry Pyongyang University of ArchitecturePyongyangDemocratic People’s Republic of Korea

The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive.In this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification catalyst was innovatively synthesized by electrostatic interaction.The Chlorella@Mn composite denitrification catalyst prepared under the optimal conditions(0.54 g/L Mn^(2+)concentration,20 million chlorellas/mL concentration,450℃ calcination temperature)exhibited a well-developed pore structure and large specific surface area(122 m^(2)/g).Compared with MnOx alone,the Chlorella@Mn composite catalyst achieved superior performance,with~100%NH_(3)selective catalytic reduction(NH_(3)-SCR)denitrification activity at 100-225℃.The results of NH_(3)temperature-programmed desorption(NH_(3)-TPD)and H_(2)temperature-programmed reduction(H_(2)-TPR)showed that the catalyst had strong acid sites and good redox properties.Zeta potential testing showed that the electronegativity of the chlorella cell surface could be used to enrich with Mn^(2+).X-ray photoelectron spectroscopy(XPS)confirmed that Chlorella@Mn had a high content of Mn^(3+)and surface chemisorbed oxygen.In-situ diffuse refectance infrared Fourier transform spectroscopy(in-situ DRIFTS)experimental results showed that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms play a role in the denitrification process on the surface of the Chlorella@Mn catalyst,where the main intermediate nitrate species is monodentate nitrite.The presence of SO_(2)promoted the generation and strengthening of Bronsted acid sites,but also generated more sulfate species on the surface,thereby reducing the denitrification activity of the Chlorella@Mn catalyst.The Chlorella@Mn composite catalyst had the characteristics of short preparation time,simple process and low cost,making it promising for industrial application.

关键词： Chlorella@Mn catalyst NH_(3)-SCR Poisoning resistance Reaction mechanism Infuence of SO_(2)

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Oligomeric donor with appropriate crystallinity for organic solar cells

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Chinese Chemical Letters 2024年第2期35卷 289-294页

作者： Kaiming Yang Min Lv Yanhong Chang Kun Lu Zhixiang Wei CAS key laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Department of Environmental Science and Engineering University of Science and Technology BeijingBeijing 100083China beijing key laboratory of resource treatment of Typical industrial pollutants Beijing 100083China

Improving the performance of all-small-molecule organic solar cells(ASM-OSCs)largely depends on the design and application of novel donors with appropriate crystallinity.Extending molecular conjugation is an effective method for regulating molecular stacking and crystallinity.In this work,we successfully designed and synthesized two novel acceptor-donor-donor-donor-acceptor(A-D-D-D-A)type oligomeric donors with three dithieno[2,3-d:2′,3′-d′]benzo[1,2-b:4,5-b']dithiophene(DTBDT)as the central unit,named as 3DTBDT-Cl and 3DTBDT,depending on with and without chlorine substitution on the thiophene side chains.We found that the introduction of chlorine atoms makes the blend films display stronger crystallinity but with large-scale phase separation morphology and more defects,which eventually leads to a power conversion efficiency(PCE)of only 10.83%,whereas the blend films based 3DTBDT with appropriate crystallinity achieved 13.74%PCE.Compared with 3DTBDT-Cl/L8-BO,the 3DTBDT/L8-BO films exhibited a nanoscale bi-continuous interpenetrating network morphology with a smaller domain size and more suitable crystallinity,which guarantees the corresponding devices obtained more efficient exciton dissociation,efficient charge transport,reduced bimolecular recombination,and performed more balanced carrier mobility.These results demonstrated that regulating the crystallinity of oligomeric donors to obtain the desired phase separation morphology in the blend films could facilitate further improving the performance of ASM-OSCs.

关键词： Linked donor unit Oligomeric donors Crystallinity regulation Organic solar cells

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Comparative analysis of DNA-SIP and magnetic-nanoparticle mediated isolation (MMI) on unraveling dimethoate degraders

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Frontiers of Environmental Science & Engineering 2024年第1期18卷 59-69页

作者： Luning Lian Yi Xing Dayi Zhang Longfei Jiang Mengke Song Bo Jiang School of Energy and Environmental Engineering University of Science&Technology BeijingBeijing 100083China beijing key laboratory of resource-oriented treatment of industrial pollutants University of Science&Technology BeijingBeijing 100083China National Environmental and Energy Science and Technology International Cooperation Base University of Science&Technology BeijingBeijing 100083China College of New Energy and Environment Jilin UniversityChangchun 130021China Guangzhou Institute of Geochemistry Chinese Academy of SciencesGuangzhou 510640China College of Natural resources and Environment South China Agricultural UniversityGuangzhou 510642China National Engineering laboratory for Site Remediation Technologies Beijing 100015China

Microorganisms are crucial in the bioremediation of organophosphorus pesticides. However, most functional microorganisms (> 99%) are yet to be cultivated. This study applied two cultivation-independent approaches, DNA-SIP and magnetic-nanoparticle mediated isolation (MMI), to identify the functional microorganisms in degrading dimethoate in agricultural soils. MMI identified five dimethoate degraders: Pseudomonas, Bacillus, Ramlibacter, Arthrobacter, and Rhodococcus, whereas DNA-SIP identified three dimethoate degraders: Ramlibacter, Arthrobacter, and Rhodococcus. Also, MMI showed higher resolution than DNA-SIP in identifying functional microorganisms. Two organic phosphohydrolase (OPH) genes: ophC2 and ophB, were involved in dimethoate metabolism, as revealed by DNA-SIP and MMI. The degradation products of dimethoate include omethoate, O,O,S-trimethyl thiophosphorothioate, N-methyl-2-sulfanylacetamide, O,O-diethyl S-hydrogen phosphorodithioate, O,O,O-trimethyl thiophosphate, O,O,S-trimethyl thiophosphorodithioate, and O,O,O-trimethyl phosphoric. This study emphasizes the feasibility of using SIP and MMI to explore the functional dimethoate degraders, expanding our knowledge of microbial resources with cultivation-independent approaches.

关键词： Stable isotope probing(SIP) Magnetic-nanoparticle mediated isolation(MMI) Dimethoate Biodegradation Cultivation-independent approach

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Metagenomic insights into microorganisms and antibiotic resistance genes of waste antibiotic fermentation residues along production,storage and treatment processes

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Journal of Environmental Sciences 2024年第2期136卷 45-55页

作者： Ziming Han Xiao Luan Haodi Feng Yanqin Deng Min Yang Yu Zhang State key laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China National Engineering Research Center of industrial Wastewater Detoxication and resource Recovery Beijing 100085China Wuhan Agricultural Inspection Center Wuhan 430016China University of Chinese Academy of Sciences Beijing 100049China

Antibiotic fermentation residue(AFR)is nutrient-rich solid waste generated from fermentative antibiotic production process.It is demonstrated that AFR contains high-concentration of remaining antibiotics,and thus may promote antibiotic resistance development in receiving environment or feeding farmed animals.However,the dominate microorganisms and antibiotic resistance genes(ARGs)in AFRs have not been adequately explored,hampering understanding on the potential antibiotic resistance risk development caused by AFRs.Herein,seven kinds of representative AFRs along their production,storage,and treatment processes were collected,and multiple methods including amplicon sequencing,metagenomic sequencing,and bioinformatic approaches were adopted to explore the biological characteristics of AFRs.As expected,antibiotic fermentation producer was found as the predominant species in raw AFRs,which were collected at the outlet of fermentation tanks.However,except for producer species,more environment-derived species persisted in stored AFRs,which were temporarily stored at a semi-open space.Lactobacillus genus,classified as Firmicutes phylum and Bacilli class,became predominant bacterial taxa in stored AFRs,which might attribute to its tolerance to high concentration of antibiotics.Results from metagenomic sequencing together with assembly and binning approaches showed that these newly-colonizing species(e.g.,Lactobacillus genus)tended to carry ARGs conferring resistance to the remaining antibiotic.However,after thermal treatment,remaining antibiotic could be efficiently removed from AFRs,and microorganisms together with DNA could be strongly destroyed.In sum,the main risk from the AFRs was the remaining antibiotic,while environment-derived bacteria which tolerate extreme environment,survived in ARFs with high content antibiotics,and may carry ARGs.Thus,hydrothermal or other harmless treatment technologies are recommended to remove antibiotic content and inactivate bacteria before recycling of AFRs in pharmaceutical industry.

关键词： Pharmaceutical manufacturing Antibiotic mycelia residue Antibiotic resistance bacteria Thermal treatment Solid waste

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Metal-based inorganic nanocrystals for biological sonodynamic therapy applications:recent progress and perspectives

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Rare Metals 2024年第2期43卷 413-430页

作者： Dong Wang Jia-Tao Zhang Institute of Medical-industrial Integration Beijing Key Laboratory of Structurally Controllable Advanced Functional Materials and Green ApplicationsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing100081China key laboratory of Medical Molecule Science and Pharmaceutics Engineering Ministry of Industry and Information TechnologySchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing100081China

With the fast development of technology for the treatment of tumor and bacteria,photo-therapeutic strate-gies emerge as a kind of highly effective and common treatment,but the low tissue penetration depth of light limits their development.Sonodynamic therapy(SDT),as an efficient and non-invasive treatment,attracts more people's attention due to the inherent property of high tissue penetration.The soft tissue penetration depth of ultrasound(US)can even reach more than 10 cm,which has great advantage over that of light.Therefore,many sonosensitizers are studied and applied to SDT-based therapy.Metal-based inorganic nanocrystals are able to generate more reactive oxygen species(ROS)due to the special composition and band structure.The representative achievements and the specific functions of the nanocrystals sonosensitizers are summarized in this work,and the relationship of structure/composition-SDT performance and the internally regulated composite is revealed.Syner-gistic effects of SDT in combination with other therapeutic modalities are mainly highlighted.At the same time,the critical and potential issues and future perspectives are addressed.

关键词： Metal-based inorganic nanocrystals Sonodynamic therapy(SDT) Tumor treatment Antibacteria

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