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Multiple effects of nitrate amendment on the transport, transformation and bioavailability of antimony in a paddy soil-rice plant system

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Journal of Environmental Sciences 2021年第2期33卷 90-98页

作者： Xiaofeng Zhang Tongxu Liu Fangbai Li Xiaomin Li Yanhong Du Huanyun Yu Xiangqin Wang Chuanpin Liu MiFeng Bing Liao Guangzhou Institute of Geochemistry Chinese Academy of SciencesGuangzhou 510640China Guangdong key laboratory of Ilntegrated Agro-environmental pollution Control and Management GuangdongInstitute of Eco-environmental Science&TechnologyGuangzhou 510650China National-Regional Joint Engineering Research Center for Soil pollution Control and remediation in South China Guangzhou 510650China University of Chinese Academy of Sciences Beijing 100049China SCNU Enuironmental Research Institute Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety&MOE Key Laboratory of Theoretical Chemistry of EnvironmentSouth China NormalUniversityGuangzhou 510006China

Nitrate(NO3^(-))is known to be actively involved in the processes of mineralization and heavy metal transformation;however,it is unclear whether and how it affects the bioavailability of antimony(Sb)in paddy soils and subsequent Sb accumulation in rice.Here,the effects of NO3^(-)on Sb transformation in soil-rice system were investigated with pot experiments over the entire growth period.Results demonstrated that NO3^(-)reduced Sb accumulation in brown rice by 15.6%compared to that in the control.After amendment with NO3^(-),the Sb content in rice plants increased initially and then gradually decreased(in roots by 46.1%).During the first 15 days,the soil p H increased,the oxidation of Sb(Ⅲ)and sulfides was promoted,but the reduction of iron oxide minerals was inhibited,resulting in the release of adsorbed and organic-bound Sb from soil.The microbial arsenite-oxidizing marker gene aox B played an important role in Sb(Ⅲ)oxidation.From days 15 to 45,after NO3^(-)was partially consumed,the soil p H decreased,and the reductive dissolution of Fe(Ⅲ)-bearing minerals was enhanced;consequently,iron oxide-bound Sb was transformed into adsorbed and dissolved Sb species.After day 45,NO3^(-)was completely reduced,Sb(V)was evidently reduced to Sb(Ⅲ),and green rust was generated gradually.Thus,the available Sb decreased due to its enhanced affinity for iron oxides.Moreover,NO3^(-)inhibited the reductive dissolution of iron minerals,which ultimately caused low Sb availability.Therefore,NO3^(-)can chemically and biologically reduce the Sb availability in paddy soils and alleviate Sb accumulation inrice.This study provides a potential strategy for decreasing Sb accumulation in rice in the Sb-contaminated sites.

关键词： Antimony Nitrate Microbial Sb(Ⅲ)oxidation Rice Paddy soil

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钙钛矿上单原子位点实现高灵敏定量化表面拉曼增强

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Science China Materials 2022年第6期65卷 1601-1614页

作者：冯冉苗清张翔崔培昕王聪冯奕博甘立勇傅加兴王仕博戴子忆胡利明罗云敬孙伟海张小娴肖家文巫金波周冰朴邹明强何大伟周小元韩晓东 beijing key laboratory of Microstructure and Properties of Solids Institute of Microstructure and Property of Advanced MaterialsFaculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China key laboratory of Luminescence and Optical Information Ministry of EducationInstitute of Optoelectronic TechnologyBeijing Jiaotong UniversityBeijing 100044China College of Physics and Center for Quantum Materials and Devices Analytical and Testing CenterChongqing UniversityChongqing 401331China key laboratory of Soil Environment and pollution remediation Institute of Soil ScienceChinese Academy of SciencesNanjing 210008China Faculty of Environment and Life Beijing Key Laboratory of Environmental and OncologyBeijing University of TechnologyBeijing 100124China Materials Genome Institute Shanghai UniversityShanghai 200444China College of Materials science and Engineering Huaqiao UniversityXiamen 361021China Joint key laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoAvenida da UniversidadeTaipaMacao 999078China Chinese Academy of Inspection and Quarantine(CAIQ) Beijing 100123China

表面增强拉曼散射(SERS)是一种快速且无损的化学和生物分子检测技术.高灵敏且定量化的SERS检测技术对其在实际中的应用至关重要,尤其是对生物分子如氨基酸和碱基的便携化检测.但是鲜有技术手段能够实现对这些最基本的生物分子进行高灵... 详细信息

表面增强拉曼散射(SERS)是一种快速且无损的化学和生物分子检测技术.高灵敏且定量化的SERS检测技术对其在实际中的应用至关重要,尤其是对生物分子如氨基酸和碱基的便携化检测.但是鲜有技术手段能够实现对这些最基本的生物分子进行高灵敏且定量化的拉曼检测.我们提出了一种无需贵金属的单原子位点修饰芯片策略,用钨单原子氧化物修饰铅卤钙钛矿芯片,实现了多种检测物的高灵敏定量化识别,包括罗丹明、酪氨酸和胞嘧啶.芯片上单原子位点技术能够实现对罗丹明、酪氨酸和胞嘧啶的线性检测,相应的定量化区间分别为:10^(−6)–1 mmol L^(−1),0.06–1 mmol L^(−1)和0.2–45 mmol L^(−1),同时我们的拉曼增强芯片对这三种分子的增强因子在非等离子激元半导体中是最高的.我们通过实验测试结合理论模拟揭示了由可控单原子位点实现拉曼增强的机理:束缚由钙钛矿基底产生的光生电子,同时高效且定量地将这些电子转移到待测分子上.不仅如此,芯片上单原子位点技术可以在便携式拉曼设备下得到与台式拉曼设备类似的增强效果,这意味着这项技术有机会应用于多种生物分子的低成本、广谱、即时检测和体外检测.

关键词： SERS single-atom site point-of-care testing in-vitro diagnosis charge-transfer mechanism lead halide perovskite

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Influencing Factors and Product Toxicity of Anthracene Oxidation by Fungal Laccase

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Pedosphere 2014年第3期24卷 359-366页

作者： LI Xuan-Zhen CHENG Qian WU Yu-Cheng FENG You-Zhi LIU Wei-Wei LIN Xian-Gui key laboratory of Soil Environment and pollution remediation Institute of Soil Science Chinese Academy of Sciences State key laboratory of Soil and Sustainable Agriculture Institute of Soil Science Chinese Academy of Sciences Technology Center of China Tobacco Hebei industrial Co. Ltd.

The transformation profiles of polycyclic aromatic hydrocarbons(PAHs)by pure laccases from Trametes versicolor and Pycnoporus sanguineus,and the optimal reaction conditions(acetonitrile concentration,pH,temperature and incubation time)were determined.Anthracene was the most transformable PAH by both laccases,followed by benzo[a]pyrene,and benzo[a]anthracene.Laccase-mediator system(LMS)could not only improve the PAH oxidation but also extend the substrate types compared to laccase alone.5%or 10%(v/v)of acetonitrile concentration,pH 4,temperature of 40?C,and incubation time of 24 h were most favorable for anthracene oxidation by laccase from T.versicolor or P.sanguineus.The gas chromatography-mass spectrometry analysis indicated that 9,10-anthraquinone was the main product of anthracene transformed by laccase from T.versicolor.Microtox test results showed that both anthracene and its laccase-transformation products were not acute toxic compounds,suggesting that laccase-treatment of anthracene would not increase the acute toxicity of contaminated site.

关键词：真菌漆酶毒性测试蒽醌氧化影响因素苯并[a]芘产品 PAHs

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Immobilization of antimony in soil and groundwater using ferro-magnesium bimetallic organic frameworks

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Journal of Environmental Sciences 2023年第3期125卷 194-204页

作者： Le Yuan JianleWang Zuqi Zhong Jiguang Li Hong Deng School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Resource RecyclingSouth China University of TechnologyGuangzhou 510006China Guangxi key laboratory of Beibu Gulf Marine Biodiversity Conservation Beibu Gulf UniversityQinzhou 535000China Guangdong Engineering and Technology Research Center for Environmental Nanomaterials South China University of TechnologyGuangzhou 510006China

Sb(Ⅲ) is often detected in contaminated soil and groundwater. Hence, high-efficiency technology is needed. In this study, bimetallic organic frameworks were used for the first time to immobilize Sb(Ⅲ) from contaminated soil and groundwater. The materials were synthesized by the hydrothermal method. Both ends of the prepared material were hexagonal tip rods,and the length became shorter as the ratio of Fe/Mg decreased. The bimetallic organic framework with a Fe/Mg feeding ratio of 0.5 was the optimum material for Sb(Ⅲ) removal, which could effectively immobilize Sb(Ⅲ). The adsorption isotherm was fitted well with the Freundlich model, and the optimal adsorption capacity can reach 106.97 mg/g. The adsorption capacity of 84% can be completed in 10 min, which conformed to the pseudo-second-order kinetics. The Fe^(3+)could enhance the stability of the material, and the Mg^(2+)was conducive to freeing up adsorption sites for binding Sb(Ⅲ) and forming stable chemical adsorption. Ion exchange is the predominant mechanism to remove Sb(Ⅲ). After 14 days of remediation of Sb(Ⅲ) contaminated soil, the Toxicity Characteristic Leaching Procedure(TCLP)-leached concentrations of Sb(Ⅲ) were reduced by 86%, 91% and 94% when the material dosages were1%, 2% and 3%, respectively. Immobilization of Sb(Ⅲ) in soil resulted in a conversion of antimony speciation from more easily bioavailable species to less bioavailable species, further contributing to reduce the environmental risk of antimony. The results indicate that ferromagnesium bimetallic organic frameworks may serve as a kind of promising materials for the immobilization of Sb(Ⅲ) in contaminated soil and groundwater.

关键词： Antimony Ferro-magnesium bimetallic organic frameworks(MOFs) Soil Groundwater

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Active site identification and engineering during the dynamic evolution of copper-based catalysts for electrocatalytic CO_(2) reduction

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Science China Chemistry 2023年第1期66卷 78-95页

作者： Bangwei Deng Xueyang Zhao Yizhao Li Ming Huang Shihan Zhang Fan Dong Yangtze Delta Region Institute(Huzhou) University of Electronic Science and Technology of ChinaHuzhou 313001China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731China key laboratory of Microbial Technology for industrial pollution Control of Zhejiang Province College of EnvironmentZhejiang University of TechnologyHangzhou 310014China

To date,copper-based catalysts are one of the most prominent catalysts that can electrochemically reduce CO_(2)towards highvalue fuels or chemicals,such as ethylene,ethanol,and acetic acid.However,the chemically active feature of Cu-based catalysts hinders the understanding of the intrinsic catalytic active sites during the initial and the operative processes of electrochemical CO_(2)reduction(CO_(2)RR).The identification and engineering of active sites during the dynamic evolution of catalysts are thereby vital to further improve the activity,selectivity,and durability of Cu-based catalysts for high-performance CO_(2)RR.In this regard,four triggers for the dynamic evolution of catalysts were introduced in detail.Afterward,three typical active-site theories during the dynamic reconstruction of catalysts were discussed.In addition,the strategies in catalyst design were summarized according to the latest reports of Cu-based catalysts for CO_(2)RR,including the tuning of electronic structure,controlling of the external potential,and regulation of local catalytic environment.Finally,the conclusions and perspectives were provided to inspire more investigations and studies on the intrinsic active sites during the dynamic evolution of catalysts,which could promote the optimization of the catalyst system to further improve the performance of CO_(2)RR.

关键词： active site dynamic reconstruction copper-based catalysts electrochemical CO_(2)reduction local catalytic environment

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The effect of interaction between Bacillus subtilis DBM and soil minerals on Cu(Ⅱ) and Pb(Ⅱ) adsorption

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Journal of Environmental Sciences 2019年第4期31卷 328-337页

作者： Jun Bai Yuanqing Chao Yanmei Chen Shizhong Wang Rongliang Qiu School of Environmental Science and Engineering Sun Yat-sen University School of Public Health Southwest Medical University Guangdong Provincial key laboratory of Environmental pollution Control and remediation Technology Sun Yat-sen University Guangdong Provincial Engineering Research Center for Heavy Metal Contaminated Soil remediation Sun Yat-sen University

The effects of interaction between Bacillus subtilis DBM and soil minerals on Cu(Ⅱ)and Pb(Ⅱ)adsorption were investigated.After combination with DBM,the Cu(Ⅱ)and Pb(Ⅱ)adsorption capacities of kaolinite and goethite improved compared with the application of the minerals independently.The modeling results of potentiometric titration data proved that the site concentrations of kaolinite and goethite increased by 80%and 30%,respectively after combination with DBM.However,the involvement of functional groups in the DBM/mineral combinations resulted in lower concentrations of observed sites than the theoretical values and led to the enhancement of desorption rates by NH_4NO_3 and EDTA-Na_2.The DBM-mineral complexes might also help to prevent heavy metals from entering DBM cells to improve the survivability of DBM in heavy metal-contaminated environments.During the combination process,the extracellular proteins of DBM provided more binding sites for the minerals to absorb Cu(Ⅱ)and Pb(Ⅱ).In particular,an especially stable complexation site was formed between goethite and phosphodiester bonds from EPS to enhance the Pb(Ⅱ)adsorption capacity.So,we can conclude that the DBM–mineral complexes could improve the Cu(Ⅱ)and Pb(Ⅱ)adsorption capacities of minerals and protect DBM in heavy metal-contaminated environments.

关键词： Bacillus subtilis DBM Goethite Kaolinite Cu Pb

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Mn-doping induced electronic modulation and rich oxygen vacancies on vertically grown NiFe2O4 nanosheet array for synergistically triggering oxygen evolution reaction

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Nano Research 2022年第5期15卷 3940-3945页

作者： Yonghao Gan Meilin Cui Xiaoping Dai Ying Ye Fei Nie Ziteng Ren Xueli Yin Baoqiang Wu Yihua Cao Run Cai Xin Zhang State key laboratory of Heavy Oil Processing College of Chemical Engineering and EnvironmentChina University of PetroleumBeijing 102249China

Large-scale electrolysis of water to produce high-purity hydrogen is one of the effective ways to solve the energy crisis and environmental pollution problems.However,efficient,cheap and stable catalysts are one of the bottlenecks for industrial application in water splitting.Herein,a facile one-step hydrothermal process was applied to fabricate Mn-doped nickel ferrite nanosheets(Mn-NiFe_(2)O_(4))which shown a low overpotential of 200 mV at 50 mA·cm^(-2)and a small Tafel slope of 47 mV·dec^(-1),together with a prominent turnover frequency(TOF)value(0.14 s^(-1))and robust stability.The in-situ UV-vis spectroscopy unveiled the surface reconstruction to generate NiOOH as active sites during oxygen evolution reaction(OER).The excellent electrocatalytic activity of Mn-NiFe_(2)O_(4)is attributed to the vertically grown nanosheets for exposure more active sites,rich oxygen vacancies,and the hybridization between Ni 3d and O 2p orbitals caused by Mn doping.This work should provide a facile strategy by Mn-doping to simultaneously engineer oxygen vacancies and electronic structure for synergistically triggering oxygen evolution reaction.

关键词： Mn doping NiFe_(2)O_(4)nanosheets oxygen vacancies electronic modulation oxygen evolution reaction

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The role of organic and inorganic substituents of roxarsone determines its binding behavior and mechanisms onto nano-ferrihydrite colloidal particles

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Journal of Environmental Sciences 2023年第7期129卷 30-44页

作者： Ming Lei Yayuan Huang Yimin Zhou Caleb Oppong Mensah Dongning Wei Bingyu Li College of Resource&Environment Hunan Agricultural UniversityChangsha 410128China Hunan Engineering&Technology Research Center for Irrigation Water Purification Changsha 410128China key laboratory of Southern Farmland pollution Prevention and Control Ministry of AgricultureChangsha 410128China

The retention and fate of Roxarsone(ROX)onto typical reactive soil minerals were crucial for evaluating its potential environmental risk.However,the behavior and molecular-level reaction mechanism of ROX and its substituents with iron(hydr)oxides remains unclear.Herein,the binding behavior of ROX on ferrihydrite(Fh)was investigated through batch experiments and in-situ ATR-FTIR techniques.Our results demonstrated that Fh is an effective geo-sorbent for the retention of ROX.The pseudo-second-order kinetic and the Langmuir model successfully described the sorption process.The driving force for the binding of ROX on Fh was ascribed to the chemical adsorption,and the rate-limiting step is simultaneously dominated by intraparticle and film diffusion.Isotherms results revealed that the sorption of ROX onto Fh appeared in uniformly distributed monolayer adsorption sites.The twodimensional correlation spectroscopy and XPS results implied that the nitro,hydroxyl,and arsenate moiety of ROX molecules have participated in binding ROX onto Fh,signifying that the predominated mechanisms were attributed to the hydrogen bonding and surface complexation.Our results can help to better understand the ROX-mineral interactions at the molecular level and lay the foundation for exploring the degradation,transformation,and remediation technologies of ROX and structural analog pollutants in the environment.

关键词： Ferrihydrite 2D-COS Surface complexation Electrostatic interaction Roxarsone

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Revealing the effect of preparation parameters on zeolite adsorption performance for low and medium concentrations of ammonium

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Journal of Environmental Sciences 2019年第11期31卷 177-188页

作者： Wenyan He Hui Gong Kuo Fang Fei Peng Kaijun Wang State key Joint laboratory of Environment Simulation and pollution Control School of Environment Tsinghua University Beijing 100084China School of Water Resources & Environment China University of Geosciences Beijing 100083 China

The effect of preparation parameters on the performance of zeolite for ammonium (20-300 mg N/L) adsorption from simulated wastewater is reported.It was found that the ratios of Na2O/SiO2 and Si/Al had a more important influence than crystallization time on zeolite adsorption properties.Relatively low Na2O/SiO2 ratios were beneficial for fabrication of zeolites with high proportions of micropore area and volume,which led to the surface adsorption mechanism being dominated by surface free energy and pore effects.However,with decreasing Si/Al ratios,the effect of ion-exchange was more prominent due to the high negative surface potential of zeolite.In addition,the concentration of weak acid sites on the zeolites was increased with lower ratios of Na2O/SiO2 and Si/Al,which may promote ammonium removal.Therefore,the most effective zeolite for ammonium removal,which was fabricated at Na2O/SiO2 =1.375,Si/Al =4 and crystallization time of 48 hr,exhibited the cooperative effects of adsorption,ion-exchange and a large amount of weak acid sites.The maximum ammonium adsorption capacity (35.06 t 0.98 mg/g) and the removal efficiency (94.44%± 4.00%) were obtained at the dosage of 4.0 g/L zeolite NaX at ammonium concentrations of 300 mg N/L and 20 mg N/L,respectively.The Freundlich isotherm and pseudo-first-order kinetics models provided excellent fitting for the ammonium adsorption process.In addition,zeolite NaX showed about 1.23-3.2 times the ammonium adsorption capacity of clinoptilolite.The stable and efficient reusability of zeolite NaX after five regeneration cycles demonstrated that this adsorbent has considerable potential for practical industrial applications.

关键词： Zeolite synthesis Ammonium nitrogen removal Ion exchange Performance optimization

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Multiple assessments, source determination, and health risk apportionment of heavy metal(loid)s in the groundwater of the Shule River Basin in northwestern China

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Journal of Arid Land 2023年第11期15卷 1355-1375页

作者： WEN Xiaohu LI Leiming WU Jun LU Jian SHENG Danrui key laboratory of Ecological Safety and Sustainable Development in Arid Lands Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000China key laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources Qinghai Institute of Salt LakesChinese Academy of SciencesXining 810008China Yantai Research Institute Harbin Engineering UniversityYantai 264006China Shandong key laboratory of Coastal Environmental Processes/CAS key laboratory of Coastal Environmental Processes and Ecological remediation Chinese Academy of SciencesYantai 264003China

Global ecosystems and public health have been greatly impacted by the accumulation of heavy metal(loid)s in water.Source-specific risk apportionment is needed to prevent and manage potential groundwater contamination with heavy metal(loid)s.The heavy metal(loid)s contamination status,water quality,ecological risk,and health risk apportionment of the Shule River Basin groundwater are poorly understood.Therefore,field sampling was performed to explore the water quality and risk of heavy metal(loid)s in the groundwater of the Shule River Basin in northwestern China.A total of 96 samples were collected from the study area to acquire data for water quality and heavy metal(loid)s risk.There was noticeable accumulation of ferrum in the groundwater of the Shule River Basin.The levels of pollution were considered to be moderately low,as evaluated by the degree of contamination,heavy metal evaluation index,heavy metal pollution index,and Nemerow pollution index.The ecological risks were also low.However,an assessment of the water quality index revealed that only 58.34%of the groundwater samples had good water quality.The absolute principal component scores-multiple linear regression model was more suited for this study area than the positive matrix factorization model.There were no obvious noncarcinogenic or carcinogenic concerns for all types of receptors according to the values of the total hazard index and total carcinogenic risk.The human activities and the initial geological environment factor(65.85%)was the major source of noncarcinogenic risk(residential children:87.56%;residential adults:87.52%;recreational children:86.77%;and recreational adults:85.42%),while the industrial activity factor(16.36%)was the major source of carcinogenic risk(residential receptors:87.96%;and recreational receptors:68.73%).These findings provide fundamental and crucial information for reducing the health issues caused by heavy metal(loid)s contamination of groundwater in arid areas.

关键词： groundwater heavy metal(loid)s ecological risk health risk Shule River Basin

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