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N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2024年第4期25卷 340-356页

作者： Yong GUO Mengxia CHEN Ting CHEN Ying GUO Zixuan XU Guowei XU Soukthakhane SINSONESACK Keophoungeun KANMANY Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes Ministry of EducationCollege of EnvironmentHohai UniversityNanjing 210093China Key Laboratory of Environmental Engineering of Jiangsu Province Jiangsu Provincial Academy of Environmental ScienceNanjing 210036China State Key Laboratory of Pollution Control and Resource Reuse Nanjing UniversityNanjing 210023China Central Environmental Laboratory Natural Resources and Environment Research InstituteMinistry of Natural Resources and EnvironmentVientiane 999012Laos

We investigated the influence mechanism of N-doping for dissolved black carbon(DBC)photodegradation of organic pollutants.The degradation performance of N-doped dissolved black carbon(NDBC)for tetracycline(TC)(71%)is better than that for methylene blue(MB)(28%)under irradiation.These levels are both better than DBC degradation performances for TC(68%)and MB(18%)under irradiation.Reactive species quenching experiments suggest that h and-O,are the main reactive species for NDBC photodegraded TC,while-OH and h*are the main reactive species for NDBC photodegraded MB.-OH is not observed during DBC photodegradation of MB.This is likely because N-doping increases valence-band(VB)energy from 1.55 eV in DBC to 2.04 eV in NDBC;the latter is strong enough to oxidize water to form-OH.Additionally,N-doping increases the DBC band gap of 2.29 to 2.62 eV in NDBC,resulting in a higher separation efficiency of photo-generated electrons-holes in NDBC than in DBC.AIl these factors give NDBC stronger photodegradation performance for TC and MB than DBC.High-performance liquid chromatography-mass spectrometry(HPLC-MS)characterization and toxicity evaluation with the quantitative structure-activity relationship(QSAR)method suggest that TC photodegradation intermediates produced by NDBC have less aromatic structure and are less toxic than those produced by DBC.We adopted a theoretical approach to clarify the relationship between the surface groups of NDBC and the photoactive species produced.Our results add to the understanding of the photochemical behavior of NDBC.

关键词： Dissolved black carbon(DBC) N-doping organic pollutants Band gap Photodegradation

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Nanoscaled MnSnO_(2)@CsPbBr_(3) quantum dots heterostructure photocatalyst as efficient organic pollutants degradation by peroxymonosulfate;DFT calculation

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Journal of Materials Science & Technology 2023年第22期153卷 41-55页

作者： Raqiqa Tur Rasool Ghulam Abbas Ashraf Mohsin Pasha Muhammad Farooq Saleem Djamel Ghernaout Mohammed M.Fadhali Hai Guo Department of Physics Zhejiang Normal UniversityJinhuaZhejiang 321004China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China GBA branch of Aerospace Information Research Institute Chinese Academy of SciencesGuangzhou 510700China Chemical Engineering Department College of EngineeringUniversity of Ha’ilPO Box 2440Ha’il 81441Saudi Arabia Chemical Engineering Department Faculty of EngineeringUniversity of BlidaPO Box 270Blida 09000Algeria Department of Physics Faculty of ScienceJazan UniversityJazan 45142Saudi Arabia Department of Physics Faculty of ScienceIbb University 70270Yemen

In this work,we developed a promising photocatalyst in CsPbBr_(3) quantum dots(QDs)because of their exceptional optoelectronic characteristics.However,QDs applications in the field of photocatalysis were mainly hampered by their poor stability and insufficient charge transfer efficiency.Herein,a novel and efficient MnSnO_(2)@CsPbBr_(3)(MSO@QDs)nanocomposite was first time effectively designed and synthe-sized by a wet impregnation method for peroxymonosulfate(PMS)activation under the light.The newly generated interface phase of QDs between MnSnO_(2)(MSO)showed great potential to improve light ab-sorption,leading to effective separation and transfer of photoelectron-hole pairs.This novel nanocompos-ite MSO@QDs showed great Flurbiprofen(FL)removal efficiency under the PMS/Light system.It should be noted that this nanocomposite removed 85.74%of FL in just 70 min,which was almost 1.11 and 2.51 times greater than using pure QDs and pure MSO,respectively.Based on thorough measurements of structural analysis,Brunauer-Emmett-Teller(BET),UV-vis spectra,electrochemical impedance spec-troscopy(EIS),transient photocurrent response,and a potential mechanism for organic pollutants degra-dation over MSO@QDs nanocomposite was envisioned.The principal reactive species of photoinduced holes(h^(+)),i.e.O_(2)^(˙−),SO_(4)^(˙−),^(˙)OH,and non-radical(^(1)O_(2))were characterized via scavengers’technique and electron paramagnetic resonance(EPR)measurements.The highest photocatalytic performance for the re-moval of MO,MB,and IBU was demonstrated by MSO@QDs nanocomposite/PMS,revealing their excellent ability to remove organic pollutants through photo-oxidation.Furthermore,the developed nanocompos-ite exhibited good stability in an aqueous medium.According to computational investigation using the density functional theory(DFT)method,the site’s higher Fukui index f^(0) value corresponds to a greater propensity to be attacked by reactive species.This work offers a fresh perspective on developing further high-efficiency,low-cost photocatalys

关键词： CsPbBr_(3)QDs MnSnO_(2) Peroxymonosulfate Nanocomposite Photocatalyst organic pollutants DFT

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Multimedia distribution and health risk assessment of typical organic pollutants in a retired industrial park

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Frontiers of Environmental Science & Engineering 2023年第11期17卷 273-285页

作者： Shijin Wu Zijing Xiang Daohui Lin Lizhong Zhu Zhejiang Provincial Key Laboratory of organic Pollution Process and Control Department of Environmental ScienceZhejiang UniversityHangzhou 310058China Zhejiang Ecological Civilization Academy Anji 313300China

The overall cross-media risk evaluation of organic pollutants in retired industrial parks is insufficiently recognized.In this study,11 semi-volatile organic compounds(SVOCs)and 27 volatile organic compounds(VOCs)were measured in 531 soil and groundwater samples taken from a retired industrial park by coast in Zhejiang Province,China.Total petroleum hydrocarbons(TPHs),Di(2-ethylhexyl)phthalate(DEHP),benzene,and ethylbenzene were identified as the critical pollutants in the soil,while TPHs,1,2-dichloropropane(1,2-DCP),toluene,benzo[a]anthracene(BaA),and benzo[b]fluoranthene(BbF)were identified as critical pollutants in the groundwater for exceeding China national standards.The spatial correlation between the concentrations of organic pollutants in soil and groundwater was explored by employing the Geodetector model.Based on the results of spatial interpolation,high-risk hotspots regarding soil and groundwater pollution were identified.Moreover,the possible harm to human health of the critical pollutants were also under evaluation.Among various critical pollutants,benzene,ethylbenzene,and DEHP in soil,and 1,2-DCP in groundwater,were the main contributors to the overall health risk of multimedia pollution.This study developed a comprehensive approach to assess the risks posed by specific organic toxicants in various environmental media.The findings of this work can serve as a valuable reference for future management strategies in retired industrial parks.

关键词： organic pollutants Retired industrial park Spatial correlation Health risk assessment

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Catalytic degradation of organic pollutants for water remediation over Ag nanoparticles immobilized on amine-functionalized metalorganic frameworks

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Nano Research 2022年第9期15卷 7887-7895页

作者： Wen-Zhe Xiao Ling-Ping Xiao Yue-Qin Yang Shang-Ru Zhai Run-Cang Sun Liaoning Key Lab of Lignocellulose Chemistry and BioMaterials Liaoning Collaborative Innovation Center for Lignocellulosic BiorefineryCollege of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalian 116034China

Developing efficient catalysts for organic pollutants degradation is crucial for remediating the current severe water environment,yet remains a great challenge.Herein,we report silver nanoparticles immobilized on an amine-functionalized metal-organic framework(MOFs)(Ag/UiO-66-NH_(2))as a robust catalyst for the reduction of 4-nitrophenol(4-NP).The fabricated Ag/UiO-66-NH_(2)catalyst exhibits the merits of superior activities(high turnover frequency(TOF)3.2×10^(4)h^(-1)and k value 6.9×10^(-2)s^(-1)),costeffectiveness under the lowest NaBH4 concentration(n[NaBH_(4)]/n[4-NP],200),outstanding cyclability(10 recycling runs),and observable long-term durability,significantly outperforming previously reported catalytic system.The excellent degradation efficiency is ascribed to the favorable microenvironment modulation of unique MOF structure,which regulates the intrinsic properties of active sites and improves the electron-transfer process.Notably,the Ag/UiO-66-NH_(2)also promotes the catalytic degradation of several organic pollutants at room temperature and hence could find a broad application for water remediation.This work offers a new avenue for the development of high-performance MOF-based catalysts with excellent activity and durability.

关键词： Ag/UiO-66-NH_(2) catalytic degradation organic pollutants 4-nitrophenol water remediation

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Nanomaterial-based biosorbents:Adsorbent for efficient removal of selected organic pollutants from industrial wastewater

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Emerging Contaminants 2022年第1期8卷 46-58页

作者： Hussein.K.Okoro Sadanand Pandey Clement O.Ogunkunle Catherine J.Ngila C.Zvinowanda Ismaila Jimoh Isiaka A.Lawal Muyiwa M.Orosun Adewale George Adeniyi Analytical-Environmental Research Group Department of Industrial ChemistryFaculty of Physical SciencesP.M.B.1515University of IlorinPostal Code 240003IlorinNigeria Department of Chemistry College of Natural ScienceYeungnam University280 Daehak-RoGyeongsanGyeongbuk38541Republic of Korea Environmental Botany Unit Department of Plant BiologyUniversity of IlorinIlorinNigeria Analytical-Environmental and Membrane Nanotechnology Research Group Department of Chemical SciencesFaculty of ScienceUniversity of JohannesburgP.O.Box 17011Doornfontein2028JohannesburgSouth Africa Psychometrics Department JAMBNigeria Chemistry Department Faculty of Applied and Computer ScienceVaal University of Technology1900VanderbijlparkSouth Africa Health and Environmental Physics Research Group Physics DepartmentUniversity of IlorinIlorinNigeria The African Academy of Sciences P.O.Box 24916-00502 NairobiKenya Physical Address:8 Miotoni LaneKarenNairobiKenya Department of Chemical Engineering Faculty of EngineeringUniversity of IlorinPMB1515IlorinNigeria

The contamination of the environment by organic pollutants is a major risk factor,particularly for developing countries.Selected organic pollutants(SOPs)like the phenolic compounds,polyaromatic hydrocarbons(PAHs),pesticides,and herbicides pose serious environmental and health issues owing to their toxic characteristics and poor degradability.Apart from their potential mutagenicity,carcinogenicity,tetragenicity and high body accumulation,these pollutants have become an increase concern worldwide.Biosorption is a promising alternative strategy for removing organic pollutants during water purification processes.Biosorbents have several advantages such as simplicity of operation,good sorption capacity,high recoverability and modifiability.As a result,the focus and novelty of this review is on recent trends in the use of biosorbents,with a particular emphasis on the removal of SOPs from wastewater.It also cover use of bacteria biosorbents,fungal,algae and chitosan/chitin biosorbents.Apart from that,we have also reviewed various classes of SOPs,their levels in the environment,classification and available characteristics techniques suitable for the adsorption experiments of these nanocomposites materials.In addition,we have provided comprehensive explanations and conclusions on possible future application of biosorbents and the mechanism of adsorption of these materials for removal of these SOPs from wastewater during water purification processes.

关键词： Biosorbents Adsorption organic pollutants Biosorption Wastewater

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Design and synthesis of polyoxovanadate-based framework for efficient dye degradation

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Tungsten 2024年第2期6卷 447-453页

作者： Qing Lan Su-Juan Jin Zheng Wang Xu-Yang Li Yan Xiong Zhuo-Cheng Wang Shan-Shan Liu Zhi-Ming Zhang Qiang Zhao Engineering Technology Research Center of Henan Province for Solar Catalysis School of Chemical and Pharmaceutical EngineeringNanyang Normal UniversityNanyang 473061China Institute of New Energy Materials&Low Carbon Technology Tianjin University of TechnologyTianjin 300384China

A new polyoxovanadate-based framework material[Cu(en)_(2)]_(4)V_(18)O_(42)(H_(2)O)·6H_(2)O(1)was designed and synthesized by hydrothermal reaction of NaVO_(3),Cu(NO_(3))_(2)·6H_(2)O and 1,2-diaminoethane(en)via carefully adjusting the pH value of the reaction system.The structure of the title compound has been determined by single-crystal X-ray diff raction analysis,thermogravimetric analysis,infrared spectra and elemental analysis.Detail structural analysis demonstrate the three-dimensional(3D)framework structure of compound 1,which was composed of the[V_(18)O_(42)(H_(2)O)]_(8)−({V_(18)O_(42)(H_(2)O)})anions linked by the Cu^(2+)cations.Compound 1 represents the fi rst 3D framework based on{V_(18)O_(42)(H_(2)O)}polyoxoanions and copper complexes.Solar-driven degradation of residual organic pollutants in industrial wastewater is still a major problem for human beings.Photocatalytic experiments reveal that compound 1 possesses of excellent photocatalytic activity for the degradation of methylene blue and rhodamine B.

关键词： Polyoxovanadate Framework Polyoxovanadate-based framework Photocatalytic organic pollutants

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Zebrafish as a possible bioindicator of organic pollutants with effects on reproduction in drinking waters

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Journal of Environmental Sciences 2015年第7期27卷 254-260页

作者： M.Martínez-Sales F.García-Ximénez F.J.Espinós Aquaculture and Environmental Research Group (ACUMA) Polytechnic University of Valencia

organic contaminants can be detected at low concentrations in drinking water, raising concerns for human health, particularly in reproduction. In this respect, we attempted to use the zebrafish as a bioindicator to detect the possible presence of these substances in drinking water, aiming to define the most relevant parameters to detect these substances, which particularly affect the development and reproduction of zebrafish. To this end, batches of30 embryos with the chorion intact were cultured in drinking waters from different sources,throughout their full life-cycle up to 5 months, in 20 L tanks. Six replicates were performed in all water groups, with a total of 24 aquariums. Two generations（F0 and F1） were studied and the following parameters were tested： in the F0 generation, survival and abnormality rates evaluated at 5 dpf（days post-fertilization） and at 5 mpf（months post-fertilization）,the onset of spawning and the fertility rate from 3 mpf to 5 mpf, and the sex ratio and underdeveloped specimens at 5 mpf. Furthermore, in the F0 offspring（F1）, survival and abnormality rates were evaluated at 5 dpf and the hatching rate at 72 hpf. These results revealed that the hatching rate is the most sensitive parameter to distinguish different levels of effects between waters during the early life stages, whereas the rate of underdeveloped specimens is more suitable at later life stages. Regarding adult reproduction, fertility rate was the most sensitive parameter. The possible reversibility or accumulative nature of such effects will be studied in future work.

关键词： organic pollutants Bioindicator Development and reproduction parameters Drinking water Zebrafish

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Genotoxicity evaluation and a primary risk assessment of organic pollutants in the drinking water sources of Nanjing, China

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Journal of Environmental Sciences 2006年第5期18卷 983-988页

作者： LI Yi-qiang WU Yu-lin CHEN Yuan-gao KONG Zhi-ming The State Key Laboratory of Pollution Control and Resource Reuse School of Environmental Nanjing University Nanjing 210093 China National Accredited Laboratory Environmental Monitoring Center of Jiangsu Province Nanjing 210036 China

An increasing number of industrial, agricultural, and commercial chemicals in the aquatic environment leads to various deleterious effects on organisms, which is becoming an increasingly serious problem in China. In this study, the comet assay was conducted to investigate the genotoxicity to human body caused by organic concentrates in the drinking water sources of Nanjing City from Yangtze River of China, and health and ecology risk due to expose to these organic pollutants were evaluated with the multimedia environmental assessment system （MEAS）. For all the water samples, they were collected from four different locations in the drinking water sourcr samples, es of Nanjing City. The results of the comet assay showed that all the organic concentrates from the water samples could induce different levels DNA damages on human peripheral blood lymphocytes, and a statistically significant difference （p〈0.01） was observed compared with the solvent control, which demonstrated the genotoxicity was in existence. According to the ambient severity （AS） of individual compound, we had sorted out the main organic pollutants in the drinking water source of the four waterworks, and the results showed that there was some potential hazard to human body for all the source water, namely the total ambient severity （TAS） of health for each water source was more than 1. However, the TAS of ecology for each water source was less than 1, which indicated that it was safe to ecology. The results of this investigation demonstrate the application of the comet assay and the MEAS in aquatic environmental monitoring studies, and the comet assay found to be fast, sensitive, and suitable for genotoxicity monitoring programs of drinking water source.

关键词： genotoxicity comet assay risk assessment organic pollutants drinking water sources Nanjing City

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Piezoelectric materials for pollutants degradation: State-of-the-art accomplishments and prospects

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Chinese Chemical Letters 2024年第4期35卷 61-72页

作者： Yuqing Zhu Haohao Chen Li Wang Liqun Ye Houle Zhou Qintian Peng Huaiyong Zhu Yingping Huang College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002China Engineering Research Center of Eco-environment in Three Gorges Reservoir Region Ministry of EducationChina Three Gorges UniversityYichang 443002China College of Hydraulic&Environmental Engineering China Three Gorges UniversityYichang 443002China School of Chemistry and Physics Queensland University of TechnologyBrisbaneQLD 4001Australia

Piezoelectric catalysis, a new catalytic method, is widely used in the field of environmental sanitation, including waste water treatment and dye degradation. However, in the face of the growing environmental pollution problem, the efficiency of piezoelectric catalysis is still hampered by the stress variation in the natural environment. Therefore, it is particularly important to improve the catalytic efficiency of piezoelectric materials. We divide piezoelectric materials into two categories: inorganic piezoelectric materials and organic piezoelectric materials. Then the mainstream inorganic piezoelectric materials are divided into four subcategories, namely:(1) MTiO_(3)(M = Ba, Sr),(2) bi-class catalytic materials,(3) MoX_(2)(X = S,Se), and(4) ZnO piezoelectric materials. The mainstream organic piezoelectric materials are divided into PVDF and g-C_(3)N_(4)materials. At the same time, the above materials are summarized to explain the excellent performance of materials from the perspective of structure and piezoelectric principle. In addition,we summarized the modification methods that can be applied to piezoelectric materials:(1) Morphology methods,(2) composites with heterojunctions, and(3) surface modification. Finally, we summarized the prospects of piezoelectric materials in the field of environment and water treatment.

关键词： Ultrasound Cavitation Piezoelectric materials Degradation organic pollutants

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Fabrication of highly efficient Bi2WO6/CuS composite for visible-light photocatalytic removal of organic pollutants and Cr(VI)from wastewater

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Frontiers of Environmental Science & Engineering 2021年第4期15卷 85-97页

作者： Wei Mao Lixun Zhang Tianye Wang Yichen Bai Yuntao Guan Guangdong Provincial Engineering Technology Research Center for Urban Water Cycle and Water Environment Safety Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen518055China State Environmental Protection Key Laboratory of Microorganism Application and Risk Control School of EnvironmentTsinghua UniversityBeijing100084China College of Resources and Environment Jilin Agricultural UniversityChangchun130000China Key Laboratory of Soil Resource Sustainable Utilization for Jilin Province Commodity Grain Bases Changchun130118China

A visible-light-driven Bi_(2)WO_(6)/CuS p-n heterojunction was fabricated using an easy solvothermal method.The Bi_(2)WO_(6)/CuS exhibited high photocatalytic activity in a mixed system containing rhodamine B(RhB),tetracycline hydrochloride(TCH),and Cr(VI)under natural conditions.Approximately 98.8%of the RhB(10 mg/L),87.6%of the TCH(10 mg/L)and 95.1%of the Cr(VI)(15 mg/L)were simultaneously removed from a mixed solution within 105 min.The removal efficiencies of TCH and Cr(VI)increased by 12.9%and 20.4%,respectively,in the mixed solution,compared with the single solutions.This is mainly ascribed to the simultaneous consumption electrons and holes,which increases the amount of excited electrons/holes and enhances the separation efficiency of photogenerated electrons and holes.Bi_(2)WO_(6)/CuS can be applied over a wide pH range(2–6)with strong photocatalytic activity for RhB,TCH and Cr(VI).Coexisiting dissolved organic matter in the solution significantly promoted the removal of TCH(from 74.7%to 87.2%)and Cr(VI)(from 75.7%to 99.9%)because it accelerated the separation of electrons and holes by consuming holes as an electron acceptor.Removal mechanisms of RhB,TCH,and Cr(VI)were proposed,Bi_(2)WO_(6)/CuS was formed into a p-n heterojunction to efficiently separate and transfer photoelectrons and holes so as to drive photocatalytic reactions.Specifically,when reducing pollutants(e.g.,TCH)and oxidizing pollutants(e.g.,Cr(VI))coexist in wastewater,the p-n heterojunction in Bi_(2)WO_(6)/CuS acts as a“bridge”to shorten the electron transport and thus simultaneously increase the removal efficiencies of both types of pollutants.

关键词： Photocatalysis Bi_(2)W〇_(6)/CuS organic pollutants Cr(VI) Synergistic effect

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