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Metal-free diatomaceous carbon-based catalyst for ultrafast and anti-interference Fenton-like oxidation

Chinese Chemical Letters 2024年第12期35卷 351-355页

作者： Kexin Yin Jingren Yang Yanwei Li Qian Li Xing Xu Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityQingdao 266237China Environment Research Institute Shandong UniversityQingdao 266237China State Environmental Protection Key Laboratory of Environmental Health Impact Assessment of Emerging Contaminants Shanghai Academy of Environmental SciencesShanghai 200233China

Herein,a diatomite biomorphic Si-O doped carbon-based catalyst(DB-SiOC)was prepared using natura mineral diatomite as the silicon source and porous *** results showed that the metal-free DB SiOC catalyst exhibited ultrafast oxidation towards chlorophenol(CP)via peroxymonosulfate(PMS)activa tion,which was almost one order of magnitudes than most of carbon-based *** DB-SiOC/PMS system also showed the high ability to resist the interference of environmental *** radicals(^(·)OH and SO_(4)^(·–))exhibited a very small contribution to the CP oxidation while the electron transfer processe(ETP)played the major role in the DB-SiOC/PMS *** electron shuttles from the electron-donating CP molecules to the adjacent DB-SiOC/PMS^(*)could be efficiently triggered via Si-O bonds as bridges,mak ing it possible for ultrafast oxidation of *** addition,the hollow-disc shaped DB-Si OC provided the biomorphic DE structures with abundant pores for enriching the PMS and pollutants,thus further ac celerating the oxidation *** work provided a new routine for the fabrication of Si-O doped carbon-based catalysts with excellent Fenton-like catalytic activity,which would greatly promote thei application prospects in Fenton-like systems.

关键词： Peroxymonosulfate Diatomite Si-O doping Fenton-like reaction Electron transfer process(ETP)

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Confinement of Fe atoms between MoS_(2) interlayers drives phase transition for improved reactivity in Fenton-like reactions

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Nano Research 2024年第3期17卷 1132-1139页

作者： Yibing Sun Yu Zhou Hongchao Li Chuan Wang Xuan Zhang Qian Ma Yingchun Cheng Jieshu Qian Bingcai Pan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China Key Laboratory of Flexible Electronics and Institute of Advanced Materials Jiangsu National Synergetic Innovation Center for Advanced MaterialsNanjing Tech UniversityNanjing 211816China Department of General Dentistry Affiliated Stomatological Hospital of Nanjing Medical UniversityJiangsu Province Key Laboratory of Oral DiseasesNanjing 210029China Research Center for Environmental Nanotechnology(ReCENT) State Key Laboratory of Pollution Control and Resources ReuseSchool of EnvironmentNanjing UniversityNanjing 210023China

Phase manipulation of MoS_(2) from thermodynamically stable 2H phase to the unstable but more reactive 1T phase represents a crucial strategy for improving the reactivity in many *** widely adopted wet chemistry approach uses intercalating entities especially alkali metal ions to achieve the phase transition;however,these entities are normally inert for the target ***,we describe the first use of iron atoms for the intercalation of 2H-MoS_(2) layers,driving the partial transition from 2H to 1T ***,in the peroxymonosulfate(PMS)-based Fenton-like reactions,the interlayered confinement of Fe atoms not only activates the inert basal plane,but also adds more reactive Fe sites for the formation of metal-PMS complex as primary reactive species for pollutant *** the degradation of a model pollutant carbamazepine(CBZ),the Fe-intercalated MoS_(2) exhibits a first order rate constant 13.3 times higher than 2H-MoS_(2).This strategy is a new direction for manipulating the phase composition and boosting the catalytic reactivity of MoS_(2)-based catalysts in various scenarios,including environmental remediation and energy applications.

关键词： confinement MoS_(2) Fe atoms Fenton-like reactions hydrogen evolution reaction

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Selective dissolution to synthesize densely populated Pt single atom catalyst

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Nano Research 2023年第1期16卷 219-227页

作者： Weinan Yang Xiaoguang Zhao Ya Wang Rong Wang Wenhao Yang Yue Peng Junhua Li State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Sinopec Research Institute of Petroleum Processing Beijing 100083China

Single atom catalysts(SACs)have become one of research focuses in heterogeneous catalysis for their effective utilization of active metal atoms and unique properties in various catalytic ***,due to their high surface energy,noble metal single atoms like Pt tend to migrate and agglomerate to form larger clusters or nanoparticles,which makes it a challenge to fabricate noble metal SACs with high loading(>5 wt.%).Furthermore,the decisive factors of loading maximum are still not ***,we reported a manganese oxide supported Pt SAC with a high loading of 5.6 wt.%synthesized by selective dissolution *** pre-stabilization of Pt by coordinated oxygen and the abundant surface defects of support are the determinants of high *** Pt SAC exhibited much better H_(2)spill-over and hydrocarbon oxidation abilities with lower adsorption and dissociation energies than the manganese oxide support because of its local electronic structure with less repulsion.

关键词： manganese oxide selective dissolution single-atom catalysis hydrogen spill-over propene oxidation

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Synthesis of Ce/BiFeO_(3)composites and activation of persulfate for pharmaceutical wastewater degradation

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Journal of Rare Earths 2025年第3期43卷 462-469,I0002页

作者： Yanting Zuo Shi Cheng Ziwen Guo Haolin Liu Huaicheng Zhang Ji Wu Ziwu Fan Wentao Li Aimin Li Key Laboratory of Taihu Basin Water Resources Management Ministry of Water ResourcesNanjing Hydraulic Research InstituteNanjing 210029China School of Urban Construction Changzhou UniversityChangzhou 213164China School of Resources and Environmental Engineering Jiangsu University of TechnologyChangzhou 213001China State Key Laboratory of Pollution Control and Resources Reuse School of the EnvironmentNanjing UniversityNanjing 210023China School of Environment and Safety Engineering Nanjing Polytechnic InstituteNanjing 210048China

Sulfamethoxazole(SMZ)is a prevalent and recalcitrant micropollutant in water,posing a significant threat to both aquatic organisms and human ***,investigating the removal of SMZ is of critical *** order to investigate the effect of rare earth metal doping on the performance of activated persulfate oxidative degradation of SMZ,BiFeO_(3)with different Ce doping amounts was successfully prepared by a hydrothermal ***,it was characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),scanning transmission electro n microscopy(STEM)and Brunauer-Emmett-Teller(BET)*** performance of porous Ce/BiFeO_(3)in the catalytic activation of persulfate(PMS)for the degradation of SMZ in water was investigated using SMZ solution as a simulated *** impact of Ce doping rate,catalyst dosage,temperature variations,common anions,natural organic matter,and PMS concentration on SMZ removal was systematically *** characterization results show that the octahedral rhombic structure of Ce can be observed on the surface of this doped catalyst,and Ce doping does not change the crystalline shape of Ce/BiFeO_(3).The specific surface area of the doped catalyst increases,accompanied by an enlargement of pore size,thereby enhancing the catalyst's adsorption capacity and resistance to contamination by *** the optimal conditions of 25℃,SMZ concentration of 20 mg/L,0.8 g/L PMS and 0.3 g/L 0.05Ce/BiFeO_(3)catalyst,the removal rate of SMZ reaches approximately 95%within35 min of reaction *** after five cycles of reuse,the degradation rate of SMZ remains above 88%,demonstrating the catalyst's good stability and *** experiments show that SO_(4)^(·-),·OH,1O_(2)and O_(2)^(·-)are involved in the catalytic degradation process,with 1O_(2)playing a dominant role.

关键词： Ce/BiFeO_(3) Persulfate Sulfamethoxazole Sulfate radicals Rare earths

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Simultaneous determination of dissolved organic nitrogen, nitrite, nitrate and ammonia using size exclusion chromatography coupled with nitrogen detector

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Journal of environmental Sciences 2023年第3期125卷 309-318页

作者： Wen-Xiang Ji Ye-Chao Tian Min-Hui Cai Bi-Cun Jiang Shi Cheng Yan Li Qing Zhou Bo-Qiang Li Bai-Yang Chen Xing Zheng Wen-Tao Li Ai-Min Li State Key Laboratory of Pollution Control and Resources Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Shenzhen Key Laboratory of Organic Pollution Prevention and Control Harbin Institute of Technology(Shenzhen)Shenzhen 518055China State Key Laboratory of Eco-hydraulics in Northwest Arid Region Xi’an University of TechnologyXi’an 710048China Quanzhou Institute for Environmental Protection Industry Nanjing UniversityQuanzhou 362008China

Accurate quantification of dissolved organic nitrogen(DON) has been a challenge due to the cumulative analytical errors in the conventional method via subtracting dissolved inorganic nitrogen species(DIN) from total dissolved nitrogen(TDN). Size exclusion chromatography coupled with an organic nitrogen detector(SEC-OND) has been developed as a direct method for quantification and characterization of DON. However, the applications of SECOND method still subject to poor separations between DON and DIN species and unsatisfied N recoveries of macromolecules. In this study, we packed a series of SEC columns with different lengths and resin materials for separation of different N species and designed an independent vacuum ultraviolet(VUV) oxidation device for complete oxidation converting N species to nitrate. To guarantee sufficient N recoveries, the operation conditions were optimized as oxidation time ≥ 30 min, injection mass(sample concentration × injection volume) < 1000 μL × mg-N/L for macromolecular proteins, and neutral p H mobile eluent. The dissolved O_(2)concentration in SEC mobile phase determined the upper limit of VUV oxidation at a specific oxidation time. Compared to conventional HW50S column(20 × 250 mm),HW40S column(20 × 350 mm) with mobile phase comprising of 1.5 g/L Na2HPO_(4)·2H_(2)O + 2.5g/L KH_(2)PO_(4)(p H = 6.85) could achieve a better separation of DON, nitrite, nitrate, and ammonia. When applied to river water, lake water, wastewater effluent, groundwater, and landfill leachate, the SEC-OND method could quantify DON as well as DIN species accurately and conveniently even the DIN/TDN ratio reached 0.98.

关键词： Size exclusion chromatography Nitrogen detector Dissolved organic nitrogen Nitrate Nitrite Ammonia

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Synergy of sodium doping and nitrogen defects in carbon nitride for promoted photocatalytic synthesis of hydrogen peroxide

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Chinese Chemical Letters 2024年第8期35卷 324-329页

作者： Fabrice Nelly Habarugira Ducheng Yao Wei Miao Chengcheng Chu Zhong Chen Shun Mao College of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource ReuseTongji UniversityShanghai 200092China Baowu Water Technology Co. Ltd.Research InstituteShanghai 201999China

Photocatalytic synthesis of hydrogen peroxide has gradually become a promising method for in-situ pro-duction of hydrogen peroxide,which relies on sustainable solar ***,the commonly used photocatalyst,i.e.,carbon nitride(CN),still suffers from the drawbacks of narrow light absorption range and fast charge ***,we report a facile method to introduce nitrogen defects into carbon nitride together with sodium *** adjusting the ratio of sodium dicyandiamide,the band gap of carbon nitride can be controlled,while the carrier separation and transfer ability of carbon nitride is *** modified CN with sodium doping and nitrogen defect(SD-CN)demonstrates outstanding H_(2)O_(2)pro-duction performance(H_(2)O_(2)yield rate of 297.2μmol L^(−1)h^(−1))under visible light irradiation,which is approximately 9.8 times higher than that of pristine *** work deepens the understanding of the coordinated effect of structural defect and element doping of carbon nitride on the photocatalytic H_(2)O_(2)production performance,and provides new insight into the design of photocatalytic system for efficient production of H_(2)O_(2).

关键词： Photocatalysis H_(2)O_(2)evolution Sodium doping Nitrogen defect Metal-free catalyst

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A bacteria-based index of biotic integrity indicates aquatic ecosystem restoration

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environmental Science and Ecotechnology 2024年第6期22卷 178-190页

作者： Qi Liu Senlu Yin Yujun Yi School of Environment Beijing Normal UniversityBeijing 100875China State Key Laboratory of Water Environment Simulation and Pollution Control Beijing Normal UniversityBeijing 100875China

Intensive ecological interventions have been carried out in highly polluted shallow lakes to improve their environments and restore their ***,certain treatments,such as dredging polluted sediment and stocking fish,can impact the aquatic communities,including benthos and *** impacts can alter the composition and characteristics of aquatic communities,which makes community-based ecological assessments *** we develop a bacteria-based index of biotic integrity(IBI)that can clearly indicate the restoration of aquatic ecosystems with minimal artificial *** applied this method to a restored shallow lake during 3-year intensive ecological *** interventions reduced nutrients and heavy metals by 27.1%and 16.7%in the sediment,while the total organic carbon(TOC)increased by 8.0%due to the proliferation of ***,the abundance of sulfur-related metabolic pathways decreased by 10.5%as the responses to improved *** score of bacteria-based IBI,which is calculated based on the diversity,composition,and function of benthic bacterial communities,increased from 0.62 in 2018 to 0.81 in *** study not only provides an applicable method for aquatic ecological assessment under intensive artificial interventions but also extends the application of IBI to complex application scenarios,such as ecosystems with significantly different aquatic communities and comparisons between different basins.

关键词： Baiyangdian lake 16S rRNA Benthic bacterial community Ecological restoration Aquatic ecological assessment

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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 *** 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 ***,the comprehensive effect of antibiotic wastewater on AR development has rarely been evaluated,and its treatment efficiency remains ***,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 *** 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 *** against ampicillin and *** may be attributed to the inhibition effect and oxidative stress of cephalosporin wastewater on *** 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 *** indicates that the antibiotic wastewater treatment had a collaborative processing effect of conventional pollutants,toxicity,and the AR induction *** 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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Enhancing ozone catalytic decomposition through acid treatment ofα-MnO_(2) for improved activity and humidity resistance

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Journal of environmental Sciences 2025年第3期149卷 35-45页

作者： Shangchao Xiong Kai Zhang Zhenghao Xu Hongjun Ou Yuanyuan Zheng Xi Li Yue Peng Xubiao Luo Junhua Li School of Life Sciences Jinggangshan UniversityJi’an 343009China Faculty of Geosciences and Environmental Engineering Southwest Jiaotong UniversityChengdu 610031China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China

Post-etching method using dilute acid solutions is an effective technology to modulate the surface compositions of metal-oxide *** theα-MnO_(2) catalyst treated with 0.1 mol/L nitric acid exhibits higher ozone decomposition activity at high relative humidity than the counterpart treated with acetic *** the increases in surface area and lattice dislocation,the improved activity can be due to relatively higher Mn valence on the surface and newly-formed Brønsted acid sites adjacent to oxygen *** remnant nitro species deposited on the catalyst by nitric acid treatment is ideal hydrophobic groups at ambient *** decomposition route is also proposed based on the DRIFTS and DFT calculations:ozone is facile to adsorb on the oxygen vacancy,and the protonic H of Brønsted acid sites bonds to the terminal oxygen of ozone to accelerate its cleavage to O_(2),reducing the reaction energy barrier of O_(2) desorption.

关键词： Ozone decomposition α-MnO_(2) Brønsted acid sites H-bonds Post-etching

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Uncovering the coupling effect with energy-related carbon emissions and human development variety in Chinese provinces

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Journal of environmental Sciences 2024年第5期139卷 527-542页

作者： Liu Chen Yiqi Tan Gengpei Lv Weiguang Cai Xiaofeng Gao Rui Li School of Management Science and Real Estate Chongqing UniversityChongqing 400044China State Key Joint Laboratory of Environment Simulation and Pollution Control(SKLESPC) School of EnvironmentTsinghua UniversityBeijing 100084China Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment Ministry of EducationCollege of Environment and EcologyChongqing UniversityChongqing 400044China

Lessening energy-related carbon emissions has become a crucial measure to achieve Chinese carbon *** study is the first to construct a Difference in Carbon pressures-adjusted Human Development Index(DCHDI)model for the purpose of exploring the coupling effect between carbon emissions and human development variety from 2000 to 2019 in Chinese *** demonstrate the following.(1)The total energy-related carbon footprint of 30 provinces in China reached 10.2 billion tons in 2019,with an average annual growth rate of 6.93% over the past two decades;and the provinces with the highest carbon emissions per capita are InnerMongolia,Ningxia,and Shanxi.(2)At the provincial level,we observed that the Human Development Index(HDI),which includes life expectancy,education,and income,has been rising,while Beijing,Shanghai,and Tianjin entered the super-high HDI level before 2008.(3)The entire coupling effect of 30 Chinese provinces has been broadly fortified in the last 20 years,but the growth rate of DCHDI values in 2011-2019 has slowed down compared with that in 2000-2010;the clustering phenomenon demonstrated that this discovery is associated with historical peaks in total carbon emissions.(4)The co-ordination degree of carbon emissions per capita and HDI was verified,and 96% of the data points were found in the range of super high coupling coordination ***,this study provides the government with worthwhile guidance for decision-making and carbon reduction strategies for other countries struggling to advance human sustainable development.

关键词： Energy-related carbon emissions Human sustainable development DCHDI model Coupling effect Chinese provinces

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