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Solid Bronsted acidity boosts adsorption reactivity of nano-adsorbent for water decontamination

Frontiers of Environmental Science & Engineering 2024年第7期18卷 23-34页

作者： Sikai Cheng Zhixian Li Kaisheng Zhang Qingrui Zhang Xiaolin Zhang Bingcai Pan State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Environmental Materials and Pollution Control Laboratory Institute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031China State Key Laboratory of Metastable Materials Science and Technology Yanshan UniversityQinhuangdao 066004China Hebei Key Laboratory of Heavy Metal Deep-remediation in Water and Resource Reused Qinhuangdao 066004China Research Center for Environmental Nanotechnology(ReCENT) Nanjing UniversityNanjing 210023China

Despite the development of various Lewis acidic nano-adsorbents for fluoride removal through innersphere coordination,strong competition for hydroxyl ions still hinders efficient water *** addition,the critical issue of polysilicate scaling that results from the ubiquitous silicates must be *** tackle these issues,an alternative approach to enhancing adsorption reactivity by modifying nano-adsorbents with dual Lewis and Bronsted acidity is *** feasibility of this approach is demonstrated by growing zirconium phosphate(ZrP)inside a gel-type anion exchanger,N201,to produce nanocomposite ZrP@N201,in which the confined ZrP contained an otherwise metastable amorphous phase with Lewis acidic Zr^(4+) sites and Bronsted acidic monohydrogen phosphate groups(-O_(3)POH).Compared with the Lewis acidic nano-zirconium oxide analog(HZ0@N201),ZrP@N201 exhibited a greatly improved adsorption capacity(117.9 vs.52.3 mg/g-Zr)and mass transfer rate(3.56×10^(-6) vs.4.55×10^(-7) cm/s),while bulk ZrP produced a thermodynamically stableα-phase with Bronsted acidity that exhibited negligible adsorption capability toward *** enhanced defluoridation activity of ZrP@N201 is attributed to Bronsted acidity and the increased outer electron density of ZA+sites,as corroborated using XPS and solid-state NMR ***,Bronsted acidity strengthens the resistance of ZrP@N201 to silicate,allowing its full regeneration during cyclic *** tests demonstrated 3-10 times the amount of clean water from(waste)for ZrP@N201 as compared to both HZO@N201 and the widely used activated aluminum *** study highlights the potential of developing nano-adsorbents with dual acidities for various environmental remediation applications.

关键词： Nanocomposite Selective adsorption Fluoride removal Dual Lewis and Bronsted acidity Regeneration

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Variations in redox properties of biochar and humic acid induced by interactive molecular exchange

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Carbon Research 2024年第1期3卷 1-13页

作者： Li, Shasha He, Pinjing Zhang, Hua Shao, Liming Lü, Fan State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China Institute of Waste Treatment and Reclamation Tongji University Shanghai200092 China

Biochar and humic substances are prevalent redox pools in the environment, which is critical to electron transfer in geochemical cycles and pollution control processes. The dissolution of biochar and the sorption of humic substances on biochar have the potential to redistribute redox substances, consequently altering the redox properties of solid and liquid phases. However, studies have often focused on either sorption or dissolution separately, overlooking the mutual effects and not involving redox properties. Herein, molecular interactions between biochar and humic acid (HA) and variations in their redox properties were elucidated using UPLC Orbitrap MS and mediated electrochemical measurement. The dissolution of biochar was far greater than the sorption of HA constituents, and HA enhanced the dissolution of biochar through molecular exchange. But preferential sorption of oxygenated aromatics to pine char (pi500) mainly by hydrogen bonding and higher saturated molecules to starch char (st700) mainly by hydrophobic interactions caused the oxygenated functional groups on biochar to increase (1 ~ 1.5 times). Thus the Electron exchange capacities (EEC) of pi500 and st700 turned to 1 ~ 3 times, and the EEC of HA decreased ca. 50%. Absorption (partition) caused more sorption of HA constituents to pi500 than to st700, while larger surface area resulted in higher EEC of st700 with sorbed HA. The enrichment of redox constituents on biochar is promising for its long-term use in waste reclamation and pollution control. The findings can aid in the understanding of variations in redox properties under interactions between pyrolytic and natural organic matter. Graphical Abstract: (Figure presented.) © The Author(s) 2024.

关键词： Hydrogen bonds

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Synergy of metal-support interaction and positive Pd species promoting efficient C-CI bond activation on Pd-based Ce-MOF-derived catalysts

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Rare Metals 2024年第11期43卷 5835-5847页

作者： Xiao-Jie Hu Yu-Han Sun Ling-Yue Liu Dan-Jun Mao Shou-Rong Zheng State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHong Kong 999077Hong KongChina

Monochloroacetic acid(MCAA)is identified as a highly carcinogenic disinfection by-product in chlorinated drinking *** this study,a series of CeO_(2)-supported Pd catalysts(Pd/MCeO_(2))were synthesized through one-step calcination of Pd-loaded Ce-UiO-66-BDC(CeMOF),and the liquid-phase catalytic hydrodechlorination of MCA A was explored using these *** comparison,Pd/CeO_(2)catalysts were additionally synthesized using the conventional impregnation *** characterization results reveal that the catalysts exhibit strong metal-support interaction,leading to high Pd dispersion and Pd^(n+)***,the calcination temperature significantly influences catalytic performance,with the catalyst calcined at 500℃(Pd/MCeO_(2)-500)demonstrating the highest catalytic activity and achieving complete dechlorination of MCA A within 50 ***,it is found that the catalytic MCAA hydrodechlorination using the catalysts adheres to the Langmuir-Hinshelwood ***,low reaction pH is favorable for the catalytic hydrodechlorination of MCAA,enhancing MCAA adsorption on the catalyst surface due to the electrostatic interaction between MCAA and the catalyst *** results suggest that the presence of Pd^(n+)efficiently facilitates MCAA adsorption and C-Cl cleavage,thus significantly enhancing the liquid-phase catalytic hydrodechlorination.

关键词： Ce-UiO-66-BDC One-step calcination Metal-support interaction Liquid-phase catalytic hydrodechlorination Monochloroacetic acid

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Identification of key precursors contributing to the formation of CX_(3)R-type disinfection by-products along the typical full-scale drinking water treatment processes

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Journal of Environmental Sciences 2023年第6期128卷 81-92页

作者： Xu Yang Shunke Ding Rong Xiao PinWang Zhenqi Du Ruihua Zhang Wenhai Chu State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Ministry of Education Key Laboratory of Yangtze River Water Environment Tongji UniversityShanghai 200092China

Identification and characterization of disinfection by-product(DBP)precursors could help optimize drinkingwater treatment processes and improve the quality of *** study comprehensively investigated the characteristics of dissolved organic matter(DOM),the hydrophilicity and molecule weight(MW)of DBP precursor and DBP-associated toxicity along the typical full-scale treatment *** results showed that dissolved organic carbon and dissolved organic nitrogen content,the fluorescence intensity and the SUVA254 value in raw water significantly decreased after the whole treatment *** treatment processes were in favor of the removal of high-MW and hydrophobic DOM,which are important precursors of trihalomethane and haloacetic *** with conventional treatment processes,Ozone integrated with biological activated carbon(O3-BAC)processes enhanced the removal efficiencies of DOM with different MW and hydrophobic fractions,leading to a further decrease in almost all DBP formation potential and DBP-associated ***,almost 50%of the detected DBP precursors in raw water has not been removed after the coagulation-sedimentation-filtration integrated with O3-BAC advanced treatment *** remaining precursors were found to be mainly hydrophilic and low-MW(<1.0 kDa)***,they would largely contribute to the formation of haloacetaldehydes and haloacetonitriles,which dominated the calculated *** current drinking water treatment process could not effectively control the highly toxic DBPs,the removal of hydrophilic and low-MW organics in drinking water treatment plants should be focused on in the future.

关键词： Disinfection by-products Drinking water Characterization key precursor Hydrophilicity MW distribution

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Identification of high oxygen-consuming substances in stormwater drainage systems illicitly connected with sewage system

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Journal of Environmental Sciences 2024年第4期138卷 132-140页

作者： Chen Xu Zuxin Xu Wenhai Chu Shanshan Wu Rong Xiao Lei Su State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Ministry of Education Key Laboratory of Yangtze River Water Environment Tongji UniversityShanghai 200092China Guangzhou Resource Environmental Protection Technology Co. Ltd.Guangzhou 510030China

The dissolved oxygen content in water is an important indicator for assessing the quality of the water environment,and maintaining a certain amount of dissolved oxygen is essential for the healthy development of the ecological *** a water body is anoxic,the activity of anaerobic microorganisms increases and organic matter is decomposed to produce a large number of blackening and odorizing substances,resulting in black and odorous water bodies,which is a very common and typical phenomenon in ***,there is still a relatively universal occurrence of illicitly connected stormwater and sewage pipes in the urban drainage pipe network in China,which makes oxygen-consuming substances be directly discharged into rivers through stormwater pipes and consume the dissolved oxygen in the water bodies,resulting in an oxygen deficiency of the *** induces seasonal or year-round black and stink phenomena in urban ***,identifying high oxygen-consuming substances,which lays the foundation for the subsequent removal of oxygen-consuming substances,is *** a series of comparisons of water quality indicators and analysis of organic characteristics,it was found that the oxygen consumption capacity of domestic sewage was higher than that of industrial wastewater in the selected area of this study,and the oxygen-consuming substances of domestic sewage were small molecular amino *** comparing 20 conventional free amino acids,it was found that seven of them consumed oxygen easily,and compared with chemical oxygen consumption,biological oxygen consumption was in a leading position.

关键词： Urban drainage system Oxygen-consuming substances Domestic sewage Amino acid

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Urban sprawl and its effects on water competition between building industry and residents: Evidence from 31 provinces in China

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Water-Energy Nexus 2024年第1期7卷 26-38页

作者： Ding, Yu Jia, Ling Wang, Chenglong Wang, Peng Faculty of Civil Engineering and Mechanics Jiangsu University Zhenjiang212013 China State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing210023 China

With accelerated urban sprawl, water scarcity and increased water stress have become global issues. Water of building industry and domestic water are two major contributors to total water consumption that cannot be ignored. This paper seeks to emphasize the effects of urban sprawl on water competition between building industry and residents. To achieve this objective, a framework for quantifying the water usage of the life cycle of the building was first constructed. Additionally, the degree of urban sprawl and water competition between domestic and building industry was computed. This study characterized the evolution path of urban sprawl and water competition using standard deviation ellipse. Spatial econometric models were used to determine the impact of urban sprawl on water competition. The results indicate that there is a high spatial correlation between urban sprawl and water competition. The center of gravity of China's urban sprawl is consistent with the north-to-south movement of water competition. As economic sprawl increases by 1%, water competition will rise by 0.440%. As the population expands by 1%, the water competition index shifts by 0.018%. Moreover, 0.017% more water was used for every 1% increase in land sprawl. © 2023

关键词： Competition

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Assessing comparable bioconcentration potentials for nanoparticles in aquatic organisms via combined utilization of machine learning and toxicokinetic models

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SmartMat 2023年第3期4卷 70-83页

作者： Shipeng Dong Zihao Wu Mingjie Wang Xiaoyan Sun Liang Mao State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjingChina Nanjing Qixia District Hospital NanjingChina

The toxicokinetic(TK)model‐derived kinetic bioconcentration factor(BCFk)provides a quantitatively comparable index to estimate the bioaccumulation potential of nanoparticles(NPs)that barely reach thermodynamic equilibrium in aquatic organisms,but experimental data are limited for various *** the present study,a machine learning model was applied to offer reliable in silico predictions for the dynamic body burden of diverse NPs to derive corresponding parameters for the TK *** developed eXtreme Gradient Boosting‐derived TK(XGB‐TK)model was applied to predict BCFk results for a broad range of metallic or carbonaceous NPs,with an appreciable prediction R2 of *** BCFk values were predicted based on a random combination of selected variable features,revealing that their bioaccumulation potential showed an overall negative correlation with NP density or organism *** applying importance analysis and partial dependence plots,NP density and organism size were revealed to be the top essential features that impact the bioaccumulation *** conjunctively used XGB‐TK model enabled a prior comparison for diverse NPs and straightforward derivation on the dependency of features,which could also guide the bioaccumulation mechanism exploration and experimental condition formulation.

关键词： aquatic organism BCF bioaccumulation machine learning nanoparticles toxicokinetic models

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Nonmicrobial mechanisms dominate the release of CO_(2)and the decomposition of organic matter during the short-term redox process in paddy soil slurry

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Eco-Environment & Health 2023年第4期2卷 227-234页

作者： Jinsong Liu Changyin Zhu Xiantang Liu Xiaolei Wang Dongmei Zhou State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China

Both biotic and abiotic mechanisms play a role in soil CO_(2)emission ***,abiotically mediated CO_(2)emission and the role of reactive oxygen species are still poorly understood in paddy *** study revealed thatOH promoted CO_(2)emission in paddy soil slurries during short-term oxidation(4 h).OH generation was highly hinged on active Fe(II)content,and theOH contribution to CO_(2)efflux was 10%–33%in topsoil and 40%–77%in deep-soil *** CO_(2)efflux was higher in topsoil slurries,which contained more dissolved organic carbon(DOC).CO_(2)efflux correlated well with DOC contents,suggesting the critical role of *** mechanisms contributed 9%–45%to CO_(2)production,as estimated byγ-ray sterilization experiments in the short-term reoxidation ***-aqueous separation experiments showed a significant reduction in net CO_(2)efflux across all soil slurries after the removal of the original aqueous phase,indicating that the water phase was the main source of CO_(2)emission(>50%).Besides,C emission was greatly affected by pH fluctuation in acidic soil but not in neutral/alkaline *** transform ion cyclotron resonance mass spectrometry and excitation-emission matrix results indicated that recalcitrant and macromolecular dissolved organic matter(DOM)components were more easily removed or attacked by·*** decrease in DOM content during the short-term reoxidation was the combined result of ·OH oxidation,co-precipitation,and soil organic matter *** study emphasizes the significance of the generally overlooked nonmicrobial mechanisms in promoting CO_(2)emission in the global C cycle,and the critical influence of the aqueous phase on C loss in paddy environments.

关键词： Soil Dissolved organic matter Abiotically mediated CO_(2)emission Reactive oxygen species

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Microstructure-Dependent Ion Selectivity in Graphene Oxide-Based Membranes

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ACS Applied Materials and Interfaces 2025年第22期17卷 32806-32815页

作者： Ren, Jing Chen, Xinran Tong, Xin State Key Laboratory of Pollution Control and Resource Reuse Shanghai Institute of Pollution Control and Ecological Security Tongji Advanced Membrane Technology Center School of Environmental Science and Engineering Tongji University 1239 Siping Road Shanghai200092 China

Graphene oxide (GO) membranes hold promise for precise separation due to their unique laminar structures and tunable separation properties. However, although water transport in GO membranes has been extensively investigated, the key mechanisms governing ion transport and selectivity remain poorly understood. In this work, we fabricated pristine and propylenediamine (PPD)/pentamethylenediamine (PTD)-cross-linked GO membranes via vacuum filtration and employed low-field nuclear magnetic resonance (LF-NMR) to elucidate their nanoscale pore architectures, including pinholes and structural defects. Our results show that cross-linking leads to a more ordered arrangement of the nanochannels and reduces the dimensions of structural defects. Ion diffusion experiments demonstrated that the membrane microstructure plays a crucial role in determining the tortuosity of the ion transport pathways. Notably, large structural defects dominate ion transport;when present, ions tend to bypass the interlayer nanochannels, leading to reduced ion selectivity. In contrast, intrinsic pinholes are too small to significantly contribute to ion transport. Molecular dynamics simulations showed that interlayer spacing, ion properties, and interactions with the membrane jointly govern ion diffusion within the GO-based nanochannels. More importantly, the simulation results deviated from experimental observations, further implying the pivotal role of large structural defects in ion transport. These findings provide valuable guidelines for designing next-generation GO-based membranes with improved ion selectivity and performance for precise separation. © 2025 American Chemical Society.

关键词： Crosslinking

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Simultaneous Degradation, Dehalogenation, and Detoxification of Halogenated Antibiotics by Carbon Dioxide Radical Anions

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Engineering 2024年第6期37卷 78-86页

作者： Yanzhou Ding Xia Yu Shuguang Lyu Huajun Zhen Wentao Zhao Cheng Peng Jiaxi Wang Yiwen Zhu Chengfei Zhu Lei Zhou Qian Sui State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process School of Resources and Environmental EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Academy of Environmental Sciences Shanghai 200233China

Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of *** moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification *** address these limitations of AOPs,advanced reduction processes(ARPs)have been ***,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated *** results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of *** detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based *** identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real ***,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halog

关键词： Carbon dioxide radical anions Advanced reduction processes Halogenated antibiotics Dehalogenation Detoxification

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