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Application of Sulfidated Microscale Zero Valent Iron to Degrade 1,1,2,2-Tetrachloroethane in Water and Soil

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SSRN 2021年

作者： Fan, Bo Li, Xiaoshuai Wang, Jiahao Hu, Jianhua Gong, Zhimin Shao, Shuai Zhu, Changyin Zhou, Dongmei Gao, Shixiang State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing210023 China

1,1,2,2-tetrachloroethane (1,1,2,2-TeCA) is a toxic chlorinated hydrocarbon that is commonly found in industrial wastewater, groundwater and soil environments. In this study, sulfidated microscale zero valent iron (S-mZVI) was prepared for the reductive degradation of 1,1,2,2-TeCA under ambient aerobic conditions. The results showed that S-mZVI could effectively degrade 1,1,2,2-TeCA and its dehydrochlorinated product trichloroethylene (TCE) in aqueous solution at pH ranging from 6 to 8, and was also more powerful in degrading the dichloroethylene products than untreated microscale zero valent iron (mZVI). The degradation rate of 1,1,2,2-TeCA increased with increasing S/Fe molar ratio (0.01-0.2) and reaction temperature (25-60°C). Further study found that S-mZVI not only performed as reductant to induce dechlorination, but also could activate oxygen to produce oxidative free radical hydroxyl radicals (such as • OH and O 2 •- ). Finally, the degradation of 1,1,2,2-TeCA and its byproducts in acidic and alkaline soils was examined, with nearly complete degradation being achieved within 24 h under S-mZVI and 50℃ conditions. This study provides valuable information for the practical application of S-mZVI in the remediation of halogenated hydrocarbon contaminated waters and soils. © 2021, The Authors. All rights reserved.

关键词： Degradation

Evolutional Solid Phase and Solid-Liquid Interface Uranium Immobilization Mechanisms by Nanoscale Zero-Valent Iron and Enhanced Uranium Stability control Strategy

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SSRN 2022年

作者： Hua, Yilong Li, Donghan Zou, Jinglan Wang, Wei Wu, Xiaoyan Zhang, Xiaowen Liu, Qing Zhao, Guodong Li, Mi Zhang, Wei-Xian Yang, Jianping School of Resource Environment and Safety Engineering University of South China Hunan Hengyang421001 China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Shanghai201620 China United Laboratory of Heavy Metal Pollution Control and Resource Reuse University of South China Hunan Hengyang421001 China Hunan Key Laboratory of Pollution Control and Resource Reuse University of South China Hunan Hengyang421001 China State Key Laboratory of Pollution Control College of Environmental Science and Engineering Tongji University Shanghai200092 China

Uranium is a carbon dioxide free nuclear energy, and uranium-contained wastewater poses serious chronic health effects toward human. Nanoscale zero-valent iron (nZVI) separates uranium from wastewater with ultrafast kinetic, high capacity and selectivity. However, the dynamic interfacial uranium binding mechanisms and its stability, controlled by the phase transformation of nZVI, is important but poorly understood. After a long-term reaction, the fresh nZVI was oxidized and transfromed to ferrihydrite and then lepidocrocite and hematite. Analysis for the structures and valence states of U, Fe species indicated that the dominate U(VI) uptake mechanism changed from Fe 0 induced reduction to adsorption as nZVI transformed to iron (oxyhydr)oxides. Density functional theory calculation revealed that uranyl formed corner-sharing configurations on the surface of iron nanoparticles, and some uranium ions prefer to incorporate into the structure of lepidocrocite than hematite during the crystallization processes of ferrihydrite. Meanwhile, 100~10000 μg/L uranyl ions were quickly captured, the residual uranium could be maintained at ~9.31 μg/L and the content of uranium in reacted iron nanoparticles reached ~24.16 wt%. Interestingly, the oxidization reduction potential (E h ) was a potential parameter to control uranium immobilization in the CSTR system, and the E h control strategy could be used to increase the fraction of U(IV)/U(V), sparingly soluble and highly stable, higher than 90%. The findings augment our understanding of U-nZVI reactions and guide nZVI technology to remedy real uranium-contained wastewater. © 2022, The Authors. All rights reserved.

关键词： Hematite

Nanoconfined Hydrated Zirconium Oxides for Improved Adsorption of Arsenate: Surface Complexation Modeling Study

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SSRN 2023年

作者： Shen, Pengfei Pan, Siyuan Huang, Xianfeng Zhang, Xiaolin State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China Nanjing University Nanjing210023 China National and Local Joint Engineering Research Center for Ecological Treatment Technology of Urban Water Pollution School of Life and Environmental Science Wenzhou University Wenzhou325035 China

Nanoscale hydrated zirconium oxide (HZO) holds great potential in groundwater purification due to its ability to form inner-sphere coordination with arsenate. Despite being frequently encapsulated inside bulky hosts, the adsorption mechanism of arsenate onto HZO, including the intrinsic coordination constants (Kintr) and the effects of nanoconfinement, remains scantily explored. In this study, we investigated the Zr-As coordination configuration and corresponding Kintr values using surface complexation modeling (SCM), and distinguished the nanoconfinement effects by comparing bare HZO with the HZO nanoparticles (NPs) encapsulated inside the strongly basic anion exchanger D201. Both samples share a similar crystalline amorphous structure and surface site density (~6 mmol/g-Zr). Potentiometric titration suggests that the protonated form (≡ZrOH2+) is the dominant surface Zr species, and D201 enhances the protonation degree by reducing electrostatic repulsion to H+. Batch adsorption experiments demonstrate that the nanocomposite (HZO@D201) has a higher adsorption capacity in a wide range of pH (3-10) and ionic strength (0.001-0.1 M NaNO3) than bare HZO. SCM simulations reveal that the coordination configuration of diprotonated monodentate mononuclear (MM-H2) dominates at pH 3-6, while deprotonated bidentate binuclear (BB-H0) dominates at pH>7. For each configuration, the Kintr values of HZO@D201 (10−0.66 and 10−16.10, respectively) are significantly higher than those of bare HZO (10−12.24 and 10−44.42, respectively), indicating a superior chemical bonding affinity caused by nanoconfinement. The obtained Kintr values are used to predict arsenate adsorption isotherms in pH 3 and 9, and the results align with the SCM simulation outcomes, verifying their reliability. © 2023, The Authors. All rights reserved.

关键词： Groundwater

Long-Term Impact of Nano Zero-Valent Iron on Methanogenesis in Anaerobic Sludge System: Evaluating Methanogenic Activity, Microbial Community Structure, and Transcription Activity

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SSRN 2023年

作者： Su, Runhua Fu, Huimin Ding, Lili Fu, Bo He, Su Ma, Haijun Hu, Haidong Ren, Hongqiang State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China National Research Base of Intelligent Manufacturing Service Chongqing Technology and Business University Chongqing400067 China School of Environmental and Civil Engineering Jiangsu Key Laboratory of Anaerobic Biotechnology Jiangnan University Wuxi214122 China

NZVI is commonly used in industrial wastewater treatment. However, its long-term inhibition mechanisms of metabolization in anaerobic sludge systems are not well understood. This study investigated the long-term effects of NZVI on methanogenic activity, microbial community, and transcription activity. The results demonstrated that only 5000 mg/L NZVI led to a significant reduction in cumulative methane production (14.4% of control) within 30 days. NZVI adversely affected cell viability, ATP production, and extracellular polymer (EPS), particularly at higher concentrations. Cell membranes played a crucial role in resisting chronic NZVI toxicity. Moreover, high NZVI levels hindered the transcription of key enzymes CoM and mcrA, while low NZVI levels down-regulated the transcription of cdh and hdr, respectively. Besides, amino-utilizing bacteria was reduced under the high NZVI concentration, while low NZVI changed dominant genus with potential protein hydrolysis function from Candidatus Cloacamonas to Sedimentibacter. The similar change was observed in the archaeal community © 2023, The Authors. All rights reserved.

关键词： Wastewater treatment

Corrigendum to "Degradation of aqueous methylparaben by non-thermal plasma combined with ZnFe2O4-rGO nanocomposites: Performance, multi-catalytic mechanism, influencing factors and degradation pathways" [Chemosphere 271 (2021) 129575]

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Chemosphere 2025年 372卷 143615页

作者： Feng, Jingwei Nian, Peng Peng, Lu Zhang, Aiyong Sun, Yabing Anhui Provincial Engineering Laboratory for Rural Water Environment and Resources School of Civil and Hydraulic Engineering Hefei University of Technology Hefei230009 China State Key Laboratory of Pollution Control & Resources Reuse School of the Environment Nanjing University Nanjing210046 China Anhui Province Key Laboratory of Industrial Wastewater and Environmental Treatment Hefei230024 China East China Engineering Science and Technology Co. Ltd. Hefei230024 China

Zirconium-grafted mesoporous SiO 2 (Zr-SBA-15) as Brønsted acid sites-free catalyst enables selective catalytic transfer hydrogenation of furfural to furfuryl alcohol

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Sustainable Chemistry and Pharmacy 2025年 46卷

作者： Sifan Bi Jinyu Lu Shourong Zheng Zhaoyi Xu State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing 210023 PR China

Zirconia-based catalysts are highly active for the transfer hydrogenation of furfural (FF) to furfuryl alcohol (FA) via the Meerwein-Ponndorf-Verley (MPV) reaction; while the inevitable presence of Brønsted acid sites in the catalysts remarkably undermines FA selectivity. In this study, zirconium-grafted catalysts were prepared by post-grafting organic zirconium (Zr(C 3 H 7 O) 4 ) on TiO 2 , Al 2 O 3 and SiO 2 via chemical liquid deposition (CLD). For comparison, supported ZrO 2 catalysts were also prepared by the conventional impregnation method, the zirconium-grafted catalysts have rich Lewis acid sites (LASs) but negligible Brønsted acid sites (BASs). Such unique acid properties of the grafted catalysts stem from the formation of covalently bonded zirconium species on the support surface. As a result, the zirconium-grafted catalysts exhibited much higher FA selectivity than conventional supported ZrO 2 ones. Characterization results further demonstrate that zirconium moiety grafted on SiO 2 displays much stronger acidity, thus delivering a higher FF conversion than those on Al 2 O 3 and TiO 2 . Additionally, we prepared zirconium-grafted mesoporous SiO 2 (Zr1-SBA-15), which exhibits 99 % FF conversion and 98.5 % FA selectivity at 120 °C with a turnover frequency (TOF) of 10.38 h −1 , outperforming previously reported zirconia-based catalysts. Furthermore, Zr1-SBA-15 shows excellent recyclability over five catalyst cycles. Our study clearly demonstrates that surface grafting of organic zirconium on oxide supports to form covalently bonded zirconium species is a universal approach to construct LASs-rich but BASs-free zirconia-based catalysts for highly selective reduction of carbonyl compounds to corresponding alcohols.

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Far-Uvc Activation of Sulfite for Carbamazepine Degradation Under Natural Reoxygenation: A Reduction-Dominated Proces

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SSRN 2025年

作者： Pan, Mingyuan Lu, Jian Zeng, Chao Peng, Zhu Zhang, Tian-Yang Pan, Ren-Jie He, Huan Dong, Zhengyu El-Din, Mohamed Gamal Xu, Bin State Key Laboratory of Pollution Control and Resource Reuse Key Laboratory of Urban Water Supply Water Saving and Water Environment Governance in the Yangtze River Delta Ministry of Water Resources College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China College of Environmental and Chemical Engineering Shanghai University of Electric Power Shanghai200090 China Department of Civil and Environmental Engineering University of Alberta EdmontonABT6G 1H9 Canada

Recent findings show that the reductive UV/sulfite (UV/S(IV)) process could convert into an oxidative pathway in the presence of dissolved oxygen, offering great potential for removing emerging contaminants (ECs). However, UV254 are inefficient at exciting S(IV) and the contributions of different reactive species under oxygenated conditions remain unclear. Herein, we propose a novel far-UV KrCl* excimer lamp (UV222) to accelerate the activation of S(IV) and improve the degradation of carbamazepine (CBZ). Results revealed that, switching from 254 nm to 222 nm enhanced the ability of the UV222/S(IV) to degrade CBZ, achieving a 3-fold increase in degradation efficiency and nearly a 9-fold increase in the degradation rate constant. The UV222/S(IV) process required only 1/10 of the electrical energy per order (EE/O) and cost compared to UV254/S(IV). Contrary to expectations, dissolved oxygen inhibited the efficiency of UV222/S(IV), rather than enhancing the oxidative pathway. Quenching experiments showed that CBZ degradation in UV254/S(IV) was driven by •OH, while in UV222/S(IV), it was mainly driven by reduction (75.1% from eₐq⁻). The high energy of UV222 accelerated S(IV) decomposition and oxygen consumption, promoting eₐq⁻ generation and limiting the formation of •OH and SO4•⁻ (with S(IV) being a precursor of both SO4•⁻ and •OH). Therefore, the UV222/S(IV) process is primarily reductive under natural reoxygenation. The degradation experiments confirmed that the process favors the reductive degradation of electron-deficient pollutants, such as benzoic acid, 2,4-dichlorophenol, iohexol and atrazine. Common anions and natural organic matter had minimal effects on the process, and the system still performed excellently in real lake water matrices, demonstrating its practical potential. This study provides new insights into the mechanisms involved in UV222/S(IV) process under natural reoxygenation. © 2025, The Authors. All rights reserved.

关键词： Rate constants

Characterization of CANON reactor performance and microbial community shifts with elevated COD/N ratios under a continuous aeration mode

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Frontiers of Environmental Science & Engineering 2019年第1期13卷 73-85页

作者： Yao Zhang Yayi Wang Yuan Yan Haicheng Han Min Wu State Key Laboratory of Pollution Control and Resources Reuse Shanghai Institute of Pollution Control and Ecological Security College of Environmental Science and Engineering Tongji University Shanghai 200092 China

The effects of increasing COD/N on nitrogen removal performance and microbial structure were investigated in a SBR adopting a completely autotrophic nitrogen removal over nitrite process with a continuous aeration mode (DO at approximately 0.15-0.2 mg/L). As the COD/N increased from 0.1 to W0.59, the nitrogen removal efficiency QMRE) increased from 88.7% to 95.5%;while at COD/N ratios of 0.59-0.82, the NRE remained at 90.7%-95.5%. As the COD/N increased from 0.82 to 1.07, the NRE decreased continuously until reaching 60.1%. Nitrosomonas sp.(AOB) and Candidatus Jet tenia (anammox bacteria) were the main functional genera in the SBR. As the COD/N increased from 0.10 to 1.07, the relative abundance of Nitrosomonas decreased from 13.4% to 2.0%, while that of Candidatus Jettenia decreased from 35% to 9.9% with COD/N < 0.82 then increased to 45.4% at a COD/N of 1.07. Aerobic heterotrophic bacteria outcompeted AOB at high COD loadings (650 mg/L) because of oxygen competition, which ultimately led to deteriorated nitrogen removal pertormance.

关键词： CANON process COD/N ratio Anammox Ammonia oxidizing bacteria Aerobic heterotrophic bacteria

A Non-Labeling Technique to Quantify and Visualize Gold Nanoparticle Accumulation at the Single-Cell Level

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SSRN 2022年

作者： Wang, Chuan Zhou, Hao-Ran Zhao, Ya-Tong Xiang, Zhi-Qian Pan, Ke Yang, Liuyan Miao, Ai-Jun State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu Province Nanjing210023 China Institute for Advanced Study Shenzhen University Shenzhen518060 China

Despite their wide bioapplications, potential health risks of gold nanoparticles (AuNPs) remain unclear. As a determinant of their risks, AuNP accumulation within a cell population is subject to cell-to-cell heterogeneity. Methods to simultaneously quantify and visualize intracellular AuNPs at the single-cell level are, however, lacking. Here we developed a novel non-labeling technique, based on hyperspectral imaging with enhanced darkfield microscopy (HSI-DFM), to visualize and quantify AuNP accumulation at the single-cell level. The identification ability of the hyperspectral libraries derived from extra- and intracellular AuNPs was compared. The spectral number in the libraries was optimized to maximize their identification ability while minimizing the identification time. In addition, a filtration method was established to merge spectral libraries from different cell lines based on their similarity. The intracellularly accumulated AuNPs as determined by HSI-DFM well correlated with those detected by inductively coupled plasma mass spectrometry. This validation allowed us to calculate the intracellular concentration of AuNPs at the single-cell level and to monitor the accumulation kinetics of AuNPs in living cells. The non-labeling method developed herein can be applied to other types of AuNPs differing in their physicochemical properties as well as other NPs, as long as they are detectable by HSI-DFM. © 2022, The Authors. All rights reserved.

关键词： Metal nanoparticles