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SSRN 2023年

作者： Li, Boyu Liu, Jiaxiang He, Xuanting Wang, Rong Tao, Wenquan Li, Zhuo State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University 1239 Siping Road Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China Defense Innovation Institute Academy of Military Sciences Beijing100071 China

Facilitated transport mixed matrix membranes (FTMMMs) separation technology has shown advantages in improving CO2 recycling efficiency and reducing the environmental impacts associated with carbon emission. The design of FTMMMs is highly dependent on the selection of a compatible combination of polymer and filler. Herein, a novel grafted nanoparticles (GNPs) filler UiO-66-NM@PEG with multiple groups prone to hydrogen bond was designed to alleviate the phase separation and performance degradation caused by filler/polymer poor compatibility. In the GNPs configuration, by employing the coexistence strategy of coupling reaction and covalent bonds, maleic anhydride (MAH) was coupled with the amino group on UiO-66-NH2 without clogging or cracking, and the generated carboxyl groups can be cross-linked with the hydroxyl groups on the poly (ethylene glycol) (PEG) by covalent bonds. The UiO-66-NM@PEGdemonstrated excellent interface compatibility between the filler and matrix phase of UiO-66-NM@PEG/PVDF, which was further convinced by molecular modelling. The resultant UiO-66-NM@PEG/PVDF achieved a simultaneous enhancement of gas permeability (537.6 Barrer) and ideal CO2/N2 selectivity (47.8), which surpassed Robenson upper bound. Moreover, the UiO-66-NM@PEG/PVDF has a lasting sustainability over 960 hours (40 days), and a valid anti-acid/alkali corrosion resistance in harsh environments. More importantly, UiO-66-NM@PEG can also be well mixed with other mixture matrices such as PDMS and PEBAX to promote permeability/ideal selectivity up to (724.1 Barrer/21.1) and (307.4 Barrer/31.4). We thus concluded that this rational-design GNPs approach provides a general toolbox for controllable engineering in GNPs whereby enhanced favorable filler/matrix compatibility in FTMMMs with optimized CO2/N2 separation properties. © 2023, The Authors. All rights reserved.

关键词： Carbon dioxide

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Peroxymonosulfate activation for preferential generation of hydroxyl radical with atomic Mn anchored TiO 2 in photoelectrochemical process

Environmental Functional Materials

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Environmental Functional Materials 2023年第1期2卷 13-24页

作者： Min Chen Jinxing Zhang Tian Yang Shun Mao Hongying Zhao Shanghai Key Lab of Chemical Assessment and Sustainability Key Laboratory of Yangtze River Water Environment School of Chemical Science and Engineering Tongji University 1239 Siping Road Shanghai 200092 PR China College of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource Reuse Tongji University 1239 Siping Road Shanghai 200092 PR China

The threaten of ubiquitous antibiotics to human and ecosystem makes it urgent to seek efficient treatment technologies. Peroxymonosulfate (PMS)-based advanced oxidation processes have revealed wide prospects for wastewater treatment via controllable PMS activation for desired ROS generation. Herein, a novel TiO 2 photoelectrode decorated with atomically distributed Mn (SA-MnTiO 2 ) was designed via a modified molten salt method (MSM) for photo-electro-catalytic (PEC) activation of PMS. The electron transfer in reduction-/oxidation-state Mn(II)/Mn(III)/Mn(IV) cycles facilitated the cleavage of intramolecular O–O bonds in PMS to preferentially generate hydroxyl radical (HO•). Almost complete degradation of norfloxacin (NOR) was occurred with optimal SA-Mn 0.6 TiO 2 within 15 min, exhibiting high turnover frequency (0.066 min −1 ). Around 74.8% of total organic carbon was eliminated with a low specific energy consumption of 0.94 kW h/g. The key operational parameters during actual wastewater treatment were inspected for SA-Mn 0.6 TiO 2 /PMS system, suggesting the satisfactory stability for practical applications.

关键词： Peroxymonosulfate Hydroxyl radical Antibiotic Advanced oxidation processes Photoelectrochemical process

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Niche Differentiation of Comammox Nitrospira and Canonical Nitrifiers in Riparian Wetland Ecosystems Around Taihu Lake

SSRN

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SSRN 2022年

作者： He, Yanqing She, Yuecheng Qi, Xin Zhang, Hui Wang, Wei Li, Zhengkui School of the Environment Nanjing University Nanjing Jiangsu210023 China State Key Laboratory of Pollution Control and Resource Reuse Nanjing University Nanjing210023 China

Complete ammonia oxidation (Comammox) overturned our perception of ammonia oxidation and challenged the traditional two-step nitrification theory. Newly discovered comammox Nitrospira and canonical nitrifiers (AOA and AOB) collaboratively perform the oxidation of ammonia in ecosystems. However, the niche distribution of comammox Nitrospira is controversial. In our study, we explored the distribution, diversity and driving environmental factors of comammox Nitrospira in riparian wetland ecosystems around Taihu Lake. Comammox Nitrospira was detected in all 15 soil samples, with the amo A gene abundance ranging from 1.83×10 5 to 8.35×10 7 copies/g. In most soil samples, the amo A gene abundance of comammox Nitrospira was lower than that of canonical nitrifiers. High-throughput sequencing indicated that the community structure of comammox Nitrospira had both spatial and temporal heterogeneity. The comammox Nitrospira detected in our study was divided into cladeA.1 cluster and clade A.2 cluster. Comammox Nitrospira clade A.2 observed in all soil samples was more prevalent, while the clade A.1 was mainly observed in the wheat field. Nitrospira sp. and Nitrospira sp. LK70 had the highest relative abundance and might be the key species of comammox Nitrospira . Temperature, soil moisture content, NH 4 + , total nitrogen, total carbon and pH were the main environmental factors causing the niche differentiation between comammox Nitrospira and canonical nitrifiers. Collectively, our study expands the general insights into the niche distribution of comammox Nitrospira and the driving environmental factors in riparian wetland ecosystems around Taihu Lake. © 2022, The Authors. All rights reserved.

关键词： Nitrification

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Simultaneous Water Softening and Selective Ammonia Nitrogen Recovery from Coal Gasification Gray Water Using an Innovative Four-Chamber Flow-Electrode Electrochemistry System

SSRN

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SSRN 2023年

作者： Chen, Taoqin Wei, Sheng Xu, Longqian Tang, Xianchun Chen, Hongbin State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Key Laboratory of Yangtze River Water Environment Ministry of Education College of Environmental Science and Engineering Tongji University Shanghai200092 China

CDI-based technologies such as flow electrode capacitive deionization (FCDI) have shown great promise for desalination and resource recovery, but simultaneous desalination and resource recovery using one FCDI device has thus far received minimal attention. In this study, a novel four-chamber FCDI coupled with a monovalent cation exchange membrane (MCEM) was proposed to realize simultaneous desalination (including water softening) and ammonia-rich solution production from coal gasification gray water (CGGW). The results showed that under optimal conditions, up to 91.2 ± 0.1% ammonia nitrogen, 88.9 ± 1.0% Ca2+, and 92.6 ± 5.5% TOC of real CGGW were removed by the desalination chamber. Furthermore, passed through the MCEM and entered the recovery chamber, while Ca2+ was effectively blocked from entering the recovery chamber by MCEM. Thus, a value-added ammonia-rich solution with purity of 98.0% was obtained. The process was superior since two typical FCDI cells are needed to realize water softening and recover ammonia-rich solutions. The mechanistic insights into the proposed four-chamber FCDI coupled with MCEM can be expanded to other simultaneous desalination, ion separation and recovery processes. Thus, the four-chamber FCDI is a promising technology for simultaneous desalination and resource recovery with the advantages of being chemical-free, capital efficient and operable. © 2023, The Authors. All rights reserved.

关键词： Desalination

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Degradation and mechanism of PFOA by peroxymonosulfate activated by nitrogen-doped carbon foam-anchored nZVI in aqueous solutions

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Chemosphere 2024年 351卷 141209页

作者： Li, Changyu Shen, Cong Gao, Bin Liang, Wenxu Zhu, Yifan Shi, Weijie Ai, Shiyun Xu, Hongxia Wu, Jichun Sun, Yuanyuan State Key Laboratory of Pollution Control and Resource Reuse Key Laboratory of Surficial Geochemistry Ministry of Education School of Earth Sciences and Engineering Hydrosciences Department Nanjing University Nanjing210023 China College of Chemistry and Material Science Shandong Agricultural University Shandong Taian271018 China Department of Civil and Environmental Engineering Rensselaer Polytechnic Institute TroyNY12180 United States

Perfluorooctanoic acid (PFOA) is an emerging pollutant that is non-biodegradable and presents severe environmental and human health risks. In this study, we present an effective and mild approach for PFOA degradation that involves the use of nitrogen-doped carbon foam anchored with nanoscale zero-valent iron (nZVI@NCF) to activate low concentration peroxymonosulfate (PMS) for the treatment. The nZVI@NCF/PMS system efficiently removed 84.4% of PFOA (2.4 μM). The active sites of nZVI@NCF including Fe0 (110) and graphitic nitrogen played crucial roles in the degradation. Electrochemical analyses and density functional theory calculations revealed that nZVI@NCF acted as an electronic donor, transferring electrons to both PMS and PFOA during the reaction. By further analyzing the electron paramagnetic resonance and byproducts, it was determined that electron transfer and singlet oxygen were responsible for PFOA degradation. Three degradation pathways involving decarboxylation and surface reduction of PFOA in the nZVI@NCF/PMS system were determined. Finding from this study indicate that nZVI@NCF/PMS systems are effective in degrading PFOA and thus present a promising persulfate-advanced oxidation process technology for PFAS treatment. © 2024 Elsevier Ltd

关键词： Paramagnetic resonance

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Competing Contributions in the Micro-Nano Bubble Ozonation Process in Degradating 2-Methylisobornyl (2-MIB) and Geosmin (GSM): Revealing the Role of Free Radicals Versus Micro-Nano Bubbles

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SSRN 2024年

作者： Wang, Yonglei Ren, Yuehua Wang, Xinglin Liu, Baozhen He, Guilin Gong, Yanli Liu, Baosen Li, Jingjing School of Municipal and Environmental Engineering Shandong Jianzhu University Jinan250101 China School of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai1239 China Jinan Environmental Research Academy Jinan250000 China

Algal contamination leads to an increase in taste and odor compounds, such as 2-methylisobornyl alcohol (2-MIB) and geosmin (GSM). In this work, a coupled micro-nano bubble ozonation deep treatment process was constructed to investigate the degradation performance and mechanism underlying the micro-nano bubble ozonation process of 2-MIB and GSM. The results showed that the micro-nano bubble ozonation process could remove 94.38% of 2-MIB and 95.45% of GSM in 15 min, which was 36.11% and 29.56% higher than that of the common bubble ozonation process, respectively. Analysis of degradation products and toxicity showed that 2-MIB was oxidized by a micro-nano bubble ozonation process with bridge ring breaking and ring opening and finally decomposed into dextro-camphor-based steric double-bridged compounds. The toxicity of the products was significantly lower than that of 2-MIB, while GSM was first decomposed into isomers and other double-ringed substances and then ring-opened and broken into ketones, naphthalenes, alkanes and alcohols;however, the toxicity of only 50% of the intermediary products was reduced. Superoxide radical oxidation was the main mechanism for the reduced toxicity of 2-MIB and GSM in the micro-nano bubble ozonation process, in which the oxidizing capacities were 4.88% and 6.72% higher than those of hydroxyl radicals. The complete removal of 2-MIB and GSM in the micro-nano bubble ozonation process relied on synergistic effects resulting from micro-nano bubble-induced volatilization of the substances and ozone oxidation, and the contribution of the micro-nano bubble process to compound removal reached 75%. © 2024, The Authors. All rights reserved.

关键词： Potable water

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Competing Contributions in the Micro-Nano Bubble Ozonation Process in Degradating 2-Methylisobornyl (2-Mib) and Geosmin (Gsm): Revealing the Role of Free Radicals Versus Micro-Nano Bubbles

SSRN

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SSRN 2024年

作者： Ren, Yuehua Wang, Yonglei Wang, Xinglin Liu, Baozhen He, Guilin Gong, Yanli Liu, Baosen Li, Jingjing School of Municipal and Environmental Engineering Shandong Jianzhu University Jinan250101 China School of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai1239 China Jinan Environmental Research Academy Jinan250000 China

Seasonal algal contamination of lake and reservoir-type water sources leads to an increase in taste and odor compounds, such as 2-methylisobornyl alcohol (2-MIB) and geosmin (GSM). As a result, the effluent quality of water purification plants and the taste of drinking water are seriously affected. In this work, a coupled micro-nano bubble ozonation deep treatment process was constructed to investigate the degradation performance and mechanism underlying the micro-nano bubble ozonation process of 2-MIB and GSM. The results showed that the micro-nano bubble ozonation process could remove 94.38% of 2-MIB and 95.45% of GSM in 15 min, which was 36.11% and 29.56% higher than that of the common bubble ozonation process, respectively. Analysis of degradation products and toxicity showed that 2-MIB was oxidized by a micro-nano bubble ozonation process with bridge ring breaking and ring opening and finally decomposed into dextro-camphor-based steric double-bridged compounds. In addition, the toxicity of the products was significantly lower than that of 2-MIB, while GSM was first decomposed into isomers and other double-ringed substances and then ring-opened and broken into ketones, naphthalenes, alkanes and alcohols;however, the toxicity of only 50% of the intermediary products was reduced. Superoxide radical oxidation was the main mechanism for the reduced toxicity of 2-MIB and GSM in the micro-nano bubble ozonation process, in which the oxidizing capacities were 4.88% and 6.72% higher than those of hydroxyl radicals. The complete removal of 2-MIB and GSM in the micro-nano bubble ozonation process relied on synergistic effects resulting from micro-nano bubble-induced volatilization of the substances and ozone oxidation, and the contribution of the micro-nano bubble process to compound removal reached 75%. This work provides new insights for the development of deep treatment processes for the removal of taste and odor compounds from drinking water. © 2024, The Authors. All r

关键词： Potable water

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Prediction of Free Radical Reactions Toward Organic Pollutants With Easily Accessible Molecular Descriptors

SSRN

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SSRN 2023年

作者： Zhang, Guoyang Zhu, Qiang Zheng, Hongcen Zhang, Shujuan Ma, Jing State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China Key Laboratory of Mesoscopic Chemistry of Ministry of Education Institute of Theoretical and Computational Chemistry School of Chemistry and Chemical Engineering Nanjing University Nanjing210023 China

Machine learning (ML) is becoming an efficient tool for predicting the fate of aquatic contaminants owing to the preponderance of big data. However, whether ML can "learn" the differences in reactivity among different free radicals has not yet been tested. In this work, the effectiveness of combining ML algorithms with molecular fingerprints to predict the reactivity of three free radicals is evaluated. Firstly, a dataset containing 211 contaminants and their rate constants with carbonate radical (CO3•−) was used to develop predictive models by linear regression and ML. The employment of topologically atomic alignment information, in terms of molecular access system (MACCS) and Morgan Fingerprint, and the electronic structure features (energy levels of the highest-occupied and lowest-unoccupied molecular orbitals, EHOMO and ELUMO, and the energy gap between ELUMO and EHOMO) gave satisfactory predictive performances (ML model with Random Forest algorithm with MACCS: RMSEtest = 0.787;linear regression model with energy levels: RMSEtest = 0.641). Additionally, the model interpretation correctly described that the key reactivity features for CO3•− were relatively close to those for SO4•− rather than those for OH. These results suggest that the combination of ML algorithms with easily accessible molecular fingerprints would be a powerful tool to accurately predict the radical reactions towards organic compounds. © 2023, The Authors. All rights reserved.

关键词： Electronic structure

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Changes in selenium bioavailability in selenium-enriched paddy soils induced by different water management and organic amendments

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Science of the Total Environment 2024年 957卷 177844页

作者： Gong, Haotian Zhai, Hui Wang, Yujian Pan, Lei Liu, Yumeng Zhang, Yunshu Shao, Huawei Tang, Guangmu Ge, Chunhui Xu, Wanli Wang, Min College of Ecology and Environment Xinjiang University Urumqi830046 China Key Laboratory of Oasis Ecology of Education Ministry Xinjiang University Urumqi830046 China Institute of Soil and Fertilizer Agricultural Water Saving Xinjiang Academy of Agricultural Sciences Urumqi830092 China State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China

Combined effects of water management and agricultural organic waste return on selenium (Se) bioavailability and mechanisms in Se-enriched paddy soils remain unclear. We investigated the effects of continuous flooding (CF) and alternating wet and dry (AWD), two types (cotton straw biochar [BC] and sheep manure [SM]) and concentrations (10 and 50 g·kg−1) of organic amendments on soil Se bioavailability, bacterial community structure in naturally Se-enriched soils (1.69 mg·kg−1). Results showed that 10 g·kg−1 SM treatment was the most effective in increasing Se bioavailability, especially under AWD treatment, whereas BC treatment reduced it. Compared with CF treatment, AWD treatment increased the Se content of root surface iron plaque and rhizosphere affinity for Se, and promoted the conversion of soil weakly organic matter bound Se to soluble-Se and exchangeable-Se. BC and SM addition significantly altered soil solution Fe(II), dissolved organic carbon, and soil bacterial community structure and function, including sulfur-oxidizing bacteria (Thiobacillus) and Se-reducing bacteria (Pseudarthrobacter), under different water management regimes. Notably, these bacteria showed a significant correlation with bioavailable Se. The present study provides theoretical guidance for agronomic practices in Se-enriched paddy soils. © 2024 Elsevier B.V.

关键词： Iron removal (water treatment)

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The ASM2d model with two-step nitrification can better simulate biological nutrient removal systems enriched with complete ammonia oxidizing bacteria (comammox Nitrospira)

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Chemosphere 2023年第1期335卷 139169页

作者： Mei, Peng Wang, Zhiqi Guo, Wenjie Gao, Yuan A. Vanrolleghem, Peter Li, Yongmei State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China Co. Ltd Shanghai200001 China ModelEAU – Université Laval QuébecQCG1V 0A6 Canada

The discovery of comammox Nitrospira, a complete ammonia-oxidizing microorganism belonging to the genus Nitrospira, has brought new insights into the nitrification process in wastewater treatment plants (WWTPs). The applicability of Activated Sludge Model No. 2 d with one-step nitrification (ASM2d-OSN) or two-step nitrification (ASM2d-TSN) for the simulation of the biological nutrient removal (BNR) processes of a full-scale WWTP in the presence of comammox Nitrospira was studied. Microbial analysis and kinetic parameter measurements showed comammox Nitrospira was enriched in the BNR system operated under low dissolved oxygen (DO) and long sludge retention time (SRT). The relative abundance of Nitrospira under the conditions of stage I (DO = 0.5 mg/L, SRT = 60 d) was about twice of that under stage II conditions (DO = 4.0 mg/L, SRT = 26 d), and the copy number of the comammox amoA gene for stage I was 33 times higher than that for stage II. Compared to the ASM2d-OSN model, the ASM2d-TSN model simulated the performance of the WWTP under stage I conditions better, and the Theil inequality coefficient values of all the tested water quality parameters were lower than using ASM2d-OSN. These results indicate that an ASM2d model with two-step nitrification is a better choice for the simulation of WWTPs with the presence of comammox. © 2023 Elsevier Ltd

关键词： Nitrification

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