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Fouling-Free electrochemical strategy based on vertically-aligned peptide layer for cardiac troponin I sensitive detection in human serum

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ANALYTICA CHIMICA ACTA 2024年 1317卷 342866页

作者： Qin, Xingao Ab, Xiaoyu Zhu, Xiaoyu Wang, Ying Tongji Univ State Key Lab Pollut Control & Resources Reuse Coll Environm Sci & Engn Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

Background: Cardiac troponin I (CTnI) is demonstrated as one of the most promising disease biomarkers for early diagnosing acute myocardial infarction (AMI). To date, electrochemical immunosensors have been extensively studied in the field of cTnI determination. But highly accurate and sensitive cTnI detection by this method is still a challenge due to non-specific adsorption on electrode interfaces in complex human serum. As a result, it is necessary to develop an antifouling electrochemical immunosensor with high sensitivity for the detection of cTnI. Results: In this work, an antifouling electrochemical immunosensor was constructed based on vertically-aligned peptide layer consisting of Au nanoparticles (AuNPs) and amphiphilic CEAK16 peptide (CEAK16@AuNPs) for sensitive and accurate detection of cTnI in human serum. The vertically-aligned CEAK16@AuNPs interface provided a stable hydration layer originated from attraction of water molecules by amino acids on the hydrophilic side of the CEAK16, which effectively reduced non-specific adsorption and enhanced electron transfer rate. The cTnI immunosensor possessed great analytical performance with a wide range from 1 fg mL-1-1 to 1 mu g mL-1-1 and a low detection limit of 0.28 fg mL-1-1 (S/N = 3). Additionally, the proposed CEAK16@AuNPs sensing interface showed excellent long-term antifouling performance and electrochemical activity that preserved 80 % of the initial signal after 20-days exposure in human serum samples. Consequently, the cTnI immunosensor displayed excellent detection accuracy compared to clinical methods and owned good selectivity, stability and reproducibility. Significance: The development of this strategy provides a versatile tool for accurate quantitative cTnI analysis in real human serum, thus helping to achieve early AMI diagnosis effectively and holding the promising potentials for other immunosensor in disease diagnosis.

关键词： Electrochemical immunosensor Antifouling Amphiphilic peptide Cardiac troponin I Human serum

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Dual acceleration of Co(III)/Co(II) redox cycle boosts peroxymonosulfate activation for superfast chloramphenicol degradation

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SEPARATION AND PURIFICATION TECHNOLOGY 2024年 334卷

作者： Xu, Bincheng Luo, Zexi Tao, Tao Wang, Ying Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

Co-based nanomaterials have been proven as excellent catalysts in activating peroxymonosulfate (PMS), owing to the high adsorption ability and efficient electron transfer toward PMS molecules. However, the slow Co sites regeneration induced by HSO5  /SO5 center dot- redox cycle alone not only deteriorates the utilization efficiency of PMS, but also restricts the overall catalytic reaction rate. Herein, we report a novel S-FeCoO nano-catalyst to active PMS for chloramphenicol (CAP) degradation. As a result, up to 97.73 % of removal efficiency was achieved within 30 min even with an initial CAP concentration of 50 mg/L, which is substantially superior to other Co or Fe-based PMS activation systems. More importantly, synergistic effects arising from the coexisting Fe and S species were identified by the control experiments and characterization results. Co served as the primary active site, while Fe (II) and S2 /S22  greatly accelerated Co(III)/Co(II) redox cycle by donating electrons. The proposed strategy of dual acceleration of Co(III)/Co(II) redox cycle, as well as its mechanism insights, is expected to provide important implications on the rational design of advanced catalysts for PMS activation.

关键词： Peroxymonosulfate Advanced oxidation process Reactive oxygen species Co(III)/Co(II) redox cycle Electron transfer

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Indirect photodegradation of typical pyrrolizidine alkaloids in water induced by triplet states of dissolved organic matter

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JOURNAL OF HAZARDOUS MATERIALS 2024年 476卷 135142页

作者： Gao, Menghong Yu, Shuili Ning, Rongsheng Ji, Xingli Xu, Ying Hou, Li'an Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

The occurrence of pyrrolizidine alkaloids (PAs) in the aquatic environment has received growing attention due to their persistent mutagenicity and carcinogenicity. In this study, the photooxidation processes of four representative PAs (senecionine, senecionine N-oxide, europine, and heliotrine) in the presence of dissolved organic matter (DOM) were investigated. The excited triplet DOM ((DOM)-D-3*) was demonstrated to play a dominant role in the phototransformation of PAs. The observed degradation rates of PAs largely depended on the DOM concentration. Alkaline conditions and the presence of HCO3-/CO32- were conducive to the photodegradation. Based on kinetic modeling, the second-order reaction rate constants of PAs with (DOM)-D-3* were predicted to be (1.7 similar to 5.3)x10(8) M-1 s(-1), nearly two orders of magnitude higher than those with singlet oxygen (O-1(2)). The monoester structure and electron-withdrawing substituent (e.g., -O atom) substantially affected the one-electron oxidation potential of PAs, which dictates the reaction rates of PAs with (DOM)-D-3*. Finally, a tentative degradation pathway of PAs was proposed, involving the formation of an N-centered radical cation through one-electron transfer, which then likely deprotonated and further oxidized to more persistent and toxic phototransformation products with an added oxygen atom into the pyrrole ring.

关键词： Excited triplet states Singlet oxygen Kinetic modeling Half-life Degradation pathway

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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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Membrane aeration accelerated nitrifying biofilm formation and optimized spatial niche differentiation in aerobic biofilm-based reactors for enhanced nitrogen removals

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CHEMICAL ENGINEERING JOURNAL 2025年 506卷

作者： Li, Jia Wang, Han Li, Zibin Xie, Junxiang Tsybekmitova, Gazhit Ts. Wang, Yayi Tongji Univ Shanghai Inst Pollut Control & Ecol Secur State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Russian Acad Sci Siberian Branch Inst Nat Resources Ecol & Cryol Nedorezova 16a Chita 672014 Russia

The membrane aerated biofilm reactor (MABR) is attractive in sewage treatment due to its robust performance and cost-effectiveness. This study characterizes the role of membrane aeration in biofilm formation, spatial niche distribution, and nitrogen transformation, aiming to deepen the understanding of how membrane aeration in MABRs differs from diffused aeration in conventional aerated biofilm reactors (CABRs). Enhanced nitrifying biofilm formation in the MABR was evidenced by increased microbial aggregation, faster biofilm maturation (20 vs. 30 days), and accelerated nitrifying bacteria proliferation (e.g., Nitrosomonas on day 20: 1.15 f 0.10 % vs. 0.49 f 0.03 %) with higher final enrichment levels (e.g., Nitrosomonas on day 90: 1.93 f 0.62 % vs. 1.23 f 0.28 %). This was attributed to membrane aeration, which facilitated initial conditioning film formation and mitigated bubble-induced disturbances, promoting microbial colonization. Ecological null model analysis indicated a sequential progression in the MABR biofilm community assembly, e.g., a deterministic-stochastic-deterministic dominant process. Membrane aeration-driven substrate counter-diffusion optimized spatial niche differentiation, with Nitrosomonas and Nitrospira abundances in the MABR biofilm (1.93 f 0.62 % and 3.85 f 0.57 %, respectively) significantly higher than in the suspended sludge (0.19 f 0.01 % and 0.20 f 0.03 %, respectively), while denitrifiers were more abundant in the suspended sludge (8.51 f 0.05 %) than in the biofilm (3.82 f 0.20 %). This spatial niche distribution contributed to a one-fold increase in nitrogen removal efficiency and a more robust microbial ecosystem with more keystone species (9 vs. 1) compared to the CABR. A self-sustaining symbiotic biofilm-flocs ecosystem was developed by introducing membrane aeration, favoring highperformance nitrogen removals and propelling the paradigm shift of wastewater treatment plants towards carbon neutrality.

关键词： Membrane aeration Nitrifying biofilm Biological nitrogen removal Community assembly Spatial niche differentiation

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Effective defluorination of novel hexafluoropropylene oxide oligomer acids under mild conditions by UV/sulfite/iodide: mechanisms and ecotoxicity

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WATER RESEARCH 2024年 258卷 121804页

作者： Zhai, Zhenyu Zhang, Chaojie Chu, Liquan Zhao, Yunmeng Zhou, Xuefei Zhang, Yalei Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

It has recently been discovered that HFPO-TA (a processing aid in the production of fluoropolymers) has high levels of bioaccumulation and biotoxicity. Hydrated electrons (eaq- ) have been proposed to be potent nucleophiles that may decompose PFAS. Unlike previous studies in which the generation of eaq- was often restricted to anaerobic or highly alkaline environments, in this study, we applied the UV/SO32- /I- process under mild conditions of neutrality, low source chemical demand, and open-air, which achieved effective degradation (81.92 %, 0.834 h-1) and defluorination (48.99 %, 0.312 h-1) of HFPO-TA. With I- as the primary source of eaq- , SO32acting as an I- regenerator and oxidizing substances scavenger, UV/SO32- /I-outperformed others under mild circumstances. The eaq- were identified as the main active species by quenching experiments and electron paramagnetic resonance (EPR). During degradation, the first site attacked by eaq- was the ether bond (C6-O7), followed by the generation of HFPO-DA, TFA, acetic and formic acid. Degradation studies of other HFPOs have shown that the defluorination of HFPOs was accompanied by a clear chain-length correlation. At last, toxicological experiments confirmed the safety of the process. This study updated our understanding of the degradation of newly PFASs and the application of eaq- mediated photoreductive approaches under mild conditions.

关键词： Degradation mechanism HFPO-TA Toxicological

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Treatment of emerging pyrrolizidine alkaloids in drinking water by UV/persulfate process: Kinetics, energy efficiency and degradation pathway

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CHEMICAL ENGINEERING JOURNAL 2024年 490卷

作者： Gao, Menghong Yu, Shuili Hou, Li'an Ji, Xingli Ning, Rongsheng Xu, Ying Li, Lei Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

Pyrrolizidine alkaloids (PAs), recognized as a group of toxic secondary metabolites, have raised growing concerns in recent years due to their potential high toxicity. However, studies on the degradation of PAs in drinking water treatments have yet to be conducted. Herein, the treatment of Heliotrine (HEL) and N-oxide (HELNO), two dominant PAs detected in the treated drinking water, are analyzed for the first time. The UV/peroxydisulfate (UV/PDS) process was demonstrated to be efficient in the degradation of PAs, achieving almost complete removal of HEL and HELNO in 30 min. SO4 center dot- plays a dominant role in the system, with second-order rate constants of 2.3 x 10(9) M-1 s(-1) and 1.0 x 10(9) M-1 s(-1) for HEL and HELNO, respectively. Based on the steady-state kinetic models, the effect of influence factors, including PDS dosage, initial pollutant concentration, pH, dissolved organic matter (DOM), and chloride (Cl), were evaluated. Acidic conditions were proven to be favorable for PA degradations, primarily contributed to the minimized quenching effect of OH and phosphate on SO4 center dot-. The inhibitory effect of DOM on radical quenching significantly overweighted the promotion effect of the generated excited triplet DOM (3DOM*), resulting in a diminished degradation efficiency. The pronounced inhibition of Cl could be attributed to the conversion of SO4 center dot- to OH center dot, involving the formation of reactive chlorine species. The UV/PDS treatment was suggested economical in the removal of PAs as a post-filtration and before-chlorination treatment through electrical energy per order (EE/O) calculation. Finally, reasonable degradation pathways of HEL and HELNO reacted with SO4 center dot- were proposed, involving the initial one-electron oxidation of HEL/HELNO by SO4 center dot- radical, and further reactions (e.g., hydroxylation, pyrrolidine ring-cleavage and self-coupling) of the formed N-centered cation radicals.

关键词： Pyrrolizidine alkaloids Drinking water Heliotrine (N -oxide) UV/persulfate Kinetic model Degradation mechanism

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Integration of seeding-induced crystallization with microbubble aeration for membrane fouling and wetting control in vacuum membrane distillation

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DESALINATION 2024年 581卷

作者： Zhang, Wei Xiao, Qian Yu, Shuili Ji, Xingli Ning, Rongsheng Xu, Ying Li, Pan Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

In this work, a bench-scale vacuum membrane distillation crystallization (VMDC) system coupled with microbubble aeration (MBA) was developed for treating high-salinity feed brine. Herein, the effect of seeding dose on membrane fouling and wetting control in the VMDC system was studied by using synthetic saturated calcium sulfate solution. The results showed that introducing gypsum seeds at a dose of 0.5 g/L effectively restricted membrane fouling and wetting. Subsequently, seeding-induced crystallization coupled with MBA was employed to investigate the control effect on membrane fouling and wetting during VMDC with simulated high-salinity feed brine treatment. As 0.5 g/L gypsum seeds were directly added at 7 h in the VMDC experiment while employing MBA, membrane fouling and wetting were effectively controlled. Finally, the mechanism behind the control of membrane fouling and wetting was elucidated during VMDC operation by integrating seeding-induced crystallization with MBA. This could be ascribed to the synergic effect of gypsum seeds and microbubbles in bulk solution. In brief, this work offers a promising approach to control membrane fouling and wetting during concentrating high-salinity wastewater by VMD.

关键词： Vacuum membrane distillation Seeding -induced crystallization Membrane fouling and wetting Microbubble aeration

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Selective electroreduction of nitrate to ammonia via NbWO_(6)perovskite nanosheets with oxygen vacancy

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Chinese Chemical Letters 2023年第5期34卷 385-388页

作者： Tao Feng Fengting Li Xiaojun Hu Ying Wang School of Chemical and Environmental Engineering Shanghai Institute of TechnologyShanghai 201418China State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Electrocatalytic nitrate reduction to ammonia(NRA)under ambient conditions is significant for carbonneutral synthetic ***,the lack of efficient electrocatalysts with tunable nanostructure for NRA remains a grand ***,Nb WO_(6)nanosheets with oxygen vacancy(NbWO_(6-x))was demonstrated via thermal treatment and exfoliation with NH_(3)selectivity of 86.8%and Faradaic efficiency of85.7%toward NRA.^(1)H nuclear magnetic resonance spectra coupled with^(15)N isotope labeling experiments proved that NH_(3)originated from NO_(3)^-.The function of oxygen vacancy was revealed by computational studies in ***,the reaction mechanism and pathway of NRA could be deduced based on the results of online differential electrochemical mass spectrometry(DEMS).This work provides a selective NH_(3)generation strategy to decarbonize the energy-chemical sector,bridging the gap between batteries and biofuels.

关键词： Nitrate reduction Ammonia generation NbWO_(6-x)nanosheets Oxygen vacancy Adsorption energy

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Self-supporting electrode incorporating active Co sites for ultrafast ammonia production from nitrate reduction

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS 2024年 687卷

作者： Xiong, Run Xu, Bincheng Chen, Zhixuan Cheng, Chen Wang, Ying Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

Electrocatalytic nitrate (NO3-) reduction reaction (NitRR) provides us a green solution to synthesize ammonia (NH3) and ease environmental problems. However, the development of robust electrodes with high NH3 yield rates and Faradaic efficiencies (FEs) is still challenging. Herein, we report a self-supporting electrode incorporating vertically aligned Co-based metal-organic framework (MOF) nanosheets (Co-NDC/NF), which facilitates electron and mass transfer for efficient NitRR to NH3 within a wide range of NO3- concentration (0.05-1.0 M). In 1.0 M KOH + 1.0 M KNO3 electrolytes, such Co-NDC/NF reaches a notable NH3 yield rate of 19,200 ug h-1 cm -2, a high FE of 93.9% and excellent electrochemical stability, which is superior to most electrocatalysts. A flowthrough reactor with large-area Co-NDC/NF also achieves the continuous production of 1096 mg L-1 NH3 under an industrial current density. Furthermore, the rapid transformation of *NO2- to *NO and selective conversion of *NO to *NOH played critical roles in NitRR toward ultrafast NH3 production. Our research not only offers a facile fabrication procedure for high -performance electrode, but also gives new insights into the enhanced electron transfer and mass transport within MOF-based electrode in electrochemical reactions.

关键词： Co-based nanosheets Electrocatalytic nitrate reduction Ammonia production Mass transport Electron transfer

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