作者机构:
[Liu, Lijuan; Zhang, Lizhi; Gong, JM; Meng, Mingxia; Gong, Jingming; Yao, Qingfeng; Cai, Zheng; Sun, Hongwei; Jiang, Fang] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Gong, JM ] C;Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.
摘要:
As emerging contaminants in the environment, antibiotic resistance genes (ARGs) have aroused a global health crisis and posed a serious threat to ecological safety and human health. Thus, efficient and accurate onsite detection of ARGs is crucial for environmental surveillance. Here, we presented a colorimetric-photoelectrochemical (PEC) dual-mode bioassay for simultaneous detection of multiple ARGs by smartly incorporating rolling circle amplification (RCA) into a stimuli-responsive DNA nanoassembly, using the tetracycline resistance genes tetA and tetC as models. The tailored DNA nanoassembly containing RCA amplicons hybridized with specific signal probes: CuO nanoflowers-anchored signal DNA1 and HgO nanoparticles-anchored signal DNA2, respectively. Upon exposure to an acidic stimulus, numerous Cu(2+) and Hg(2+) were released, serving as the reporting agent of colorimetric/PEC dual-mode assay. The released Cu(2+) and Hg(2+) induced localized surface plasmon resonance shifts in Au nanorods and triangular Ag nanoplates through an etching process, respectively, enabling visual analysis of ARGs with distinguishing color changes. Meanwhile, numerous Cu(2+) and Hg(2+) triggered the amplified PEC variations via reacting with the photoactive layers of CuS/CdS and ZnS, respectively. Thus, a rapid and ultrasensitive colorimetric/PEC dual-mode detection of multiple ARGs was achieved with the detection limit down to 17.2 aM. Furthermore, such dual-mode bioassay could discriminate single-base mismatch and successfully determine ARGs in E. coli plasmids and sludge samples, holding great promise for point-of-care genetic diagnostics.
通讯机构:
[Gong, JM ] C;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词:
Ammonia nitrogen;6-Trichlorophenol;Peroxymonosulfate;Dechlorination;Active chlorine species
摘要:
Halogenated phenol and ammonia nitrogen (NH4+-N) are typical composite pollutions in wastewater. It is still unclear how the transformation of halogenated phenol affects the fate of co-existing NH4+-N. In this study, the removal performance of the NH4+-N containing the co-existed halogenated organic, using 2, 4, 6-trichlorophenol (TCP) as the model pollutant was firstly investigated in the waste lithium-ion batteries (LIBs) material-derived catalysts activating peroxymonosulfate system (LIBs/PMS). The rapid degradation of TCP and the selective transformation of NH4+-N to N2 were simultaneously achieved. TCP could be degraded rapidly (within 2 min) whether with or without NH4+-N. Interestingly, the NH4+-N removal was initiated by the co-present TCP, strongly dependent on TCP dechlorination. And NH4+-N removal displayed a thermally accelerated process in the temperature range of 25 to 60 degrees C. With the co-present TCP (60 mg/L), 93.7% of NH4+-N could be removed at 50 degrees C. Based on the capture and the electron spin resonance (ESR) experiments, the generated reactive oxygen species (& BULL;OH, SO4 & BULL; and 1O2) participated in the TCP dechlorination, particularly 1O2 with dominant roles, whereas ClO & BULL; played an important role on NH4+-N removal. Theoretical calculations were used not only to predict the possible reactive site of TCP, but also evaluate the difficulty of reaction between NH4+-N and different active species. Moreover, NH4+-N could be removed 80% in outdoor simulated experiment (in Wuhan) and 100% for chlorobenzene and nitrogen-containing wastewater. This study unveiled the influence of the co-existed halogenated phenol toward the fate of NH4+-N in LIBs/PMS system and enriched the treatment of NH4+-N wastewater strategies.
作者机构:
[Feng, Lizhen; Zhang, Lizhi; Gong, Jingming; Yuan, Yijin; Wu, Mengsi; He, Xianqin] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Coll Chem,Minist Educ, Inst Environm & Appl Chem,Key Lab Pesticide & Che, Wuhan 430079, Peoples R China.
通讯机构:
[Lizhi Zhang; Jingming Gong] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要:
Sulfite (S(IV)) is a promising substitute for sulfate radical-based advanced oxidation processes. Here, a composite of in-situ anchoring NiCo2O4 nanosheets on biochar (BC) was firstly employed as a heterogeneous activator for sulfite (NiCo2O4@BC-sulfite) to degrade atrazine (ATZ) in the neutral environment. The synergistic coupling of BC and NiCo2O4 endows the resulting composite excellent catalytic activity. 82% of the degradation ratio of ATZ (1 mg/L) could be achieved within 10 min at initial concentrations of 0.6 g/L NiCo2O4@BC, 3.0 mmol/L sulfite in neutral environment. When further supplementing sulfite into the system at 20 min (considering the depletion of sulfite), outstanding degradation efficiency (similar to 100%) were achieved in the next 10 min without any other energy input by the NiCo2O4@BC-sulfite system. The features of the prepared catalysts and the effects of some key parameters on ATZ degradation were systematically examined. A strong inner-sphere complexation ( Co2+/Ni2+-SO32-) was explored between sulfite and the metal sites on the NiCo2O4@BC surface. The redox cycle of the surface metal efficiently mediated sulfite activation and triggered the series radical chain reactions. The generated radicals, in particular the surface-bound radicals were involved in ATZ degradation. High performance liquid chromatography-tandem mass spectrometry (LC-MS) technique was used to detect the degradation intermediates. Density functional theory (DFT) calculations were performed to illustrate the possible degradation pathways of ATZ. Finally, an underlying mechanism for ATZ removal was proposed. The present study offered a low-cost and sustainable catalyst for sulfite activation to remove ATZ in an environmentally friendly manner from wastewater. (C) 2022 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
通讯机构:
[Zhihui Ai] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, PR China
关键词:
Chloronitrobenzenes;Environmental remediation;H(2)O(2);Reduction-oxidation coupling;Zero-valent iron
摘要:
Chloronitrobenzenes (CNBs) are typical refractory aromatic pollutants. The reduction products of CNBs often possess higher toxicity, and the electron-withdrawing substituent groups are detrimental to the ring-opening during the oxidation treatment, leading to ineffective removal of CNBs by either reduction or oxidation technology. Herein we demonstrate a controllable reduction-oxidation coupling (ROC) process composed of zero-valent iron (ZVI) and H(2)O(2) for the effective removal of CNBs from both water and soil. In water, ZVI first reduced p-CNB into 4-chloronitrosobenzene and 4-chloroaniline intermediates, which were then suffered from the subsequent oxidative ring-opening by ·OH generated from the reaction between Fe(II) and H(2)O(2). By controlling the addition time of H(2)O(2), the final mineralization rate of p-CNB reached 6.6×10(-1) h(-1), about 74 times that of oxidation alone (9.0×10(-3) h(-1)). More importantly, this controllable ROC process was also applicable for the site remediation of CNBs contaminated soil by either ex-situ treatment or in-situ injection, and, respectively decreased the concentrations of p-CNB, m-CNB, and o-CNB from 1105, 980, and 94mg/kg to 3, 1, and < 1mg/kg, meeting the remediation goals (p-CNB: < 32.35mg/kg, o-CNB and m-CNB: < 1.98mg/kg). These laboratory and field trial results reveal that this controllable ROC strategy is very promising for the treatment of electron-withdrawing groups substituted aromatic contaminates.
摘要:
Due to the low sensitivity of traditional colorimetric sensors, complex and time-consuming signal amplification processes are often required in the actual detection process. In this work, with the aid of the porous nature of the gel matrix, a unique "All-in-One" ultra-portable colorimetric sensor has been constructed for highly sensitive and instant detection of low-abundance Hg2+ without signal amplification. Here, by dropping the prepared "Pill" sensor into the sample solution, the Hg2+ can specifically trigger the colorimetric reaction, so as to realize the on site instant detection of Hg2+. Under the confinement effect, the porous structure of the gel matrix can serve as a preconcentrator to enrich the analyte, thus enhancing detection sensitivity of the sensor. Additionally, all colorimetric reactants are integrated into a small "Pill", which greatly improves the portability of the sensor. Such an unusual sensor exhibits an outstanding linear response to the concentration in the range between 0.1 and 100 mu M, and the detection limit is as low as 0.04 mu M (S/N = 3). The as fabricated assay is sensitive, easy operation, and versatile. It has been successfully used for measuring Hg2+ in four different actual samples, demonstrating great promise for practical applications. <comment>Superscript/Subscript Available</comment
期刊:
Colloids and Surfaces A: Physicochemical and Engineering Aspects,2022年655:130286 ISSN:0927-7757
通讯作者:
Li Xin<&wdkj&>Gong Jingming<&wdkj&>Lai Guosong
作者机构:
[Liang, Pan; Wang, Yuxin; Li, Xin; Lai, Guosong] Hubei Normal Univ, Coll Chem & Chem Engn, Hubei Key Lab Pollutant Anal & Reuse Technol, Huangshi 435002, Peoples R China.;[Gong, Jingming] Cent China Normal Univ, Inst Environm & Appl Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Li Xin; Lai Guosong] H;[Gong Jingming] K;Hubei Key Laboratory of Pollutant Analysis & Reuse Technology, College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002, PR China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, PR China
关键词:
Double central atom coordination;Electron transfer;g-C3N4;Molecular oxygen activation;Photo-Fenton oxidation
作者机构:
[Liu, Lijuan; Zhang, Lizhi; Gong, Jingming; Yao, Qingfeng; Sun, Hongwei; Hu, Yachen; Li, Xin] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Jingming Gong] K;Key Laboratory of Pesticide and Chemical Biology of the Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
摘要:
A smart temperature stimuli-driven multiplex photoelectrochemical (PEC) assay was constructed for antibiotic resistance genes (ARGs) detection, where the stimuli-responsive gatekeeping by regulating the alternative release of "cargo" allowed for the simultaneous detection of multiple tetracycline resistance gene, using tetA (T(DNA1)) and tetC (T(DNA2)) as the model. Dual temperature-responsive nanoassemblies were embedded in the PEC bioassay as signal DNA tages: one thermoresponsive polymer (poly(N-isopropylacrylamide), PNIPAM)-capped mesoporous silica nanoparticles (MSN) with loading the "cargo" of HgO nanoparticles as signal DNA1 tags (S(DNA1)-PNIPAM@MSN@HgONPs) and the other antimony tartrate (SbT)-anchored silica nanospheres as signal DNA2 tags (S(DNA2)-SbT@SiO(2)NSs). At 20 °C, below the lower critical solution temperature (LCST) of PNIPAM, the "gatekeeper" PNIPAM in S(DNA1)-PNIPAM@MSN@HgONPs was in an ON state, igniting Hg(2+) release through the pore of SiO(2). While at above LCST (40 °C), it was in an OFF state. Likewise, the thermo-dependent dissociation of SbT endowed the grafted S(DNA2) tags switching from the OFF (at 20 °C) to ON state (at 40 °C), igniting SbO(+) release. The released Hg(2+) and SbO(+) triggered the amplified photocurrents due to the structure evolution of the photoactive layer into HgS/ZnS or Sb(2)S(3)/ZnS heterostructure, thus achieving sensitive detection of multiple ARGs: tetA, tetC, tetG, tetM, tetO, tetZ, tetX, and tetW. Combined with heat map analysis, rapid screening of the ARGs profiles in 12 samples could be realized. This bioassay is simple and accessible for multiple genes analysis with the detection limit down to 0.50 nM. And it was successfully applied for measuring tetracycline ARGs in real sludge samples.
通讯机构:
[Jingming Gong] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079, PR China
关键词:
Hydrated electron;Integrated oxidation and reduction;Nitrate;Perfluorooctanoic acid;Reactive nitrogen species
摘要:
The environmental persistence, high toxicity and wide spread presence of perfluorooctanoic acid (PFOA) in aquatic environment urgently necessitate the development of advanced technologies to eliminate PFOA. Here, the simultaneous application of a heterogeneous In(2)O(3) photocatalyst and homogeneous persulfate oxidation (In(2)O(3)/PS) was demonstrated for PFOA degradation under solar light irradiation. The synergistic effect of direct hole oxidation and in-situ generated radicals, especially surface radicals, was found to contribute significantly to PFOA defluorination. Fourier infrared transform (FTIR) spectroscopy, Raman, electrochemical scanning microscope (SECM) tests and density functional theory (DFT) calculation showed that the pre-adsorption of PFOA and PS onto In(2)O(3) surface were dramatically critical steps, which could efficiently facilitate the direct hole oxidation of PFOA, and boost PS activation to yield high surface-confined radicals, thus prompting PFOA degradation. Response surface methodology (RSM) was applied to regulate the operation parameters for PFOA defluorination. Outstanding PFOA decomposition (98.6%) and near-stoichiometric equivalents of fluorides release were achieved within illumination 10h. An underlying mechanism for PFOA destruction was proposed via a stepwise losing CF(2) unit. The In(2)O(3)/PS remediation system under solar light provides an economical, sustainable and environmentally friendly approach for complete mineralization of PFOA, displaying a promising potential for treatment of PFOA-containing water.
作者:
Ning Xie;Dongmei Li;Yaqian Li;Jingming Gong;Xianluo Hu
期刊:
Chemical Engineering Journal Advances,2021年8:100163 ISSN:2666-8211
通讯作者:
Jingming Gong<&wdkj&>Xianluo Hu
作者机构:
[Li D.; Gong J.; Xie N.] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China;[Li Y.; Hu X.] State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China
通讯机构:
[Jingming Gong] K;[Xianluo Hu] S;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
关键词:
Lithium iron phosphate;Lithium metal recovery;Low energy consumption;Solar-assisted electrolysis;Spent batteries
期刊:
Biosensors and Bioelectronics,2021年194:113575 ISSN:0956-5663
通讯作者:
Jingming Gong
作者机构:
[Chen, Yuxin; Gong, Jingming; Jiang, Shumin; Hu, Yachen] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Jingming Gong] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, 430079, PR China
摘要:
An intracellular leakage-trigged signal-on solid-state electrochemiluminescent (ECL) assay is developed for the detection of Escherichia coli (E. coli). A self-assembled multilayer ensemble of N, S co-doped carbon dots -poly dimethyl diallylammonium chloride grafted carbon nanospheres is used as ECL luminophores with peroxydisulfate (PS) ions as coreactants. The incorporation of molecularly imprinted electrospun nanofibers with the multilayer ensemble enables a robust, highly selective solid-state ECL probe without using any expensive and fragile biological receptor. Upon the imprinted E. coli exposed to the assay, under bactericidal effects of PS ions by destroying the integrity of E. coli cell membrane, intracellular leakage K(+)-triggered ECL enhancement is first disclosed via prompting the involved (1)O(2)-mediated ECL process. Benefiting from the ECL enhancement upon increasing the concentration of E. coli, a unique intracellular leakage-trigged signal-on ECL system is created for sensing E. coli. Such a assay is proved to be highly specific and sensitive for sensing E. coli in the concentration range from 5 to 10(7)cfumL(-1), achieving a detection limit of 1cfumL(-1) (S/N=3). This label-free, simple and facile assay provides a promising point-of-care diagnostic tool for pathogen detection.
作者机构:
[Gu, Wenling; Wang, Hengjia; Jiao, Lei; Wu, Yu; Chen, Yuxin; Gong, Jingming; Zhu, Chengzhou] Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan;430079, China;[Hu, Liuyong] School of Materials Science and Engineering, Wuhan Institute of Technology, Wuhan;430205, China;[Du, Dan] School of Mechanical and Materials Engineering, Washington State University, Pullman
摘要:
An elaborated 3D printing "all-in-one" dual-modal immunoassay (3D-AIO) has been constructed for the colorimetric and photoelectrochemical (PEC) detection of alpha-fetoprotein (AFP), which integrates all step-analysis functional components (including immune/enzyme reaction, separation and detection) together using automatic microfluidics. The released ascorbic acid (AA) from the enzyme-linked immunoreactions can induce the aggregation of gold nanoparticles (AuNPs) by reducing cystine into cysteine, serving as the reporting agent of colorimetric assay. Meanwhile, the released AA induces hole-trapping of the photoactive nanostructured ZnIn(2)S(4) (ZIS), thus triggering a noticeable photocurrent enhancement at ZIS modified screen printed electrode (labeled as ZIS/SPE) slotted in PEC detection chamber. By smart controlling, the colorimetric assays exhibits a distinguishable color change once AFP contents in serum exceed its cut-off value (20ngmL(-1)), achieving fast screening and rapid identification purpose for plasma samples as negative or positive, especially in point of care (POC) analysis. And then the PEC immunoassay could be used for more accurate quantitative analysis with the detection limit as low as 0.01ngmL(-1) (S/N=3). The proposed assay offered bimodal readout for realizing both qualitative fast screening and quantitative PEC determination of AFP concentration, thereby meeting the requirements of quick and precise POC analysis. The direct detection of AFP from human blood makes it promising for on-site POC diagnostics.
摘要:
Developing efficient methods to degrade perfluorochemicals (PFCs), an emerging class of highly recalcitrant contaminants, are urgently needed in recent years, due to their persistence, high toxicity, and resistance to most regular treatment procedures. Here, a UV-photolysis system is reported for efficient mineralization of perfluorooctanoic acid (PFOA) via irradiation of ferric nitrate aqueous solution, where in-situ generating *NO2 and the effective Fe(3+)/Fe(2+) redox cycle synergistically play great roles on rapidly mediating the mineralization of PFOA. A fast PFOA removal kinetics with first-order kinetic constants of 2.262 h(-1) is observed at initial PFOA concentration of 5 ppm (50 mL volume), reaching approximately 92 % removal efficiency within only 0.5-h irradiation. Near-stoichiometric fluoride ions liberation and high total organic carbon (TOC) removal efficiency ( approximately 100 %) further validated the capability for completely destructive removal of PFOA. A tentative pathway for PFOA destruction is proposed. This work, by UV photolysis of abundant existing iron/nitrate-based systems in natural environment, provides an economical, sustainable and highly efficient approach for complete mineralization of perfluorinated chemicals.