INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Dun Fu,Tonni Agustiono Kurniawan,Herong Gui,Heng Li,Songbao Feng,Qingbiao Li,Yuanpeng Wang
This study investigated the effects of pyrolysis temperature on the physicochemical properties of pyrolyzed hydrochars (PHCs) and H2O2-catalyzed tetracycline (TC) degradation in a combined treatment with PHC and CuxO@PHCs. The effects of pH on TC degradation by CuxO@PHCs were also evaluated in the presence of H2O2 and compared with that by CuxO@GAC. To analyze their physicochemical changes due to the oxidant, the carbocatalysts were characterized using scanning electron microscopy (SEM), X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) analysis, and Fourier transform infrared (FTIR) spectroscopy. To sustain its cost-effectiveness, spent CuxO@PHC700 was regenerated using NaOH. Based on the characterization results, increasing the pyrolysis temperature from 300 to 700 °C enlarged their specific surface area and pore volume. The X-ray diffraction (XRD) analysis revealed that the Cu anchored in the carbocatalyst existed as Cu2O/CuO. The H2O2-catalyzed degradation by CuxO@PHC700 (0.231 min–1) was faster than that by CuxO@PHC500 (0.107 min–1), CuxO@PHC300 (0.013 min–1), and CuxO@GAC (0.041 min–1) (p ≤ 0.05; analysis of variance (ANOVA)). The maximum TC removal was achieved by CuxO@PHC700 at pH 6 due to the H-bonding and Cu-bridging effects between the Cu-loaded carbocatalyst and TC molecules in solutions. Treated effluents could meet the maximum discharge limit standard of 1 mg/L set by the local legislation. After the first regeneration, the spent CuxO@PHC700 could attain about 96% of TC degradation. This implies that the saturated carbocatalyst still had promising catalytic activity for reuse. Overall, CuxO@PHC is a cost-effective option for TC removal from contaminated water.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 51
·77771-77787
·
IF 5.19
Yu Jinming,Yan Weiwen,Zhu Bin,Xu Zimu,Hu Shuheng,Xi Wenhao,Lan Yan,Han Wei,Cheng Cheng
Carbamazepine (CBZ) is a typical psychotropic pharmaceutical which is one of the most commonly detected persistent pharmaceuticals in the environment. The degradation of CBZ in the aqueous solution was studied by a direct current (DC) gas–liquid phase discharge plasma combined with different catalysts (H 2 O 2 or Fe 2+ ) in this study. The concentrations of reactive species (H 2 O 2 , O 3 , and NO 3 − ) and •OH radical yield in the liquid were measured during the discharge process. The various parameters that affect the degradation of CBZ, such as discharge powers, initial concentrations, initial pH values, and addition of catalysts, were investigated. The energy efficiency was 25.2 mg·kW −1 ·h −1 at 35.7 W, and the discharge power at 35.7 W was selected to achieve the optimal balance on the degradation effect and energy efficiency. Both acidic and alkaline solution conditions were conducive to promoting the degradation of CBZ. Both H 2 O 2 and Fe 2+ at low concentration (10–100 mg/L of Fe 2+ , 0.05–2.0 mmol/L of H 2 O 2 ) were observed contributing to the improvement of the CBZ degradation rate, while the promotional effect of CBZ degradation was weakened even inhibition would occur at high concentrations (100–200 mg/L of Fe 2+ , 2.0–5.0 mmol/L of H 2 O 2 ). The degradation rate of CBZ was up to 99.1%, and the total organic carbon (TOC) removal efficiency of CBZ was up to 67.1% in the plasma/Fe 2+ (100 mg/L) system at 48 min, which suggested that high degradation rate and mineralization efficiency on CBZ could be achieved by employing Fe 2+ as a catalyst. Based on the intermediate products identified by Ultra Performance Liquid Chromatography Tandem Mass Spectrometry (UPLC–MS), the possible degradation pathways were proposed. Finally, the growth inhibition assay with Escherichia coli ( E. coli ) showed that the toxicity of plasma/Fe 2+ -treated CBZ solution decreased and a relatively low solution toxicity could be achieved. Thus, the plasma/catalyst could be an effective technology for the degradation of pharmaceuticals in aqueous solutions.
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Journal of Environmental Sciences
·
2022
·
IF 6.796
Jie Xu,Yang Guo,Qian Yang,Xueling Bai,Runhua Lu,Menghui Liu,Zichen Kuang,Luo Zhang,Jing Li
Ultraviolet/persulfate (UV/PS) and Ultraviolet/hydrogen peroxide (UV/H 2 O 2 ) have attracted much attention in recent years as advanced oxidation processes for water treatment. However, it is not all clear how these two methods affect the formation of cyanogen chloride (CNCl) in the subsequent water chlorination process. In this study, it was found that both UV/H 2 O 2 and UV/PS pre-oxidation promoted the formation of CNCl in six actual water samples collected from urban rivers. Glycine, uric acid, arginine and histidine were investigated as the model compounds to explore the effects of different methods on the production of CNCl. The results showed that compared with chlorination alone, pre-oxidation by UV/H 2 O 2 and UV/PS can reduce the production of CNCl for glycine and uric acid by up to 95% during post-chlorination process. However, they can greatly promote the formation of CNCl for arginine and histidine by up to 120-fold. In a more detailed investigation, pre-oxidation of histidine formed highly reactive intermediates to chlorine, leading to increased CNCl formation and chlorine consumption. The results showed that the precursors of CNCl was altered after pre-oxidation, and need to be re-evaluated.
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高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 5
·2661-2672
·
IF 9.3
Songcheng Bo,Haoyi Lin,Jiaxing Zhang,Weiping Liao,Kaixuan Yang,Ting Su,Hongying Lü,Zhiguo Zhu
Oxidative desulfurization is an appealing alternative technology to eliminate organic sulfides in fuel oil in response to environmental and economic requirements. The supported metal oxide catalysts generally possess low catalytic activity and/or deactivation due to the loss and sintering of their metal oxides during the reaction or removal of carbon deposition at elevated temperature. In this work, beta zeolite-fixed MoO3 (MoO3@beta) was hydrothermally synthesized via structural reconstruction. A series of characterizations confirmed that MoO3 nanoparticles with an ultrasmall crystal size of 1.5–2.5 nm were fixed into the beta zeolite. Owing to the small particle size of MoO3, the MoO3@beta material exhibited nearly three times higher catalytic activity, weight-based space–time-yield, and active site-based turnover frequency than an impregnated MoO3/beta sample with MoO3 in an extra-framework position during the process of oxidative desulfurization with the oxidant H2O2. As for the oxidant molecular O2, MoO3@beta also possessed superior catalytic activity in a deep eutectic solvent under mild reaction conditions of 90 °C and ambient pressure, regardless of the model oil or actual fuel oil. Besides, excellent reusability was observed for the MoO3@beta catalyst via the elimination of carbon deposition through simple calcination, resulting from its unique feature to resist the loss and sintering of MoO3 fixed in the zeolite. More importantly, the catalytic mechanism of MoO3@beta was also revealed. This work opens a new avenue for effectively synthesizing zeolite-fixed metal oxide and establishing a green heterogeneous reaction system for catalytic oxidations.
研究领域:
催化
·
环境化学
·
材料科学
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 6
·2558-2568
·
IF 2.7
Shiman Zhou,Qianqian Zhu,Denan Li,Lifeng Zhang,Yanshuo Li,Zhenxin Zhang
Tetrabromobisphenol A (TBBPA), a prevalent brominated flame retardant, poses significant environmental and health risks, necessitating its removal. In this study, WO3 with different structures was synthesized for TBBPA photodegradation under visible light using H2O2 and O2 as oxidants. The catalyst exhibited robust stability and reusability, rendering it suitable for practical applications. The crystalline structure and surface structure of WO3 controlled its catalytic activity towards TBBPA photodegradation. Monoclinic WO3 with the (022) plane was found to be the most active for ˙O2− active species generation from H2O2 and thus active for TBBPA degradation. Degradation product analysis showed that the catalyst was active not only for the removal of TBBPA, but also for the debromination of TBBPA. Nearly 100% debromination was achieved.
研究领域:
环境科学
·
材料科学
·
化学工程
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高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Xiaoyu Wang,Li Qin,Minjie Lin,Hang Xing,Hui Wei
While breakthroughs in peroxidase-like nanozymes for bioanalysis have been made, most of current nanozyme biosensing systems are based on a single signal output. Such sensing systems could be easily influenced by environmental and personal factors. We envision that nanozyme sensing systems with ratiometric signal outputs would provide more reliable and robust sensing performance. Herein, to construct such ratiometric sensing systems, three fluorescent graphitic carbon nitride (C3N4)-based nanozymes (i.e., C3N4–Ru, C3N4–Cu, and C3N4–hemin) with excellent peroxidase-like activities were prepared. These fluorescent nanozymes emitted a fluorescence at 438 nm when excited at 385 nm. Interestingly, when o-phenylenediamine (OPD) was catalytically oxidized to oxidized OPD (OPDox) in the presence of H2O2 and nanozymes, the OPDox not only emitted an emerging fluorescence at 564 nm but also quenched the fluorescence at 438 nm of the nanozymes. We therefore employed the ratio of the fluorescent intensity at 564 and 438 nm (i.e., F564/F438) as the signal output to construct the ratiometric biosensing systems. First, we used the C3N4–Ru nanozyme to construct the ratiometric H2O2 sensing system, which showed not only the enhanced robustness but also wider linear range and better sensitivity than most reported H2O2 sensors based on nanozymes. Second, with the assistance of glucose oxidase, glucose can be detected by such ratiometric sensing systems. Third, we used three different C3N4-based nanozymes to construct ratiometric sensor arrays for the detection and discrimination of five phosphates. This study provides new insights for constructing robust nanozyme biosensing systems.
研究领域:
生物化学
·
纳米医学
·
分析化学
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高影响因子
Biomaterials Science
·
2021
·Vol. 9
·期 7
·2647-2657
·
IF 6.843
Xiaojuan Wang,Xuejian Zhou,Kai Yang,Qiong Li,Rongxin Wan,Guoying Hu,Jin Ye,Yue Zhang,Jiahui He,Hanqing Gu,Yongfang Yang,Lei Zhu
In this study, UiO-66-NH2 metal–organic framework (MOF) nanoparticles with peroxidase and oxidase mimetic activities were incorporated into a chitosan (CS) matrix by a simple and environmentally friendly method. The UiO-66-NH2/CS composite membrane possesses the peroxidase mimicking activity in the presence of traces of H2O2, thus resulting in good antibacterial properties. Intriguingly, 30 min of UV pre-irradiation of the UiO-66-NH2/CS composite membrane, in the absence of H2O2, still leads to a good antibacterial activity. This was attributed to the oxidase mimetic activity and the peroxidase mimicking activity of UiO-66-NH2. In such a way, the side effects of direct exposure to UV irradiation and H2O2 can be avoided for wound-healing treatments. The antibacterial mechanism was further proved by antibacterial experiments, TMB·2HCl color development experiments, reactive oxygen species generation tests and electron spin resonance tests. As a potential medical antibacterial dressing, in vitro membranes were also investigated.
研究领域:
材料科学
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纳米技术
·
生物材料
·
生物医学工程
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高影响因子
Nature Protocols
·
2018
·Vol. 13
·期 10
·2362-2386
·
IF 12.423
Zou Yejun,Wang Aoxue,Shi Mei,Chen Xianjun,Liu Renmei,Li Ting,Zhang Chenxia,Zhang Zhuo,Zhu Linyong,Ju Zhenyu,Loscalzo Joseph,Yang Yi,Zhao Yuzheng
Cellular oxidation–reduction reactions are mainly regulated by pyridine nucleotides (NADPH/NADP + and NADH/NAD + ), thiols, and reactive oxygen species (ROS) and play central roles in cell metabolism, cellular signaling, and cell-fate decisions. A comprehensive evaluation or multiplex analysis of redox landscapes and dynamics in intact living cells is important for interrogating cell functions in both healthy and disease states; however, until recently, this goal has been limited by the lack of a complete set of redox sensors. We recently reported the development of a series of highly responsive, genetically encoded fluorescent sensors for NADPH that substantially strengthen the existing toolset of genetically encoded sensors for thiols, H 2 O 2 , and NADH redox states. By combining sensors with unique spectral properties and specific subcellular targeting domains, our approach allows simultaneous imaging of up to four different sensors. In this protocol, we first describe strategies for multiplex fluorescence imaging of these sensors in single cells; then we demonstrate how to apply these sensors to study changes in redox landscapes during the cell cycle, after macrophage activation, and in living zebrafish. This approach can be adapted to different genetically encoded fluorescent sensors and various analytical platforms such as fluorescence microscopy, high-content imaging systems, flow cytometry, and microplate readers. A typical preparation of cells or zebrafish expressing different sensors takes 2–3 d; microscopy imaging or flow-cytometry analysis can be performed within 5–60 min.
研究领域:
细胞生物学
·
分子生物学
·
生物化学
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 3
·1-10
·
IF 6.408
Wang Lijun,Zhou Hong,Wu Xue,Song Yanfei,Huang Yukun,Yang Xiao,Chen Xianggui
A novel colorimetric aptasensor has been developed for highly sensitive tetracycline (TC) detection based on the peroxidase-like activity of Fe 3 O 4 @Cu nanoparticles and “sandwich” oligonucleotide hybridization. The Fe 3 O 4 @Cu nanoparticles with high peroxidase-like activity were successfully synthesized under mild conditions. Then, a “sandwich” oligonucleotide hybridization probe (a short amino-modified complementary sequence of a portion of the TC aptamer (cDNA1), TC aptamers, and a long complementary to 5′ terminal TC aptamer sequence (cDNA2)) was created in 96-wells plates via DNA hybridization in the absence of TC from the detection system. The unique “sandwich” oligonucleotide hybridization probe adsorbed large numbers of Fe 3 O 4 @Cu nanozymes while further enhancing its peroxidase-like activity. Based on the 3,3′,5,5′-tetramethylbenzidine (TMB)-hydrogen peroxide (H 2 O 2 ) reporting system, the blue color of the solution decreased linearly with the increase of TC concentration, ranging from 10 −3 to 10 3 μg/L with an ultralow limit of detection (LOD) of 0.91 ng/L (2 pM). The proposed method was successfully applied to detect TC in spiked milk samples, with recoveries of 81.8 to 112%, demonstrating the excellent potential for highly sensitive TC detection in milk. Graphical abstract
研究领域:
分析化学
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纳米技术
·
环境科学
·
食品安全
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Yonghong Wang,Zeyang Fang,Ge Ning,Shaoming Mao,Yaohui Wu,Shun Wu,Gao-Qiang Liu
After successively introducing elements of a triple-helix aptamer probe (TAP) and a luminol–hydrogen peroxide (H 2 O 2 ) solution, we proposed a brand-new chemiluminescence (CL)-based biosensor for the assay of ochratoxin A (OTA). Primarily, the TAP contains an aptamer loop, two DNA segment stems, and a triplex-forming oligonucleotide (signal probe). In the presence of a target, the aptamer sequence binds to the target with an impressive affinity. This association leads to a conformational change in the TAP, thus releasing the signal probe. Sequentially, with the participation of hemin and potassium ions, the dissociated probe forms into a G-quadruplex structure that is capable of catalyzing luminol to produce CL mediated by H 2 O 2 . In contrast, in the absence of the target, a low background signal remains. Using this approach of combining a novel TAP switch with a G-quadruplex-catalyzed luminol-H 2 O 2 system, we presented a label-free and signal-on CL strategy for the measurement of OTA. Under optimal conditions, the gradually strengthened signal maintained a linear dependence on target concentrations ranging from 0.1 ng/mL to 2.0 ng/mL, and the detection limit was as low as 0.07 ng/mL. This newly designed, simple, and cost-effective protocol affords high sensitivity, specificity, suitability, and efficacy for biosensing. Thus, this protocol is attractive for a range of target quantifications, with only the matched aptamer requiring replacement (no redesign of signal probes).
研究领域:
分析化学
·
食品安全
·
生物技术
·
分子诊断
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高影响因子
ACS Nano
·
2024
·
IF 15.8
Xu Li,Wenlong Tan,Jinsong Fan,Kun Li
Although the past decade has witnessed a rapid development of oxidoreductase-mimicking nanozymes, the mimicry of cofactors that play key roles in mediating electron and proton transfer remains limited. This study explores how surface Au–H species conjugated to Au nanoparticles (NPs) that imitate formate dehydrogenase (FDH) can serve as cofactors, analogous to NADH in natural enzymes, offering diverse possibilities for FDH-mimicking Au nanozymes to mimic various enzymes. Once O2 is present, Au–H species assist Au NPs to complete the on-demand H2O2 generation for cascade reactions. Alternatively, when oxidizing organic molecules are introduced as substrates, Au–H species confer nitro reductase- and aldehyde reductase-like activities on Au NPs under anaerobic conditions. Furthermore, similar to the dehydrogenase–NADH complex, Au NPs possessing Au–H species are gifted with esterase-like activity for ester hydrolysis. By revealing that Au–H species are prosthetic groups for FDH-mimicking Au nanozymes, this work may inspire explorations into future self-generated cofactor mimics for nanozymes, thereby circumventing the need for exogenous cofactors.
研究领域:
催化
·
生物化学
·
纳米技术
·
酶学
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高影响因子
ANALYST
·
2024
·
IF 3.6
Haiying Cai,Peiting Dong,Xiuping Li,Lulu Wang,Tao Li
It is known that the abnormal expression of specific cellular miRNAs is closely related to cell apoptosis, and so monitoring the level change of these miRNAs can in principle be used to evaluate the process of apoptosis stimulated by drugs. Towards this goal, here we construct an ultrasensitive electrochemiluminescence (ECL) nanoplatform via the target miRNA-triggered immobilization of spherical nucleic acid enzymes (SNAzymes) onto tetrahedral DNA nanostructures on the electrode surface, which catalyzes the luminol–H2O2 reaction to output an ECL signal. This enables the sensitive and specific detection of two apoptosis-related miRNAs, miR-21 and miR-133a, with a detection limit of 33 aM. Furthermore, we employed the developed ECL nanoplatform to monitor the levels of these two miRNAs inside cancer cells stimulated by DOX, showing that the level of miR-21 decreases, while that of miR-133a increases in the early apoptotic cells. This difference highlights the distinct roles of the two target miRNAs, where miR-21 promotes the early apoptosis of cancer cells, whereas miR-133a suppresses it, providing new insight into cell physiological processes.
研究领域:
生物技术
·
纳米技术
·
分子生物学
·
癌症研究
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高影响因子
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