Materials
·
2023
·Vol. 16
·期 7
·2606
·
IF 3.4
Wei Cui,Jiahui Fang,Yuanyuan Wan,Xueyu Tao,Litong Guo,Qiyan Feng
In this study, an E-fenton oxidation system based on Co-N co-doped carbon nanotubes (Co-N-CNTs) was designed. The Co-N-CNTs system showed fast degradation efficiency and reusability for the degradation of rhodamine B (RhB). The XRD and SEM results showed that the Co-N co-doped carbon nanotubes with diameters ranging from 40 to 400 nm were successfully prepared. The E-Fenton degradation performance of Co-N-CNTs was investigated via CV, LSV and AC impedance spectroscopy. The yield of H2O2could reach 80 mg/L/h within 60 min, and the optimal voltage and preparation temperature for H2O2yield in this system was −0.7 V (vs. SCE) and 800 °C. For the target pollutant of RhB, the fast removal of RhB was obtained via the Co-N-CNTS/E-Fenton system (about 91% RhB degradation occurred during 60 min), and the •OH played a major role in the RhB degradation. When the Fe2+concentrations increased from 0.3 to 0.4 mM, the RhB degradation efficiency decreased from 91% to about 87%. The valence state of Co in the Co-N-C catalyst drove a Co2+/Co3+cycle, which ensured the catalyst had good E-Fenton degradation efficiency. This work provides new insight into the mechanism of an E-Fenton system with carbon-based catalysts for the efficient degradation of RhB.Keywords:carbon nanotubes;E-Fenton;rhodamine B;degradation;mechanism
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Environmental Science-Nano
·
2023
·Vol. 10
·期 5
·1428-1440
·
IF 7.3
Xixi Chen,Yanjun Li,Wanyi Fu,Shuanghong Tian,Yulong Yang,Kai Yang,Xuanbo Xu,Xihui Zhang
The importance of nonradical Fenton-like catalysis in environmental fields has motivated research for effective singlet oxygen (1O2) production, but realizing the accurate design and regulation of active sites for manipulating oriented 1O2 generation is still highly challenging. In this study, α-, β-, and γ-MnO2 catalysts with different oxygen vacancy (OV) abundance were fabricated to activate H2O2 to generate 1O2 for the degradation of oxytetracycline (OTC). The OV-rich α-MnO2 had a high OTC removal efficiency (>93.5%) at the pH range from 4.0 to 11.0. Moreover, α-MnO2 exhibited great applicability for a real water matrix, and the total removal of various kinds of emerging contaminants from hospital wastewater reached up to 97.4%. The excellent performances of α-MnO2 were attributed to the rich contents of OVs that induced the oriented generation of 1O2. Theoretical density functional theory (DFT) calculations validated that the OV-rich α-MnO2 had the highest H2O2 adsorption ability (−1.39 eV) and the lowest energy barrier (0.41 eV) for the dissociation of *OH to form the *O intermediate, which promoted the oriented formation of 1O2. This work provides a strategy of manipulating the oriented generation of 1O2 towards water decontamination via regulating the abundance of oxygen vacancies in α-MnO2 nanocatalysts.
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WATER RESEARCH
·
2023
·
IF 12.8
Xixi Chen,Wanyi Fu,Zhichao Yang,Yulong Yang,Yanjun Li,Hui Huang,Xihui Zhang,Bingcai Pan
Hydrogen peroxide (H 2 O 2 ) is the most commonly used oxidant in advanced oxidation processes for emerging organic contaminant degradation. However, the activation of H 2 O 2 to generate reactive oxygen species is always accompanied by O 2 generation resulting in H 2 O 2 waste. Here, we prepare a Ti doped Mn 3 O 4 /Fe 3 O 4 ternary catalyst (Ti-Mn 3 O 4 /Fe 3 O 4 ) to create abundant oxygen vacancies (OVs), which yields electron delocalization impacts on enhancing the electrical conductivity, accelerating the activation of O 2 to produce H 2 O 2 . In Ti-Mn 3 O 4 /Fe 3 O 4 /H 2 O 2 system, OVs-mediated O 2 /O 2 •− /H 2 O 2 redox cycles trigger the activation of locally generated O 2 , boost the regeneration of O 2 •− and on site produce H 2 O 2 for replenishment. This leads to a 100% removal of tiamulin in 30 min at an unprecedented H 2 O 2 utilization efficiency of 96.0%, which is 24 folds higher than that with Fe 3 O 4 /H 2 O 2 . Importantly, further integration of Ti-Mn 3 O 4 /Fe 3 O 4 catalysts into membrane filtration achieved high rejections of tiamulin (> 83.9%) from real surface water during a continuous 12-h operation, demonstrating broad pH adaptability, excellent catalytic stability and leaching resistance. This work demonstrates a feasible strategy for developing OVs-rich catalysts for improving H 2 O 2 utilization efficiency via activation of locally generated oxygen during the Haber-Weiss reaction.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 30
·11325-11334
·
IF 4.569
Yale Hong,Qinfeng Tao,Yuan-Yuan Liu,Zhuo Wang,Haifang Wang,Lining Sun
Chemodynamic therapy (CDT) can convert endogenous hydrogen peroxide (H2O2) to highly reactive hydroxyl radical (˙OH) through Fenton or Fenton-like reaction to kill tumor cells, which is a promising anticancer strategy. However, the limited H2O2 and overexpressed glutathione (GSH) in tumor cells make CDT ineffective. Here, an efficient nanocomposite, UCN@CuO2–GOx (UCCuG), was synthesized, realizing both starvation therapy and H2O2 self-supplying CDT in vitro. In this case, the glucose oxidase (GOx) of the nanocomposite could consume glucose for starvation therapy after the UCCuG nanocomposite entered tumor cells. In addition, the acidic environment of the lysosome triggered the release of Cu2+ and H2O2 by the decomposition of UCCu; then, Cu2+ was reduced to Cu+ by GSH in tumor cells; and finally, Cu+ catalyzed the released H2O2 to generate ˙OH for CDT. The in vitro experiments demonstrated starvation-enhanced CDT with remarkable results. Meanwhile, under 980 nm laser irradiation, the upconversion luminescence signal of UCN in the UCCuG nanocomposite was reduced due to the CuO2–GOx coating, while it gradually recovered after the UCCuG nanocomposite reacted with glucose and GSH under the tumor microenvironment (TME). Such a luminescent intensity recovery process is expected to monitor the TME-activated therapeutic effect in real time. This strategy may solve the problem of insufficient CDT efficacy caused by limited endogenous H2O2 and overexpressed GSH in tumor cells. This multifunctional nanocomposite demonstrates the promising application of starvation-enhanced CDT in tumor treatment.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Xuyun Lu,Xiaorong Zhu,Zhangyu Ma,Zhiwen Che,Yafei Li,Jianchun Bao,Ying Liu
Carbon-based nanomaterials are well-recognized catalysts for H 2 O 2 production though remain insufficient for practical applications, and their photothermal effect is usually ignored. Herein, two typical carbon nanomaterials, mesoporous carbon hollow spheres (MCHS) and carbon hollow spheres (CHS), are selectively synthesized to explore the influence of oxygen-containing surface functional groups, mesoporous structure and photothermal effect on their electrocatalytic and application ability. It was found that the abundant oxygen-containing surface functional groups in MCHS can optimize the adsorption energy of *OOH while the mesoporous structure of MCHS provides plenty of electrochemical active sites, both of which significantly enhance H 2 O 2 production selectivity of the MCHS (96.0% versus 87.0% for the CHS counterpart). Furthermore, the notable photothermal effect of the MCHS can promote the generation of more ·OH radicals and accelerate related reaction kinetics (3.5 times higher than those without NIR light irradiation) under the in-situ electro-Fenton degradation of methyl orange. As a result, remarkable degradation efficiency of 98.1% was achieved for the MCHS under the illumination of near infrared (NIR) light, outperforming those without NIR light irradiation (70.1% for MCHS and 54.7% for CHS). By integrating oxygen-containing surface functional groups, mesoporous structure and photothermal effect, this work achieves remarkable H 2 O 2 production ability and pollutant degradation application simultaneously, providing a new avenue for the design of advanced electrocatalysts and may promote their energy related applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yi Yang,Bicheng Zhu,Libo Wang,Bei Cheng,Liuyang Zhang,Jiaguo Yu
Artificial photosynthesis offers a promising strategy for converting solar energy into environmental-friendly H 2 O 2 . Herein, robust photocatalytic H 2 O 2 production through dioxygen reduction is achieved, reaching a high H 2 O 2 yield of 873 μmol L −1 h −1 . The photocatalyst was prepared by in-situ chemical vapor deposition of N, S co-doped graphene on TiO 2 nanofibers. Thanks to the intimate interface with large area and Schottky junction, the H 2 O 2 yield of the composite can be increased by eight times than that of pristine TiO 2 . Experimental results and density functional theory calculations clarify that the strong synergistic effect between the doped N and S atoms provides abundant active sites to facilitate the electron transfer, promote the adsorption of O 2 molecules, and restrain the decomposition of formed H 2 O 2 by suppressing H 2 O 2 adsorption. This work not only provides a novel approach to build close contact between photocatalyst and co-catalyst, but also develops a highly efficient photocatalyst for H 2 O 2 production.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Ying Cai,Jinhong Fan,Zhigang Liu
This study constructed a FeS-based Fenton-like process to explore the degradation of TTC in the presence of copper ions . The acidic condition of pH 3 was more favorable to the H 2 O 2 decomposition and TTC degradation , and it was slightly enhanced by Cu(II). The production of •OH from H 2 O 2 was revealed through radical scavenging and benzoic acid probe experiments, and the ratio of H 2 O 2 decomposition to •OH production was about 1–1.5, which is comparatively consistent with the theoretical ratio. FeS-based Fenton process was proved to be a homogenous system, the slow release of Fe(II) source and the autocatalytic cycle of Fe(III) to Fe(II) resulting from the reductive species of TTC and dissolved S(-II) improved the production of •OH and the degradation of TTC, which was proved by comparing TTC degradation, TOC removal, H 2 O 2 decomposition and Fe(II) concentration with different iron sources (FeS, Fe(II) and Fe(III)) and external addition of dissolved S(-II). The possible degradation pathways of TTC were subsequently inferred according to the detected products by LC-MS. Understanding these autocatalytic processes is essential to reveal the transformation of redox-active substances in environments and may have potential significance in applying FeS-based Fenton-like process for the treatment of wastewater containing reductive organic matters.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Suhang Jiang,Lijuan Tan,Yujia Tong,Lijian Shi,Weixing Li
Hydrogen peroxide synthesis by electro-reduction of O 2 to substitute the current anthraquinone process has attracted a great deal of attention. Low oxygen utilization rate and low hydrogen peroxide production remain obstacles to electro-Fenton application. In situ H 2 O 2 generated by electrochemical reaction depends on the electrochemical performance of the cathode and the structure of the reactor. Here, novel graphite felt (GF) modified by La-doped CeO 2 (La–CeO 2 ) was developed as a cathode. A new double chamber electro-Fenton reactor was proposed, where an organic ultrafiltration membrane was used to prevent H 2 O 2 from spreading to the anode. The effects of hydrothermal temperature, time and urea concentration on the electrochemical properties of graphite felt were investigated. The accumulated concentration of H 2 O 2 on the modified cathode reached 218.4 mg·L –1 in 1 h when the optimal conditions of hydrothermal temperature 120 °C and urea concentration 0.55% (mass) in 24 h. The degradation rate of methyl orange reached 98.29%. The new electro-Fenton reactor can efficiently produce hydrogen peroxide to degrade various organic substances and has a high potential for treating wastewater in the chemical industry.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 11
·5176-5187
·
IF 3.925
Yuzhen Li,Shaojie Wang,Yunsheng Xia,Lizhen Gao
A series of Z-scheme CuSnO3/g-C3N4 heterojunctions were synthesized by a precipitation–calcination method. Morphological features, chemical composition, optical properties and crystallographic information of the prepared materials were obtained using scanning electron microscopy (SEM), transmission electron microscopy (TEM), powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), UV–Vis diffuse reflection spectroscopy (UV-Vis DRS), and photoluminescence spectroscopy (PL). The as-fabricated catalysts assisted by H2O2 showed remarkably enhanced photocatalytic performance for the degradation of tetracycline (TC) under visible light irradiation. The 20 wt% CuSnO3/g-C3N4 composite exhibited the highest photocatalytic degradation activity, which could be up to 93.6% at 60 min for the degradation of TC under visible light irradiation. Reactive species scavenging experiments revealed that superoxide radicals were the main active species during the photocatalytic process. This work will be useful for the design of other direct Z-scheme photocatalytic systems for applications in energy conversion and environmental remediation.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Huang Wei,Xu Yun,Sun Yimin
The rational design and construction of high-performance flexible electrochemical sensors based on hierarchical nanostructure functionalized microelectrode systems are of vital importance for sensitive in situ and real-time detection of biomolecules released from living cells. Herein, we report a novel and facile strategy to synthesize a new kind of high-performance microelectrode functionalized by dual nanozyme composed of rime-like Cu2(OH)3NO3 wrapped ZnO nanorods assembly [Cu2(OH)3NO3@ZnO], and explore its practical application in electrochemical detection of hydrogen peroxide (H2O2) released from living cells. Benefiting from the merits of the unique hierarchical nanohybrid structure and high catalytic activities, the resultant Cu2(OH)3NO3@ZnO-modified AGF microelectrode shows remarkable electrochemical sensing performance towards H2O2 with a low detection limit of 1 μM and a high sensitivity of 272 μA cm−2 mM−1, as well as good anti-interference capability, long-term stability, and reproducibility. These properties enabled the proposed microelectrode-based electrochemical platform to be applied for in situ amperometric tracking of H2O2 released from different types of human colon cells, thus demonstrating its great prospect as a sensitive cancer cell detection probe for the early diagnosis and management of various cancer diseases.
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Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 11
·2544-2556
·
IF 7.779
Xuwen Da,Zhanhua Wang,Yao Jian,Chao Zhang,Yuanjun Hou,Yishan Yao,Xuesong Wang,Qianxiong Zhou
The bottleneck problems of chemodynamic therapy (CDT) are the dependence on an acidic pH (2.0–4.0), insufficient H2O2 level in tumor tissues, and potential systematic toxicity of inorganic nanomaterials-based CDT agents. In this study, the new tricks of two old compounds, i.e. [Ru(phen)2(PIP-OCH3)](PF6)2 (Ru3, phen = 1,10-phenanthroline, PIP-OCH3 = 2-(4-methoxy phenyl)-1H-imidazo[4,5-f][1,10]phenanthroline) and Fe(tpy)Cl3 (tpy = 2,2′:6′,2′-terpyridine), were harnessed to construct an ideal CDT system. Ru3 was able to efficiently photo-catalyze NADH oxidation accompanied by the production of H2O2in situ with a high yield of 73.2%, which can be converted into cytotoxic hydroxyl radicals by the biocompatible Fe(tpy)Cl3 at a neutral pH. By loading both Ru3 and Fe(tpy)Cl3 in tumor-targeting bovine serum albumin (BSA), the obtained BSA@Fe/Ru nanoparticles exhibited a highly efficient, selective, and photo-controlled CDT activity both in vitro and in vivo. This work may provide new sights for overcoming the issues confronted in CDT.
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ANALYST
·
2022
·Vol. 147
·期 9
·1815-1823
·
IF 5.227
Yue Wang,Cheng Cheng,Ruofei Ma,Zhangrun Xu,Yukihiro Ozaki
Visualization of signaling molecules in single living cells is crucial for understanding cellular metabolism and physiology, which can provide valuable insights into early diagnoses and treatments of diseases. Highly sensitive in situ monitoring of intracellular analytes released from single living cells by virtue of label-free nanosensors is urgently needed, which can avoid interferences from molecular labeling. Here, we proposed an ultrasensitive strategy for in situ imaging of intracellular H2O2 in single living cancer cells by surface-enhanced Raman scattering (SERS) spectroscopy with the utilization of label-free Fe3O4@Ag core–satellite nanoparticles (NPs). The Fe3O4@Ag NPs can efficiently and selectively catalyze the oxidation of the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2. Additionally, they exhibit excellent SERS activity that allows for in situ monitoring of intracellular H2O2 in living cells through establishing the correlation between the H2O2 level and the SERS intensity of the catalytic oxidation product of TMB. The H2O2 concentration is revealed through the SERS intensity of oxidized TMB with a good linear response in a wide range from 1 fM to 1 mM. Moreover, the intracellular H2O2 level in live cancer cells and imaging of the distribution of H2O2 inside single cells can be achieved by using such a label-free nanosensor based strategy. Our work demonstrates that the label-free Fe3O4@Ag NP-based SERS imaging and quantification strategy is a promising and powerful approach to assess intracellular H2O2 in living cells and allows us to monitor single-cell signaling molecules with nanoscale resolution.
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