CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han
Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.
研究领域:
材料科学
·
环境科学
·
化学工程
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-20
·
IF 14.7
Bi Guoshu,Liang Jiaqi,Bian Yunyi,Shan Guangyao,Huang Yiwei,Lu Tao,Zhang Huan,Jin Xing,Chen Zhencong,Zhao Mengnan,Fan Hong,Wang Qun,Gan Boyi,Zhan Cheng
Targeting ferroptosis, an iron-dependent form of regulated cell death triggered by the lethal overload of lipid peroxides, in cancer therapy is impeded by our limited understanding of the intersection of tumour’s metabolic feature and ferroptosis vulnerability. In the present study, arginine is identified as a ferroptotic promoter using a metabolites library. This effect is mainly achieved through arginine’s conversion to polyamines, which exerts their potent ferroptosis-promoting property in an H 2 O 2 -dependent manner. Notably, the expression of ornithine decarboxylase 1 (ODC1), the critical enzyme catalysing polyamine synthesis, is significantly activated by the ferroptosis signal——iron overload——through WNT/MYC signalling, as well as the subsequent elevated polyamine synthesis, thus forming a ferroptosis-iron overload-WNT/MYC-ODC1-polyamine-H 2 O 2 positive feedback loop that amplifies ferroptosis. Meanwhile, we notice that ferroptotic cells release enhanced polyamine-containing extracellular vesicles into the microenvironment, thereby further sensitizing neighbouring cells to ferroptosis and accelerating the “spread” of ferroptosis in the tumour region. Besides, polyamine supplementation also sensitizes cancer cells or xenograft tumours to radiotherapy or chemotherapy through inducing ferroptosis. Considering that cancer cells are often characterized by elevated intracellular polyamine pools, our results indicate that polyamine metabolism exposes a targetable vulnerability to ferroptosis and represents an exciting opportunity for therapeutic strategies for cancer.
研究领域:
肿瘤学
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细胞生物学
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分子生物学
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DOI
PubMed
高影响因子
Scientific Reports
·
2017
·Vol. 7
·期 1
·1-8
·
IF 4.259
Yang Yufang,Shen Dongjun,Long Yijuan,Xie Zhixiong,Zheng Huzhi
Ficin is classified as a sulfhydryl protease isolated from the latex of fig trees. In most cases, a particular enzyme fits a few types of substrate and catalyzes one type of reaction. In this investigation, we found sufficient proofs for the intrinsic peroxidase-like activity of ficin and designed experiments to examine its effectiveness in a variety of scenarios. Ficin can transform peroxidase substrates to colored products in the existence of H 2 O 2 . Our results also indicate that the active sites of peroxidase-like activity of ficin are different from that of protease, which reveals that one enzyme may catalyze more than one kind of substrate to perform different types of reactions. On the basis of these findings, H 2 O 2 releasing from MCF-7 cells was detected successfully. Our findings support a wider application of ficin in biochemistry and open up the possibility of utilizing ficin as enzymatic mimics in biotechnology and environmental monitoring.
研究领域:
生物化学
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酶学
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生物技术
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环境监测
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ruoyun Lin,Fangjie Lv,Hao Zhang,Yang Li,Jiangang Lu,Jiansheng Li
Efficient removal of multiple pollutants from discharged antibiotic wastewater effluents by a single processing unit is highly desirable, yet challenging. In this study, intrinsically synergizing Fenton oxidation and in-situ coagulation were achieved in the tannic acid (TA)/Fe(III)/H 2 O 2 process, demonstrating the simultaneous removal of multiple pollutants over a wide pH range. Under the optimal conditions (TA/Fe(III)/H 2 O 2 = 25 mg/L/0.1 mM/0.5 mM), 95.43 % of SMR and 98.41 % of turbidity were simultaneously removed at pH = 7. Moreover, the applicability of this process was validated by treating a spiked actual secondary effluent. Compared with polymer ferric sulphate coagulation and conventional Fe(II)/H 2 O 2 Fenton, TA/Fe(III)/H 2 O 2 process exhibited significantly enhanced removal performance in terms of SMR, COD, UV 254 and turbidity without any pH adjustment. The mechanism analysis revealed that the introduction of TA can not only promote the iron redox cycle for the production of ∙OH, but also neutralize the charge for the generation of the porous flocs. Due to the bridging of TA, the synergy of Fenton oxidation and in-situ coagulation was achieved in a single processing unit. Finally, the synergy mechanism proposed that a four-step process sequentially proceeded during the treatment. This study may provide new insights into the simultaneous removal of multiple pollutants in the advanced treatment of refractory industrial wastewater.
研究领域:
环境科学
·
废水处理
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DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Yu Liu,Yanan Cao,Cong Zhang,Cheng Ye,Qinglai Bian,Xue Cheng,Hui Xia,Junping Zheng,Hongtao Liu
The inhibition of hydrogen peroxide (H 2 O 2 ) on the cysteine-mediated aggregation of gold nanoparticles (AuNPs) has great potential to rapidly visualize H 2 O 2 and disease-associated biomarkers. However, associated applications have been rigid due to the low cysteine-oxidation efficiency or the insufficient interference-resistance of previous catalysts. Here, we proposed a novel AuNPs colorimetric method termed Fe 2+ -catalyzed H 2 O 2 -preventing aggregation of AuNPs by oxidizing Cysteine (FeHOAuC) for the visible and rapid detection of H 2 O 2 with high specificity. Formed Fe 2+ -cysteine composites in the beginning, Fe 2+ accelerates the oxidation of cysteine by H 2 O 2 with an intramolecular electron-transferring model, and the generated cysteine oxides (including cysteic acid or cystine , dependent on the ratio of cysteine to H 2 O 2 molecules) lose the pro-aggregation effect on AuNPs. Notably, FeHOAuC can quantify 2–30 μM of H 2 O 2 within 5 min, and the monitoring process works well with tolerance to the impact of dissolved oxygen. The FeHOAuC paired with lactate oxidase was successfully used for measuring lactic acids in real sweat samples with a practicable detection window (2–60 μM) and a low variable coefficient (<10%). In summary, FeHOAuC is a feasible platform for rapid and convenient detection of H 2 O 2 and oxidase-specific substrates.
研究领域:
分析化学
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生物传感器
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纳米技术
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生物化学
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DOI
PubMed
高影响因子
CRYSTENGCOMM
·
2017
·Vol. 20
·期 5
·679-688
·
IF 3.474
Huihui Chen,Mei Yang,Sha Tao,Guangwen Chen
A facile, template-free and easily scalable approach has been developed for the preparation of Co3O4 nanorings, which can be divided into two stages: (1) formation of CoOOH nanorings and (2) high-temperature calcination of CoOOH nanorings in air. The key step for the synthesis of Co3O4 nanorings is the formation of CoOOH nanorings, prepared by the oxidation of β-Co(OH)2 nanoplates with H2O2 under strong basic conditions. The plausible growth mechanism governing the formation of CoOOH nanorings was correlated with Ostwald ripening. It was found that the dosage of H2O2 played a vital role in the formation of CoOOH nanorings. To a large extent, other experimental variables including the H2O2 concentration, Co2+ concentration, the molar ratio of Co2+ to OH− and the reaction temperature did not affect the preparation of the CoOOH nanorings. Furthermore, the as-prepared Co3O4 nanorings exhibited superior activity in comparison with Co3O4 nanoplates and commercial Co3O4 towards the catalytic decomposition of H2O2. The apparent rate constant of the as-prepared Co3O4 nanorings was 0.38 min−1, which is 2.2 times the value of Co3O4 nanoplates.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jun Young Kim,Kang Hoon Lee,Jae Won Lee,Imtiaz Afzal Khan,Jong-Oh Kim
In this study, the removal efficiency of chemicals of emerging concerns (CECs) was evaluated under exposure to various doses of UV/H 2 O 2 -based oxidation processes in combination with membrane filtration for three cleaning cycles. Polyethersulphone (PES) and polyvinylidene fluoride (PVDF) materials based membranes were used for this study. The chemical cleaning of the membranes was performed by immersion of the membranes into 1 N HCl followed by adding 3000 mg.L −1 NaOCl for 1hr. Degradation and filtration performance was evaluated using Liquid Chromatography with tandem mass spectrometry (LC-MS/MS) and total organic carbon (TOC) analysis. Membrane fouling analysis for assessing the comparative performance of PES and PVDF membranes was determined by specific fouling and fouling indices evaluation. Membrane characterization results show that the alkynes and carbonyl group formation are due to dehydrofluorination and oxidation of PVDF and PES membranes under the attack of foulants and cleaning chemicals, which resulted in a reduction of fluoride percentage and an increase in sulfur percentage in the PVDF and PES membranes. A decrease in the hydrophilicity of the membranes in underexposed conditions was observed and is consistent with an increase in dose. Degradation results of CECs follow with the highest removal efficiency of chlortetracycline (CTC) followed by atenolol (ATL), acetaminophen (ACT), and caffeine (CAF) degradation due to attack on the aromatic ring and the carbonyl group of CECs by OH exposure. Membrane exposed at 3 mg.L-1 dose of UV/H 2 O 2 -based CECs shows minimum alteration with higher filtration efficiency and lower fouling, particularly in PES membranes.
研究领域:
环境科学
·
材料科学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Mengzhen Song,Jingru Han,Yingzhi Wang,Lungang Chen,YanYan Chen,Xiaoyuan Liao
Fe-based MOFs (Fe-MOFs) are deemed promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, their inferior catalytic activity, iron leaching, and low H2O2 utilization always hinder their application as Fe-based MOF catalysts. In this work, we manipulated the structure of Fe-oxo nodes in MIL-88B(Fe) via a CuI species substitution method, affording a mixed-valence (Cu-incorporated Fe-MOFs) with highly improved Fenton-like performance. It is found that the CuI serves as a shuttle to promote transfer between FeII/FeIII, inducing the formation of a larger amount of stable FeII sites, which was proven by experimental and DFT calculation results. A linear relationship was observed for the Fenton-like performance and the amount of CuI species for the catalysts. The corresponding value of the •OH formation is 2.17 eV for Cu-incorporated MIL-88B(Fe), which is significantly lower than that of MIL-88B(Fe) (2.69 eV). Meanwhile, the enriched CuI species suppress Fe species leaching during the catalytic reaction. The Fe-ion leakage of 0.4Cu@MIL-88B is very tiny (0.01–0.03 mg/L), significantly less than that of MIL-88B (2.00–3.02 mg/L). At the same time, H2O2 utilization for 0.4Cu@ MIL-88B(Fe) is 88%, which is almost 4.4 times that of pure MIL-88B(Fe). This work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for wastewater treatment.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huiru Zhang,Lulu Liu,Hao Zhang,Yinhua Wan,Jianquan Luo
Inspired by the photo-enzyme-coupled catalytic system in chloroplasts, we developed a composite catalyst with both photocatalytic and biomimetic catalytic activity for H 2 O 2 production by loading gold nanoparticles (AuNPs, enzyme mimics) on graphite carbon nitride (GCN, photocatalyst) nanosheets using polyethyleneimine (PEI) as the “bridge”. The introduction of PEI and AuNPs can adjust the electronic structure of GCN, facilitating the rapid separation of photogenerated carriers. Moreover, surface plasmon resonance of AuNPs excited by incident light promotes the activation of glucose molecules, elevating their reactivity with O 2 , thereby improving the glucose oxidase-mimicking catalytic production of H 2 O 2 . Furthermore, the grafting of PEI and the addition of glucose enhance the O 2 adsorption on the catalyst surface. Thus, both biomimetic catalytic and photocatalytic reduction of O 2 to H 2 O 2 are boosted, achieving a significant synergistic enhancement effect of 175%. This study provided a novel design strategy for catalysts and a green routine for efficient H 2 O 2 production.
研究领域:
催化
·
光化学
·
材料科学
·
环境化学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Guanqing Ding,Changlong Li,Wendong Liu,Xiaoxue Zhao,Yuanyuan Jiang,Yizhong Lu
Electrochemical oxygen reduction reaction (ORR) via two-electron pathway is a viable method to produce hydrogen peroxide (H 2 O 2 ). Here, oxidized carbon nanotubes (O-CNTs) rich in oxidized functional groups are obtained by rapid kneading oxidation within two hours. The optimal sample, O-CNTs-7, exhibits remarkable electrocatalytic performance for the H 2 O 2 production under alkaline environment. The O-CNTs-7 shows a high onset potential of 0.74 V (vs. RHE), and could delivers up to 90% selectivity for H 2 O 2 production over a wide voltage window (0.3 V to 0.7 V). In situ attenuated total reflection infrared (ATR-IR) spectroscopy show the certain relationship between potential and the adsorption behavior of *HOOH and *OOH, which confirm the associative two-electron pathway for O-CNTs-7. This study provides a general method to obtain highly oxidized carbon materials with abundant oxygen-containing groups towards highly efficient H 2 O 2 electrosynthesis.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
MOLECULES
·
2026
·Vol. 31
·期 9
·1512
·
IF 5.1
Boyi Ma,Degang Li,Weimin Zhang,Siru Hao
Hydrogen peroxide (H2O2) is widely regarded as a clean and high-value chemical; however, its conventional industrial production remains both energy-intensive and environmentally unsustainable. In this study, sulfur-deficient ZnIn2S4(denoted SDZIS) was developed as an efficient photocatalyst for H2O2generation through oxygen reduction under visible-light irradiation. SDZIS photocatalysts with controllable sulfur-vacancy concentrations were synthesized via a one-step citric-acid-assisted hydrothermal process combined with NaOH etching. The results of transient photocurrent response and electrochemical impedance spectroscopy show that the separation efficiency of charge carriers has been improved. Compared with pristine ZnIn2S4, the optimized SDZIS catalyst achieved a nine-fold enhancement in the H2O2production rate, reaching 2711.81 μmol g−1h−1. Results of experimental and density functional theory calculations suggest that sulfur vacancies can modulate the catalyst work function and the adsorption energy of O2. Comparative experiments indicate that an appropriate concentration of sulfur vacancies can lead to a high H2O2yield. Combined with scavenger tests, DMPO-EPR, and rotating ring disk electrode measurements, these results support a sulfur-vacancy-associated enhancement in charge separation and a tendency toward a superoxide-involved 2e−ORR pathway for H2O2production.
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DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Shi Gang Liu,Shi Mo,Lei Han,Na Li,Yu Zhu Fan,Nian Bing Li,Hong Qun Luo
Ratiometric sensing suffers from less interference and can obtain more accurate results than single-signal assay. Here, a new ratiometric optical sensing strategy for H 2 O 2 detection is developed by etching silver nanoparticles (AgNPs) to deactivate fluorescence resonance energy transfer (FRET) and reduce Rayleigh scattering based on a hyphenated technique of fluorescence and second-order Rayleigh scattering (SRS). The ratiometric detection of H 2 O 2 is achieved through exploiting a hybrid system fabricated by fluorescent carbon dots and silver nanoparticles (CDs/AgNPs). In the CDs/AgNPs system, the fluorescence of CDs is quenched because of FRET, and the scattering is strong due to the intrinsic high light-scattering power of AgNPs. With the introduction of H 2 O 2 , the AgNPs are etched and the CDs are released from the AgNP surface, resulting in the fluorescence enhancement and scattering decline. As a result, ratiometric sensing of H 2 O 2 can be achieved based on the CDs/AgNPs system by simultaneous collection of fluorescence and SRS signals. The sensing system is further used for H 2 O 2 -generation bioanalysis, and as a proof-of-concept, ratiometric assay of glucose and evaluation of glucose oxidase activity are performed successfully. This work provides a new perspective for sensing applications of plasmonic nanoparticles.
研究领域:
分析化学
·
纳米技术
·
生物传感器
·
生物医学工程
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）