Advanced Science
·
2022
·Vol. 10
·期 2
·2204079
·
IF 17.521
Xu Chen,Ziqi Tian,Qihao Yang,Linjuan Zhang,Qiu Yang,Liang Chen,Zhiyi Lu
The reuse of powdered activated carbon (PAC) vitally determines the economics and security of the PAC-based adsorption process, while state-of-the-art PAC regeneration technologies are usually unsatisfactory. Here, it is demonstrated that isolated Fe sites anchored on commercial PAC enable fast H 2 O 2 activation to produce Fe-based reactive oxygen species for highly efficient PAC regeneration at room temperature. Taking rhodamine B as a representative pollutant, PAC decorated with isolated Fe sites realize H 2 O 2 based regeneration with negligible adsorption capacity degradation for 10 cycles. Moreover, in terms of the PAC loss rate, this technology is greatly superior to traditional Fenton-based regeneration technology. Further operando experiments and theoretical calculations reveal that the high regeneration performance can be attributed to the isolated HO FeO motifs, which activate H 2 O 2 via a nonradical reaction pathway. These findings provide a very promising strategy toward reducing the cost of H 2 O 2 -based PAC regeneration technology.
研究领域:
环境科学
·
化学工程
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材料科学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Chunyu Zhang,Chan Wu,Li Wang,Guozhu Liu
The controllable synthesis of specific defective carbon catalysts is crucial for two-electron oxygen reduction reaction (2e– ORR) to generate H2O2 due to the great potential applications. Herein, the defective carbon catalysts (Mo-CDC-ns) were prepared by an electrochemical activation (ECA) method with Mo2C/C as a parent. Electrochemical cyclic voltammetry curves, X-ray photoelectron spectroscopy, inductively coupled plasma-mass spectrometry, scanning electron microscopy, and high-resolution transmission electron microscopy confirm the evolution process of a defective carbon structure from the Mo2C phase in which Mo species are first oxidized to Mo6+ species and then the latter are dissolved into the solution and defective carbon is simultaneously formed. Raman and electron paramagnetic resonance spectra reveal that the defect types in Mo-CDC-ns are the edge defect and vacancy defect sites. Compared with the parent Mo2C/C, Mo-CDC-ns exhibit gradually increased kinetic current density and selectivity for H2O2 generation with an extension of activation cycles from 10 (Mo-CDC-10) to 30 (Mo-CDC-30). Over Mo-CDC-30, a kinetic current density of 19.4 mA cm–2 and a selectivity close to 90% in 0.1 M KOH solution were achieved, as well as good stability for H2O2 production in an extended test up to 12 h in an H-cell. Graphene planes and Stone Wales 5757-carbon were constructed as basic models for density functional theory calculations. It revealed that the obtained defective structure after the removal of Mo atoms contains the double vacancy at the edge of graphene (Edge-DVC) and the topological defect on the plane of 5757-carbon (5757C-D), which show more moderate reaction free energy for forming *OOH and smaller energy barrier of 2e– ORR.
研究领域:
材料科学
·
电化学
·
催化反应
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DOI
PubMed
高影响因子
Engineering
·
2023
·
IF 12.8
Lei Li,Jing Bai,Panyu Jiang,Yan Zhang,Tingsheng Zhou,Jiachen Wang,Changhui Zhou,Jinhua Li,Baoxue Zhou
Hydrogen peroxide (H 2 O 2 ) in situ electrosynthesis by O 2 reduction reaction is a promising alternative to the conventional Fenton treatment of refractory wastewater. However, O 2 mass transfer limitation, cathodic catalyst selectivity, and electron transfer in O 2 reduction remain major engineering obstacles. Here, we have proposed a systematic solution for efficient H 2 O 2 generation and its electro-Fenton (EF) application for refractory organic degradation based on the fabrication of a novel ZrO 2 /CMK-3/PTFE cathode, in which polytetrafluoroethylene (PTFE) acted as a hydrophobic modifier to strengthen the O 2 mass transfer, ZrO 2 was adopted as a hydrophilic modifier to enhance the electron transfer of O 2 reduction, and mesoporous carbon (CMK-3) was utilized as a catalyst substrate to provide catalytic active sites. Moreover, feasible mass transfer of O 2 from the hydrophobic to the hydrophilic layer was designed to increase the contact between O 2 and the reaction interface. The H 2 O 2 yield of the ZrO 2 /CMK-3/PTFE cathode was significantly improved by approximately 7.56 times compared to that of the conventional gas diffusion cathode under the same conditions. The H 2 O 2 generation rate and Faraday efficiency reached 125.98 mg·cm − 2 ·h − 1 (normalized to 5674.04 mmol·g − 1 ·h − 1 by catalyst loading) and 78.24% at −1.3 V versus standard hydrogen electrode (current density of −252 mA·cm − 2 ), respectively. The high H 2 O 2 yield ensured that sufficient ·OH was produced for excellent EF performance, resulting in a degradation efficiency of over 96% for refractory organics. This study offers a novel engineering solution for the efficient treatment of refractory wastewater using EF technology based on in situ high-yield H 2 O 2 electrosynthesis.
研究领域:
环境工程
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化学工程
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水处理
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DOI
高影响因子
Materials Today Energy
·
2023
·
IF 9.3
Yuhang Gao,Xu Zhang,Chaogang Ban,Ran Feng,Jixiang Hou,Jiazhi Meng,Guo Yang,Chunlang Gao,Lu Xia,Peijie Ma,Kaiwen Wang,Xianlin Qu
A typical photocatalytic H 2 O 2 production reaction primarily comprises three processes: photoabsorption, electron–hole separation and transfer, and surface oxygen reduction reaction. Previous researches have focused on revealing the origin of the facet effect in photocatalysis. However, an comprehensive understanding of the structure–activity relationship for facet effect at atomic scale remains limited. Herein, we provide fundamental insights into photocatalytic H 2 O 2 production performance of three types of TiO 2 with predominantly exposed (101), (100), or (001) facets. The TiO 2 nanosheets with exposed (001) facet exhibit the highest H 2 O 2 yield rate of 649.2 μmol g -1 h -1 , which is 29.2 and 5.2 times higher than those of TiO 2 with (101) facet and (100) facet, respectively. Band alignment, charge carrier behavior and surface reaction are studied systematically and correlated with unique surface atom arrangement. Even with narrowed light-response range, short charge carrier lifetime, inferior charge separation, and inconspicuous specific surface area, the (001) facet exposed TiO 2 still performs best. The experimental results and density functional theory (DFT) calculations reveal that the under-coordinated Ti atoms on (001) surface serve as active sites and have strong interaction with oxygen molecule, while the Ti atoms on (101) and (100) surface can hardly adsorb and activate oxygen molecule. Hence, we suggest that the significantly lowered barrier for oxygen molecule adsorption and activation results from intrinsic surface sites rather than band-alignment and charge carrier behavior plays the principal role in this case. This work may provide semiquantitative insights into the origin of facet effect in photocatalysis.
研究领域:
材料科学
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化学
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催化
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表面科学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Kangkang Li,Xu Yan,Yaxin Du,Sheng Chen,Yang You,Wenshu Wu,Xingyu Liu,Liang Dong,Qian Wang,Qiuliang Wang,Yang Lu,Jingzhe Xue
Peroxidase-mimicking nanozyme therapy has emerged as a powerful tool in antibacterial therapy. Due to the critical role in reactive oxygen species (ROS) generation, various in situ H2O2 supplying nanoagents have been developed to guarantee the therapeutic effect. However, the challenges in reliance on external stimulus, instability of the H2O2 donor, and risk of leakage limited their antibacterial efficiency and actual application. In this work, we fabricated an injectable silk fibroin/ZnO NP/mica–Fe3O4 (SFZM) composite nanozyme hydrogel with spontaneous H2O2 generation and peroxidase-mimicking nanozyme properties. The ZnO NPs could produce H2O2 without light or other external stimulus. Under a weak acid environment, the H2O2 produced from ZnO NPs could be in situ transformed to ROS by magnetic mica–Fe3O4 nanosheets, leading to nearly 50% enhancement in antibacterial activity compared with a silk fibroin–ZnO hydrogel. Meanwhile, the SFZM nanozyme hydrogel displayed in vivo adhesion and hemostasis properties. As a result, the SFZM hydrogel could accelerate the healing of bacteria-infected wounds in rats. More interestingly, the ZnO exhibited continued H2O2 generation during at least 12 days, suggesting the long-term enhanced antibacterial effect of the SFZM hydrogel. Also, the SFZM nanozyme hydrogel showed low nanomaterial leakage and demonstrated biocompatibility both in vitro and in vivo.
研究领域:
生物医学工程
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材料科学
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纳米医学
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DOI
高影响因子
RSC Advances
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2023
·Vol. 13
·期 17
·11720-11727
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IF 3.9
Wanqian Cai,Chongbiao Zhang,Yourong Wu,Wei Wang,Mei Lin,Tengfei Lin,Cong Lin,Min Gao,Chunlin Zhao,Xiao Wu
As emerging contaminants, antineoplastic drugs are widely used, but their residues in water may cause long-term genotoxicity to aquatic organisms and human beings. Here, waste moxa ash was selected as biomass raw material and modified by ball milling to obtain carbon-based materials with excellent adsorption performance, which were used to remove the antineoplastic drug mitoxantrone (MTX) from water. The experimental results indicate that moxa ash modified by ball milling in hydrogen peroxide exhibits ultrafast removal of MTX (the removal efficiency reaches 97.66% in 1 min and 99.72% in 30 min). The pseudo-second-order kinetics and Freundlich isotherm models accurately describe the MTX adsorption process, and the mechanism of adsorption probably involves pore filling, hydrogen bond, π–π interaction and electrostatic attraction. Not only that, moxa ash also has the ability to remove dyes such as malachite green (97.81%) and methylene blue (99.97%). In this study, a simple and environmentally friendly process was used to convert waste moxa ash into an effective MTX adsorbent, providing a feasible solution for controlling MTX pollution and identifying a circular and economic way to reuse the waste.
研究领域:
环境科学
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材料科学
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药学
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产品关联
DOI
PubMed
高影响因子
Materials Advances
·
2023
·Vol. 4
·期 22
·5585-5593
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IF 5
Tinglei Wang,Jiayu Xin,Zhen Li,Yong Fan,Yu Wang
Synthesizing highly effective photocatalysts for hydrogen peroxide (H2O2) generation is still a challenge. In this work, the doping of graphite carbon nitride nanosheets with single-atom titanium, using TiCl3 as a precursor, to form single Ti atom-doped graphitic carbon nitride (Ti-SAC/g-C3N4) photocatalysts can efficiently address this challenge. The photocatalytic activity is enhanced by increasing the concentration of titanium to 0.09%, and subsequently decreases with further increases in the concentration of titanium, thus confirming that the concentration of titanium atoms can modulate the performance of the single-atom catalysts. Furthermore, an in-depth investigation indicates that the bottom of the conduction band (CB) and the maximum of the valence band (VB) can be controlled by varying the concentration of titanium atoms. A high bottom of the CB is beneficial to increase the photocatalytic efficiency. Under acidic conditions and utilizing sacrificial agents, the H2O2 production rate of Ti-C3N4-100 can reach 356.45 μmol L−1 h−1 and is 2.44 and 2.13 times higher than that of BCN and g-C3N4, respectively. The electron spin resonance (ESR) spectra suggest that the generation of superoxide radicals is crucial in the photocatalytic process. This work provides a distinctive strategy to realize single titanium atom doping and offers new insights into structure–property relationships.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
ANALYST
·
2019
·Vol. 144
·期 23
·6968-6974
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IF 4.019
Jianqiao Liu,Li Quan,Xuelian Yu,Lin Wang
In this work, a sandwich-type electrochemical immunosensor for the detection of procalcitonin (PCT) is constructed layer-by-layer with a novel label based on MoO3/Au@rGO nanocomposites. The high surface area and electroconductivity of graphene contributes to the transfer of electrons. Besides, the introduction of Au modulates the morphology of the MoO3@rGO nanocomposites from hexagonal prisms to agglomerated particles. Compared to rGO, Au@rGO and MoO3@rGO, the synergistic effect of MoO3/Au@rGO nanocomposites leads to the highest electrocatalytic activity towards H2O2 reduction. The electrochemical immunosensor exhibits a wide working range from 0.01 pg mL−1 to 10 ng mL−1 and a detection limit of 0.002 pg mL−1 at a signal-to-noise ratio of 3. Additionally, we also obtain excellent sensing performance for the immunosensor, including excellent selectivity, good reproducibility and stability. This work will give insight into the application of the nanocomposites based on noble metals combined with transition metal oxides in the fields of electroanalytical chemistry and biosensors.
研究领域:
分析化学
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生物医学工程
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DOI
PubMed
高影响因子
Nanomaterials
·
2019
·Vol. 9
·期 2
·E210
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IF 4.034
Qingtong Zhang,Mingfu Li,Chenyan Guo,Zhuan Jia,Guangcong Wan,Shuangfei Wang,Douyong Min
Lignin is the second largest naturally renewable resource and is primarily a by-product of the pulp and paper industry; however, its inefficient use presents a challenge. In this work, Fe₃O₄ nanoparticles loaded on lignin nanoparticles (Fe₃O₄@LNPs) were prepared by the self-assembly method and it possessed an enhanced peroxidase-like activity. Fe₃O₄@LNPs catalyzed the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of H₂O₂ to generate a blue color, was observable by the naked eye. Under the optimal conditions, Fe₃O₄@LNPs showed the ability of sensitive colorimetric detection of H₂O₂within a range of 5⁻100 μM and the limit of detection was 2 μM. The high catalytic activity of Fe₃O₄@LNPs allows its prospective use in a wide variety of applications, including clinical diagnosis, food safety, and environmental monitoring.
研究领域:
生物化学
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纳米材料科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
NANO
·
2018
·
IF 1.1
Chang Liu,Qianqian Su,Li Li,Jie Sun,Jian Dong,Weiping Qian
In this work, we designed a simple substrate-immersed solvothermal route for the one-step synthesis of novel ordered SiO 2 /Ag arrays, employing SiO 2 colloidal crystals as templates and alcohol as reducing agent. The Ag nanoparticles were uniformly deposited in situ onto SiO 2 colloidal crystals, which exhibited high surface enhanced Raman spectroscopy (SERS) activity and uniform SERS intensity. It was found that ordered SiO 2 /Ag arrays could rapidly scavenge the absorbed-Nile blue A (NBA) molecules from the surfaces with the assistance of H 2 O 2 , while the SERS signals of NBA decreased sharply and almost completely disappeared within four minutes. This can be attributed to the superior catalytic activity of Ag nanoparticles. After five times of re-immersion and re-absorbing process of NBA, the substrates could still keep ∼ 74.8% SERS intensity versus the original. The high activity and durability of the as-prepared SiO 2 /Ag SERS substrate endow them as a promising candidate for trace detection.
研究领域:
材料科学
·
化学
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产品关联
DOI
高影响因子
Frontiers in Nutrition
·
2022
·
IF 6.59
Tao Liang,Gu Fan,Liu Yan,Yang Min,Wu Xing-Zhong,Sheng Jun,Tian Yang
Moringa oleifera leaves are a kind of new food raw materials, rich in functional factors, M. oleifera leaves aqueous extract have antioxidant activity and M. oleifera leave protein is an important active ingredient in the aqueous extract. Numerous studies have shown that peptides have strong antioxidant activity. To reveal the antioxidant effects of M. oleifera (MO) leaves peptides, MO leave antioxidant peptides were isolated and prepared to clarify their antioxidant activity. MLPH1 (<1 kDa), MLPH3 (1~3 kDa), MLPH5 (3~5 kDa), and MLPH10 (5~10 kDa) fractions were obtained by the membrane ultrafiltration classification of MO leaves proteolytic hydrolysate (MLPH). MLPH1 was further separated by centrifugal filters, and the fraction separated by <1 kDa (MLPH1-1) was identified and analyzed by LC–MS/MS. The purpose of this study was to investigate the effect of MO leaves antioxidant peptide pretreatment on H2O2-treated HepG2 cells and to refine the antioxidant activity. The results showed that MLPH1 had the strongest antioxidant activity, and three MO leaves antioxidant peptides (LALPVYN, LHIAALVFQ, and FHEEDDAKLF) were obtained. The peptide with the sequence LALPVYN and a molecular weight of 788.44 Da had the strongest antioxidant activity. After 24 h of LALPVYN pretreatment, the cell viability and the CAT, GSH-Px, and SOD enzyme activity were significantly increased, and the MDA, ROS, and apoptosis rates were significantly decreased. These results provide a theoretical basis for further research on the antioxidant mechanism of MO leaves peptides.
研究领域:
生物化学
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药理学
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细胞生物学
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食品科学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2014
·Vol. 5
·期 13
·9374-9380
·
IF 3.708
Nan Li,Wangyang Lu,Kemei Pei,Wenxing Chen
The rapid diffusional mass transfer process (DMTP) always results in a highly efficient reaction. Herein, cobalt phthalocyanine (CoPc) was covalently anchored on to multiwall carbon nanotubes (MWCNTs) by an easy and moderate one-step deamination method to obtain the catalyst MWCNT-immobilized CoPc (CoPc-MWCNT). The interfacial peroxidase-like catalytic activity of CoPc-MWCNTs is described for controllable H2O2 activation. According to the experimental results and density functional theory calculations, we can be confident that high-valent cobalt-oxo intermediates are formed during the H2O2 activation. Such active species are anchored and exposed on the surface of MWCNTs, shortening the DMTP and enhancing the resistance of CoPc-MWCNTs to oxidative decay. The introduction of linear alkylbenzene sulphonates (LAS) facilitates the catalytic H2O2 activation by CoPc-MWCNTs, and at the same time, CoPc-MWCNTs could maintain a high and sustained catalytic activity because of the specific hydrophobic interactions between the long-chain alkyl group of LAS and the π-conjugated surface of the MWCNTs.
研究领域:
材料科学
·
催化化学
·
生物医学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）