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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

A three-stage oxidation method improves sludge dewaterability by achieving sustained oxidation and phased enhanced coagulation: Ingeniously using H2O2 as a “converter”

Wei Lin,An Ding,Chuangxin Gong,Xiuxiang Ding,Peter Desmond,Piotr Oleskowicz-Popiel,Xu He,Jun Ma,Huu Hao Ngo

Sludge reduction is essential for mitigating the environmental hazards associated with sludge. The use of ferric chloride (Fe(III)) catalyzed ferrate (Fe(VI)) can significantly enhance sludge dewaterability by increasing the Fe(VI) oxidation rate and maintaining in-situ enhanced coagulation. However, its weak oxidation ability at the sludge’s original pH limits its practical application. To address this, hydrogen peroxide (H 2 O 2 ) strengthened Fe(VI)/Fe(III) was employed to efficiently improve sludge dewaterability without pH adjustment, thereby enhancing the environmental utilization capacity of sludge. Compared to raw sludge, the treatment of Fe(VI)/Fe(III)–H 2 O 2 resulted in approximately the 95% reduction in specific resistance to filtration (SRF) and increased the bioavailable phosphorus (P) content in dewatered sludge. During the oxidation process, highly reactive species such as tetravalent iron (Fe(IV)) and hydroxyl radicals ( OH) were generated, facilitating the release of tightly bound water in extracellular polymeric substances (EPS). Importantly, the oxidation process was divided into three stages (persistent moderate oxidation — fast strong oxidation — sustained weak oxidation) based on the predominant reactive species (Fe(IV) or OH). This division promoted more robust and more durable oxidation processes. Phased enhanced coagulation occurred during the oxidation process. The gradual increase in Fe(III) content led to the re-flocculation of damaged EPS, enlarging the size of sludge drainage pores/channels and improving water discharge efficiency. Additionally, the costs and carbon emissions of chemicals for the Fe(VI)/Fe(III)–H 2 O 2 process were 18% and 52% lower than those of the traditional Fenton method. This study not only achieves the goals of sludge reduction and resource collection but also provides insights into selecting sludge conditioning methods that meet pollution reduction and carbon emission reduction requirements.

CAS / MDL: 39469-86-8
研究领域: 环境科学 · 污水处理
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CLAYS AND CLAY MINERALS · 2019 ·Vol. 67 ·期 4 ·253-264 · IF 1.835

Photocatalytic Activity of La-Containing Mixed- Metal Oxides Derived from Layered Double Hydroxides to Degrade Methylene Blue in the Presence of H2O2

Xu Minhong,Qian Mengxia,Pan Guoxiang,Guo Yuhua,Wu Tao

Photocatalytic degradation of polluted water by means of minerals, such as clays and oxides, which have surfaces that exhibit catalytic properties, has been suggested to be a useful new strategy to promote both organic and inorganic pollutant degradation. Nevertheless, much still remains to be studied about the capability of mixed metal oxides derived from lanthanum-containing layered double hydroxides to promote pollutant removal by means of photocatalytic degradation with the mineral surfaces. The objective of the present study was to investigate the synthesis of ternary MgAlLa mixed-metal oxides (MgAlLa-M) with various Mg/Al/La molar ratios through a hydrotalcite-like precursor route by co-precipitation of appropriate amounts of metal salts from homogeneous solution, followed by calcination at 600°C. The crystal structure, surface morphology, and optical properties of the samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR), and UV-Vis diffuse reflectance spectroscopy (DRS). Analysis by XRD showed that MgO, La 2 O 3 , MgAl 2 O 4 , and La 10 Al 4 O 21 phases coexisted in calcined samples as MgAlLa-M. The samples showed a small band gap of 3.11–3.35 eV according to DRS. The photocatalytic activities of the samples were evaluated by degradation of methylene blue (MB) under visible light irradiation. MgAlLa-M had better photocatalytic properties than hydrotalcite precursors, and the MgAlLa-0.5-M possessed the best photocatalytic activity. The photocatalytic degradation efficiency of MB dye with MgAlLa-0.5-M under visible light irradiation for 1 h was 99.89% in the presence of H 2 O 2 , which exceeded the binary MgAl-M (84.06%) under the same conditions. The high photocatalytic activity of the sample was attributed to the addition of La(III). In addition, the possible mechanism of photocatalytic degradation of MB by MgAlLa-M was discussed. The results showed that •O 2 – plays a major role in the MgAlLa-0.5-M/H 2 O 2 system.

研究领域: 环境科学 · 材料科学
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Polymers · 2020 ·Vol. 12 ·期 1 ·72 · IF 3.426

Magnetic Template Anion Polyacrylamide–Polydopamine-Fe3O4 Combined with Ultraviolet/H2O2 for the Rapid Enrichment and Degradation of Diclofenac Sodium from Aqueous Environment

Qiang Sun,Huaili Zheng,Xuebin Hu,Jun Li,Rui Zhao,Chun Zhao,Wei Ding

In this study, a novel system was set up by preparing a magnetic flocculant combining with ultraviolet/H2O2to realize the rapid enrichment and degradation of diclofenac sodium (DCFS). For the magnetic flocculant, template anion polyacrylamide (TAPAM) with anion micro-block structure was prepared. Thereafter, polydopamine was used to modify TAPAM, Fe3O4nanoparticles was grafted to the modified TAPAM by chelation, named template anion polyacrylamide-polydopamine-Fe3O4(TAPAM-PDA-Fe3O4). Furthermore, the TAPAM-PDA-Fe3O4preparation protocol was optimized by the response surface method (RSM). In the DCFS enrichment section, the rapid separation of flocs from water was realized by an external magnetic field and it indicated that the π–π stacking effect was dominant in neutral/alkaline condition, whereas charge neutralization was favored in acidic conditions. Meanwhile, a DCFS enrichment kinetic curve was much fitted by the pseudo-second-order kinetic model and DCFS enrichment isothermal curve was close to the Freundlich isothermal model, indicating the dependence of DCFS quantity enriched by TAPAM-PDA-Fe3O4and a multilayer heterogeneous enrichment process. The degradation experiment confirmed that DCFS was effectively degraded by ultraviolet/H2O2/TAPAM-PDA-Fe3O4and the maximum value of DCFS degradation efficiency reached 98.1%. Furthermore, the regeneration experiment showed that the enrichment and degradation efficiency of DCFS could maintain a relatively high level in the initial three recycles.Keywords:diclofenac sodium;π–π stacking;charge neutralization;enrichment;degradation

CAS / MDL: 7727-54-0 62-31-7
研究领域: 环境科学 · 材料科学
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JOURNAL OF SOLID STATE CHEMISTRY · 2023 · IF 3.3

Effective enhanced photocatalytic H2O2 production through synergistic oxygen vacancy defects and In situ-growth Z-scheme BiOBr/WO3 heterojunction with compact interface

Tianxiang Zhang,Tao Zhang,Hanping Fu,Li Feng,Qing Zhang,Shufen Ren,Jiayun Cheng,Qingshuang Liang,Xiufeng Xiao

Rational heterojunction interface construction and defect engineering have been regarded as significant strategies to enhance the photocatalytic performance of hydrogen peroxide (H 2 O 2 ) production. Herein, a novel 2D/1D BiOBr/WO 3 Z-scheme heterostructure with compact interface and rich oxygen vacancies (OVs) was successfully fabricated by an in situ -growth procedure. The rational design architecture and electronic structure allow the photocatalytic system to fully optimize light absorption, charge separation, and surface redox reaction . Benefited from synergistic effect of the formation of compact Z-scheme heterostructur and oxygen vacancies , the as-prepared BiOBr/WO 3 photocatalysts exhibit a greatly improved photocatalytic performance in the production of H 2 O 2 with a yield of 82.4 mM/h/g. We believe that this work provides a novel sight to develop high-efficiency photocatalyst via microstructure nanointerface control and defect engineering.

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PLANT JOURNAL · 2023 · IF 7.2

Wounding induces a peroxisomal H2O2 decrease via glycolate oxidase-catalase switch dependent on glutamate receptor-like channel-supported Ca2+ signaling in plants

Xiangyang Li,Linru Chen,Xiaoyue Zeng,Kaixin Wu,Jiayu Huang,Mengmeng Liao,Yue Xi,Guohui Zhu,Xiuying Zeng,Xuewen Hou,Zhisheng Zhang,Xinxiang Peng

SUMMARY Sensing of environmental challenges, such as mechanical injury, by a single plant tissue results in the activation of systemic signaling, which attunes the plant's physiology and morphology for better survival and reproduction. As key signals, both calcium ions (Ca 2+ ) and hydrogen peroxide (H 2 O 2 ) interplay with each other to mediate plant systemic signaling. However, the mechanisms underlying Ca 2+ -H 2 O 2 crosstalk are not fully revealed. Our previous study showed that the interaction between glycolate oxidase and catalase, key enzymes of photorespiration, serves as a molecular switch (GC switch) to dynamically modulate photorespiratory H 2 O 2 fluctuations via metabolic channeling. In this study, we further demonstrate that local wounding induces a rapid shift of the GC switch to a more interactive state in systemic leaves, resulting in a sharp decrease in peroxisomal H 2 O 2 levels, in contrast to a simultaneous outburst of the nicotinamide adenine dinucleotide phosphate (NADPH) oxidase-derived apoplastic H 2 O 2 . Moreover, the systemic response of the two processes depends on the transmission of Ca 2+ signaling, mediated by glutamate-receptor-like Ca 2+ channels 3.3 and 3.6. Mechanistically, by direct binding and/or indirect mediation by some potential biochemical sensors, peroxisomal Ca 2+ regulates the GC switch states in situ , leading to changes in H 2 O 2 levels. Our findings provide new insights into the functions of photorespiratory H 2 O 2 in plant systemic acclimation and an optimized systemic H 2 O 2 signaling via spatiotemporal interplay between the GC switch and NADPH oxidases.

CAS / MDL: 52665-69-7
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ACS Nano · 2023 · IF 17.1

Regulating the H2O2 Activation Pathway on a Well-Defined CeO2 Nanozyme Allows the Entire Steering of Its Specificity between Associated Enzymatic Reactions

Bo Yuan,Zicong Tan,Qiang Guo,Xiutong Shen,Chao Zhao,Jian Lin Chen,Yung-Kang Peng

Nanozymes are promising alternatives to natural enzymes, but their use remains limited owing to poor specificity. For example, CeO2 activates H2O2 and displays peroxidase (POD)-like, catalase (CAT)-like, and haloperoxidase (HPO)-like activities. Since they unavoidably compete for H2O2, affecting its utilization in the target application, the precise manipulation of reaction specificity is thus imperative. Herein, we showed that one can simply achieve this by manipulating the H2O2 activation pathway on pristine CeO2 in well-defined shapes. This is because the coordination and electronic structures of Ce sites vary with CeO2 surfaces, wherein the (100) and (111) surfaces display nearly 100% specificity toward POD-/CAT-like and HPO-like activities, respectively. The antibacterial results suggest that the latter surface can well-utilize H2O2 to kill bacteria (cf., the former), which is promising for anti-biofouling applications. This work provides atomic insights into the synthesis of nanozymes with improved activity, reaction specificity, and H2O2 utilization.

CAS / MDL: 143-74-8 54827-17-7
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Amorphous cobalt sulphide introduced atomic H*/H+ for H2O2 electrosynthesis and enhanced Fe(II) regeneration in electro-Fenton process at macroneutral pH

Zhenglin Chen,Guangzhen Liu,Shuiping Yu,Lixia Yang,Lingyi Zheng,Zhihui Wei,Shenglian Luo

Cathode materials with high hydrogen peroxide (H 2 O 2 ) selectivity and Fe 2+ regeneration under macroneutral conditions are the essential for practical electro-Fenton processes. Herein, we develop an amorphous cobalt sulphide (CoSx(t = x)@Cu) cocatalytic electro-Fenton (EF) system capable of effectively degrading organic pollutants, such as sulfamethoxazole, at macroneutral pH conditions. Owing to the flexible electronic properties of amorphous structures and charge redistribution triggered by S defects, the optimum CoSx(t = 8)@Cu cathode successfully introduces H*/H + and promotes the in-situ evolution of H 2 O 2 . Additionally, an acidic microenvironment was constructed on the CoSx(t = 8)@Cu surface by the unreduced H*/H + , enabling a self-adjustment from alkalinity to acidity in the EF reaction without adding acid. Such self-adjustment effectually inhibits iron sludge production and promotes Fe 2+ regeneration, assuring 80% Fe 2+ cycling efficiency. More importantly, the EF system possesses outstanding stability and applicability for organic pollutant remediation regardless of water matrices. This work elucidates the intrinsic mechanism of amorphous electrocatalysts in overcoming the pH limitation of EF reactions, extending the applicability of Fenton technology.

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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 33 ·15721-15730 · IF 3.3

The fabrication of CuBTC@PW12 with prominent peroxidase-mimicking activity for colorimetric detection of H2O2 and ascorbic acid via “on–off” switch

Wanyu Song,Peng Sun,Jihong Zhou,Xu Han,Qijun Dai,Fang Chai

The Keggin phosphotungstic acid (PW12) embedded metal–organic framework copper benzene-1,3,5-tricarboxylate (CuBTC), CuBTC@PW12, was fabricated by a facile hydrothermal synthesis technique. With a unique tetrakaidecahedron structure and multiple active sites, the obtained CuBTC@PW12 exhibited peroxidase-mimicking activity, which promoted a novel strategy for qualitative and quantitative detection of hydrogen peroxide (H2O2) and sequential sensing of ascorbic acid (AA) via colorimetric evolution. Notably, with the advantages of strong redox performance of POMs and the unique porous structure of metal organic frameworks (MOFs), as peroxidase mimics, CuBTC@PW12 achieved highly selective and sensitive detection of H2O2via oxidizing TMB to a blue oxidation product (ox-TMB), with a limit of detection of 2.67 μM within the 0.01 to 1.0 mM scale. Concomitantly, the AA can be monitored consecutively by reducing the ox-TMB with fading blue color quantitatively with a limit of detection at 0.15 μM in the range of 0.01–0.10 μM. The recoveries for the determination of AA in human serum were obtained at 94.63–105%. These results manifested that CuBTC@PW12 could be used as a peroxide-mimetic enzyme for the continuous detection of H2O2 and AA with the advantages of simplicity, efficiency, sensitivity and accuracy.

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ANALYTICAL CHEMISTRY · 2023 · IF 7.4

Remarkably Enhanced Luminol/H2O2 Chemiluminescence with Excellent Peroxidase-like Activity of FeCoNi-based Metal-Organic Xerogels for the Sensitive Detection of Dopamine

Fangshuo Liu,Shiyu Xia,Ala’a Mhmoued Abdllh Alboull,Zhiyong Dong,Hongzhan Liu,Chengda Meng,Fengxia Wu,Guobao Xu

Metal-organic gels (MOGs) are a category of metal-organic smart soft materials with large specific surface areas, loose porous structures, and open metal active sites. In this work, trimetallic Fe(III)Co(II)Ni(II)-based MOGs (FeCoNi-MOGs) were synthesized at room temperature via a simple and mild one-step procedure. Fe3+, Co2+, and Ni2+ were the three central metal ions in it, while 1,3,5-benzenetricarboxylic acid (H3BTC) served as the ligand. The solvent enclosed in it was then removed by freeze-drying to get the corresponding metal-organic xerogels (MOXs). The as-prepared FeCoNi-MOXs have excellent peroxidase-like activity and can significantly enhance luminol/H2O2 chemiluminescence (CL) by more than 3000 times, which is very effective compared with other reported MOXs. Based on the inhibitory effect of dopamine on the CL of the FeCoNi-MOXs/luminol/H2O2 system, a simple, rapid, sensitive, and selective CL method for dopamine detection was established with a linear range of 5–1000 nM and a limit of detection of 2.9 nM (LOD, S/N = 3). Furthermore, it has been effectively used for the quantitative measurement of dopamine in dopamine injections and human serum samples, with a recovery rate of 99.5–109.1%. This research brings up prospects for the application of MOXs with peroxidase-like activity in CL.

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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Facile microwave-assisted synthesis of Pt single atom anchored on poly (ionic liquids) functionalized reduced graphene oxide for ultrasensitive detection of H2O2

Mehdihasan I. Shekh,Tao Lu,Amit Kumar,Gaurav Sharma,Guangming Zhu,Florian J. Stadler,Bing Du

Theoretically, Single atoms are providing the maximum atomic efficiency and are very promising to improve the performance of the noble metal catalysts for high-active electrochemical sensors. In this work, Pt single atom anchored on surficial modified, reduced graphene oxides with poly(ionic liquids) (Pt 1 _rGO@PILs) for detecting hydrogen peroxide (H 2 O 2 ) was synthesized via a facile microwave-assisted method. Due to the high active sites from PILs, 1.2 wt% isolated Pt atoms were steadily loaded on the surface of rGO@PILs and formed Pt-S 4 coordination with the modified PILs layer. Such atomical dispersion of Pt atoms and their unique coordination environment promoted electronic transfer during the electrochemical reaction. The Pt 1 _rGO@PILs composite presented a detection limitation of 1.5 µM in a liner range from 2.3 to 250 µM with high sensitivity up to 725.95 µA/µM. The catalysts also showed good stability for 30 days while active and the lowest detected concentration of approximately 15 μM for H 2 O 2 in the real commercial samples.

CAS / MDL: 7722-84-1 7722-64-7
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Food & Function · 2022 ·Vol. 14 ·期 1 ·160-170 · IF 6.317

Identification, molecular docking, and protective effects on H2O2-induced HEK-293 cell oxidative damage of antioxidant peptides from Pacific saury (Cololabis saira)

Junjia Luan,Lei Wang,Junnan Yang,Xuepeng Li,Jinxiang Wang,Fangchao Cui,Hongbo Mi,Yongxia Xu,Shumin Yi,Jianrong Li

We identified novel antioxidant peptides from Pacific saury (Cololabis saira). Enzymatic hydrolysates were isolated, purified, and identified by ultrafiltration, gel chromatography, reverse phase high-performance liquid chromatography (RP-HPLC), and matrix-assisted laser desorption/ionization-time of flight (MALDI-TOF) mass spectrometry (MS). Twenty putative peptides were identified from five components of HPLC, among which sixteen peptides were predicted to have good water solubility and non-toxicity by online tools. Fifteen peptides were successfully docked with myeloperoxidase, and we observed that Arg31, Arg323, and Lys505 played a key role in the antioxidant mechanism, with van der Waals forces and conventional hydrogen bonds as important interaction forces. Six identified peptides with lower CDOCKER energy values were synthesized to verify the antioxidant activity, and the results showed that the synthetic peptide QQAAGDKIMK displayed the strongest 2,2-diphenyl-1-picrylhydrazyl (DPPH) radical scavenging rate (31.05 ± 0.27%) and reducing power (0.29 ± 0.01). The synthetic peptide KDEPDQASSK at a concentration of 300 μg mL−1 exhibited the strongest protective effects on H2O2-induced oxidative damage of HEK-293 cells, with cell viability and ROS level of 0.38 ± 0.03 and 0.08 ± 0.01, respectively.

CAS / MDL: 7705-08-0 76-03-9
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Self-supply of H2O2 and O2 by a composite nanogenerator for chemodynamic therapy/hypoxia improvement and rapid therapy of biofilm-infected wounds

Junjie Wu,Peng Shen,Xian Qin,Yulu Yang,Chuanchuan Lin,Xuan Li,Wenbo Geng,Pengfei Gao,Lixue Chen,Li Miao,Yang Jiao,Bailong Tao

Bacterial wound infection is a major challenge to human health worldwide. In this study, a composite nanogenerator, CaO 2 @ZIF-67-PLL, was fabricated via a bottom-up approach with chemodynamic therapy (CDT)/hypoxia improvement for rapid therapy of biofilm-infected wounds. Under a pathologically acidic microenvironment, the out layer ZIF-67 can be decomposed to rapidly release Co 2+ and CaO 2 ; Subsequently, the unprotected CaO 2 reacts with H 2 O to produce O 2 and H 2 O 2 . The self-supply of O 2 relieves hypoxia and inflammatory response induced by infections, while the generated H 2 O 2 and poly- l -lysine (PLL) exhibited synergistic strong anti-biofilm capability against Escherichia coli ( E. coli) and Staphylococcus aureus (S. aureus) as assessed by reactive oxygen species (ROS) generation, membrane permeability change, ATP reduction, o -nitrophenyl-β-d-galactopyranoside (ONPG) hydrolysis and intracellular component leakage. Meanwhile, CaO 2 @ZIF-67-PLL exhibited good cytocompatibility and promoted the adhesion, proliferation, and migration of NIH-3T3 cells by enhancing the expression of wound healing-related genes (TGF-β1, VEGF, α-SMA, Col I, Col III, and Wnt-5a). Notably, CaO 2 @ZIF-67-PLL could significantly improve the healing process of S. aureus -infected wounds via suppressed inflammatory responses, enhanced collagen disposition and angiogenesis, and stimulated HIF-1α, CD31, and Wnt-5a/β-Catenin signaling pathways. These results indicated the potential of CaO 2 @ZIF-67-PLL nanogenerator for clinical application in infected wound treatment.

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