APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Qingru Xie,Yanping Zhu,Haiyang Xian,Qingze Chen,Chengshuai Liu,Fei Wu,Xiaoliang Liang,Runliang Zhu
Doping transition metal into ferrihydrite (Fh) may significantly affect its structure and Fenton reactivity. The comparative study of Fh and M(II)-Fh (M = Cu, Co, or Mn), for the first time, reveals that doping metal ions can alter the property and content of oxygen vacancy (OVs) and the oxidation potential of Fh, which subsequently affects H 2 O 2 decomposition, HO . generation, and Fenton reactivity of the catalysts. The overall Fenton activity of the samples in decomposing bisphenol A decreases in the order Cu-Fh > Fh > Co-Fh > Mn-Fh. In specific, Cu-Fh is the most efficient catalyst as it has the lowest energy barrier for decomposing H 2 O 2 into HO . at OVs sites and the highest oxidation potential (benefiting the reduction of Fe(III) to Fe(II) by H 2 O 2 ). Our findings show the complex heterogeneous Fenton reactivity of M-Fh, and doping can be an efficient strategy for achieving highly efficient Fenton catalysts.
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ChemNanoMat
·
2023
·Vol. 9
·期 5
·e202200569
·
IF 3.8
Yanyu Li,Xiaoyue Zhang,Jinglin Shen,Wei Qi
Graphical A new type of nanocomposite enzymes has been developed, composed of Pd−Pt nanoparticles, hemin-rGO and CNTs-COOH. The nanocomposites show a high peroxidase-like activity and a linear response toward H 2 O 2 in the range of 0.05–500 μM with a determination limit of 0.01 μM. Based on this, a paper sensor was constructed for H 2 O 2 detection in real samples. Nanocomposite enzymes are attracting intensive attention worldwide. In the present study, a novel colorimetric H 2 O 2 paper sensor was developed based on a new type of nanocomposites composed of Pd−Pt nanoparticles, hemin functionalized reduced graphene oxide (hemin-rGO) and carboxylated carbon nanotubes (CNTs-COOH). The proposed nanocomposites show a high peroxidase-like activity. It provides a sensitive platform showing a linear response toward H 2 O 2 in the range of 0.05–500 μM with a determination limit of 0.01 μM. Based on this, the composites were applied to construct a paper sensor for H 2 O 2 detection in real samples. The cost-effectiveness, simplicity and efficiency of this paper sensor could be developed for “point-of-care” analysis and other related areas.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yi Xing,Mengyun Zhou,Xiangmei Liu,Minghang Qiao,Liping Zhou,Tailin Xu,Xueji Zhang,Xin Du
Chemodynamic therapy (CDT), which catalyzes the production of highly toxic reactive oxygen species (ROS), has been widely used in tumor therapy in the past five years. However, most of the current nanomaterials for CDT are difficult to penetrate into the tumor effectively due to the lack of motility, resulting in an unsatisfactory CDT effect. Herein, bioinspired jellyfish-like carbon/manganese nanomotors (JCMNs) are designed to achieve hydrogen peroxide (H 2 O 2 ) and NIR light dual-propulsion for the enhanced CDT therapy. Based on the jellyfish-like asymmetric structure, the manganese component can catalyze H 2 O 2 to generate chemical concentration gradient, propelling JCMNs to dynamically generate ROS in cells by self-diffusiophoresis. In addition, the carbon component of JCMNs can absorb near-infrared (NIR) light to produce a temperature gradient, driving JCMNs to enhance tumor penetration by self-thermophoresis. The combination of chemical and NIR light propulsions significantly improves the efficiency of tumor CDT, revealing that it should be a reasonable strategy to promote the development of nanobiomedicine by endowing nanosystems with propulsion capacity.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Ao Zhang,Zhongqing Jiang,Shaoda Zhang,Penghua Lan,Naihua Miao,Weiheng Chen,Ning Huang,Xiaoning Tian,Yangjie Liu,Zhongyu Cai
We report the development of non-noble transition metal sulfide catalysts Mn-CuS-x for high-efficiency and selective H 2 O 2 production. In this study, we synthesized Mn-CuS-x with coral-shaped hierarchical porous structure through one-pot hydrothermal reaction. The Mn-CuS-x possesses large specific surface area with plenty of crystalline defects via heteroatom doping of Mn. The Mn-CuS-x kinetically favored 2e − pathway over 4e − pathway, resulting in high selectivity (>92%) to H 2 O 2 production and high H 2 O 2 concentration (∼24.5 mM at 0.6 V vs. RHE) within 3 h for the optimized Mn-CuS-2 catalysts (synthesized with a molar ratio of 1:3:8 (MnCl 2 ·4 H 2 O: CuCl 2 ·2 H 2 O: C 2 H 5 NS)). The Mn-CuS-2 showed excellent stability, indicating that the Mn-CuS electrocatalysts can simultaneously achieve both high stability and enhanced H 2 O 2 production. Our first-principles calculations further confirmed that the heteroatom Mn doping to CuS thermodynamically makes the 2e – -ORR pathway more favorable. This study provides a green, low-cost, and efficient route to produce H 2 O 2 , which is very promising for generating chemicals and liquid fuels.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2023
·
IF 6
Die Zhao,Chunji Li
Microbial carotenoids and lipids are two groups of versatile biomolecules widely used in the food, fuel, pharmaceutical, and cosmetic industries. Rhodotorula glutinis is one of the best-known oleaginous red yeasts that has the remarkable capability to produce an assortment of valuable carotenoids and lipids. Here, the effects of different concentrations of TiO 2 and H 2 O 2 treatments on carotenoid and lipid production in R. glutinis ZHK were investigated. After 120 h of cultivation, the total amount of carotenoids was significantly increased in the TiO 2 (100 mg/L: 23.165 μg/gdw, 750 mg/L: 19.65 μg/gdw) and H 2 O 2 (5 mM: 21.51 μg/gdw, 10 mM: 118.858 μg/gdw) treatments than the control (6.099 μg/gdw). In contrast, as compared to the control, the relative abundance of total lipids was significantly decreased in the TiO 2 (100 mg/L) and H 2 O 2 (10 mM) treatments, respectively. In response to TiO 2 and H 2 O 2 stresses, the increased carotenoids were probably attributed to the down-regulated lipid biosynthesis flux, while the decreased lipids might be ascribed to the down-regulated fatty acid biosynthesis flux. Our results presented herein not only provide an effective strategy for modulating carotenoid and lipid biosynthesis in R. glutinis ZHK but also reveal the molecular foundation to further enhance their bioproductivity by molecular manipulation.
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ANALYTICAL CHEMISTRY
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2022
·
IF 8.008
Jing Lei,Xiaoqing Sun,Yan Jin,Chunli Xu,Baoxin Li
Fe and Co single-atom catalysts (SACs) have been widely explored in many fields, while Zn SACs are still in their infancy stage. Herein, we unexpectedly found that atomically dispersed Zn2+ on N-doped carbon material (Zn-N-C) exhibited high catalytic activity on luminol-H2O2 chemiluminescence (CL) reaction. The Zn-N-C SACs were readily prepared through simple pyrolyzation of the cheap precursors (dopamine and ZnCl2). The mechanism of Zn SAC-catalyzed CL reaction of luminol-H2O2 was investigated in detail. The activity of Zn SACs originated from the Zn-N sites in the Zn-N-C structure. The monoatomic dispersion makes Zn2+ catalytic performance change from no activity to high activity in luminol-H2O2 CL reaction. This study demonstrated the particularity of the monatomic metal catalyst over the conventional metal ion. This work provides the unprecedented perspective for design of new metal SACs in CL reaction.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Fangmin Wu,Jun Nan,Tianzuo Wang,Zhencheng Ge,Bohan Liu,Meng Chen,Xuesong Ye
The activity and selectivity of the cathode towards electrosynthesis of H 2 O 2 are critical for electro-Fenton process. Herein, nickel-foam modified with N, O co-doped graphite nanosheets (NO-GNSs/Ni-F) was developed as a cathode for highly efficient and selective electrosynthesis of H 2 O 2 . Expectedly, the accumulation of H 2 O 2 at pH= 3 reached 494.2 mg L −1 h −1 , with the selectivity toward H 2 O 2 generation reaching 93.0%. The synergistic effect of different oxygen-containing functional groups and N species on the performance and selectivity of H 2 O 2 electrosynthesis was investigated by density functional theory calculations, and the combination of epoxy and graphitic N (EP + N) was identified as the most favorable configuration with the lowest theoretical overpotential for H 2 O 2 generation. Moreover, NO-GNSs/Ni-F was applied in the electro-Fenton process for p-nitrophenol degradation, resulting in 100% removal within 15 min with the kinetic rate constant of 0.446 min −1 and 97.6% mineralization within 6 h. The efficient removal was mainly attributed to the generation of bulk ·OH. Furthermore, NO-GNSs/Ni-F exhibited excellent stability. This work provides a workable option for the enhancement of H 2 O 2 accumulation and the efficient degradation of pollutants in electro-Fenton system.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Dongqin He,Dongli Wang,Hongwei Luo,Yifeng Zeng,Ganning Zeng,Jun Li,Xiangliang Pan
The most important factor that restricts the decomposition of H 2 O 2 in the Fe 3+ /H 2 O 2 reaction is the slow cycling efficiency of reducing Fe 3+ to Fe 2+ . In this study, the addition of tungsten disulfide (WS 2 ) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant enhancement of H 2 O 2 decomposition, which resulted in the effective degradation of acetaminophen (APAP). Results show that 99.6% of APAP (5 mg L −1 ) could be degraded by H 2 O 2 /Fe 3+ /WS 2 system within 2.5 min. The conversion of Fe 3+ to Fe 2+ occurred mainly on the surface of WS 2 due to the redox reaction of the exposed W 4+ active sites with Fe 3+ after the unsaturated S atoms were bound to protons. Electron paramagnetic resonance (EPR) and radical quenching experiments evaluated the contribution of hydroxyl radical (•OH) and superoxide radical (O 2 • − ) in the degradation of pollutants. WS 2 showed good recoverability after four cycles of the reaction. This study provides a new perspective to improve the efficiency of Fe 3+ /H 2 O 2 and provides a reference for the involvement of transition metal sulfides in advanced oxidation processes (AOPs).
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Acta Biomaterialia
·
2022
·
IF 10.633
Ying Wang,Chuanjiang Jian,Yiqing Long,Xiaowen Xu,Yang Song,Zongning Yin
Pathological coagulation within an injured artery and the subsequent cardiovascular complications, such as stroke and heart attack, greatly threaten human life. Inspired by the biochemical features of acute arterial thrombosis, such as abundant activated platelets and hydrogen peroxide (H 2 O 2 ), we constructed platelet-targeted theranostic nanoparticles (CyBA/PFM NPs) with H 2 O 2 -triggered photoacoustic contrast enhancement and antithrombotic capabilities. CyBA/PFM NPs were designed to target platelet-rich clots via fucoidan segment within the carrier, which could be activated by H 2 O 2 to produce fluorescent “CyOH” molecules, thus turning on the photoacoustic signal. CyBA/PFM NPs showed obvious amplification of fluorescence following incubation with fresh clots, exhibiting efficient scavenging ability of intracellular reactive oxygen species (ROS). In a FeCl 3 -induced mouse model of carotid thrombosis, CyBA/PFM NPs significantly amplified the photoacoustic contrast in thrombogenic tissues, effectively eliminated ROS within the occlusion site, and suppressed the thrombus formation , accompanied by a normalization of the soluble CD40L level. Given their accurate imaging potential, potent antithrombotic activities and acceptable biosafety, CyBA/PFM NPs hold strong potential as nanoscale theranostics for H 2 O 2 -correlated cardiovascular diseases. Statement of significance In this study, we developed a platelet-targeted and H 2 O 2 -triggered nanosystem self-assembled from phenylboronated fucoidan/maltodextrin polymers and responsive near-infrared probes. The fucoidan segment within the carrier could facilitate the specific delivery of the therapeutic polymers and probes to the platelet-rich arterial thrombus. In a mouse model of FeCl 3 -induced arterial thrombosis, the system could be activated by H 2 O 2 to produce fluorescent “CyOH” molecules, thus turning on the photoacoustic signal and specifically imaging thrombosed tissues. Besides, CyBA/PFM NPs significantly effectively eliminated ROS within the occlusion site and suppressed the thrombus formation. Given their theranostic potential and acceptable biosafety, this system has great potential for H 2 O 2 -correlated cardiovascular diseases.
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Small
·
2022
·Vol. 18
·期 32
·2203020
·
IF 15.153
Kai Deng,Wenxin Wang,Qiqi Mao,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Tailoring the morphology and crystal structure of metallene is critical to improve its electrocatalytic performance. In this work, hetero-phase RhB metallene ( h -RhB metallene) with amorphous/crystalline structure is readily prepared by a two-step method. The h -RhB metallene is very unique in its non-metallic heteroatom doping and amorphous/crystalline structure. Benefiting from the unique metallene structure and the optimized electronic states induced by the incorporation of B atoms, the h -RhB metallene exhibits superior performance for hydrogen evolution reaction and hydrogen peroxide electro-oxidation reaction (HPOR). When coupled with HPOR, the h -RhB metallene|| h -RhB metallene water electrolysis two-electrode system exhibits a lower cell voltage of 0.379 V (@ 10 mA cm −2 ) compared with the overall water splitting (1.35 V). The presented synthetic method provides a powerful strategy to design metallene with hetero-phase for energy-saving H 2 production.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Jing Yang,Xiaoqin Zhang,Jia Tang,Jinlan Li,Aiping Zhang
In this study, molybdenum disulfide (MoS 2 ) was used to enhance a zero-valent iron/hydrogen peroxide (Fe 0 /H 2 O 2 ) Fenton-like system, which was able to remove refractory organic matter from the effluent produced during the treatment of landfill leachate by a membrane bioreactor (MBR). The MoS 2 /Fe 0 /H 2 O 2 system could efficiently remove refractory organic matter (i.e., fulvic acid-like substances and humic-like substances) from the MBR effluent and also exhibited a strong synergistic effect. Under the conditions of initial pH = 3, H 2 O 2 = 40 mmol/L, Fe 0 = 0.4 g/L, MoS 2 = 0.1 g/L, and t = 30 min, compared with a Fe 0 /H 2 O 2 system, the absorbance UV 254 , chroma (CN), and total organic carbon (TOC) removal rates in MBR effluent treated with MoS 2 /Fe 0 /H 2 O 2 increased to 48.68%, 63.85%, and 35.85%, respectively. Through the identification of reactive oxygen species (ROS), the hydroxyl radical (HO • ) concentration and an analysis of the effective utilization rate of H 2 O 2 , as well as an analysis of the morphology of the material, the distribution of Fe compounds, valence changes, and the Fe ion concentration , it was proven that MoS 2 promoted the cycling of Fe 3+ /Fe 2+ in the Fe 0 /H 2 O 2 process. The addition of MoS 2 promoted the Fe 3+ /Fe 2+ cycling reaction through the exposed Mo 4+ active center, significantly promoting the decomposition of H 2 O 2 and the formation of HO • . The MoS 2 /Fe 0 /H 2 O 2 system was able to remove a wide range of aromatic organics, indicating the wide applicability of the system. This study developed a new method for the efficient removal of refractory organic matter from landfill leachate.
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CHEMOSPHERE
·
2022
·
IF 8.943
Chao Gong,Jinli Zhai,Xi Wang,Wenjie Zhu,Daoli Yang,Yongming Luo,Xiaoya Gao
Herein, a heterogeneous photo-Fenton and photo-catalytic system was constructed using oxide pyrite (FeS 2 /Fe 2 O 3 ) mineral and organic acids including tartaric acid (TA), ascorbic acid (AA), and citric acid (CA). In the proposed system, FeS 2 /Fe 2 O 3 can be successfully activated through irradiation to generate photogenerated carriers, which generated H 2 O 2 in-situ through the reduction reactions between e - and O 2 . The addition of organic acids enhanced the dissolution of iron from FeS 2 /Fe 2 O 3 . Based on the iron and in-situ generated H 2 O 2 , •OH was produced through a photo-Fenton reaction. Furthermore, h + , e - , and •O 2 − , which were generated through the photo-catalytic activation of FeS 2 /Fe 2 O 3 , also played a certain role in the degradation of carbamazepine (CBZ). Therefore, the synergistic photo-Fenton and photo-catalytic reaction improved the degradation of CBZ, with the degradation efficiencies of 86%, 62%, and 68% in FeS 2 /Fe 2 O 3 /TA, FeS 2 /Fe 2 O 3 /AA, and FeS 2 /Fe 2 O 3 /CA systems, respectively. This investigation provides an innovative strategy for the removal of organic pollutants using natural minerals.
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