FlatChem
·
2023
·
IF 6.2
Anchao Zhou,Tianqi Yu,Xincheng Liang,Shibin Yin
Hydrogen peroxide (H 2 O 2 ) is required to reduce the residual potassium permanganate (KMnO 4 ) in the traditional Hummers method for preparing graphene oxide (GO), which is dangerous and uncontrollable. In this work, spontaneous-reduction of high-valence Mn ions is induced by simply adjusting the reaction temperature/time and the dosage of concentrated sulfuric acid (H 2 SO 4 ) to prepare high quality GO without H 2 O 2 , avoiding the high risk of the dramatically exothermic reduction reaction caused by the quenching reaction of adding H 2 O 2 . Notably, the C/O ratio of GO prepared by this H 2 O 2 -free method is 1.986, which is less than commercial GO. Herein, this work provides a novel and efficient strategy for the safe and environmentally-friendly preparation of GO with high quality.
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高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 7
·2101-2107
·
IF 5
Jianhao Qiu,Lu Zhang,Guanglu Xia,Dingliang Dai,Yong Tang,Jianfeng Yao
Different ligand functionalized UiO-66 (UiO-66-X, X = OH, (OH)2 and NH2) were prepared and then modified by ZnIn2S4 lamellas to form ZnIn2S4/UiO-66-X heterostructures for visible-light-driven H2O2 evolution in pure water. The H2O2 yields using ZnIn2S4/UiO-66-NH2, ZnIn2S4/UiO-66-(OH)2 and ZnIn2S4/UiO-66-OH are 799, 733 and 165 μmol L−1, respectively, which are 9.5, 8.7 and 2.0 times that of ZnIn2S4/UiO-66. The high performance of ZnIn2S4/UiO-66-NH2 and ZnIn2S4/UiO-66-(OH)2 is ascribed to the benign visible-light response and Z-scheme heterostructures, and the H2O2 evolution abides by indirect O2 reduction with ˙O2− as an intermediate species. Additionally, H2O2 yields using ZnIn2S4/UiO-66-NH2 on tap water and Xuanwu Lake (Nanjing, China) water can be comparable to that on the above-deionized water. This study sheds light on the great promise of functionalized MOFs and their applications on green (photo)catalytic energy conversion.
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MICROCHIMICA ACTA
·
2022
·Vol. 190
·期 1
·1-12
·
IF 6.408
Yan Zhengquan,Zheng Xiaoyu,Meng Guoqing,Tang Yulian,Zhou Xuemei,Hao Junkai,Feng Jing,Lin Naibo,Hu Lei
A portable sensor for visual monitoring of Fe 2+ and H 2 O 2 , two-dimensional Co 3 O 4 modified by nano-IrO 2 (IrO 2 @2D Co 3 O 4 ) was prepared in this work, for the first time, with the help of microwave radiation at 140 °C, which was further stabilized onto common test strips. The present IrO 2 @2D Co 3 O 4 possessed superior dual-function enzyme-like activity with low toxicity and excellent biocompatibility. Especially, trace Fe 2+ and H 2 O 2 could exclusively alter their enzyme-like catalytic activity with discriminating hyperchromic or hypochromic effect, i.e., from blue to colorless or to dark blue for both IrO 2 @2D Co 3 O 4 dispersion and its functionalized test strips. The linear regression equations were A 652 = 0.5940 − 0.00041 c Fe 2+ (10 −8 M, R 2 = 0.9927) for Fe 2+ and ∆A 652 = 0.0023 c H2O2 + 0.00025 (10 −7 M, R 2 = 0.9982) for H 2 O 2 , respectively. When applied to visual monitoring of aqueous Fe 2+ and intercellular H 2 O 2 , the recoveries were 101.2 ~ 102.5% and 95.8 ~ 103.7% with detection limits of 1.25 × 10 −8 mol/L and 1.02 × 10 −7 mol/L, respectively, far below the permitted values in drinking water set by the World Health Organization. The mechanisms for the enhancing enzyme-mimetic activity of IrO 2 @2D Co 3 O 4 and its selective responses to Fe 2+ and H 2 O 2 were investigated in detail. Graphical Abstract
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Guanglu Xia,Jianhao Qiu,Lu Zhang,Dingliang Dai,Jianfeng Yao
Photocatalytic H 2 O 2 production by reducing O 2 has drawn great interest, but most reactions were conducted in pure O 2 which requires extra energy input. Here, TpPa-1 was facilely decorated by ZnIn 2 S 4 nanosheets for H 2 O 2 production in ambient air under visible light . Profiting from the hierarchical heterostructure , efficient visible-light absorption and O 2 capture of ZnIn 2 S 4 /TpPa-1, an H 2 O 2 yield of 516 μmol·L −1 was obtained with 2 h irradiation, which is 3.0 and 3.9 times those of blank TpPa-1 and ZnIn 2 S 4 , respectively. The intimate interface contact between ZnIn 2 S 4 and TpPa-1 also contributes to the performance improvement. It is noted that the photocatalytic H 2 O 2 formation over ZnIn 2 S 4 /TpPa-1 hybrids experienced an indirect reduction of O 2 that ·O 2 - served as the key intermediate. Additionally, the reactions under different atmospheres and ethanol concentrations demonstrate that both O 2 and ethanol play important roles in the efficient evolution of H 2 O 2 . This work could enlighten the heterostructure construction and (photo)catalytic H 2 O 2 production based on covalent organic frameworks .
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 12
·126508
·
IF 4.386
Li Feng,Yan Xu,Wanting Deng,Yadong Wang,Xiaoqin Min,Xiaoyun Lin,Yongnian Ni
A novel electrochemical non-enzymatic sensor for glucose and H2O2 based on metal organic framework (MOF)-derived cobalt-nickel bimetallic oxides (NiCo2O4) and gold nanoparticle (AuNPs) composite modified glassy carbon electrode (GCE) was fabricated in this paper. The structure and morphology of the prepared materials was successfully characterised by X-ray diffraction (XRD), element mapping images and scanning electron microscopy (SEM). Moreover, the electrocatalytic activity for glucose and H2O2 was investigated at the NiCo2O4/AuNPs/GCE using cyclic voltammetry (CV) and amperometric i–t technique. The catalytic currents for glucose and H2O2 are proportional to their concentrations in the range of 0.2 μM–581 μM and 0.5 μM–1774.5 μM, respectively. The corresponding limits of detection (LOD) were calcuated be 0.0081 μM and 0.181 μM for glucose and H2O2. Furthermore, the NiCo2O4/AuNPs/GCE shows excellent stability, reproducibility and anti-interference ability.
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CHEMOSPHERE
·
2023
·
IF 8.8
Baizhou Lu,Zhanqiang Fang,Pokeung Eric Tsang,Jinhua Wu
To overcome the bottlenecks of the conventional zero-valent iron Fenton-like (ZVI/H 2 O 2 ) process, such as low reagent utilization, low applicable pH, and iron sludge contamination, guava leaf extract (GLE) was used as a green promoter to enhance ZVI/H 2 O 2 process in this study. Compared with the ZVI/H 2 O 2 system, the removal rate and k obs of norfloxacin by the ZVI/H 2 O 2 /GLE system were increased by 33.76% and 2.19 times, respectively. The experimental investigation of the mechanism showed that the attack of reactive oxygen species was the main pathway for the removal of pollutants, and three types of reactive oxygen species ( 1 O 2 , O 2 − ,·OH) generations in the ZVI/H 2 O 2 /GLE system were effectively promoted by the introduction of GLE. The reactivity improvement was mainly due to the decrease of pH. At the same time, the chelation of iron ions by GLE promoted the Fe(III)/Fe(II) cycle on the catalyst surface was also a minor mechanism to improve the reactivity. This study provides a crucial reference for the practical application of guava leaf to promote the ZVI/H 2 O 2 process in environmental pollution control .
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Fengxia Deng,Shilin Yang,Baojian Jing,Shan Qiu
In the electro-Fenton process, there still suffers concern of low H 2 O 2 generation caused by inadequate mass transfer of oxygen and low selectivity of oxygen reduction reaction (ORR). To solve it, in this study, various particle sizes (850 μm, 150 μm, and 75 μm) of granular activated carbon filled in a microporous titanium-foam substate was used to develop a gas diffusion electrode (AC@Ti–F GDE). This facile-prepared cathode has seen a 176.15% improvement in H 2 O 2 formation compared to the conventional one. Aside from a much higher oxygen mass transfer by creating gas-liquid-solid three-phase interfaces coupled with much high dissolved oxygen, the filled AC played a significant role in H 2 O 2 accumulation. Among these particle sizes of AC, the one in 850 μm has observed the highest H 2 O 2 accumulation, reaching 1487 μM in 2 h electrolysis. Because there is a balance between chemical nature for H 2 O 2 formation and micropore-dominant porous structure for H 2 O 2 decomposition, resulting in an electron transfer of 2.12 and H 2 O 2 selectivity of 96.79% during ORR. In a word, the facial AC@Ti–F GDE configuration is promising for H 2 O 2 accumulation.
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高影响因子
Materials
·
2023
·Vol. 16
·期 3
·1261
·
IF 3.4
Qian Wang,Yuzhe Wang,Guiyong Xiao,Xinde Zhu
In this work, the facile fabrication of Co3O4particles/reduced graphene oxide (Co3O4/rGO) composites on Indium tin oxide (ITO) slide was achieved by an electrophoretic deposition and annealing process. The deposition time and ratio of the precursors were optimized. Structural characterization and chemical composition investigation indicated successful loading of Co3O4particles on graphene sheets. When applied as a non-enzymatic H2O2sensor, Co3O4/rGO showed significant electrocatalytic activity, with a wide linear range (0.1–19.5 mM) and high sensitivity (0.2247 mA mM−1cm−2). The good anti-interference ability, reproducibility, and long-term stability of the constructed sensor were also presented. The application of Co3O4/rGO in real sample analysis was evaluated in human urine sample with satisfactory results, indicating the feasibility of the sensor in physiological and medical applications.
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Hao Ding,Gongsong Tong,Jingchun Sun,Jiewei Ouyang,Fangge Zhu,Zhi Zhou,Nan Zhou,Mei’e Zhong
Biochar, as an adsorbent, is widely used for the removal of organic pollutants in water body. Hence, after saturated adsorption, regeneration treatment is required to recover the adsorption performance of biochar. In this study, a biochar (P-GBC) prepared by phosphoric acid activation showed high adsorption capacity for methylene blue (MB) with the maximum adsorption capacity (Q m ) of 599.66 mg/g. Then, regeneration treatments using 4 mM peroxymonosulfate (PMS), 0.2 M hydrogen peroxide (H 2 O 2 ) and their mixture were used to regenerate MB-saturated biochar with regeneration efficiencies of 58.24%, 66.01% and 94.88%, respectively. Combining with degradation and quenching experiments, it is found that synergistic effect of H 2 O 2 desorption and PMS degradation is responsible for the enhancement of regeneration efficiency of P-GBC in H 2 O 2 -PMS system and enables a high mineralization rate of 82.68% for the MB adsorbed on P-GBC. Furthermore, EPR tests indicate that singlet oxygen ( 1 O 2 ) is assigned as the primary activate species for the degradation of MB and XPS analyses confirm that graphite nitrogen and carbonyl on P-GBC are the main active sites for the activation of PMS. Compared with conventional regenerants, H 2 O 2 -PMS system has the advantages of low dosage, high mineralization efficiency, and easy accessibility, and is also effective, sustainable and environmentally friendly for the regeneration of organic pollutants-saturated biochar.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2022
·
IF 5.999
Yuyan Yan,Renlu Han,Huijun Zhang,Pengxin Song,Xiangjun Wei,Yafei Hou,Jiancheng Yu,Keqi Tang
Chemodynamic therapy (CDT), which employs Fenton/Fenton-like agents to decompose hydrogen peroxide (H 2 O 2 ) into toxic hydroxyl radical (•OH) to induce cancer cell apoptosis and necrosis, holds great promise in tumor therapy due to its high selectivity . Nevertheless, its efficiency is impaired by the insufficient intracellular H 2 O 2 concentration and/or the insensitive response of Fenton/Fenton-like agents to the slightly acid tumor microenvironment (pH∼7.0–6.5). Herein, we develop a novel CDT reagent based on CeO 2 quantum dot (QD) decorated MgO 2 nanosheets engineered with cascade reactions to boost the intracellular H 2 O 2 level and high pH-activated (pH = 6.5) characteristic for an enhanced CDT. Under the tumor microenvironment (pH = 6.5), MgO 2 nanosheets that are highly reactive can react with H 2 O to produce nontoxic Mg 2+ and abundant H 2 O 2 , boosting the intracellular H 2 O 2 level. The self-generated H 2 O 2 is subsequently converted into •OH by CeO 2 QD, which is served as a relatively high pH-activated (pH = 6.5) Fenton-like agent. The sufficient intracellular H 2 O 2 supply and sensitive response to the slightly acid tumor sites significantly improve the Fenton reaction, leading to the excellent in vivo CDT results with tumor growth inhibition effect. Our work presents a distinctive paradigm for self-boosting CDT efficacy.
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RSC Advances
·
2022
·Vol. 12
·期 44
·28349-28358
·
IF 4.036
Xin Zhang,Siqin Wang,Jiahao Dao,Jiajing Guo,Yanfang Gao
A novel colorimetric platform based on nano-composites of two-dimensional (2D) molybdenum disulfide nanosheets (MoS2 NSs) and one-dimensional (1D) carbon nanotubes (CNTs), called 2D–1D MoS2-CNT nanozyme, was fabricated for the selective and sensitive determination of hydrogen peroxide (H2O2) in soda water. The MoS2-CNT nanozyme was synthesized through a one-step solvothermal reduction method. The introduced CNTs could effectively prevent the stacking of MoS2 nanosheets (NSs) and not only expanded the interlayer distance of MoS2 NSs from 0.620 nm to 0.710 nm but also improved their specific surface. Under acidic conditions, the as-prepared 2D–1D MoS2-CNT nanozymes could oxidize the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue-oxidized TMB (oxTMB) in the presence of H2O2, resulting in enhanced peroxidase-like (POD-like) activity. The kinetic study showed that MoS2-CNT nanozyme had stronger catalytic activity than natural horseradish peroxidase (HRP). The linear range for H2O2 colorimetric determination was 5.00–500 μmol L−1 with a limit of detection (LOD) of 1.40 μmol L−1. Furthermore, the established determination method was applied to actual samples and the recoveries of H2O2 spiked in soda water were in the range of 92.3–107%, showing feasibility for the analysis of food.
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高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Bo Sheng,Chaoyuan Deng,Yangfan Li,Shijie Xie,Zhaohui Wang,Hua Sheng,Jincai Zhao
In Fenton or Fenton-like reactions, ·OH obtained by the reductive activation of H2O2 is regarded as the major reactive oxygen species (ROS); however, the generation of other ROS like O2·– and 1O2 cannot be negligible. Since the degradation capability of a certain ROS would be varied to distinctive pollutants, the regulation of ROS production from H2O2 activation should be applicable for a more targeted pollutant degradation. Herein, a series of carbon nitride (C3N4)-supported Fe catalysts with the state of Fe ranging among single-atom, oxide-cluster, and nanoparticle catalysts were fabricated and their activities in photo-Fenton reactions were evaluated. It was uncovered that the single-atom catalyst favored the generation of O2·– and 1O2 via the oxidative activation of H2O2 and the selectivity of 1O2 toward ·OH dynamically increased with the proceeding of H2O2 activation, while the catalysts with an abundance of oxide clusters exhibited a significantly higher conversion of H2O2 to ·OH. In situ FT-IR studies demonstrated that during the H2O2 activation, the single-atom catalyst underwent a more significant surface hydroxylation than the oxide-cluster catalyst. Such a result was further consolidated by the theoretical calculation that the adsorption energy of surface hydroxyl was remarkably higher on the single-atom catalyst. Thereafter, distinctive from the easy desorption of hydroxyl during the reduction of H2O2 to ·OH in oxide-cluster catalysts, the in situ surface hydroxylation on the single-atom catalyst alters the adsorption mode of H2O2 to a H-bonded structure, which steers the selectivity of ROS generation to a more favored oxidative transformation of H2O2 to O2·–/1O2. This work uncovers the decisive role of surface hydroxyl in regulating ROS generation in a heterogeneous Fenton reaction.
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