ANALYST
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2022
·Vol. 147
·期 5
·956-964
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IF 5.227
Yiyin Zhang,Xiang Gao,Yingwang Ye,Yizhong Shen
Rapid and accurate monitoring of food freshness to provide consumers with high-quality meat continues to be of tremendous importance to the food industry. In this report, an efficient Fe-doped polydopamine (Fe-PDA) nanozyme with peroxidase-mimicking activity was synthesized by a high-temperature hydrothermal method, and was applied to a spectrophotometric sensing system, which successfully reports the concentration of hypoxanthine (Hx) related to meat freshness. The Fe-PDA nanozyme showed excellent peroxidase simulation activity, which was primarily verified by steady-state kinetics experiments. In the presence of xanthine oxidase (XOD), Hx can react quantitatively with dissolved O2 to generate H2O2, which can be further catalyzed and produce hydroxyl radicals (•OH) under acidic conditions via the Fe-PDA nanozyme and oxidize colorless TMB to blue oxTMB with absorbance at 653 nm. The absorbance at 653 nm expressed a clear linear relationship with hypoxanthine concentration in the range of 5.13–200 μM, and the detection limit was 1.54 μM. This method was further assessed by measuring the recovery of Hx added to meat samples, which showed promising accuracy. Overall, the developed Fe-PDA nanozyme with excellent peroxidase-mimicking activity is cost-effective, high-performance and easy to produce, offering an efficient and low-cost sensing system based on spectrophotometry for meat freshness determination as an alternative to conventional methods.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Shan Wang,Zunfu Hu,Qiulian Wei,Ping Cui,Huimin Zhang,Weina Tang,Yunqiang Sun,Haiqiang Duan,Zhichao Dai,Qingyun Liu,Xiuwen Zheng
Recently, extending single-atom catalysts from mono- to binary sites has been proved to be a promising way to realize more efficient chemical catalytic processes. In this work, atomically dispersed Fe, Pt dinuclear catalysts ((Fe, Pt)SA-N-C) with an ca. 2.38 Å distance for Fe1 (Fe-N3) and Pt1 (Pt-N4) could be precisely controlled via a novel secondary-doping strategy. In response to tumor microenvironments, the Fe-N3/Pt-N4 moieties exhibited synergistic catalytic performance for tumor catalytic therapy. Due to its beneficial microstructure and abundant active sites, the Fe-N3 moiety effectively initiated the intratumoral Fenton-like reaction to release a large amount of toxic hydroxyl radicals (•OH), which further induced tumor cell apoptosis. Meanwhile, the bonded Pt-N4 moiety could also enhance the Fenton-like activity of the Fe-N3 moiety up to 128.8% by modulating the 3d electronic orbitals of isolated Fe-N3 sites. In addition, the existence of amorphous carbon revealed high photothermal conversion efficiency when exposed to an 808 nm laser, which synergistically achieved an effective oncotherapy outcome. Therefore, the as-obtained (Fe, Pt)SA-N-C-FA-PEG has promising potential in the bio-nanomedicine field for inhibiting tumor cell growth in vitro and in vivo.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
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IF 8.91
Tong Zhu,Jinping Jiang,Jisheng Wang,Zhening Zhang,Jiao Zhang,Jing Chang
A magnetic FeCo 2 O 4 /Co 3 O 4 nanocomposite was successfully synthesized by a facile hydrothermal method as an efficient activator for persulfate (PS) activation to degrade tetracycline (TC) in an aqueous solution. TC removal and mineralization efficiencies reached up to 91.63% and 43.57% in 120 min in the FCC-3/PS system, respectively. The mixed-valence of Fe/Co in the nanocomposite catalyst was beneficial for electrons transfer between Co and Fe elements and enhanced the redox circulation of Fe and Co in between divalent and trivalent. Surficial analysis and phosphate adsorption test confirmed the existence of –OH groups on the surfaces of FeCo 2 O 4 /Co 3 O 4 nanocomposite. Fe/Co redox and surficial hydroxyl in the catalyst played significant roles in the TC potentiation degradation, which was contributed by the plenty of adsorbed –OH groups and excellent dispersity of FeCo 2 O 4 in the FeCo 2 O 4 /Co 3 O 4 composite. The sulfate radicals were major species followed by the hydroxyl radicals , and the surficial adsorbed hydroxyl made great contributions to radical generation. The cycling test and intermediate toxicity analysis indicated that the nanocomposite was considered stable and practicable in water treatment . This work demonstrated that the FeCo 2 O 4 /Co 3 O 4 nanocomposite was an effective and environ-friendly catalyst towards PS activation for removing organic pollutants from water.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yi-Hao Tong,Yu-Zhe Wu,Zhen-Liang Xu,Li-Han Luo,Sun-Jie Xu
This work was expected to develop a new loose NF membrane with facile materials to conduct dye/salt separation and endow it with versatile capacities to offer an applicable solution to treat textile wastewater. Ethylene vinyl alcohol (EVAL) was first chosen to fabricate loose nanofiltration (NF) membrane through non-solvent induced phase separation (NIPS) method. Besides, MIL-101(Fe) showed outstanding photocatalytic capacity in degrading organic molecules while a low-cost bio-inspired coating, catechol, was utilized to modify MIL-101(Fe). A combination of modified MIL-101(Fe) and EVAL could have a high water permeability (43.2 L·m −2 ·h −1 ·bar −1 ) with superior rejection to small molecule negative charged dyes (Chlorazol black T: 99.8%, Congo Red: 99.7%, Eriochrome black T: 98.4%) and low rejection to various salts (Na 2 SO 4 : 4.8 %, NaCl: 2.1 %, MgCl 2 : 2.9%, MgSO 4 : 4.9% and CaCl 2 : 3.3%). Meanwhile, the EVAL loose NF membrane with the best performance had excellent antifouling capacity and long-term stability in EBT/Na 2 SO 4 separation. Moreover, the membrane could degrade dyes to self-clean the membrane surface through photocatalytic process, which originated from the Fe-O clusters in MIL-101(Fe).
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Shuai Liu,Mengmeng Jin,Jiaqiang Sun,Yongji Qin,Sanshuang Gao,Yu Chen,Shusheng Zhang,Jun Luo,Xijun Liu
Electrocatalytic CO 2 reduction reaction (CRR), powered by renewable energy sources, is a promising route to address energy and environmental issues. Herein, we fabricate single atomic Fe sites anchored on B and N co-doped carbon (Fe-SA/BNC), which showed excellent CRR activity, achieving a highest Faradaic efficiency of ∼ 94% at −0.7 V versus reversible hydrogen electrode. The performance is much better than that of the B-free sample. Furthermore, an outstanding current density of ∼ 130 mA cm −2 , as well as ∼ 99% Faradaic efficiency, has been achieved using the membrane electrode assembly (MEA). Details of density functional theory (DFT) calculations revealed that the introduction of B was beneficial for the desorption of *CO. The Zn-CO 2 battery was then assembled, which reached a high peak power density of 1.18 mW cm −2 at a current density of 4 mA cm −2 , as well as showing remarkable stability for CO production.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yucheng Li,Xiangyu Wang,Zhengyin Duan,Dehai Yu,Qiang Wang,Dandan Ji,Wenxia Liu
Treating dye-contaminated wastewater using the visible light–driven photo-Fenton reaction is beneficial to environmental remediation. This paper reports the synthesis of a novel, highly effective photo-Fenton catalyst, the Zn/Co-ZIFs@MIL-101(Fe) composite, by a facile internal-growth method. The composite, which had an MOF-in-MOF structure, activated H 2 O 2 to decompose RhB, a polluting-dye model, under visible-light illumination. The transfer of the electron–hole pair was synergistically accelerated by the reaction centers of the composite (the MIL-101(Fe) shell and Zn/Co-ZIFs core), which enhanced H 2 O 2 activation. The generated OH, O 2 − , and 1 O 2 effectively decomposed RhB. The composite’s catalytic performance was significantly enhanced by the electronic hybridization of its Fe 3+ , Co 2+ , and Zn 2+ metal centers. Thus, the composite demonstrated a remarkable capability to remove RhB. The composite polymetallic MOFs loaded with 3% Zn/Co-ZIFs prepared by us showed good reusability and water stability, and their morphology and structure did not change significantly after four runs, depending on the iron, cobalt, and zinc metal leaching concentrations 0.134 mg/L, 0.06 mg/L and 0.054 mg/L respectively. This study provides a novel method to construct an Zn/Co-ZIFs@MIL-101(Fe) catalyst with dual reaction centers that enhance the transfer of electron–hole pairs. Our findings inspire the application of MOF-based photo-Fenton catalysts to wastewater treatment and environmental remediation.
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2022
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IF 1.193
Yan-Yan XING,Mei-Ling CHEN,Xin-Ai SHEN,Ning LIANG,Xiao-Hong HOU
In consideration of the promising application of peroxidase (POD)-like nanozymes in biomedical analysis, the development of POD mimics with good catalytic performance under neutral conditions remains significant. As a new catalyst, metal-organic frameworks have been explored as candidate nanozymes owing to their high catalytic activity, good stability, flexible and simple synthesis methods, diverse types, and properties. Herein, rod-like Fe-MIL-88A was successfully synthesized via a simple hydrothermal method. Fe-MIL-88A exhibited POD-like properties under neutral conditions and a stronger affinity for substrate 3,3 ' ,5,5 ' -tetramethylbenzidine and H 2 O 2 than natural horseradish POD. This result was primarily due to the additional exposed (100) facets of rod-like Fe-MIL-88A, which can catalyze the decomposition of H 2 O 2 to •OH more easily. Based on the POD-like properties of Fe-MIL-88A under neutral conditions, combined with glucose oxidase, a one-pot colorimetric analysis method for glucose detection was established. The proposed measurement had a linear range of 1–100 µM and a limit of detection of 0.45 µM. The colorimetric method was accurate, reliable, highly selective, convenient, and time-saving. Furthermore, the one-pot method was successfully applied to detect the concentration of glucose in human blood samples, and the measured results were consistent with those of commercial glucose meters, indicating that the proposed method can be a potential candidate for glucose detection.
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RSC Advances
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2022
·Vol. 12
·期 16
·9543-9549
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IF 4.036
Tanlun Wang,Chenxiang Sun,Yong Yan,Fan Li
Metal–N–C-based catalysts prepared by pyrolysis are frequently used in the oxygen reduction reaction (ORR). Zeolitic imidazolate frameworks (ZIFs), a type of metal organic framework (MOF), are selected as precursors due to their special structure and proper pore sizes. A series of Fe–N–C catalysts with different concentrations of 2-methylimidazole were prepared with a simple solvothermal-pyrolysis method, and the transformation productivity, morphology and ORR activity were investigated. It was found that the Fe–N–C catalyst with a 2-methylimidazole concentration of 0.53 mol L−1 had the best performance. In 0.1 M KOH solution, the half-wave potential was 0.852 V (vs. RHE), with the highest electrochemically active surface area (ECSA) of 94.1 cm2, and the ORR reaction was dominated by a 4-electron process. The current only decreased by 10.5% after 50 000 s of chronoamperometry (CA), while the half-wave potential only decreased 20 mV in 3 M methanol. Additionally, this catalyst cannot be poisoned by Cl− and SO32− ions in the ORR process. Finally, some typical ions including SCN−, Fe(CN)63− and Fe(CN)64− were used to inhibit the active sites, and it was determined that Fe(II) is the real active species. The series of synthesis and testing experiments has significance in guiding optimization of the synthesis conditions and analysis of the mechanism of active sites in Fe–N–C materials.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Yang Liu,Fenxian Cun,Dongqi Tian,Peng Zhou,Yue Yuan,Zhaokun Xiong,Chuanshu He,Ye Du,Zhicheng Pan,Bo Lai
Sodium bismuthate dihydrate (NaBiO 3 .2 H 2 O, NBH) nanosheets were successfully prepared in this study using the persulfate oil bath oxidation method. Benefited from the unique layered structure of NBH, the Fe(III) as a variable valence metal ion was explored for enhancing NBH activation of peroxymonosulfate (PMS) to degrade levofloxacin (LVF) in the visible-light catalytic system. Based on results of the reactive oxygen species (ROS) quenching experiments and electron paramagnetic resonance (EPR) analysis, singlet oxygen ( 1 O 2 ) and superoxide radical (O 2 ·- ) were identified as the main ROS. The morphology, chemical structure, and optical properties of NBH were analyzed using various characterization methods. It was confirmed that Fe(III) embedded in the NBH via the ion exchange with Na, resulting in lattice oxygen vacancies on the surface of the NBH, after the formation of oxygen defect sites, reacts with PMS in the solution to produce active oxygen species with oxidizing efficiency. This study expands the technological application of NBH in the catalytic oxidation of variable valence metals, which are essential for the removal of fluoroquinolone antibiotics.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Xiaobo Ma,Lijun Gao,Qiyu Zhang,Weibo Hua,Yating Zhang,Xinyang Li,Juan Yang,Shujiang Ding,Chao Hu
The traditional Haber-Bosch N 2 fixation process suffers from rigorous reaction conditions and massive CO 2 emission. By contrast, N 2 electroreduction by water to the direct production of NH 3 can be conducted at room temperature and atmospheric pressure, and thus has been attracting increasingly attention. Herein, we develop a nano-CaCO 3 template route for the synthesis of Fe, N co-doped porous carbon materials from zeolitic imidazolate framework-8 (ZIF-8). The Fe atoms are atomically dispersed in the skeleton of carbon and bonded with four nitrogen atoms . Interestingly, the morphology and pore structure of these carbons have notable effects on their performance for the electrocatalytic reduction of N 2 . With an optimized morphology and pore structure tuned by the addition of nano-CaCO 3 template, the ZIF-8 derived Fe, N co-doped carbon catalyst shows a Faradaic efficiency of 13.14% and a NH 3 yield as high as 13.01 µg h −1 mg cat −1 (−0.2 vs . reversible hydrogen electrode) for N 2 reduction reaction in 0.1 M KOH aqueous electrolyte . Morphology engineering strategy may open a new path to designing and synthesizing high-performance carbon-based catalysts for the electroreduction of N 2 to NH 3 .
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Wei Yuan,Lichun Cheng,Tianrui Xia,Yucheng Chen,Qianxing Long,Qingrong Yao,Shunkang Pan,Chaohao Hu
Perovskite LaCoO 3 has unique mixed ionic electronic and structural defects, which has high research value in microwave absorption field. LaCoO 3 precursor was prepared by sol-gel method, and LaCo 1− x Fe x O 3 (Fe-LCO, x = 0, 0.05, 0.1 and 0.15) with rhombic symmetric structure was successfully synthesized at 600 °C. By refinement of X-ray diffraction (XRD) (Rietveld analysis), it was found that Fe doping makes LaCoO 3 lattice constant and cell volume increase. As a dielectric loss microwave absorbing material, the electromagnetic attenuation of LaCoO 3 is mainly due to the conduction loss, while the interface and dipole polarization are secondary reasons. It finds that Fe doping can improve the wave absorption performance of LaCoO 3 . The best absorbing performance was obtained when Fe content is x = 0.1, with the maximum reflection loss of − 38.99 dB at 10.8 GHz and the effective absorption bandwidth (RL<−10 dB) is 4.48 GHz, while the corresponding thickness was only 3 mm. In summary, LaCoO 3 has broad application prospects in X and Ku bands.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yangjun Luo,Yanwei Wang,Youyuan Wang,Heming Huang,Li Zhang,Huijuan Zhang,Yu Wang
Although various alloys have been extensively explored to enhance catalyst activity and stability in oxygen reduction, degradation of performance due to long-term operation has plagued the crowd. Here, we develop a catalyst synthesis strategy based on the coexistence of monoatomic Fe and Pt-based clusters/alloys on NC/TiO x . Fe/PtCo-NC/TiO x exhibits a half-wave potential of 0.948 V and mass activity of 3.69 A mg Pt −1 at 0.9 V, the latter being approximately 32.1 times higher than that of 20% Pt/C (0.115 A mg Pt −1 ). Additionally, it also shows maximum power densities of 952.2 mW cm −2 and 215.8 mW cm −2 in the H 2 /O 2 fuel cell and Zn-air battery, respectively. The combination of illumination and calcination promotes the electron transfer between Pt and TiO x , thus enhancing the catalytic activity and stability. We also explore the approach and mechanism of using illumination to suppress catalyst performance degradation. The intermittent irradiation inhibits the dissolution of Pt to facilitate the Fe/PtCo-NC/TiO x durability beyond that of most reported metal catalysts, with a half-wave potential degradation of only 14 mV after 30,000 cycles. The ingenious use of illumination provides a simple and feasible strategy for the sustainable utilization of catalysts.
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