MICROCHIMICA ACTA
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2022
·Vol. 189
·期 4
·1-5
·
IF 6.408
Tian Dazhi,Xiang Wen,Wang Hao,Jiang Wentao,Li Ting,Yang Minghui
B-doped core–shell Fe@BC nanozyme was synthesized. The peroxidase (POD) like activity of Fe@BC nanozyme was studied and utilized for detecting the activity of alanine aminotransferase (ALT). In the presence of ALT as well as ALT co-substrates l -alanine and α-ketoglutarate, l -glutamate is generated. The following catalytic oxidation of l -glutamate by glutamate oxidase leads to the generation of H 2 O 2 . The POD-like activity of Fe@BC can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to oxTMB in the presence of H 2 O 2 , generating a blue-colored compound. Through the detection of the amount of H 2 O 2 generated, ALT activity can be determined through measuring the absorbance intensity variation at 450 nm. The limit of detection of the assay is 4 U/L, with a linear range from 10 to 1000 U/L. For human serum samples, the ALT levels determined by our assay are comparable to those determined by the hospital with a correlation coefficient of 0.991, demonstrating the reliability of our assay results. Graphical abstract
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高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Tianwei Hao,Yao Huang,Fangbai Li,Yundang Wu,Liping Fang
Fe(II) redox chemistry is a pivotal process of biogeochemical Fe cycle and the transformation of organic pollutants in subsurface aquifers, while its interfacial reactivity on iron oxides with varying surface chemistries remains largely unexplored. In this study, the redox processes of Fe(II) on two hematite with highly exposed {001} and {110} facets and their impacts on the transformation of nitrobenzene were investigated. Results suggest that Fe(II) adsorption is the rate-limiting step of the redox chain reactions, controlling the reduction potential ( E H ). Nitrobenzene activates the facet electron transfer on hematite, leading to nitrobenzene reduction and Fe(II) oxidation. Moreover, {001} facet exhibits a higher reactivity and electron transport efficiency than {110} facet, which is attributed to a lower site density (0.809 #Fe/nm 2 ) and a lower E H of hematite {001} facet than that of {110} facet. It is worth noting that the facet-dependent reduction activity is more intense at low pH or high Fe(II) activity. A slight dissolution of {110} facet was observed, indicating hematite {001} facet exhibits higher thermodynamic stability than {110} facet. This study confirms the facet-dependent reducing activity of surface bound Fe(II) on hematite, providing a new perspective for in-depth understanding of the interfacial reactions on hematite. The findings of this work broaden the biogeochemical process of Fe cycle in subsurface environments and its impact on the fate of organic pollutants in groundwater.
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 15
·2200276
·
IF 6.389
Dong Liu,Chenxi Huyan,Yuanyuan Zhao,Terence Xiaoteng Liu,Ding Wang,Jining Sun,Sheng Dai,Fei Chen,Ben Bin Xu
Carbon-based single-atom iron electrocatalysts with nitrogen coordination (CSAIN) have recently shown enormous promise to replace the costly Pt for boosting the cathodic oxygen reduction reaction (ORR) in fuel cells. However, there remains a great challenge to achieve highly efficient CSAIN catalysts for the ORR in acidic electrolytes. Herein, a novel CSAIN catalyst is synthesized by pyrolyzing a precursor mixture consisting of metal–organic framework and conductive polymer hybrid. After pyrolysis at a high temperature, the CSAIN with a structure of carbon nanosheet supported polyhedral carbon is achieved, where the unique structure endows CSAIN with expediting electron transfer and mass transport, as well as largely exposed surface to host atomically dispersed iron active sites. As a result, the optimal CSAIN catalyst shows a high ORR activity with its half-wave potential of 0.77 V (vs RHE) and a Tafel slope of 74.1 mV dec –1 , which are comparable to that of commercial Pt/C catalyst (0.80 V and 81.9 mV dec –1 ).
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Wan Xin,Liu Qingtao,Liu Jieyuan,Liu Shiyuan,Liu Xiaofang,Zheng Lirong,Shang Jiaxiang,Yu Ronghai,Shui Jianglan
Simultaneously increasing the activity and stability of the single-atom active sites of M–N–C catalysts is critical but remains a great challenge. Here, we report an Fe–N–C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe–N 4 active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe–N 4 due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe–N 4 and also shorten the bond amplitude of Fe–N 4 with incoherent vibrations. As a result, both the activity and stability of Fe–N 4 sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.
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Nanomaterials
·
2022
·Vol. 12
·期 5
·811
·
IF 5.719
Kang-Ping Cui,Yu-Ying He,Kai-Jie Xu,Yu Zhang,Chang-Bin Chen,Zheng-Jiang Xu,Xing Chen
In this work, the combination of high surface area diatomite with Fe and Cu bimetallic MOF material catalysts (Fe0.25Cu0.75(BDC)@DE) were synthesized by traditional solvothermal method, and exhibited efficient degradation performance to tetracycline hydrochloride (TC). The degradation results showed: Within 120 min, about 93% of TC was degraded under the optimal conditions. From the physical–chemical characterization, it can be seen that Fe and Cu play crucial roles in the reduction of Fe3+because of their synergistic effect. The synergistic effect can not only increase the generation of hydroxyl radicals (•OH), but also improve the degradation efficiency of TC. The Lewis acid property of Cu achieved the pH range of reaction system has been expanded, and it made the material degrade well under both neutral and acidic conditions. Loading into diatomite can reduce agglomeration and metal ion leaching, thus the novel catalysts exhibited low metal ion leaching. This catalyst has good structural stability, and less loss of performance after five reaction cycles, and the degradation efficiency of the material still reached 81.8%. High performance liquid chromatography–mass spectrometry was used to analyze the degradation intermediates of TC, it provided a deep insight of the mechanism and degradation pathway of TC by bimetallic MOFs. This allows us to gain a deeper understanding of the catalytic mechanism and degradation pathway of TC degradation by bimetallic MOFS catalysts. This work has not only achieved important progress in developing high-performance catalysts for TC degradation, but has also provided useful information for the development of MOF-based catalysts for rapid environmental remediation.Keywords:Fenton-like catalyst;bimetallic MOF;diatomite;synergistic effect;antibiotics
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APPLIED CLAY SCIENCE
·
2022
·
IF 5.907
Qiushi Jiang,Zhaolian Han,Nan Qu,Lianzhi Sun,Yafeng Yuan,Yating Ren,Zhiqiang Cheng
A low-cost palygorskite (Pal)/MIL-101(Fe) was prepared by solvothermal method and calcined under nitrogen protection to form the magnetic derivant Pal/MIL-101(Fe)-400, the successful combination of which was confirmed. The band gap (1.47 eV) of Pal/MIL-101(Fe)-400 was lower than 2.25 eV of Pal/MIL-101(Fe), indicating a significant improvement in light absorption performance. In addition, Pal/MIL-101(Fe)-400 exhibits stronger photocurrent response and lower impedance due to the formation of Fe 3 O 4 clusters with high electrical conductivity and new active centers by calcination. The prepared Pal/MIL-101(Fe)-400 can achieve 90 mg/g RhB removal completely, which is better than 77.0% adsorption of MIL-101(Fe) and 67.2% adsorption-photocatalytic of Pal/MIL-101(Fe), which also shows superparamagnetism properties and excellent cyclic stability. In addition, Pal/MIL-101(Fe)-400 mainly relies on the action of peroxy radical to oxidize organic pollutants, which is different from Pal/MIL-101(Fe). This work provides a new perspective for the construction of magnetic MOF multifunctional materials for the efficient treatment of pollutants in water.
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Small Structures
·
2022
·Vol. 3
·期 4
·2100211
·
IF 11.343
Fan Tang,Sijie Guo,Yonggang Sun,Xijie Lin,Jianhua Qiu,Anmin Cao
Developing high-performance, low-cost, and robust electrocatalysts is of great importance to boost the efficiency of oxygen evolution reaction (OER). Herein, based on the integrated design of chemical composition and geometric structure, Fe-doped CoO nanotubes (NTs) with high OER activity are prepared by a facile template-free approach. The construction of this tubular structure is realized via a simple wet-chemical reaction to prepare solid nanorods as precursor and a subsequent calcination treatment of the precursor to form hollow cavity. The favorable composition and unique hollow structure endow these Fe-doped CoO NTs with remarkable activity toward OER. When used as the electrocatalyst for OER, the Fe-doped CoO NTs show a small overpotential of 282 mV at the current density of 10 mA cm −2 , a low Tafel slope of 78.26 mV dec −1 , and a high turnover frequency of 0.0965 s −1 at the overpotential of 282 mV, which is superior to those of CoO NTs and solid CoO nanoparticles. Moreover, the Fe-doped CoO NTs also exhibit excellent long-term stability of 24 h at the current density of 10 mA cm −2 .
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BIOSENSORS & BIOELECTRONICS
·
2021
·
IF 10.618
Yu Wang,Xitong Zhou,Wanxin Dong,Qinsong Zhong,Xinxin Mo,He Li
In this work, we synthesized Fe-Tcpp@ICG(ICG, Indocyanine green) with light stimuli-response through 5,10,15,20-tetrakis (4-carboxyphenyl) porphyrin (Fe-Tcpp) loaded ICG by electrostatic adsorption. The morphology and properties of Fe-Tcpp and Fe-Tcpp@ICG were characterised by ultraviolet–visible absorption spectrometer, X-ray diffraction, thermogravimetric analyzer and transmission electron microscope , respectively. A non-enzymatic photoelectrochemical sensor based on Fe-Tcpp@ICG was constructed to quantitatively detect hydrogen peroxide in tumor microenvironment . Under the optimal conditions, the linear range of detecting hydrogen peroxide was 0.01–50 mmol/L with detection limit of 0.2 μmol/L (S/N = 3). This sensor proposed a simple, fast, sensitive and label-free method for the detection of hydrogen peroxide. Moreover, the results also showed that the Fe-Tcpp@ICG can catalyze the decomposition of hydrogen peroxide to generate singlet oxygen, which can kill tumor cells. These indicated that this material was expected to be used for detecting hydrogen peroxide and inhibition of tumor cell growth.
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ACS Catalysis
·
2023
·
IF 12.9
Xiaoxue Han,Qiao Zhao,Huiyong Gong,Chongyang Wei,Jing Lv,Yue Wang,Mei-yan Wang,Shouying Huang,Xinbin Ma
Fe-based catalysts undergo complex reduction, carburization, and phase interconversion as well as oxidation during Fischer–Tropsch synthesis (FTS). Unraveling the evolution of carbides and establishing the dominant factors are essential for rational design and modulation of Fe-based catalysts. In this work, Fe–oxide interfaces were constructed to investigate the effect on phase transformation and FTS performance. By correlating performance to the composition of iron species, the crucial role of Fe2.2C in high CO conversion and C5+ productivity has been confirmed. More importantly, a heterogeneous spatial distribution of iron carbides and oxides induced by Fe–oxide interfaces was observed. Fe3O4 preferentially forms at interfaces with the coexistence of carbon-rich Fe2.2C at subadjacent interfaces, while Fe5C2 locates at the region away from oxides or in the bare Fe catalyst. Further ex/in situ characterizations, including XPS, TPO, in situ XRD, and in situ IR, were conducted for revealing the mechanism. This study provides insights for iron carbides formation and stability by modulating interfaces, which guides the further development of Fe-based FTS catalysts.
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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 107
·期 13
·4301-4309
·
IF 5
Wang Xueqin,Chen Xuyang,Liu Junyan,Tao Haizhen,Shao Ninghan,Li Wenlin,Huang Shiyu,Zhang Xiyan,Li Na
Abstract Total antioxidant capacity (TAC) is currently considered as a vital indicator of food quality in antioxidant ability and attracts much attention for human healthcare. It is thus of great significance to realize the accurate and rapid detection of TAC in foods. Herein, we have constructed a preferable hybrid nanozyme based on the mesoporous silica-stabilized CuO composited Fe 3 O 4 nanoparticles (Fe 3 O 4 @MSNs@CuO, FMC NPs), which possess the enhanced peroxidase (POD)-like activity via cascade response for specific and sensitive determination of TAC in fruit foods. The results showed the hybrid nanozyme displayed a remarkable POD-like activity, excellent selectivity and sensitivity, and the limit of detection (LOD) of the colorimetric sensor was 6.13 mM with the concentration range from 10 to 45 mM. Therefore, the fabricated hybrid nanozyme can be regarded as an effective biosensor for the evaluation of antioxidant quality in fruit foods in future. Key points
• The stabilized bimetallic nanozyme was constructed for TAC analysis in fruits.
• The hybrid nanozyme possessed the enhanced POD-like activity by cascading effects.
• The nanozyme was an effective biosensor for antioxidant quality evaluation in fruits.
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LWT-FOOD SCIENCE AND TECHNOLOGY
·
2021
·
IF 4.952
Yaru Han,Linpin Luo,Liang Zhang,Yi Kang,Hao Sun,Jie Dan,Jing Sun,Wentao Zhang,Tianli Yue,Jianlong Wang
Nanozymes have become a frontier of research recently and possess broad application prospects in the field of analytical sensing. Herein, a Fe–Mn bimetallic nanozyme (FeMnzyme) was proposed for colorimetric analysis of ascorbic acid (AA). The FeMnzyme, with high specific surface area, consisted of Fe–Mn mixed oxide amorphous core and α-FeOOH nanorod shell characterized by scanning electron microscope (SEM) and Powder X-ray diffraction (XRD). It exhibits typical oxidase-like properties to catalyze oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to generate visible blue oxidized TMB (oxTMB) without exogenous H 2 O 2 . Due to the reducibility of AA to oxTMB, the FeMnzyme/oxTMB system can be employed as a promising colorimetric sensor for quantitative analysis of AA. The method has a good linear concentration range of 8 μmol L −1 to 56 μmol L −1 , and the detection limit is as low as 0.88 μmol L −1 (3σ). Finally, the proposed biosensor has been favorably put into use to determine AA content in kiwi fruit, indicating its reliability for practical application.
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CARBON
·
2021
·
IF 9.594
Yu Ma,Ding Chen,Dongdong Zhang,Hao Yu,Yapeng Zheng,Weijun Li,Lin Wang,Qiao Liu,Weiyou Yang
Freestanding air cathode catalyst with exceptional catalytic bifunctions for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is highly desirable for exploring rechargeable Zn–air batteries (ZABs) with low cost and high reliability. Here, a facile and scalable approach is demonstrated to prepare efficient and robust freestanding cathode catalyst that consists of dispersed Fe 3 C nanoparticles , rich Fe-N x /N-C species and carbon fibers networks with large specific surface area, which is based on one-pot in-situ coupling of Fe and N induced active sites within bacterial cellulose-derived carbon fibers networks. Its bifunctional activity parameter (Δ E ) for ORR and OER is 0.79 V, superior to those of single Fe- or N- modulated counterparts, and comparable to the state-of-the-art Pt/C + RuO 2 catalyst (0.79 V). This material can be directly used as freestanding and binder-free catalyst layer , and as-assembled ZABs exhibit a larger peak power density (173 mW cm −2 ), higher specific capacity (717 mA h g −1 , 10 mA cm −2 ) and better cycle stability (negligible activity decay after 165 h charge/discharge cycles) than those of Pt/C + RuO 2 -based devices, representing their potential applications in advanced energy conversion systems.
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危险品化学品经营许可证（带存储）