APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Wenlan Ji,Xinyu Miao,Tian C. Zhang,Yuan Wang,Shaojun Yuan
The elimination of arsenic pollution has attracted increasing concerns due to its toxicity and severe carcinogenicity. Herein, we proposed an in-situ crystal growth strategy without surfactant to fabricate MIL-88B uniformly anchored on the surface of MnO 2 /GAC (MIL-88B/MnO 2 /GAC). Such innovative MIL-88B/MnO 2 /GAC nanostructured composites not only exhibited the synergetic functions of simultaneously oxidizing As(III) and adsorbing the generated As(V), but also effectively reduced the cost of metal–organic frameworks (MOFs) adsorbents. Impressively, the as-prepared sample achieved remarkably boosted As(III) removal capacity of 15.13 mg g −1 compared to 4.1 mg g −1 of MnO 2 /GAC composite and 2.1 mg g −1 of GAC , which was mainly ascribed to the synergistic effect between the excellent adsorption abilitiy of MIL-88B and oxidation property of MnO 2 /GAC. Owing to the unique construction and properties, the constructed MIL-88B/MnO 2 /GAC composites presented a desirable As(III) removal ability under a wide pH scope of 2 to 10. Moreover, the possible mechanism of the synergistic removal over MIL-88B/MnO 2 /GAC was elucidated by X-ray photoelectron spectroscopy (XPS), electron spin resonance (ESR) and radical trapping experiment. This work not only offers a superior bifunctional catalyst for high-efficient removal of arsenic, but also provides a new perspective for rational construction of MOF derivatives for their further applications.
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Hao Liu,Huan Wang,Lu Zhang,Yanjuan Sang,Fang Pu,Jinsong Ren,Xiaogang Qu
Since excess fluoride ions may lead to a severe health hazard, it is imperative to design a facile and sensitive sensor to detect it in both environmental and biological systems. The reported methods are always subjected to some limits, hampering their practical application. Herein, a two-dimensional turn-on fluorescent sensor, Fe 3+ -integrated oxidized graphitic-phase carbon nitride nanosheets (Fe-g-CNO), was synthesized via a facile and green method for sensitive detection of fluoride ions. The interactions between the C-N/C = N moieties of oxidized graphitic-phase carbon nitride (g-CNO) and Fe 3+ caused fluorescence quenching of g-CNO. Upon addition of F- ions, the fluorescence was recovered through the formation of complex of Fe 3+ and F-. The limit of detection of the sensor was 1 × 10 -6 M. Furthermore, this probe could be used as an imaging agent of fluoride ions in living cells and teeth for diagnosis of dental fluorosis. The work provides a safe and efficient platform for further environmental and biomedical uses.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shuai Yang,Dongqi Tian,Xinhao Wang,Peng Zhou,Zhaokun Xiong,Heng Zhang,Yang Liu,Gang Yao,Bo Lai
Fenton-like technology has been widely used in the field of water treatment as an advanced oxidation processes (AOPs), and a multitude of non-homogeneous catalysts have been reported effectively to enhance it. Herein, nitrogen and sulfur co-doped nanocarbon materials (NSC) was designed and synthesized, which formed a unique mesoporous structure and abundant functional groups on the surface. It exhibits superior catalytic performance to enhance the Fe(III)/H 2 O 2 system for sulfamethoxazole (SMX) degradation, k obs is 18 times higher than Fe(III)/H 2 O 2 system after the introduction of NSC under the same experimental conditions. Also, the working pH of Fe(III)/H 2 O 2 system was broadened by NSC. Quenching and probe experiments demonstrate that hydroxyl radical (∙OH) was the dominant active species. Both dissociative and surface-bound iron species were observed, which indicates direct reduction and in-situ binding of Fe(III), respectively. Further investigation found nitrogen and sulfur co-doped attribute to the formation of abundant functional groups, the C O bond and C S C bond on the surface of NSC result in the directly reduce of Fe(III), while –COOH contributes to the in-situ binding. The intermediates and possible degradation pathway of SMX degradation were proposed based on the results of liquid chromatography-quadrupole time of flight-mass spectrometer (LC-QTOF-MS). The results of cycling and co-existing ions experiments demonstrate that NSC has outstanding potential for application. This work provides a novel insight into the sustained removal of micropollutants from the aqueous environment based on the nanocarbon materials enhancing the Fenton-like oxidation.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Zhaoxu Li,Xinyi Luo,Meifang Luo,Yuan Qin,Chaozhong Guo,Yao Liu,Zhongli Luo
To design inexpensive carbon catalysts and enhance their oxygen reduction reaction (ORR) activity is critical for developing efficient energy-conversion systems. In this work, a novel Fe-N-C hybrid electrocatalyst with carbon nanolayers-encapsulated Fe 3 O 4 nanoparticles is synthesized successfully by utilizing the molecular-level confinement of graphitic C 3 N 4 structures via hemin biomaterial. Benefiting from the Fe-N structure prevalent on the carbon nanosheets and large mesopore-dominated specific surface area, the synthesized catalyst under optimized conditions shows excellent electrocatalytic performance for ORR with an E ORR at 1.08 V versus reversible hydrogen electrode (RHE) and an E 1/2 at 0.87 V vs. RHE, and outstanding long-term stability, which is superior to commercial Pt/C catalysts (E ORR at 1.04 V versus RHE and E 1/2 at 0.84 V versus RHE). Moreover, the low hydrogen peroxide yield (<11%) and average electron transfer number (~3.8) indicate a four-electron ORR pathway. Besides, the maximum power density of the home-made Zn-air battery using the obtained catalyst is 97.6 mW cm −2 . This work provides a practical route for the synthesis of cheap and efficient ORR electrocatalysts in metal-air battery systems.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Tian Meng,Qun Li,Mengxia Yan,Dewen Wang,Libing Fan,Xiaojuan Liu,Zhicai Xing,Xiurong Yang
Self-reconstruction of oxygen evolution reaction (OER) catalyst, especially metal (oxy)hydroxides or oxides, has attracted much attention. Herein, an in-situ self-reconstruction process for Ni, Fe, Zn ternary-metal hydroxides (NFZ-TH) involving significant morphology transformation, and self-modulated electronic structure change of Ni and Fe owing to the etching of Zn species under anodic polarization potential is revealed. NFZ-TH derived materials, undergoing in-situ self-reconstruction (NFZ-TH-SR), exhibits superior OER performance (η = 217 mV @ j = 10 mA cm −2 geometry ) and excellent stability over a period of ~48 h. Nano-pitted surface resulting from etching of Zn species improves the electrochemical surface area. Meanwhile, in NFZ-TH-SR, large amounts of defects induced defect-/corner-sited Fe and adjustability of NiOOH species are verified by Mössbauer spectra and in-situ Raman spectra respectively. Density functional theory calculations give insight that both defect-/corner- sited Fe and Ni at next-nearest-neighbour defect-site have high activity. This paper helps understand that the proposed in-situ self-reconstruction strategy can improve the electrochemical performance of OER catalysts.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Kun Li,Luxin Liang,Peng Du,Zeyun Cai,Tao Xiang,Hiroyasu Kanetaka,Hong Wu,Guoqiang Xie
Magnesium (Mg) alloys can be regarded as the most promising biodegradable implant materials for orthopedic and stent applications due to their good biocompatibility and low Young's modulus which is near to that of natural bone. However, its applicability is hindered because it exhibits a high corrosion rate in the physiological environments. In this work, we fabricated Mg 66 Zn 30 Ca 4 /Fe bulk metallic glass composites via spark plasma sintering (SPS). We studied the influence of different contents of Fe on the properties of the composites. The results indicated that Fe was uniformly distributed on the surface of Mg 66 Zn 30 Ca 4 metallic glass (MG) as a second phase, which led to an improvement in the corrosion resistance and mechanical strength. The standard potential of Mg 66 Zn 30 Ca 4 /Fe bulk metallic glass (BMG) composites increased as compared to Mg 66 Zn 30 Ca 4 , while their mechanical strength improved from 355 MPa to 616 MPa. Furthermore, cytotoxicity was investigated via the CCK-8 assay and calcein-AM staining, which revealed that the extraction mediums diluted 6 times (EM × 6) of the Mg 66 Zn 30 Ca 4 and Mg 66 Zn 30 Ca 4 /Fe did not cause cell toxicity on day 3 and 5, while the EM × 6 of the Mg 66 Zn 30 Ca 4 showed cytotoxicity on day 1, 3 and 5. Thus, Mg 66 Zn 30 Ca 4 /Fe BMG composites exhibit significant potential for fabricating implants with good mechanical strength and corrosion resistance.
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Environmental Science-Nano
·
2020
·Vol. 7
·期 9
·2573-2583
·
IF 7.683
Jie Yang,Jia Li,Dickon H. L. Ng,Ping Yang,Wenning Yang,Yong Liu
Self-propelled micro- and nanomotors are a current research focus and have shown attractive potential in environmental applications. Here, we report a biomass approach to construct a novel tubular micromotor decorated with a nanozyme/natural enzyme hybrid, which integrated the advantages of the self-propelled movement, selectivity of a natural enzyme and catalytic activity of artificial nanozymes. Such a micromotor had a unique hierarchical structure where laccase immobilized-Fe-BTC MOF nanoparticles grew uniformly on Mn2O3–NiFe2O4 nanosheets, which was constructed using natural kapok fiber as a template. This laccase-integrated Fe-BTC/NiFe2O4 micromotor was capable of self-propulsion with a speed of 120 μm s−1 by oxygen bubbles via the decomposition of H2O2 catalyzed by Mn2O3. Owing to the incorporation of autonomous motion with high selectivity of natural laccase and high peroxidase-like activity of the Fe-BTC/NiFe2O4 nanozyme, these micromotors exhibited much higher catalytic activity to methylene blue degradation than their passive counterparts. Besides as a substrate to accommodate laccase immobilized-Fe-BTC, magnetic NiFe2O4 also enabled the remote magnetic control on the movement direction.
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2021
·
IF 10.618
Li-Ping Zong,Ling-Yu Ruan,Junji Li,Robert S. Marks,Jun-Song Wang,Serge Cosnier,Xue-Ji Zhang,Dan Shan
Enzyme mimetics have attracted wide interest due to their inherent enzyme-like activity and unique physicochemical properties , as well as promising applications in disease diagnosis, treatment and monitoring. Inspired by the attributes of nonheme iron enzymes , synthetic models were designed to mimic their capability and investigate the catalytic mechanisms . Herein, metal-organic gels (Fe-MOGs) with horseradish peroxidase (HRP) like Fe-N X structure were successfully synthesized though the coordination between iron and 1,10-phenanthroline-2,9-dicarboxylic acid (PDA) and exhibited excellent peroxidase-like activity. Its structure-activity relationship and the in-situ electrochemiluminescence (ECL) detection of H 2 O 2 secreted by Hela cells were further investigated. The highly dispersed Fe-N X active sites inside Fe-MOGs were able to catalyze the decomposition of H 2 O 2 into large amounts of reactive oxygen species (ROS) via a Fenton-like reaction under a low overpotential. Due to the accumulation of ROS free radicals , the luminol ECL emission was significantly amplified. A proof-of-concept biosensor was constructed with a detection limit as low as 2.2 nM and a wide linear range from 0.01 to 40 μM. As a novel metal organic gels based enzyme mimetic, Fe-MOGs show great promises in early cancer detection and pathological process monitoring.
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Chenhui Hu,Chunhong Liu,Kaimin Du,Chengkai Pang,Zuoxi Zhuo,Qiangsheng Gao
An energy-saving catalyst 4%Fe/Ce-Mn-TiO 2 was prepared via a simple one-step impregnation-annealing process and used as a denitration catalyst at low temperature (≤180 °C) and high water content (∼20%). The results show that 4%Fe/Ce-Mn-TiO 2 catalyst exhibits good low-temperature catalytic activity and water resistance attributed to its highly dispersed metal oxide species, more surface-adsorbed oxygen and high stability of particles. The denitrification efficiencies of 4%Fe/Ce-Mn-TiO 2 catalyst are 90% (5% H 2 O) and 70% (20% H 2 O) at 170 ℃ respectively, which are superior to the commercial vanadium catalyst in service usually needs heating up to 220 ℃.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yan Li,Liangmin Gao,Yu Wang,Shuo Cheng,Guowei Wu,Xuan Yang,Shunli Wan
Biochar-supported metallic oxides are attractive adsorbents for heavy metal cleanup, but the adsorption performance is still unsatisfactory as a result of the self-aggregation of the incorporated metallic oxides. A new hybrid nano-material was prepared through impregnating hydrated ferric oxide (HFO) nanoparticles within biochar bearing high-density charged oxygen-containing groups (e.g., carboxyl and hydroxyl groups) (ABC) derived from HNO 3 treatment. The as-made adsorbent, denoted as HFO-ABC, possesses highly dispersed HFO nanoparticles with typical size lower than 20 nm, and exhibits greater sorption capacity for Cd(II) and Cu(II) than the pristine biochar-supported HFO. It also shows great sorption preference toward Cd(II) and Cu(II) in co-presence of high levels of Ca 2+ , Mg 2+ and humic acid (HA). Such prominent performance is put down to the high-density charged functional groups on the host ABC, which not only promote the dispersion of the immobilized HFO nanoparticles but also generate the potential Donnan membrane effect, i.e., the pre-concentration and permeation of target metals prior to their preferable adsorption by nano-HFO. The predicted effective coefficients of intra-particle diffusion for Cu(II) and Cd(II) are 3.83 × 10 −9 and 4.33 × 10 −9 cm 2 /s, respectively. HFO-ABC exhibits excellent performance for fixed-bed column application, and yields 513 and 990 BV effluents for Cd(II) and Cu(II) to achieve their discharge standards, respectively. The spent HFO-ABC could be in situ regenerated using binary HCl-CaCl 2 solution with desorption efficiency higher than 95%. All results manifest that increasing charged functional groups via HNO 3 treatment is an effective measure for boosting sorption performance of biochar-based nanocomposites.
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DOI
PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2018
·Vol. 44
·期 5
·3455-3474
·
IF 1.674
Sun Xiao,Guo Rui-tang,Li Ming-yuan,Sun Peng,Pan Wei-guo,Liu Shu-ming,Liu Jian,Liu Shuai-wei
Fe was used as the modifier to improve the performance of CeZr 2 O
x
catalyst for the selective catalytic reduction (SCR) reaction with ammonia. Experimental results revealed that proper Fe species (Fe/Ce molar ratio = 2) could effectively improve the SCR activity of CeZr 2 O
x
, along with the elevated resistance to SO 2 and H 2 O. The characterization results including BET, XRD, H 2 -TPR and NH 3 -TPD confirmed that Fe species in Fe 2 CeZr 2 O
x
catalyst could inhibit the formation of ZrO 2 crystals and lead to higher reducibility and surface acidity. In addition, more Ce 3+ and surface active oxygen species could be detected on Fe 2 CeZr 2 O
x
compared with CeZr 2 O
x
. By means of in situ DRIFT technique, it could be deduced that the SCR reaction process over Fe 2 CeZr 2 O
x
was accelerated mainly through theL–H pathway due to the advanced adsorption of NH 3 and NO
x
species, along with the promoted NO conversion to NO 2 . Therefore, the modification of CeZrO
x
catalyst by Fe had a significant stimulation effect on its low-temperature SCR performance.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Yuping Gai,Wei Deng,Junbo Hu,Dan Li,Wenshuo Xie,Xiang Li,Jingjing Zhang,Dewu Long,Fei Jiang
The preparation of stable electrocatalyst for oxygen evolution reaction is of the utmost importance to realize high performance water decomposition reaction . Metal-organic framework (MOF) nanostructures have become promising materials. Herein, we report three kinds of electrocatalysts with different structures and properties for the oxygen evolution reaction, which were constructed by using different binding sites of three kinds of ligands following a mechanism which involved only *O and *OH species as intermediates. CoFeBTC-MOF shows excellent overpotential η = 261 mV at 10 mA cm −2 (1.481 V vs. RHE), Tafel slope of 59.29 mV dec −1 and pretty excellent stability (48 h of continuous testing), making it become one of the best acid-resistant catalysts for oxygen evolution reaction. The DFT calculations show that there are different ways to transfer electrons . In addition, the coupling effect between Co and Fe metals is the key to regulate the electrocatalytic activity , confirming the cooperative catalysis mechanism with a reduced energy barrier.
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