Nano Energy
·
2021
·
IF 17.881
He Zhang,Liang Huang,Jinxing Chen,Ling Liu,Xinyang Zhu,Weiwei Wu,Shaojun Dong
Designing an artificial enzyme, from the perspective of bionics, to mimic the catalytic activity of natural enzymes is highly desirable but remains challenges. In response to the simulation of biological structure, we developed cytochrome c oxidase (CcO)-like single-atom nanozymes with FeN 5 active centers (FeN 5 SAs) in this work. Similar to the spatial structure of heme a 3 in natural CcO, the active center of FeN 5 SAs is axial N-coordinated heme-like structure and can be served as oxygen-binding site to complete oxygen reduction reaction (ORR) in respiratory electron transport chain by catalyzing the oxidation of cytochrome c (Cyt c). Depending on this bionic structure, furthermore, FeN 5 SAs exhibited competitive electrocatalytic performance towards ORR with a half-wave potential of 0.67 V (vs. RHE) at neutral condition. Coupling a glucose dehydrogenase (GDH) bioanode , the FeN 5 SAs-based glucose/O 2 enzymatic biofuel cell (EBFC) obtained a maximum power density of 149.2 ± 4.0 μW cm −2 with an open circuit potential of 0.40 ± 0.01 V. In this study, inspired by the native structure of enzymes, we develop CcO-like FeN 5 SAs and expand its application in EBFCs, which may provide an rational research approach to advance the development of nanozymes.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 48
·21183-21191
·
IF 3.288
Pengyao Yu,Sheng Liu,Yuchen Cui,Kun Sun,Ling Zhang,Hailing Guo,Yongming Chai,Chenguang Liu,Lili Fan,Ge Yang,Chunzheng Wang,Svetlana Mintova
A uniform bimetallic hollow ZnFe–N/C (80–180 nm) electrocatalyst is synthesized using a precursor ZnFe-ZIF-8 (100–200 nm) subjected to pyrolysis in an argon atmosphere at 800 °C for 2 hours. The ZnFe–N/C catalyst was deposited on a glassy carbon electrode (GCE), and exhibited a superior electrocatalytic activity with a high onset potential (0.97 V vs. RHE) and half-wave potential (0.85 V vs. RHE), high stability in an alkaline electrolyte, and remarkable resistance to methanol. The high performance of the ZnFe–N/C-3 electrocatalyst is attributed to the hollow structure containing metallic Fe/Fe3C and N doping.
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MATERIALS CHEMISTRY AND PHYSICS
·
2021
·
IF 4.094
Yixin Li,Li Liu,Xiaoyang Liu,Yi Feng,Beichen Xue,Liyun Yu,Lijie Ma,Yanchao Zhu,Yimin Chao,Xiaofeng Wang
The comprehensive utilization of Si-rich biomass is restrained by macromolecular lignin and a large amount of ash. In this study, rice husks (RHs) are treated as a representative by alkali extraction and acid precipitation, and the obtained lignin-SiO 2 composite is modified by carbonazation, ball milling, magnesiothermic reduction and additives. Through these processes, a Si/C composite with excellent electrochemical properties is obtained and performs stable cycling performance with high specific capacity retention of 572 mA h g −1 at 1 A g −1 after 1000 cycles. This introduced method provides a potential for utilizing Si-rich biomass comprehensively and preparing desirable Si/C anode materials from Si-rich biomass derived lignin-SiO 2 composites.
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RSC Advances
·
2020
·Vol. 11
·期 1
·501-509
·
IF 3.119
Shan Huang,Ming Lu,Lei Wang
Based on cytochrome c-multiwalled carbon nanotubes (Cyt c-MWCNTs) and cobalt metal–organic frameworks/gold nanoparticles (Co-MOFs/AuNPs), an electrochemical biosensor was proposed for the detection of nitrite. Herein, Co-MOFs and AuNPs were immobilized on gold electrodes via surface layer assembly. Their advantages including large surface area and high conductivity provided an excellent platform for the immobilization of Cyt c-MWCNTs. Cyt c-MWCNTs were prepared via electrostatic adsorption and possessed good biocompatibility and superior electrocatalytic activity towards nitrite. Notably, MWCNTs and AuNPs could provide a good microenvironment for the electron transfer of Cyt c, which further significantly promoted the dispersion of MWCNTs. All of the above features led to outstanding electrochemical performance and achieved signal amplification for nitrite detection. Therefore, the biosensor displayed a linear range from 0.005 μmol L−1 to 1000 μmol L−1 with a detection limit of 0.0044 μmol L−1 for nitrite detection. In addition, the designed biosensor exhibited excellent selectivity and could be applied in real samples.
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Nanoscale Research Letters
·
2020
·Vol. 15
·期 1
·1-14
·
IF 3.578
Guo Chaozhong,Li Yanrong,Li Zhaoxu,Liu Yao,Si Yujun,Luo Zhongli
Designing appropriate methods to effectively enhance nitrogen-doping efficiency and active-site density is essential to boost the oxygen reduction reaction (ORR) activity of non-platinum Fe/N/C-type electrocatalysts. Here, we propose a facile and effective strategy to design a mesopore-structured Fe/N/C catalyst for the ORR with ultrahigh BET surface area and outstanding conductivity via nanochannels of molecular sieve-confined pyrolysis of Fe 2+ ions coordinated with 2,4,6-tri(2-pyridyl)-1,3,5-triazine complexes as a novel precursor with the stable coordination effect. Combining the nanochannel-confined effect with the stable coordination effect can synergistically improve the thermal stability and stabilize the nitrogen-enriched active sites, and help to control the loss of active N atoms during pyrolysis process and to further obtain a high active-site density for enhancing the ORR activity. The as-prepared Fe/N/C electrocatalyst has exhibited excellent catalytic activity with an onset potential of ~ 0.841 V (versus RHE) closely approaching the Pt/C catalyst and high long-term stability in alkaline electrolyte. Besides, low-hydrogen peroxide yield (< 6.5%) and high electron transfer number (3.88–3.94) can be found on this catalyst, indicating that it is a valuable substitute for traditional Pt/C catalysts. This work paves a new way to design high-performance Fe/N/C electrocatalysts and deepens the understanding of active site and ORR catalysis mechanism.
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CARBON
·
2020
·
IF 8.821
Minglong Yang,Ye Yuan,Ying Li,Xianxian Sun,Shasha Wang,Lei Liang,Yuanhao Ning,Jianjun Li,Weilong Yin,Renchao Che,Yibin Li
Lightweight, low-cost electromagnetic (EM) wave absorption materials are in urgent need, as EM interference pollution is increasingly serious. Carbon material as EM absorber has attracted ever increasing attention. However, their absorption property is still limited. Herein, we propose a very simple strategy to prepare hierarchical carbon fiber coated with Co/C nano-dodecahedron particles where CNTs were anchored (HCF@CZ-CNTs), using cotton and metal-organic-framework (MOF) as raw materials. One of MOF, ZIF-67 particles were in-situ grown onto the surface of cotton fibers . Lightweight HCF@CZ-CNTs samples were obtained by direct carbonization , the apparent density of which is only 0.0198 g/cm 3 . The minimum reflection loss (RL min ) of hierarchical HCF@CZ-CNTs was dramatically enhanced to −53.5 dB at 7.8 GHz, compared with pure carbonized cotton fiber (RL min = −18.9 dB at 16 GHz). Meanwhile the effectively absorption bandwidth was also remarkably enlarged to 8.02 GHz. The excellent EM wave absorption performance is attributed to the micro-to-nano hierarchical hollow fibrous structure , as well as the synergetic effect of polarization relaxation and magnetic loss. These results illuminate a low-cost and sustainable strategy to prepare ultra-lightweight microwave absorbers with excellent EM wave absorbing ability utilizing biomass precursor and MOF.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Qi Yang,Dan Chen,Libing Chu,Jianlong Wang
In present work, we studied a novel Fe/C nanomaterial fabricated using Fe-based metal organic frameworks (MOFs) as precursors through thermal pyrolysis to catalyze gamma irradiation-induced degradation of antibiotics, cephalosporin C (CEP-C) and sulfamethazine (SMT) in aqueous solution. The MOFs-derived Fe/C nanomaterials (DMOFs) had the regular octahedrons structure of MOFs and contained element C, Fe and O, while Fe° with a fraction of Fe 3 O 4 and Fe 2 O 3 were identified. Results showed that DMOFs addition could accelerate the generation of OH during gamma irradiation, while the intermediates of bonds cleavages of antibiotic molecules and OH addition were identified. DMOFs were more effective to improve the decomposition of antibiotic having the higher adsorption capacity like SMT. The degradation rate of CEP-C and SMT increased by 1.3 times and 1.8 times, and TOC reduction at 1.0 kGy reached 42 % and 51 %, respectively by gamma/DMOFs treatment, while only 20.2 % (CEP-C) and 4.5 % (SMT) of TOC reduction were obtained by γ-irradiation alone. The crystal structure, functional groups and magnetism of DMOFs changed slightly after gamma irradiation, which made it possible to be reused. DMOFs were promising to enhance the degradation of antibiotics during gamma irradiation.
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ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Shukun Le,Weishan Yang,Gonglai Chen,Aoyu Yan,Xiaojing Wang
The carbon dots (C-dots) mediated Sn 2 Ta 2 O 7 /SnO 2 heterostructures with spongy structure were successfully assembled by simple hydrothermal route. The photocatalytic removal efficiency of amoxicillin (AMX, 20 mg L −1 ) over C-dots/Sn 2 Ta 2 O 7 /SnO 2 was estimated to reach up 88.3% within 120 min simulated solar light irradiating. Meanwhile, the HPLC-MS/MS analysis and density functional theory (DFT) computation were examined to clarify the photo-degradation pathway of AMX. The mechanism investigation proposed that with the modification of C-dots, the photocatalysts improves the utilization of solar energy by harvesting the long wavelength solar light due to their unique up-converted photoluminescence (UCPL). In addition, the porous spongy structure and plenty of tiny C-dots promote the ability of adsorption by enlarged specific surface area. Furthermore, the C-dots mediated Z-type heterojunction of Sn 2 Ta 2 O 7 /SnO 2 facilitates the efficient separation and transfer of photo-induced carriers. Our work affords a promising approach for the design of the high-efficient photocatalysts to remedy poisonous antibiotics in aqueous environment.
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CERAMICS INTERNATIONAL
·
2020
·
IF 3.83
Qian Dai,Bingnan Yuan,Minghui Guo,Kun Zhang,Xueqi Chen,Zihui Song,Tat Thang Nguyen,Xiaojing Wang,Shudong Lin,Jincheng Fan,Yingchun Li,Hu Liu,Zhanhu Guo
To improve the photocatalytic efficiency of niobium pentoxide (Nb 2 O 5 ) for the degradation of organic pollutants, a novel nano-fibriform C-modified Nb 2 O 5 (F–C/Nb 2 O 5 ) photocatalyst was successfully synthesized by niobium oxalate as precursor and nanofibrillated cellulose (NFC) as template and carbon source. Vacuum induced self-assembly method was used to form the nano-fibriform morphology. Compared to ordinary C/Nb 2 O 5 and commercial Nb 2 O 5 , F–C/Nb 2 O 5 exhibited a typical three-dimensional nanorod structure with plenty of pores. The specific surface area of F–C/Nb 2 O 5 was 3 times that of C/Nb 2 O 5 . The prepared F–C/Nb 2 O 5 exhibited a 3.01 eV bandgap and was able to be activated under visible light while that was unable for commercial Nb 2 O 5 with 3.19 eV bandgap. The F–C/Nb 2 O 5 showed the best photocatalytic efficiency in pH value ≤ 3. After cycling for 5 times, the photocatalytic efficiency of F–C/Nb 2 O 5 was still 2.4 times of the ordinary C/Nb 2 O 5 under visible light. Meanwhile, the self-assembly mechanism and photodegradation mechanism were proposed. This study provides a new strategy to form a special nano-fibriform C-modified niobium pentoxide with extremely high photocatalytic efficiency in aqueous solutions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Runping Wu,Qing Ye,Kai Wu,Shuiyuan Cheng,Tianfang Kang,Hongxing Dai
The alkali metal (M = Na, K, Rb, and Cs)-modified C-FDU-15 (M-C-FDU-15( x ); x was the M/C-FDU-15 M ratio, and equal to 0.01–0.03) samples were prepared through an in situ process, and characterized by means of the TG, XRD, TEM, EDS, N 2 adsorption–desorption, O 2 -TPD, and CO 2 -TPD techniques. The (NO + O 2 ) adsorption mechanism was investigated using the (NO + O 2 )-TPD and DRIFTS techniques. The results show that the sequence of (NO + O 2 ) adsorption performance was Na-C-FDU-15(0.01) (104.1 mg/g) > K-C-FDU-15(0.01) (92.4 mg/g) > C-FDU-15 (76.2 mg/g) > Rb-C-FDU-15(0.01) (65.1 mg/g) > Cs-C-FDU-15(0.01) (62.3 mg/g). The alkali metal was uniformly distributed in C-FDU-15 and its doping enhanced the amount of the basic sites in the sample. Moreover, the optimal Na/C-FDU-15 M ratio was 0.02. (NO + O 2 ) were chemically adsorbed mainly in the forms of nitrite (NO 2 − ) and nitrate (NO 3 − ) on M-C-FDU-15( x ). A more amount of NO was converted to nitrate than to nitrite. There were three key factors of enhancing the (NO + O 2 ) adsorption capacity of C-FDU-15 due to alkali metal doping: the first factor was the increasing of surface area and pore volume of the sample, the second one was the enhancement in amount of the active sites in the sample, and the third one was the smaller alkali metal ionic radius in the sample.
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CELLULOSE
·
2020
·Vol. 27
·期 11
·6677-6689
·
IF 4.21
Ren Yuanlin,Liu Yansong,Wang Yang,Guo Xun,Liu Xiaohui
Abstract Lyocell fibers, one of the green and regenerated cellulose fibers, are widely used in the textile fields. However, lyocell fibers are highly flammable which will cause fire accidents. Herein, a novel biomass-based flame retardant derived from vitamin C (VCFR) was designed and synthesized. Then, the lyocell fabrics were finished with VCFR through esterification to fabricate durable flame retardant lyocell fabrics (RF-lyocell). The structure of the different fabrics was characterized by X-ray photoelectron spectroscopy and Fourier transform infrared analysis analysis. The limiting oxygen index value of the FR-lyocell was as high as 39.8%, which still remained 26.4% after 30 washing cycles, indicating excellent flame retardancy and durability. Thermogravimetric-Fourier transform infrared analysis proved that non-combustion compounds, such as CO 2 and water were generated, and provided an obvious flame retardant effect in the gas phase. Cone calorimeter tests showed that the peak of heat release rate and total heat release had a reduction of 89.5% and 54.5%, respectively. These results suggested that VCFR can be used as an effective biomass-based flame retardant for lyocell fabrics. Graphic abstract
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CHEMISTRY & BIODIVERSITY
·
2020
·Vol. 17
·期 7
·e2000241
·
IF 2.039
Nan Wang,Yuan Dong,Yu Yang,Rui Xu,Chang-Wei Li,Cheng-Bin Cui
Penicimutanin C, a new alkaloidal compound, was isolated from the neomycin-resistant mutant strain 3-f-31 of the marine-derived fungus, Penicillium purpurogenum G59, together with four known compounds. The structure of penicimutanin C, including the absolute configuration, was determined by spectroscopic and chemical methods. The absolute configuration of penicimutanin A was also re-confirmed by Marfey's and chiral HPLC analyses of the hydrolyzed products. Penicimutanins C and A inhibited the proliferation of five human cancer cell lines to some extent. Penicimutanin C is the third dimer of diketopiperazine and penicimutanolone, which are only produced by mutants of P. purpurogenum G59 isolated to date, and it showed cytotoxic activity against human cancer cell lines. The neomycin-resistant screening strategy has been previously successfully used to discover new compounds by activating silent metabolites in fungi, and the present results provide an additional example of the effectiveness of this method. Graphical
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