ELECTROCHIMICA ACTA
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2018
·
IF 5.116
Xuedong Wei,Na Li,Xianming Zhang
Two kinds of three-phase composite materials, Co/Co(OH) 2 /C@B directly from ZIF67 modified by NaBH 4 and Co/CoO/C@B through pyrolyzation of Co/Co(OH) 2 /C@B material, are successfully synthesized and used as catalysts for the oxygen evolution reaction (OER). The structure and morphology are mainly characterized by X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), energy dispersive X-ray analysis (EDX), X-ray photoelectron spectroscopy (XPS). HBZ-1 sample with the structure of Co/Co(OH) 2 /C@B has the best onset potential of 1.075 V vs. RHE at 0.1 mA cm −2 and the best catalyst stability among all of the materials researched. Especially as its pyrolyzing product, the CBZ-1 sample with the structure of Co/CoO/C@B behaves the most excellent synthetically electrocatalytic performance with low onset potential of 1.444 V vs. RHE at 0.1 mA cm −2 and a small overpotential of 390 mV at 10 mA cm −2 , which is better than that of RuO 2 . This good catalytic activity is mainly attributed to the generation of CoO phase and synergistic effect of all the phases in the composite structure. Furthermore, the CBZ-1 sample has the appropriate catalytic stability which attributed to the three-phase structure of Co/CoO/C@B composite and the existing of a little B element.
研究领域:
材料科学
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电催化
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纳米材料
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能量转换
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无机化学
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 12
·33587-33597
·
IF 5.19
Zhang Ying,Zhang Shici
A series of porous photocatalysts, Au-carbon-doped ZnO (Au/C/ZnO), were synthesized successfully via calcination using MOF-5 as template, with the matrix impregnated with Au nanorods through the seed-mediated method. The catalytic performance was investigated by the photodegradation of tetracycline hydrochloride (TC-HCl). Ninety percent of TC was degraded by Au/C/ZnO sample within 360 min under visible light, showing an efficient photocatalytic activity. The enhanced activity was mainly ascribed to the effect of oxygen vacancies produced by C doping during calcination process of MOF-5 and Au nanorods. The density functional theory (DFT) calculation shows that due to the intermediate energy level, the electron–hole pairs generated by photoelectricity transition were transitioned from valence band (VB) to the intermediate energy level, and further to the conduction band (CB) under irradiation. Thus, the separation efficiency of photogenerated carrier was improved in this process. Meanwhile, the surface plasmon resonance (SPR) and electromagnetic field effect of Au nanorods which were loaded on the C/ZnO promoted the separation efficiency of change carriers, and this process also provided more hot electrons for free radicals generation. This work provides an efficient method for the design and synthesis of noble metal– and non-metal-doped oxide photocatalysts and provides an effective photocatalytic technique for the antibiotic degradation under visible light, which possesses the huge application potential in the environmental purification.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Youpu Zhao,Qing Sun,Jian Zhang,Jiawei Sheng
In this study, natural porous diatomite was utilized as a conciliatory carrier for the fabrication of Fe/N/C nano-clusters with assistance of binary molten salt of NaCl-ZnCl 2 under different annealing temperature and used to removal of norfloxacin (NFA). The sample Fe/D m900 (prepared at 900 °C) exhibited a high surface area and great catalytic performance for antibiotics in the presence of PMS. Over 97% NFA can be decomposed within 5 min and the final degradation rate reached 98%. Meaningfully, high-efficiency Fe/D m900 -PMS system was nearly impervious to pH values and inorganic cations in aqueous solution and could be a likely candidate for degradation of multiple contaminants in pharmaceutical outlet water. Furthermore, the other impacting variables such as catalyst dosage, PMS dosage, NFA concentration and initial pH were moreover explored towards debasement, and conceivable degradation pathways of NFA were presented through LC-MS. This work builds up a compelling procedure to synthesize super-dispersed Fe clusters, which may be amplified to other transition metal-based catalyst via molten salt.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Rui Jiao,Yanming Wang,Yuxia Pang,Dongjie Yang,Zhixian Li,Hongming Lou,Xueqing Qiu
Metal–organic frameworks (MOFs) have become promising accommodation for enzyme immobilization in recent years. However, the microporous nature of MOFs affects the accessibility of large molecules, resulting in a significant decline in biocatalysis efficiency. Herein, a novel strategy is reported to construct macroporous MOFs by metal competitive coordination and oxidation with induced defect structure using a transition metal (Fe2+) as a functional site. The feasibility of in situ encapsulating β-glucosidase (β-G) within the developed macroporous MOFs endows an enzyme complex (β-G@MOF-Fe) with remarkably enhanced synergistic catalysis ability. The 24 h hydrolysis rate of β-G@MOF-Fe (with respect to cellobiose) is as high as approximately 99.8%, almost 32.2 times that of free β-G (3.1%). Especially, the macromolecular cellulose conversion rate of β-G@MOF-Fe reached 90% at 64 h, while that of β-G@MOFs (most micropores) was only 50%. This improvement resulting from the expansion of pores (significantly increased at 50–100 nm) can provide enough space for the hosted biomacromolecules and accelerate the diffusion rate of reactants. Furthermore, unexpectedly, the constructed β-G@MOF-Fe showed a superior heat resistance of up to 120 °C, attributing to the new strong coordination bond (Fe2+–N) formation through the metal competitive coordination. Therefore, this study offers new insights to solve the problem of the high-temperature macromolecular substrate encountered in the actual reaction.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Na Ye,Pengcheng Zhao,Xiaoying Qi,Riguang Zhang,Binhang Yan,Wenchao Sheng,Zhao Jiang,Tao Fang
Engineering high-performance inexpensive TaN-modified Pd-based nanostructures for alkaline methanol oxidation reaction(MOR) has attracted extensive attention, yet the related enhancement mechanism of TaN for MOR remains lacked. The core-shell like Pd 3 Ni 1 -TaN/C catalyst decorated with Ni(OH) 2 /NiOOH that contains highly dispersed Ni sites and nitrogen defects has been fabricated for the first time. The unsaturated coordination environment and core-shell like morphology of Pd 3 Ni 1 -TaN/C bring fruitful active sites and a down-shifted d -band center, making it a highly-efficient electrocatalyst for alkaline MOR (17.3-fold that of commercial Pd/C). Besides the electronic effects and surface defect sites of Pd 3 Ni 1 -TaN/C, TaN also helps MOR proceed via HCOO ad pathway (non-CO) accompanied by enhanced OH adsorption induced by the addition of Ni. DFT(Density Functional Theory) calculations also further confirm the energy barrier of the formation of HCOO ad intermediate and desorption energy of CO on Pd 3 Ni 1 -TaN/C are reduced. The introduction of Ni species and nitrogen vacancies enhances the CO tolerance evidently.
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MOLECULES
·
2023
·Vol. 28
·期 4
·1529
·
IF 4.6
Zhixiang Wang,Wentao Liu,Guohu Li,Jiacheng Wang,Bin Zhao,Peishan Huang,Wenjie Mei
Herein, two novel ruthenium(II) complexes coupled by erianinviaa flexible carbon chain, [Ru(phen)2(L1-(CH2)4-erianin)](ClO4)2(L1= 2-(2-(tri-fluoromethyphenyl))-imidazo [4,5f][1–10]phenanthroline (1) and [Ru(phen)2(L2-(CH2)4-eria)](ClO4)2(L2= 2-(4-(tri-fluoromethyphenyl))-imidazo [4,5f][1,10]phenanthroline (2), have been synthesized and investigated as a potential G-quadruplex(G4) DNA stabilizer. Both complexes, especially 2, can bind toc-mycG4 DNA with high affinity by electronic spectra, and the binding constant calculated for 1 and 2 is about 15.1 and 2.05 × 107M−1, respectively. This was further confirmed by the increase in fluorescence intensity for both complexes. Moreover, the positive band at 265 nm in the CD spectra ofc-mycG4 DNA decreased treated with 2, indicating that 2 may bind toc-mycG4 DNA through extern groove binding mode. Furthermore, fluorescence resonance energy transfer (FRET) assay indicated that the melting point ofc-mycG4 DNA treated with 1 and 2 increased 15.5 and 16.5 °C, respectively. Finally, molecular docking showed that 1 can bind toc-mycG4 DNA in the extern groove formed by base pairs G7–G9 and G22–A24, and 2 inserts into the small groove ofc-mycG4 DNA formed by base pairs T19–A24. In summary, these ruthenium(II) complexes, especially 2, can be developed as potentialc-mycG4 DNA stabilizers and will be exploited as potential anticancer agents in the future.Keywords:ruthenium(II) complexes;erianin;c-mycG-quadruplex DNA;stabilizer
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Jiajin Zhong,Na Li,Xiaoxuan Xu,Limin Wei,Huijian Liu,Huijuan Li,Zheng Fang,Haifeng Bao
High temperature thermally stable fiber materials with flexibility are expected to be applicable to severe conditions. In this article, ZrO 2 /Si–C–O ceramic fibers have been synthesized by the sol-gel process combined with the electrospinning technique. We focus on the changes of composition, structure and morphology with the increasing heat treatment temperature. More importantly, the effects of ZrO 2 crystalline phase transformation on mechanical property of ZrO 2 /Si–C–O ceramic fibers have been investigated. The results show that the increased temperature can lead to an increase of the fiber diameter and grain size, as well as the transformation of ZrO 2 phase. It is also found that the ZrO 2 /Si–C–O ceramic fibers possess refined crystalline grain and improved mechanical properties at a heat treatment temperature of 800 °C, which is mainly due to the fact that the amorphous Si–C–O phase containing free carbon facilitates the refinement of the crystalline grain, and the ZrO 2 in the tetragonal structure improves the flexibility of ceramic fibers. Furthermore, the obtained fibers exhibit excellent thermal stability up to 1300 °C, therefore they have broad application prospect in high temperature environment.
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PLANTA MEDICA
·
2022
·Vol. 88
·期 13
·1233-1244
·
IF 3.007
Shipeng Chen,Yinan Liao,Jinyan Lv,Huaxin Hou,Jie Feng
The aim of the present study was to investigate the cytotoxic effects and underlying molecular mechanisms of nitidine chloride (NC) in hepatocellular carcinoma cells via quantitative proteomics. MTT assays were used to detect the inhibitory effects of NC in Bel-7402 liver cancer cells, and the number of apoptotic cells was measured by flow cytometry. Quantitative proteomics technology based on iTRAQ was used to discover differential expressed proteins after NC treatment, and bioinformatic techniques were further used to screen potential targets of NC. Molecular docking was applied to evaluate the docking activity of NC with possible upstream proteins, and their expression was detected at the mRNA and protein levels by quantitative reverse transcription PCR and western blotting. NC inhibited the proliferation of Bel-7402 cells after 24 h of treatment and stimulated apoptosis in vitro. The proteomics experiment showed that NC triggers mitochondrial damage in HCC cells and transcription factor AP-1 (c-Jun) may be a potential target of NC (fold change = 4.36 ± 0.23). Molecular docking results revealed the highest docking score of NC with c-Jun N-terminal kinase (JNK), one of the upstream proteins of c-Jun. Moreover, the mRNA and protein expression of c-Jun and JNK were significantly increased after NC treatment (p
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PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Jia-Pei Guo,Fang-Jing Liu,Lei-Lei Bie,Xing-Gang Si,Yan-Hong Li,Ping Song,Nian Liu,Yun-Peng Zhao,Zai-Xing Huang,Jing-Pei Cao,Xian-Yong Wei
The utilization of lignin to produce high value-added chemicals is conducive to alleviating the fossil energy crisis. Herein, Ni nanoparticles supported on iron/nitrogen co-doped carbon was prepared by co-pyrolysis and solvothermal reduction method for catalytic hydrogenolysis (CH) of dealkaline lignin and its model compounds. The catalysts were prepared under different calcination temperature, N/C ratio and Ni loading, and the optimal catalyst was Ni 10% @Fe/NC 0.33 – 800 (calcination temperature: 800 °C, N/C ratio: 0.33, Ni loading: 10%) based the on the CH of benzyl phenyl ether (BPE). Ni 10% @Fe/NC 0.33 – 800 showed good catalytic performance on the selective cleavage of C-O bond of lignin and its model compounds. The BPE conversion reached up to 97.7% over Ni 10% @Fe/NC 0.33 – 800 under mild conditions (230 °C, 1 MPa H 2 , and 0.5 h) with toluene and cyclohexanol as major products. Catalyst characterizations suggest that N content affects the formation of NiFe alloy and the synergistic effect between Ni and Fe plays an important role in CH of BPE. Moreover, Ni 10% @Fe/NC 0.33 – 800 could promote the cleavage of C-O bonds in dealkaline lignin through CH and hence enhance producing aromatics such as phenols, aromatic ethers, and aromatic esters, among which phenols are the main aromatics with guaiacols predominant.
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Fundamental Research
·
2022
·
IF 0
Feng Ma,Xuan Liu,Xiaoming Wang,Jiashun Liang,Jianyu Huang,Cameron Priest,Jinjia Liu,Shuhong Jiao,Tanyuan Wang,Gang Wu,Yunhui Huang,Qing Li
Transition metal supported N-doped carbon (M-N-C) catalysts for oxygen reduction reaction (ORR) are viewed as the promising candidate to replace Pt-group metal (PGM) for proton exchange membrane fuel cells (PEMFCs). However, the stability of M-N-C is extremely challenging due to the demetalation, H 2 O 2 attack, etc. in the strongly oxidative conditions of PEMFCs. In this study, we demonstrate the universal effect of Zn on promoting the stability of atomically dispersed M-N x /C (M = Co, Fe, Mn) catalysts and the enhancement mechanism is unveiled for the first time. The best-performing dual-metal-site Zn-Co-N-C catalyst exhibits a high half-wave potential ( E 1/2 ) value of 0.81 V vs. reversible hydrogen electrode (RHE) in acid and outstanding durability with no activity decay after 15,000 accelerated degradation test (ADT) cycles at 60 °C, surpassing most reported Co-based PGM-free catalysts in acid media. For comparison, the Co-N-C in the absence of Zn suffers from a rapid degradation after ADT due to the demetalation and higher H 2 O 2 yield. X-ray adsorption spectroscopy (XAS) and density functional theory (DFT) calculations suggest the more negative formation energy (by 1.2 eV) and increased charge transfer of Zn-Co dual-site structure compared to Co-N-C could strength the Co-N bonds against the demetalation and the optimized d-band center accounts for the improved ORR kinetics.
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Yuting Yang,Yi Huang,Shuqing Zhou,Yi Liu,Luyan Shi,Tayirjan Taylor Isimjan,Xiulin Yang
Surface vacancy defects, as the bridge between theoretical structural study and the design of heterogenous catalysts, have captured much attention. This work develops a metal-organic framework-engaged replacement-pyrolysis approach to obtain highly dispersed Ru nanoparticles immobilized on the vacancy-rich Ni-NiO@C hollow microsphere (Ru/Ni-NiO@C). Fine annealing at 400 °C introduces nickel and oxygen vacancies on Ru/Ni-NiO@C surface, resulting in an improved electrical conductivity and rapid mass-charge transfer efficiency. Ru/Ni-NiO@C with a hollow micro/nanostructure and interconnected meso-porosity favors the maximal exposure of abundant active sites and elevation of hydrogen oxidation reaction (HOR) activity. Experimental results and density functional theory (DFT) calculations reveal that an electronic effect between Ru and Ni-NiO@C, in conjunction with nickel/oxygen vacancies in the NiO species could synergistically optimize hydrogen binding energy (HBE) and hydroxide binding energy (OHBE). The HBE and OHBE optimizations thus created confer Ru/Ni-NiO@C with a mass activity over 7.75 times higher than commercial Pt/C. Our work may provide a constructive route to make a breakthrough in elevating the hydrogen electrocatalytic performance.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Guojun Weng,Xun Shen,Jianjun Li,Jingyuan Wang,Jian Zhu,Junwu Zhao
The etching of gold nanorods/nanobipyramid, or silver-coated nanorods/nanobipyramid inducing plasmon changes represents an efficient strategy to improve the performance of enzyme-linked immunosorbent assay (ELISA). However, the effect of shape on the sensitivity was negligible, especially the thickness of coated silver shell. Here, we propose a plasmonic ELISA for multi-colorimetric detection of CRP based on the etching of Ag-coated Au nanobipyramid (Au [email protected] ). The effect of silver shell thickness on the sensitivity of plasmon peak shifting was investigated by experiments and DDA calculations. The relationship between the Ag shell thickness and the sensitivity of plasmon peak shifting was obtained. Our results reveal that the thickness of coated Ag shell acts as a key factor in the multi-color change of Au [email protected] etching. It is found that Au [email protected] with medium Ag shell thickness and rod-like shape has the higher sensitivity and is suitable for sensing. At the optimized most sensitive Ag shell, the detection limit of proposed plasmonic ELISA for CRP was determined to be 0.09 ng/mL with a spectrometer in the range from 0.09 ng/mL to 25 ng/mL. Importantly, the visual detection limit was 0.78 ng/mL, which allows the differential diagnosis with the naked eye. Compared with traditional ELISA with the monochromatic intensity variations, the multi-color ELISA proposed in this study has a large linear range and rich color variation for high-sensitivity and naked-eye semi-quantitative detection.
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