LUMINESCENCE
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2021
·Vol. 36
·期 8
·1901-1909
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IF 2.464
Yan-hong Liu,Xiao-guang Ma,Li-ye Zhu,Meng Li,Xiao-xia Ren,Man Zhang
The SiO 2 @SiO 2 :Tb(1,2-BDC) 3 phen microspheres with monodispersed core-shell structure, are kind of fluorescent particles, which are prepared by a seeded growth method under the catalysis of glacial acetic acid (1,2-BDC, 1,2-benzenedicarboxylic acid; phen, 1,10-phenanthroline). Firstly, silica seed was fabricated by the hydrolysis of ethyl orthosilicate, and the Tb(1,2-BDC) 3 phen was prepared by using 1,2-BDC and phen. Then, a thin mesoporous silica shell doped with Tb(1,2-BDC) 3 phen was grown on the prepared monodisperse silica colloids. The prepared phosphor was analyzed by Fourier-transform infrared spectroscopy, X-ray diffraction analysis, scanning electron microscopy, transmission electron microscopy, thermogravimetric and fluorescence spectroscopy. The experimental results showed that the diameter of the SiO 2 @SiO 2 :Tb((1,2-BDC) 3 phen microsphere was about 200 nm with a typical core-shell structure, among which the diameter of the silica core was 180 nm, and that of the mesoporous silicon shell doped with terbium complex was about 10 nm. The fluorescence intensity of SiO 2 @SiO 2 :Tb((1,2-BDC) 3 phen microsphere is nearly three times higher than that of Tb((1,2-BDC) 3 phen complexes. The prepared microspheres could be widely used in bio-imaging, optoelectronic appliances and medical diagnosis.
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ENVIRONMENTAL TECHNOLOGY
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2021
·
IF 3.247
Binchao Lu,Liang Wang,Xin Zheng,Zhongce Hu,Zhiyan Pan
Environmental contamination by 4-chlorophenol (4-CP) is a major concern. Photosynthetic bacteria have the ability to biodegrade 4-CP under dark aerobic conditions. In this study, we found that using different carbon sources (i.e. glucose, sodium acetate, sodium propionate sucrose, and malic acid) as co-metabolic substrates accelerated the biodegradation of 4-CP, and this acceleration was especially pronounced in the glucose treatment. A maximum degradation rate of 96.99% was reached under a concentration of 3.0 g·L−1 after 6 days of culture. The optimum conditions were pH 7.5, a temperature of 30°C, and a rotation speed of 135 rpm. The biodegradation of 4-CP was achieved at a range of salinities (0–3.0% NaCl, w/v). The biodegradation kinetics agreed with the Haldane model, and the kinetic constants were rmax = 0.14 d−1, Km = 33.9 mg·L−1, and Ki = 159.6 mg·L−1. Additionally, the coexistence of phenol or 2,4-dichlorophenol (2, 4-DCP) had a certain impact on the degradation of 4-CP under dark aerobic conditions. When the coexisting phenol concentration reached 100 mg·L−1, the maximum degradation rate of 4-CP reached 90.20%. The degradation rate of 4-CP decreased as the concentration of coexisting 2, 4-DCP increased.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Xingyu Fang,Lu Gan,Linjie Wang,Han Gong,Lijie Xu,Ying Wu,Haiqin Lu,Shuguang Han,Juqing Cui,Changlei Xia
In this study, mixed metal cobalt zinc oxide embedded nitrogen enriched porous carbon composites (CoZnO-PC) were prepared via pyrolyzing polyvinylpyrrolidone (PVP) encapsulated Co, Zn-bimetal centered zeolitic imidazolate frameworks (ZIF). The prepared composites were then used to activate peroxymonosulfate (PMS) for bisphenol A (BPA) removal in water. When mole ratio of Co/Zn was 2/1, the resulted Co 2 Zn 1 O-PC possessed spinel structure with prominent degradation capability, in which the introduction of Zn accelerated the PMS activation performance of Co through establishing bimetal synergistic interactions. Both radical and non-radical activation pathways were existed in the Co 2 Zn 1 O-PC/PMS system, in which Co 2 Zn 1 O dominated the radical pathway whereas PC dominated the non-radical way. Since PVP contained abundant nitrogen atoms and could form strong coordination interactions with the ZIF precursor, the introduction of PVP in the ZIF precursor prevented pore collapsing during pyrolysis process , as well as enhancing the nitrogen content in the pyrolzed composites, which significantly promoted the generation of singlet oxygen. With combined pathways, the Co 2 Zn 1 O-PC/PMS system showed a wide pH application range with promising mineralization rate. Meanwhile, the spinel-structured Co 2 Zn 1 O-PC was magnetically separable with desirable recyclability . This study presents a novel composite with remarkable performance for the removal of refractory organic pollutants in municipal wastewater .
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ANALYST
·
2021
·Vol. 146
·期 14
·4566-4575
·
IF 4.616
Feng Li,Qi-Le Li,Lei Hu,Hong-Yu Zhu,Wen-Juan Wang,Fen-Ying Kong,Heng-Ye Li,Zhong-Xia Wang,Wei Wang
p-Nitrophenol and its derivatives can cause serious harm to the health of mankind and the earth's ecosystem. Therefore, it is necessary to develop a novel and rapid detection technology for p-nitrophenol and its derivative. Herein, excellent water-soluble, large-size and dual-emissive neuron cell-analogous carbon-based probes (NCNPs) have been prepared via a solvothermal approach, using o-phenylenediamine as the only precursor, which exhibit two distinctive fluorescence (FL) peaks at 420 and 555 nm under 345 nm excitation. The NCNPs show a neuron cell-like branched structure, are cross-connected, and are in the range of 10–20 nm in skeleton diameter. Interestingly, their blue-green dual-colour fluorescence is quenched by p-nitrophenol or its derivative due to the specific mechanism of the π⋯π stacking interactions or internal filtration effect. Accordingly, a simple, rapid, direct and free-label ratiometric FL detection of p-nitrophenol is proposed. An excellent linear relationship shows linear regions over the range of 0.1–50 μM between the ratio of the FL intensity (FL555 nm/FL420 nm) and the concentrations of p-nitrophenol. The detection limit is as low as 43 nM (3σ). Importantly, the NCNP-based probe also shows acceptable repeatability and reproducibility for the detection of p-nitrophenol and its derivatives, and the recovery results for p-nitrophenol in real wastewater samples are favourable.
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ANALYST
·
2021
·Vol. 146
·期 13
·4280-4289
·
IF 4.616
Jinyan Du,Shuangqing Qi,Tingting Fan,Ying Yang,Chaofeng Wang,Qin Shu,Shujuan Zhuo,Changqing Zhu
Herein, a simple and facile one-step hydrothermal carbonization synthesis procedure for the fabrication of N, Cu-doped carbon quantum dots (N, Cu-CQDs) as a peroxidase-mimicking enzyme was reported. The peroxidase-like performance of N, Cu-CQDs was assessed based on the oxidative coupling reaction of phenol with 4-aminoantipyrine (4-AAP) in the presence of hydrogen peroxide (H2O2). The N, Cu-CQDs/4-AAP/H2O2 system was applied to sensing phenol based on double signals of absorption spectra (or colorimetric visualization) as well as fluorescence spectra. The obtained limits of detection (LODs) were as low as 0.12 μM and 0.02 μM, respectively. Moreover, the proposed method was successfully applied to the determination of phenol in sewage with satisfactory recovery. Our results demonstrate that the N, Cu-CQDs/4-AAP/H2O2/phenol sensing system has a great potential prospect for applications in environmental chemistry and biotechnology.
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BIOMATERIALS
·
2021
·
IF 12.479
Kuo Zhang,Hui Zhang,Xiao-Ran Zou,Ying Hu,Da-Yong Hou,Jia-Qi Fan,Chao Yang,Zi-Ming Chen,Shi-Fang Wen,Hui Cao,Pei-Pei Yang,Lei Wang
Different from chemical (small molecular inhibitor) and biological (monoclonal antibody) drugs, herein, based on angiogenesis-related neuropilin-1 (NRP-1), we develop a biomimetic superstructure drug, i.e. an antibody-like peptidic network (ALPN) to achieve the high-efficient treatment of choroidal neovascularization (CNV). The ALPN in nanoparticulated formulation (ALPN-NP S ) can bind NRP-1 through targeting unit and form fibrous peptidic networks trapping NRP-1 on the surface of endothelial cells (ECs), leading to anti-angiogenesis. The ALPN shows high-efficacy against angiogenesis in CNV rat model ascribed to the superstructure-enhanced binding and blockage of NRP-1. The very low dose of ALPN (0.263 μg/Kg) exhibits similar anti-angiogenesis effect comparing with monoclonal antibody bevacizumab (23.5 μg/Kg), which shows potential advantages over traditional monoclonal antibodies.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yihao Li,Lu Jiang,Rui Wang,Pingxiao Wu,Juan Liu,Shanshan Yang,Jiahao Liang,Guining Lu,Nengwu Zhu
In this paper, Phenol , 4-Chlorophenol (4-CP), 2,4-Dichlorophenol (2,4-DCP) and 2,4,6-Trichlorophenol (2,4,6-TCP) were selected as model pollutants to explore the oxidant mechanism by ferrate (Fe(VI)). The reactions between ferrate (1000 μM) and four phenolic compounds (100 μM) were conformed to the second-order reaction kinetics at pH 9.2, and the order of k obs followed as: k 4-CP (129 M −1 s −1 ) > k 2,4-DCP (96 M −1 s −1 ) > k 2,4,6-TCP (44 M −1 s −1 ) > k Phenol (12 M −1 s −1 ). Meanwhile, the degradation rates of all four compounds by Fe(VI) increased with increased pH (3.1–9.2). A total of 14 degradation products were identified by Liquid chromatography-Time-of-Flight-Mass Spectrometry (LC-TOF-MS), and two pathways including hydroxylation of benzene ring and substitution of chlorine atom were proposed. Hydroxyl radicals , played a vital role during the degradation of phenolic compounds. Moreover, density functional theory calculations were used to explore the degradation mechanisms. The results showed that the hydroxyl radical was more favorable to substitute chlorine atom than hydrogen atom , and the substitution on ortho-position was more favorable than para-position for all four compounds. The findings of this study could greatly improve our understanding on the degradation mechanism of chlorophenol-like compounds by Fe(VI) for environmental remediation.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 8
·1-8
·
IF 5.833
Hu Cong Yi,Jiang Zhong Wei,Huang Cheng Zhi,Li Yuan Fang
Based on the laccase-mimicking activity of Cu 2+ -modified University of Oslo (UiO) metal–organic framework (UiO-67-Cu 2+ ), we developed a colorimetric sensor array for distinguishing a series of phenols with different number and position of substituted hydroxyl group (-OH) and different substituent group on the benzene ring, including phenol, catechol, quinol, resorcinol, pyrogallol, phloroglucinol, o -chlorophenol, o -aminophenol, and o -nitrophenol. The highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy levels of phenolic compounds were obtained by theoretical calculation. The results show that the lower the LUMO energy level, the easier the chromogenic reaction occurs. The UiO-67-Cu 2+ -catalyzed phenol chromogenic reaction showed a good linearity in the range from 0.1 to 200 μM with limit of detection approximately 61 nM. Through the detection of phenol in tap water and river water, the recovery rate and RSD ( n = 3) were calculated as 94.1~103% and 1.0~3.3, respectively, showing good recovery, reliable results, and outstanding stability. Therefore, the proposed colorimetric sensor array will have a great potential for the detection of phenols in the environment. Graphical abstract
Schematic presentation of a simple and sensitive colorimetric strategy based on the laccase-mimicking activity of Cu 2+ -modified UiO-type metal–organic framework (MOFs, Uio-67-Cu 2+ ) to distinguish phenols with analogous structures.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Wang Jia-Wei,Jiang Long,Huang Hai-Hua,Han Zhiji,Ouyang Gangfeng
The fulfillment of a high quantum efficiency for photocatalytic CO 2 reduction presents a key challenge, which can be overcome by developing strategies for dynamic attachment between photosensitizer and catalyst. In this context, we exploit the use of coordinate bond to connect a pyridine-appended iridium photosensitizer and molecular catalysts for CO 2 reduction, which is systematically demonstrated by 1 H nuclear magnetic resonance titration, theoretical calculations, and spectroscopic measurements. The mechanistic investigations reveal that the coordinative interaction between the photosensitizer and an unmodified cobalt phthalocyanine significantly accelerates the electron transfer and thus realizes a remarkable quantum efficiency of 10.2% ± 0.5% at 450 nm for photocatalytic CO 2 -to-CO conversion with a turn-over number of 391 ± 7 and nearly complete selectivity, over 4 times higher than a comparative system with no additional interaction (2.4%±0.2%). Moreover, the decoration of electron-donating amino groups on cobalt phthalocyanine can optimize the quantum efficiency up to 27.9% ± 0.8% at 425 nm, which is more attributable to the enhanced coordinative interaction rather than the intrinsic activity. The control experiments demonstrate that the dynamic feature of coordinative interaction is important to prevent the coordination occupancy of labile sites, also enabling the wide applicability on diverse non-noble-metal catalysts.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Lingxiao Xue,Lijing Hao,Hui Ding,Rui Liu,Dan Zhao,Jianfeng Fu,Mengling Zhang
Glyphosate , a common broad-spectrum herbicide, is a serious environmental pollutant that causes a significant threat to humans. Hence, there is a pressing task to remove glyphosate from the environment. Here, we report an excellent Fe 3 Ce 1 O x catalyst synthesized via the one-step co-precipitation method for activating peroxymonosulfate (PMS) to degrade glyphosate at 25 °C. As a result, glyphosate is completely degraded with a high degradation rate of 400 mg L −1 ·h −1 , and the TOC and TN removals are 85.6% and 80.8%, respectively. As proven by systematic characterizations, the Fe–Ce synergistic effect plays a significant role in promoting PMS activation . The main reactive oxygen species for glyphosate oxidation are surface-bound SO 4 − · and ·OH, produced by activating PMS by electron transfer between Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ of Fe 3 Ce 1 O x . In light of the products determined, the possible degradation process of glyphosate is also speculated: C–N and C–P bonds of glyphosate molecules are attacked to form aminomethylphosphonic acid (AMPA) and orthophosphate (PO 4 3− ) by surface-bound SO 4 − · and ·OH that continuously mineralize and dephosphorylate AMPA to generate small molecules and inorganic ions, such as H 2 O and PO 4 3− . The results of this work suggest that Fe 3 Ce 1 O x /PMS could provide a potential candidate for efficiently removing organic compounds containing nitrogen or phosphorus from wastewater.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Leizhi Zheng,Guoqiang Yang,Xingbang Hu,Zhibing Zhang
The capture and conversion of carbon dioxide (CO 2 ) into useful and valuable chemicals are receiving more and more research interesting. Herein, we designed a new and efficient route to synthesize methyl phenyl carbonate (MPC) via the carbonylation of phenol (PhOH) with CO 2 and methanol (CH 3 OH). PhOH and CH 3 OH react with 1,8-diazabicyclo-[5.4.0]undec-7-ene (DBU) to form ionic liquids [DBUH][PhO] and [DBUH][CH 3 O]. The DBU-based ionic liquids exhibited outstanding performance in CO 2 capture and in situ conversion at room temperature. The reusability of the system had no obviously change after 6 cycles. This protocol provides a sustainable and environmentally friendly preferential technique for the production of MPC, and extends the chemical utilization of CO 2 .
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wenyang Fu,Xuedong Du,Pei Su,Qizhan Zhang,Minghua Zhou
As nitrate contamination causes serious environmental problems, it is necessary to develop stable and efficient electrocatalysts for efficient electrochemical nitrate reduction reaction (ENRR). Here, a nonprecious Co3O4/carbon felt (CF) electrode with a 3D structure was prepared by integrating electrodeposition with calcination methods. This 3D structured Co3O4/CF electrode exhibits a high-rate constant of 1.18 × 10–4 s–1 cm–2 for the ENRR, surpassing other Co3O4 electrodes in previous literature. Moreover, it also has an excellent stability with a decrease of 6.4% after 10 cycles. Density functional theory calculations, electron spin resonance analysis, and cyclic voltammetry were performed to study the mechanism of the ENRR on the Co3O4/CF electrode, proving that atomic H* (indirect pathway) plays a prominent role in NO3– reduction and clarifying the synergistic effect of Co(III) and Co(II) in the Co(II)–Co(III)–Co(II) redox cycle for the ENRR: Co(III) prefers the adsorption of NO3– and Co(II) favors the production of H*. Based on this synergy, a relatively large amounts of Co(II) on the surface of the Co3O4/CF electrode (1.3 Co(II)/Co(III) ratio) was maintained by controlling the temperature of calcination to 200 °C with a lower energy barrier of H* formation of 0.46 eV than other ratios, which is beneficial for forming H* and enhancing the performance of the ENRR. Thus, this study suggests that building 3D structure and optimizing Co(II)/Co(III) ratio are important for designing efficient Co3O4 electrocatalyst for ENRR.
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