CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xiaojie Qiu,Shengjiong Yang,Mawuli Dzakpasu,Xiaoping Li,Dahu Ding,Pengkang Jin,Rongzhi Chen,Qionghua Zhang,Xiaochang C. Wang
Mn 0.8 Fe 2.2 O 4 magnetic nanocrystals (Mn 0.8 Fe 2.2 O 4 MNCs) are synthesized by thermal treatment of a metal-organic framework (MOF) template, and their physicochemical properties are characterized in detail. The Mn 0.8 Fe 2.2 O 4 MNCs exhibited highly efficient performance for the catalytic degradation of Bisphenol A (BPA) by peroxymonosulfate (PMS) activation at various initial pH, catalyst dosage, and PMS concentration. A leaching solution experiment evidenced that PMS activation by the Mn 0.8 Fe 2.2 O 4 MNCs is a heterogeneous process. Interestingly, scavenging experiments and electron paramagnetic resonance (EPR) analysis demonstrated that HO is the dominant radical for BPA degradation, rather than SO 4 − . The scavenger experiment indicated that the surface-bound radicals may play the crucial role for BPA degradation. Increasing Cl − or decreasing bicarbonate concentrations in solution enhanced the catalytic degradation process significantly through non-radical pathways. The Mn 0.8 Fe 2.2 O 4 MNCs exhibited desirable stability and reusability, that the spent Mn 0.8 Fe 2.2 O 4 MNCs could be significantly regenerated by thermal treatment at 450 °C in open air. Findings from this study would expand the applications of MOFs and also provide new insights into the enhancement of degradation efficiency during PMS activation processes.
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ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Shi Gang Liu,Haoyu Wang,Qian Zhao,Wenli Gao,Xingbo Shi,Zhonghua Liu
Background Dichlorvos (DDVP), as a highly effective insecticide, is widely used in agricultural production. However, DDVP residue in foodstuffs adversely affects human health. Conventional instrumental analysis can provide highly sensitive and accurate detection of DDVP, while the need of bulky and expensive equipment limits their application in resource-poor areas and on-site detection. Therefore, the development of easily portable sensing platforms for convenient, rapid and sensitive quantification of DDVP is very essential for ensuring food safety. Result A portable colorimetric sensing platform for rapid and sensitive quantification of DDVP is developed based on nanozyme-participated highly efficient chromogenic catalysis. The Fe-Mn bimetallic oxide (FeMnOx) nanozyme possesses excellently oxidase-like activity and can efficiently catalyze oxidation of 3, 3′, 5, 5′-tetramethylbenzidine (TMB) into a blue oxide with a very low Michaelis constant (K m ) of 0.0522 mM. The nanozyme-catalyzed chromogenic reaction can be mediated by DDVP via inhibiting the acetylcholinesterase (AChE) activity. Thus, trace DDVP concentration-dependent color evolution is achieved and DDVP can be sensitively detected by spectrophotometry . Furthermore, a smartphone-integrated 3D-printed miniature lightbox is fabricated as the colorimetric signal acquisition and processing device. Based on the FeMnOx nanozyme and smartphone-integrated lightbox system, the portable colorimetric sensing platform of DDVP is obtained and it has a wide linear range from 1 to 3000 ng mL −1 with a low limit of detection (LOD) of 0.267 ng mL −1 for DDVP quantification. Significance This represents a new portable colorimetric sensing platform that can perform detection of DDVP in foodstuffs with simplicity, sensitivity, and low cost. The work not only offers an alternative to rapid and sensitive detection of DDVP, but also provides a new insight for the development of advanced sensors by the combination of nanozyme, 3D-printing and information technologies.
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Nanoscale
·
2017
·Vol. 9
·期 8
·2824-2835
·
IF 7.367
Zhi-Qiang Zhou,Li-Yun Yang,Ren Yan,Jie Zhao,Yu-Qi Liu,Lu Lai,Feng-Lei Jiang,Thomas Maskow,Yi Liu
Although cation exchange (CE) has been studied for many years and some mechanisms were proposed, there is still a knowledge gap in CE and problems such as the need for high temperature and it being time-consuming are still unaddressed. We developed a new mild strategy for CE by introducing a new ideal template and first applied this doping strategy to detect Cd2+ and Hg2+. This strategy adopted Mn-doped ZnSe quantum dots (QDs) as the template and the introduction occurs via a two-step CE reaction: first Zn2+ was partially substituted by X (X = Cd2+, Hg2+, Cu2+, Ag+ or Pb2+), later Mn2+ (in the deep structure of QDs) was substituted by X. Remarkably, Mn2+ in the lattice can be easily substituted by a dopant and its replacement by a dopant helps to bury the metal ions. The ultra-fast introduction of Cd2+ and Hg2+ (70 minutes for Cd2+ and 19 minutes for Hg2+) was realized at room temperature; other metal ions such as Ag+, Cu2+ and Pb2+ can be buried at 50 °C. This mild reaction temperature offers a solution for introducing impurities without sacrificing the interfacial structure of nanocrystals. HRTEM, XPS and ICP measurements were applied to analyze the introduction process. Furthermore, the spectroscopic method was employed to analyze the introduction, migration and distribution of metal ions. Then, we proposed a mechanism for the chemical conversion of nanocrystals by CE. Through this strategy, full-color light-emitting doped QDs were fabricated. Strikingly, a new turn-on probe for the detection of Cd2+ and Hg2+ with improved selectivity was developed by adopting this doping strategy. The detection limit is 36 nM for Cd2+ and 20 nM for Hg2+, which is competitive with the limit of detection reported by other groups using QDs as sensors.
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International Journal of Minerals Metallurgy and Materials
·
2016
·Vol. 23
·期 11
·1346-1351
·
IF 0.882
Jiang Peng,Yang Wen-hui,Zhou Yun-cheng,Kuang Jian-lei,Li Yong,Xiao Ting
Brownmillerite-type oxides Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
(0 ≤ x ≤ 0.6, 0 ≤ y ≤ 0.5) were prepared at 1300°C through solid-state reaction. X-ray diffraction (XRD) analysis showed that the structure symmetry evolved from orthorhombic to cubic with increasing Mn and Al contents. When y was greater than 0.3, peaks associated with small amounts of BaAl 2 O 4 and Ba 2 InAlO 5 impurities were observed in the XRD patterns. When substituted with a small amount of Mn ( x ≤ 0.3), the Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
samples exhibited an intense turquoise color. The color changed to green and dark-green with increasing Mn concentration. UV–vis absorbance spectra revealed that the color changed only slightly upon Al doping. The valence state of Mn ions in Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
was confirmed to be +5 on the basis of X-ray photoelectron spectroscopic analysis. According to this analysis, the intense turquoise color of the Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
samples is rooted in the existence of Mn 5+ ; thus, the introduction of Al does not affect the optical properties of the compounds.
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Small
·
2024
·
IF 13
Lian-Hua Xu,Qichang Wang,Liangdong Hu,Dekui Shen,Sheng Chu,Huiyan Zhang
The electrochemical reduction of oxygen is pivotal for advancing emerging energy technologies. Precise control over morphology and electronic structure is essential for enhancing catalytic activity and stability in the oxygen reduction reaction (ORR). In this study, a freestanding carbon electrode is developed by in-situ growth of carbon nanotube (CNT)-encapsulated bimetallic CoM (M = Ni, Fe, Mn, Cu) nanoparticles (NPs) within a hierarchical carbonized wood matrix (CoM@NWCC). The hierarchically porous architecture of the electrode promotes efficient mass transfer during the ORR. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) analyses revealed that incorporating metals such as Ni, Fe, Mn, and Cu modulates the electronic structure of Co, specifically adjusting the distance between the d-band center (E d ) and the Fermi level (E F ), thus optimizing ORR kinetics. Among these, CoNi@NWCC, with its asymmetric electronic configuration, achieves an optimal balance between OH * and OOH * adsorption, significantly enhancing catalytic performance. This study demonstrates the potential of band structure engineering to precisely tailor catalyst properties, offering a cost-effective and high-performance solution for zinc-air batteries (ZABs) suitable for large-scale deployment.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Zihao Li,Zewen Chen,Chen Ye,Lixi Gong,Hui Wang,Jie Zhou
Despite the low cost of supported non-precious metal catalysts, their catalytic activity is significantly lower than that of precious metal catalysts in the catalytic oxidation reaction of volatile organic compounds (VOCs). In order to enhance the catalytic activity of supported non-precious metal catalysts, we introduced an ultra-low loading of palladium into the existing catalytic system and employed a plasma preparation process instead of the conventional impregnation method. The approach significantly improves the catalytic activity of the active sites on the catalyst. The results indicate that, compared to the supported Pd and CuMnCeO x catalysts prepared by conventional impregnation method, the Pd/CuMnCeO x /SiO 2 -P catalysts prepared via plasma exhibit a higher proportion of lattice defects (oxygen vacancies). Furthermore, the doping of the ultra-low Pd could facilitate the formation of additional lattice defects in the composite oxide. As a result, it can improve the content of surface active oxygen and enhance the adsorptive strength of hexane on the surface of the catalyst. The Pd/CuMnCeO x /SiO 2 -P catalysts exhibit high catalytic activity and stability in the catalytic oxidation of n-hexane. This work promotes the potential application in the preparation of catalyst with ultra-low precious metal loading.
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POLYHEDRON
·
2024
·
IF 2.4
Firdous Bibi,Adeel Ahmed,Yathrib Ajaj,Ahmed Abd Al-Sattar Dawood,Muhammad Usman,Abdullah Alodhayb,Saikh Mohammad,Zubair Ahmad,Ambreen Kalsoom,Shahid Iqbal
Herein, we have synthesized Ni and Mn co-doped ZnFe 2 O 4 ferrites using the simple co-precipitation method and their nanocomposites (NCs) with 10 % rGO using the ultra-sonication route. The structural investigation revealed the successful formation of single-phase ZnFe 2 O 4 NPs with cubic spinel ferrite geometry. The crystallite size was determined to be in the range of 21 nm to 28 nm. The current–voltage (I-V) analysis revealed that Ni and Mn co-doping and the addition of rGO nanosheets in ZnFe 2 O 4 NPs boosted the electrical responses of the fabricated Zn 1-x Ni x Fe 2-y Mn y O 4 /rGO NCs. The BET analysis indicates an increase in the surface area of Zn 1-x Ni x Fe 2-y Mn y O 4 /rGO NCs (132 m 2 /g) that might be attributed to the inclusion of rGO nanosheets, which prevents the NPs from agglomeration. The photocatalytic evaluation of the pristine ZnFe 2 O 4 NPs, Ni and Mn co-doped Zn 1-x Ni x Fe 2-y Mn y O 4 NPs, and Zn 1-x Ni x Fe 2-y Mn y O 4 /rGO NCs photocatalysts was tested by photodegradation of malachite green (MG) dye under sunlight irradiation. Results exhibited improved photocatalytic responses and degraded 94.6 % of MG dye in 45 min using Zn 1-x Ni x Fe 2-y Mn y O 4 /rGO NCs, which was much higher compared to the Ni and Mn co-doped Zn 1-x Ni x Fe 2-y Mn y O 4 NPs (58.7 %) and pristine ZnFe 2 O 4 NPs (38.3 %). The increased degradation potential of Zn 1-x Ni x Fe 2-y Mn y O 4 /rGO NCs was accredited to the highly conducting nature and 2D nano-sheets of rGO, which efficiently inhibited the recombination of charge carrier species. Ultimately, the remarkable photocatalytic capability exhibited by Zn 1-x Ni x Fe 2-y Mn y O 4 /rGO NCs implies that the synthesized NCs could have auspicious practical applications in the elimination of dyes from wastewater.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Chengzhi Wang,Zhenbang Tian,Weiqing Huang,Jingyuan Hu,Xing Xing
Owing to the different reaction properties and deactivation mechanisms caused by the structural discrepancy of monolithic catalysts, abundant scientific results of powder or granular NH 3 -SCR catalysts have still not sufficiently robustly applied in recent years. Furthermore, minimal research has been focused on monolithic catalysts. As a result, this work prepared monolithic Mn-Fe-Ce/Al 2 O 3 catalysts by active component impregnation (ACI-Mn-Fe-Ce/Al 2 O 3 ) and precursor impregnation methods (PI-Mn-Fe-Ce/Al 2 O 3 ) and investigates the long-term SO 2 and H 2 O resistance of the catalysts. Compared with the PI-Mn-Fe-Ce/Al 2 O 3 catalyst, the monolithic ACI-Mn-Fe-Ce/Al 2 O 3 catalyst showed better performance. The catalytic activity follows a bell-shaped curve with an optimal performance at a drug loading of 5 %. The ACI-Mn-Fe-Ce/Al 2 O 3 catalyst exhibits long-term resistance to SO 2 and H 2 O and can still convert more than 70 % NO x after 168 h of SO 2 and H 2 O resistance test. Characterization of the ACI-Mn-Fe-Ce/Al 2 O 3 catalysts before and after the reaction showed that the reducibility decreased after the reaction, and more Mn 4+ was transformed into Mn 2+ to weaken the catalytic activity. However, more Fe 2+ and Ce 3+ were generated during the reaction, increasing the number of oxygen vacancies, oxygen defects, and hydroxyl-like groups, all of which would contribute to a certain extent to counteract the passivation effect of SO 2 on the catalysts. In situ DRIFTs analysis shows that the formation of surface sulfates has a minimal effect on the adsorption of NO, but it does affect the adsorption of coordinated NH 3 on Lewis acid sites. This work elucidates the deactivation details of Mn-Fe-Ce/Al 2 O 3 catalysts from the perspective of physicochemical properties, which provides a reference for the development of better low-temperature SO 2 -resistance catalysts for industrial applications.
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FOOD CHEMISTRY
·
2020
·
IF 6.306
Xinyue Yuan,Dianwei Zhang,Xuecheng Zhu,Huilin Liu,Baoguo Sun
Manganese-doped zinc sulfide quantum dots (Mn-ZnS QDs) are promising candidates for multi-channel sensing analysis due to their multi-dimensional optical properties. In this study, we integrated amino-silane and ionic liquid co-modified Mn-ZnS QDs and covalent organic frameworks (COFs) into optosensing nanoparticles to provide triple-dimensional optical response signals and combined them with chemometrics for the analysis of multiple pesticide residues . Through the exploration and optimization of a series of conditions, fluorescence, room temperature phosphorescence, and ultraviolet−visible combined with chemometrics were used for the discrimination and recognition of multiple pesticide residues in fruits and vegetables. The ionic liquid of 1-vinyl-3-ethylimidazolium tetrafluoroborate was used to modify Mn-ZnS QDs to improve the optical response and enrichment of pesticide adsorption sites, which were also synergistically enhanced by the COF support. This is a potential method to discriminate pesticides efficiently and enables fast and reliable analysis of pesticides in the agricultural and food industries.
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JOURNAL OF COORDINATION CHEMISTRY
·
2024
·
IF 2.2
Ying Zhou,Xiao-Tong Song,Hui-Chao Guan,Shu-Mei Yue
In this investigation, six new metal complexes with 2-(pyridin-2-yl)benzo[d]imidazole (bpm) were synthesized and analyzed by single-crystal X-ray diffraction (XRD), including catena-bis[(µ-2,2-bis(4-carobxyphenyl)hexafluoropropane)-(2-(pyidin-2-yl)-1H-benzimidazole)-aqua-zinc] (1), catena-[(µ-2,2-bis(4-carobxyphenyl)hexafluoropropane)-(2-(pyidin-2-yl)-1H-benzimidazole)-aqua-cadmium] (2), aqua-[2,2-bis(4-carobxyphenyl)hexafluoropropane]-bis[2-(pyridin-2-yl)-1H-benzimidazole]-manganese (3), μ-[2-nitrobenzene-1,4-dicarboxylato]-μ-[2-nitrobenzene-1,4-dicarboxylato]-bis[2-(pyridin-2-yl)-1H-benzimidazole]-di-zinc (4), catena-[bis(µ-2-nitrobenzene-1,4-dicarboxylato)-diaqua-bis(2-(pyridin-2-yl)-1H-benzimidazole)-di-cadmium] (5), aqua-[pyridine-2,6-dicarboxylato]-[2-(pyridin-2-yl)-1H-benzimidazole]-copper hydrate (6) (H2hfipbb = 2,2-bis(4-carboxyphenyl)hexafluoropropane, H2nbdc acid = Nitroterephthalic acid, and H2pda = 2,6-pyridinedicarboxylic acid). Complex 1 crystallized in a monoclinic system with space group P21/n; 2 crystallized in a monoclinic system with space group C2/c; 3 crystallized in an orthorhombic system with space group Pna21; 5 crystallized in a monoclinic system with space group P21/c; 4 and 6 crystallized in triclinic systems with space group P-1. The DNA-binding modes of the complexes were investigated by several analysis methods (e.g. viscosity analysis, circular dichroism spectroscopy, fluorescent spectroscopic analysis, as well as UV spectroscopic analysis). Complexes 1-6 bind to calf thymus DNA via an intercalative mode. The results of this study provide insights into the mechanism of DNA binding and provide a basis for rationally designing new powerful reagents for DNA detection and targeting.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Rui Tian,Shiying Fan,Guohua Chen,Xinyong Li
The photocatalytic conversion of methane into valuable liquid oxygenates presents a promising strategy for advancing a sustainable chemical industry. However, achieving both high conversion efficiency and high selectivity using non-precious metal catalysts under ambient conditions remains a significant challenge. Inspired by the functional characteristics of natural enzymatic catalytic systems, this study has constructed a multicomponent synergistic catalytic system with ZnMn₂O₄ as the support. Through the defective engineering design of fluorine doping and in situ growth of tungsten species, it achieves efficient construction of the microenvironment of active centers and precise regulation of free radical intermediates. The optimized 3W20F-ZnMn₂O₄ catalyst achieved a liquid-phase product yield (including methanol and ethanol, etc.) of 442.02 μmol·g⁻¹ ·h⁻¹ with a selectivity of 98.6 % under ambient temperature and pressure—surpassing the performance of most reported non-precious metal-based catalytic systems. Studies have demonstrated that catalysts doped with the two elements exhibit significant differences in the oxygen sources of products, which reflects the distinct pathways they follow in catalyzing methane oxidation. Specifically, the oxygen vacancy (FVo) sites formed by F doping primarily adhere to a single reaction pathway using water as the oxygen source, where the active oxygen species are mainly dominated by ·OH generated from the dissociation of water molecules, ultimately yielding ethanol and small amount of methanol. In contrast, the active sites formed by W doping involve multiple reaction pathways. The production of ethanol relies more on ·OH from water molecule dissociation, while the generation of methanol and methyl hydroperoxide is more dependent on active oxygen species derived from oxygen activation. This study deepens the understanding of the multi-element synergistic catalytic mechanism and lays a foundation for the development of sustainable and efficient catalytic systems.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Fangfang Du,Gan Li,Xiaojuan Gong,Guo Zhonghui,Shaomin Shuang,Ming Xian,Chuan Dong
We rapidly synthesized N,P-dual-doped carbon dots (N,P-CDs) via the acid-base neutralization spontaneous heat using a simple blend of phthalic acid, 1,2-ethylenediamine, and concentrated phosphoric acid. The approach is automatic without external heat treatment to speedily produce dozens of N,P-CDs, which refrain high temperature, sophisticated manipulations, and long reaction times. As-fabricated N,P-CDs with excellent luminescent properties, superior biocompatibility and respectable fluorescence quantum yield (QY) of 15% have been employed for the development of a label-free multifunctional fluorescence sensing platform for the detection of Mn(VII), temperature sensing and cellular imaging. Mn(VII) is able to effectively quench the fluorescence of N,P-CDs based on inner filter effect (IFE) because the absorption bands of Mn(VII) can perfectly overlap the emission and excitation wavelengths of N,P-CDs. The system had high selectivity toward Mn(VII) and the detection limit was 48.3 nM in the broad linear span from 10 μM to 200μM. Moreover, the N,P-CDs were extended for sensing Mn(VII) in living cell due to favorable biocompatibility and negligible cytotoxicity. Furthermore, the sensors showed a linear and reversible variation of emission intensity for a temperature range from 25℃ to 80℃, with a sensitivity of −1.79% per ℃. The practical implications of N,P-CDs for Mn(VII) detection have been demonstrated in Teas leaves and Medicinal herbs samples with satisfactory results.
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