EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2021
·Vol. 2021
·期 48
·5069-5076
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IF 2.524
Qiao Han,Hui Wang,Mooeez Ur Rehman,Xin Shang,Haijun Chen,Na Ji,Xinli Tong,Hui Shi,Yujun Zhao
Graphical A phyllosilicate-derived NiFe/SiO 2 catalyst with both metallic Ni and NiFe alloy active sites prepared by ammonia-evaporation method shows excellent intrinsic activity in the hydrodeoxygenation of phenol to cyclohexane. A phyllosilicate-derived NiFe/SiO 2 catalyst (NiFe/SiO 2 −AE) was successfully prepared by the ammonia evaporation method and applied in the hydrodeoxygenation of phenol to cyclohexane. Another two catalysts were also prepared for a comparison by impregnation (NiFe/SiO 2 −IM) and deposition-precipitation (NiFe/SiO 2 −DP) methods, respectively. It was found that Ni−Fe alloy, the active sites for the hydrogenolysis of C−O bond, can be obtained by the reduction of NiFe 2 O 4 (IM) or phyllosilicate (DP and AE) by H 2 . The AE strategy can generate more phyllosilicate structure, which improves the dispersion of both Ni−Fe alloy and metallic Ni sites and allows the formation of more interface between these two kinds of sites as well. Therefore, the NiFe/SiO 2 −AE exhibits a significantly high catalytic performance in the HDO of phenol to cyclohexane. Moreover, the turnover frequency of Ni−Fe alloy sites over NiFe/SiO 2 −AE catalysts is much higher than those of other two catalysts. It is suggested that the enhanced synergy between the two kinds of active sites in the adsorption of C−O groups and hydrogen molecules ensures the superior intrinsic activity in HDO process.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Qing Zhang,Yi Zhai,Fumin Wang,Xubin Zhang,Guojun Lv,Yongkui Liu,Mengyue Li,Mengyao Li
Hierarchical Fe-doped MFI/MCM-41 composites (Fe-HMZs) were one-pot hydrothermal synthesized by partial transformation strategy using conventional CTAB as a dual-functional template. The hierarchical Fe-doped MFI/MCM-41 composites possess ordered mesopores and crystallized MFI structure. The effect of addition amount of NaOH and CTAB as well as the type of the alkali source on the formation of hierarchical Fe-MFI/MCM-41 composites have been investigated in detail. In addition, the temperature-gradient treatment plays the vital roles in the formation of MFI and the possible formation mechanism has been proposed. The obtained hierarchical Fe-HMZ-40 sample exhibits outstanding catalytic performance for phenol hydroxylation and 48% of phenol conversion as well as 89% of dihydroxybenzene selectivity could be achieved, which are ascribed to the more accessible active sites endowed by the significant diffusion ability of ordered mesopores. Compared with Fe-MCM-41 sample, the hydrothermal stability is improved because of the presence of MFI structure.
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Journal of Chemistry
·
2021
·
IF 2.506
Renjie Zhou,Gui Chen,Yuejun Ouyang,Hairui Ni,Nonglin Zhou,Bailin Xiang
Using MOF-5 as a template, the porous carbon (MDPC-600) possessing high specific surface area was obtained after carbonization and acid washing. After MDPC-600 was loaded with Cu ions, the catalyst Cu/MDPC-600 was acquired by heat treatment under nitrogen atmosphere. The catalyst was characterized by X-ray powder diffraction (XRD), N2 physical adsorption (BET), field emission electron microscope (SEM), energy spectrum, and transmission electron microscope (TEM). The results show that the Cu/MDPC-600 catalyst prepared by using MOF-5 as the template has a very high specific surface area, and Cu is uniformly supported on the carrier. The catalytic hydrogen peroxide oxidation reaction of phenol hydroxylation was investigated and exhibits better catalytic activity and stability in the phenol hydroxylation reaction. The catalytic effect was best when the reaction temperature was 80°C, the reaction time was 2 h, and the amount of catalyst was 0.05 g. The conversion rate of phenol was 47.6%; the yield and selectivity of catechol were 37.8% and 79.4%, respectively. The activity of the catalyst changes little after three cycles of use.
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JOURNAL OF SEPARATION SCIENCE
·
2021
·Vol. 45
·期 4
·976-983
·
IF 3.645
Xiu Liu,Junli Pu,Jianming Li,Bolin Gong
Using monodisperse poly(glycidyl methacrylate- co -ethylene glycol dimethacrylate) as the matrix, and pefloxacin template molecules, a novel restricted-access medium molecularly imprinted polymers with Bovine serum albumin crosslinked on its surface was prepared through reversible addition–fragmentation chain-transfer polymerization. Then, the obtained material was employed in dispersive solid-phase extraction to analyze the fluoroquinolones in untreated egg samples by high-performance liquid chromatography–ultraviolet detection. Adsorption performance revealed a good binding amount (40.72 mg/g), fast binding kinetics (25 min), satisfactory selectivity, and good ability to eliminate matrix interference. The reusability experiments indicated the materials have good reusable performance after repetition. Under the optimized conditions, restricted access media-molecularly imprinted polymers-dispersive solid-phase extraction was combined with high-performance liquid chromatography–ultraviolet to enrich fluoroquinolones in untreated eggs, good limit of detection (1.31–3.15 μg/L) and high recovery (89.5–96.8%) were obtained. The results showed that the prepared restricted-access material is promising for the direct detection of antibiotics in complex samples.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Linghao Li,Wei Wang,Jian Huang,Rongmin Dun,Rui Yu,Yiwei Liu,Zile Hua
Nanosized hierarchical titanosilicate-1 zeolites ( nano TS-1_D) with variable Ti doping content were synthesized by a simple and sequent two-step procedure consisting of microporous TS-1 nanocrystal synthesis through steam-assisted dry-gel conversion and post alkali-etching treatment for mesopore formation. Comprehensive characterizations, e.g. XRD, N 2 sorption isotherms, DLS, UV-Vis, SEM, TEM and water-droplet contact angle, indicated that the resultant nano TS-1_D materials not only possess abundant intracrystal mesopores and high surface area, but importantly maintain the intrinsic surface hydrophobicity as those of microporous TS-1 zeolites. Consequently, they showed the expected superior catalytic performance in both bulky cyclohexene/cyclooctene epoxidation and phenol hydroxylation probe reactions, contrast to the microporous TS-1 and amorphous Ti-MCM-41 mesoporous counterparts. In the oxidative desulfurization of fuels, they exhibited 100% removal ability for thiophene and its bulky derivatives and excellent recyclability. In addition, a new Ti-dopant directed alkali-etching mechanism has been proposed to illustrate the synthesis of high-specific-surface-area nano TS-1_D.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 9
·2607-2624
·
IF 3.186
Zhang Qian,Chen Si,Yu Yong Bo,Hong Jun-ming
Simultaneous pollution degradation and disinfection were seldom discussed in the field of electrocatalytic oxidation. In this work, N-doped graphene (N-GN) was selected as anode to ensure the high performance of paracetamol (APAP) degradation. With N doping, the activity of N-GN is evidently improved because of the better surface area, active defects, and conductivity compared with graphene. The generation of active chlorine and O 2 . − on the N-GN surface played an important role in APAP degradation. Compared with other operation parameters (such as pH and current density), environmental microorganisms exhibited more negative interference for APAP degradation. However, evident disinfection effects can be observed because of the release of fulvic and humic acids from microorganisms. In particular, active chlorine is evidently more effective than O 2 . − for disinfection. The simultaneous APAP degradation and disinfection observed in this research provided the possible technology of electrocatalytic oxidation via N-GN for practical application. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Peizhen Yang,Songrong Li,Liang Xiaofu,An Xiaojing,Dongfang Liu,Wenli Huang
The degradation of organic contaminants via traditional radical-dominated advanced oxidation processes (AOPs) under high salinity conditions was limited due to side reactions between coexisting inorganic anions and radicals. Herein, a nonradical oxidation process via peroxymonosulfate (PMS) activation by CuO/MXene for treating high-salinity organic wastewater was developed. Rapid removal efficiency of target pollutant carbamazepine (CBZ) was significantly enhanced to 95.88% within 20 min by CuO/MXene under high salinity conditions (NaCl, 200 mM), compared to the efficiency of 4.30% exhibited by PMS alone. Besides, CBZ maintained a higher removal efficiency of > 81.04% in complex highly saline wastewater composed of eight common inorganic anions. Radical quenching experiments and electron paramagnetic resonance (EPR) analysis confirmed that radical and nonradical oxidation processes were involved in the catalytic process. However, singlet oxygen ( 1 O 2 ) was identified as the primary reactive species, and its contribution rate to CBZ degradation was > 73.58% in a wide pH range (3.0-9.0). The oxygenated functional groups and the interaction between CuO/MXene and PMS facilitated the production of 1 O 2 . The degradation pathway was proposed based on the detection of intermediates. This work provided a new inspiration for the decontamination of organic contaminants under high salinity conditions via a nonradical oxidation process.
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Aggregate
·
2021
·Vol. 3
·期 2
·e147
·
IF 0
Bingyan Han,Qifang Yan,Ze Xin,Qingdong Liu,Dan Li,Jiao Wang,Gaohong He
Nonconjugated polymer dots (PDs) without largely conjugated structures entitle their advantages such as environment friendliness, nontoxicity, and intrinsic fluorescence. However, color-tunable PDs remain a challenge. Herein, polyvinyl pyrrolidone (PVP) and ascorbic acid (AA) are used to synthesize nonconjugated PDs, namely, PA PDs with intensive blue emission. The introduction of a third component, m-phenylenediamine (MPD), redshifted the emission to green. The as-prepared color-tunable blue to green emissive PDs exhibit excellent properties, whether in solution or in solid state, originated from the mechanism of clustering-triggered emission (CTE) induced by the overlap of electron-rich atoms, the strong inter/intrachain interaction. The quantum yields of blue and green PDs reached up to 15.07% and 28.22%, respectively. Furthermore, PA PDs were successfully applied to the highly efficient photocatalytic degradation for dyes: methylene blue (MB) and methyl orange (MO) were degraded by 89.9% and 93.8% within 20 min under visible light, respectively.
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ANALYST
·
2021
·Vol. 146
·期 24
·7593-7600
·
IF 4.616
Ling Lei,Caoling Li,Wensheng Huang,Kangbing Wu
Developing a sensitive and rapid detection method for 4-chlorophenol (4-CP) and 4-nitrophenol (4-NP) is very important due to their high toxicity. In this work, bulk Ti3AlC2 powder was etched to Ti3C2Tx for the first time through a hydrothermal reaction in NaF/HCl solution. After ultrasonication in N-methylpyrrolidone (NMP), Ti3C2Tx powder was successfully exfoliated into multilayered Ti3C2Tx nanosheets (i.e. Ti3C2Tx MXene). The prepared Ti3C2Tx MXene not only has a large electrochemical surface area for the oxidation of 4-CP and 4-NP, but also lowers their electron transfer resistance. As a result, the oxidation signals of 4-CP and 4-NP are significantly improved on the surface of the Ti3C2Tx MXene. Based on the remarkable signal amplification of the Ti3C2Tx MXene, a sensitive and rapid method was developed for the simultaneous detection of 4-CP and 4-NP. The linear range is from 0.1 to 20.0 μM for 4-CP, and from 0.5 to 25.0 μM for 4-NP, with detection limits of 0.062 μM (4-CP) and 0.11 μM (4-NP). This method was used in wastewater samples, and the accuracy was confirmed to be good by high-performance liquid chromatography.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2021
·Vol. 139
·期 3
·51508
·
IF 3.125
Lilan Huang,Shaofei Wang,Haimei Chen,Xiaoyang Hou,Han Zhang,Jian Pan,Yuzhong Zhang
Phenolic waster has a pervasive problem afflicting people throughout the word due to negative impacts for ecosystems and humans. Herein, isolated iron/polyethersulfone (4A-Fe/PES) mixed-matrix membrane as a catalytic non-permselective membrane reactor is developed for rapid reduction of phenol in continuous flow-through reaction. The forced flow of the reactants through the membrane intensifies the contact between reactants and immobilized catalysts, allowing for high catalytic activity with negligible mass transport resistances. In the presence of H 2 O 2 , the 4A-Fe/PES catalytic membrane can remove 99.9 ± 1.6% phenol after 6 min at pH 2 with a catalyst/phenol mass ratio of 1/3. The catalytic membranes show much higher performances than 4A-Fe particles even under neutral or alkaline conditions. In particular, at pH 9, the catalytic membrane exhibits a phenol degradation rate of 92.5 ± 3.4% after 12 h. This strategy provides guidance to the design of high-performance catalytic membranes for efficient removal of phenolic pollutants.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Jianhui Jia,Jianbo Chen,Huan Ding,Xianggui Xue,Shichun Li,Jichun Huang,Yu Liu
N- oxide based explosives display better explosive performances than traditional explosives, because of the introduction of N- oxide group with strong hydrogen bonding (H-bonding). However, the strong H-bonding results in poor dissolution of N- oxide based explosives, and thus poses a significant challenge for their potential applications. Deep eutectic solvents (DESs), a new generation of green solvents, display promising dissolution toward strong H-bonding materials in recent years. In this study, 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) was used as a prototype of N- oxide based explosives to study the dissolution in DESs. The dissolution conditions for LLM-105 were optimized by using different types of DESs. The DES-3 - 2 based on choline chloride and urea displayed higher dissolving capacity with 0.52 g/100 g at 80 °C, which was determined by traditionally gravimetric method. Further, the dissolution process of LLM-105 in DES-3 - 2 under different temperatures was investigated by comprehensive analysis including ultra-high-performance liquid chromatography, high-resolution mass spectrum and theoretical calculations. The dissolution of LLM-105 under ≤80 °C was demonstrated to be real dissolution referring to the formation of Zundel-type complex and Meisenheimer complex between DES-3 - 2 and LLM-105. Abnormally high solubility of LLM-105 at >80 °C was attributed to the self-collapse of its H-bonding network by losing a nitro group and an oxygen of N- oxide group.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yangke Long,Jian Dai,Shiyin Zhao,Shixin Huang,Zuotai Zhang
Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as Co@NC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation , surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation.
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