Sustainability
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2022
·Vol. 14
·期 3
·1318
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IF 3.889
Haijie He,Erpei Xu,Zhanhong Qiu,Tao Wu,Shifang Wang,Yuhua Lu,Guannian Chen
Bentonite was modified with cetyltrimethylammonium bromide (CTAB). The organically modified bentonite (OMB) was used to remove phenol from aqueous solution, the microstructural changes were characterized by X-ray diffraction (XRD) and scanning electronic microscopy (SEM), and phenol adsorption kinetic was obtained using batch adsorption test results. The results indicated that the rate of adsorption of phenol onto the OMB was positively correlated with the initial concentration, and the maximum adsorption capacity was found to be 10.1 mg/g at the initial concentration of 150 mg/L at 25 °C and pH 10. The investigations of adsorption kinetics models showed that the adsorption kinetic was better reflected by the pseudo-second-order kinetic model. Furthermore, the properties of the OMB samples with different adsorption times were obtained by SEM and XRD. The statistic analysis revealed that the pore diameter of the OMB samples decreased with the increasing adsorption time and gradually reached equilibrium.Keywords:organically modified bentonite;adsorption;kinetics
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
·
IF 10.753
Jun Wang,Ying Zhao,Chunting Li,Zijun Yu,Yang Zhang,Yuan Li,Xiaoyao Tan,Shaomin Liu,Shaobin Wang,Xiaoguang Duan
Hierarchically porous iron/nitrogen-doped carbons (Fe-N-PC) were developed for the oxidation of ibuprofen (IBP) with peroxymonosulfate (PMS). The incorporation of trace-level iron and nitrogen dopants promoted the catalytic performance remarkably, leading to 4.8, 16.4 and 22.9-fold enhancement over N-doped carbon (N-PC), porous carbon (PC), and Fe-doped carbon (Fe-PC), respectively. Fe(III) was anchored in nitrogen-coordinated pots (Fe-N x ) in the sp 2 -hybridized carbon network, and graphitic-N could synergistically boost the catalysis. Notably, methyl phenyl sulfoxide (PMSO) transformation, quenching tests, in situ electrochemical analysis and Raman spectroscopy verified high-valent iron-oxo species and direct electron transfer pathway accounted for pollutant oxidation. The relationship between the kinetic constants (ln k obs ) and the oxidation peak potential ( E op ) of pollutants was established with good correlation, manifesting particular selectivity toward oxidizing electron-rich pollutants and great immunity to background inorganic ions and natural organic matters (NOMs) for real wastewater treatment . The deactivation mechanisms of Fe-N-PC were revealed via surface oxidation and dopant refabrication. This work delicates to deepen the understanding of the nonradical mechanisms and structure-oriented PMS activation by engineered carbonaceous materials .
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Liang Zhu,Xuecui Mei,Zhengchun Peng,Jiao Yang,Yingchun Li
Paper-based microfluidic analytical devices (μPADs) have recently attracted attention as a rapid test kit owing to their low cost and nonrequirement for external driving pump. However, low accuracy and poor anti-interference ability of μPADs under complex detection condition limit their practical applications. Here, we present a facile way to prepare a novel fluorescence sensor-array μPAD for multi-analyte discrimination based on molecular imprinting technology , and its sensing behavior was studied by using three nitrophenol (NP) isomers (2-, 3-, and 4-NP) as the testing models. Carbon quantum dots (CQDs) emitting blue light were grafted on glass-fiber paper, followed by in-situ modification of three types of molecularly imprinted polymers (MIPs) with 2-, 3-, and 4-NP as template. Each sensing unit on the array showed differential yet cross-reactive binding affinity to NP isomers, resulting in distinct fluorescence quenching efficiency. Thus, precise distinguishment of the three NPs was realized with the MIPs/CQDs/paper-based sensor array. Furthermore, the discrimination ability of the platform was evaluated in mixtures of the NP isomers. Practicability of this apparatus was validated by identification of blind samples and 100% accuracy was achieved. The μPAD has proven to be highly sensitive and accurate, which will serve as an ideal analytical tool in the fields of environment monitoring, disease prognosis, food safety and so on.
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POLYMER
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2022
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IF 4.432
Qisong Lin,Feng Gao,Yongjun Wang,Wangyang Lu,Wenxing Chen
Antimony-free poly(ethylene terephthalate) (PET) has been synthesized through polycondensation of p -phthalic acid and ethylene glycol , and then subjected to a viscosity-increasing process by liquid-state polycondensation (LSP). For both of these processes, a novel environmentally benign ethylene glycol-soluble Ti/Mg bimetal (TM) catalyst has been used. The structure of the TM catalyst has been comprehensively characterized and its catalytic activity in the polycondensation reaction has been evaluated and compared with those of other titanium-based catalysts. The results reveal that the TM catalyst is a chelated complex with high catalytic activity for polycondensation to afford PET without significant side reactions. Indeed, the LSP process catalyzed by TM affords a PET product with high intrinsic viscosity suitable for industrial yarn production (1.08 dL/g) within 60 min, and that exhibits higher thermostability with increasing intrinsic viscosity. Finally, the kinetics of the TM-catalyzed polycondensation has been probed based on the variation of intrinsic viscosity with increasing polycondensation time.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Xiaobo Min,Chu Chu,Zonghao Luo,Junye Ma,Yifu Fu,Zongsu Wei,Richard Spinney,Dionysios D. Dionysiou,Ruiyang Xiao
In this study, the kinetics and mechanisms of superoxide radical ( O 2 · - )-mediated transformation of two monosubstituted aromatic contaminants with diametrically opposed electronic effect, namely phenol (PhOH) and nitrobenzene (NB), were investigated through combined experimental and theoretical approaches. The reaction rate constant between O 2 · - and PhOH was determined to be 269 M −1 s −1 via competition kinetic method. Such weak role of O 2 · - was confirmed by density functional theory (DFT) calculations at SMD/CAM-B3LYP/6-311++G(2d,2p)//CAM-B3LYP/6-31+G(d,p) level of theory. However, NB exhibited a higher reactivity towards O 2 · - than PhOH, demonstrating the selectivity of O 2 · - to electron withdrawing group. Despite the difference in reactivity, O 2 · - shows very limited removal capacity for PhOH and NB. These results were also in reasonably good agreement with an indication from a quantitative structure–property relationship model. With these quantitative and mechanistic results, we provided a more comprehensive understanding on the O 2 · - -mediated transformation of organic pollutants bearing different electron donating/withdrawing groups.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Zihui Jia,Yangyang Lv,Yu Guo,Qiaohui Gao,Hexiang Lan,Aimal Khan,Aihua Xu,Xiaoxia Li
The abundant and low-cost manganese oxides have attracted increasing interest in peroxymonosulfate (PMS) activation. Nevertheless, the low zeta potentials and surface area of the catalysts lead to weak adsorptions of PMS and pollutants under neutral and basic conditions, and thus the low degradation efficiency. Herein, a promising hybrid from graphite nanosheets (GNs) and cryptomelane-type manganese octahedral molecular sieves (OMS-2) was developed by a simple redox method at room temperature. The catalysts possessed a high surface area and a great number of surface defects , which enhanced the adsorption of PMS; while the introduction of GNs increased the capacity of pollutants adsorption and the rate of electron transfer. Compared with pure OMS-2 and other catalysts, the hybrid catalyst showed a much higher performance for acid orange 7 degradation at pH 8.2 with a first-order rate constant of 0.414 min −1 , due to the above synergistic effects between OMS-2 and GNs. Based on quenching experiments, PMS decomposition and degradation of pollutants with different oxidation potentials, a direct electron transfer process through Mn-O-PMS complexes was identified to contribute the degradation. Moreover, a galvanic oxidation system was set up to further confirm the occurrence of the mechanism. Overall, this work provides an important step in developing Mn-based hybrids for organic pollutants degradation.
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CHEMOSPHERE
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2022
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IF 8.943
Haixia Wu,Ruoyu Liu,Yongjun Sun,Yiyun Wen,Quanfa Zhao,Shaohua Lin,Yong Wang
Molybdenum disulfide (MoS 2 ) was added to the system after being treated with high-voltage pulse discharge plasma to improve the degradation efficiency of pollutants and reduce energy consumption. The discharge plasma-treated solution contains hydrogen peroxide and metal iron ions, and MoS 2 addition can cause co-catalytic Fenton reaction . The effects of discharge time, initial pH, phenol concentration, MoS 2 dosage, discharge voltage, and gas type on phenol removal and aqueous H 2 O 2 concentration were mainly investigated. Results showed that the addition of MoS 2 after plasma treatment can reduce the plasma treatment time by 70% and maintain or even increase the degradation efficiency of phenol from 40% (after 20 min of discharge plasma) to 92% (after turning off the discharge and dosing with MoS 2 for 30 min). Acidic conditions (pH = 3–4) and oxygen were beneficial to phenol removal. MoS 2 addition greatly improved the catalytic oxidation of discharge plasma. This study provides a promising direction for water treatment based on plasma technology .
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ACS Catalysis
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2022
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IF 13.7
Hui Wang,Wenru Zhao,Mooeez Ur Rehman,Wei Liu,Yuxi Xu,Huijiang Huang,Shengping Wang,Yujun Zhao,Donghai Mei,Xinbin Ma
In the utilization of renewable resources derived from biomass, hydrodeoxygenation (HDO) is one of the most critical steps in the bio-oil upgrading process. Herein, a series of copper phyllosilicate nanotube (CuPSNT) catalysts were successfully prepared and applied in the chemosynthesis of cyclohexane via the phenol HDO reaction. Against the presumption that mono-metal copper was not active for the complete hydrogenation of aromatic compounds, a cyclohexane yield of 97.8% at the total conversion of phenol was achieved at 230 °C on the CuPSNT catalysts with a Cu/Si ratio of 1:1. The kinetic analysis suggested that further conversion of cyclohexanol to cyclohexane is the rate-determining step in the phenol HDO. Cu0 accounts for the hydrogenation, while Cu+ is responsible for the adsorption of phenol and cyclohexanol and in charge of further cyclohexanol dehydration. This conclusion is further confirmed by density functional theory calculations. This work demonstrates that the synergy between Cu0 and Cu+ species of CuPSNT catalysts plays a critical role in the HDO process of phenol, and mono-metal Cu can accomplish both the saturation of aromatic rings and the removal of oxygen groups.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 17
·10394-10407
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IF 3.945
Jing Xiao,Cong Wang,Bai-Qi Feng,Tian-Yu Liu,Shao-Yi Jia,Hai-Tao Ren,Yong Liu,Song-Hai Wu,Xu Han
Although synthesis of oligoaniline (OANI) by persulfate and aniline has been investigated in the recent years, the impact of phenol on the synthesized soluble OANI is still not clear. In this study, our results indicate that phenol and pH mediate the production of the blue water-soluble OANI (OANIblue) in the reaction between sodium persulfate (SPS) and aniline under alkaline conditions, and the yields of OANIblue increase with increasing concentrations of phenol and pH values. Quenching experiments rule out the contributions of SO4˙− and ˙OH to aniline oxidation and imply that the non-radical activation of SPS is an important pathway in the formation of OANIblue. MALDI-TOF-MS analysis indicates that phenol apparently inhibits the polymerization degree of aniline in that the molecular weights of OANIblue gradually decrease from 1586.4 to 684.6 when phenol is increased from 0 to 2.0 mM. FTIR and Raman analyses confirm the structure of aniline oligomers in OANIblue and indicate that phenol inhibits the phenazine-like structure in OANIblue and facilitates the transformation of benzenoid rings to quinoid rings in the oxidation products. However, simultaneous activation of SPS by phenol and aniline is likely to occur in the reaction system with the formation of PhNH˙, as indicated by DFT calculations. The high scavenging reactivity of phenol towards both PhNH2˙+ and PhNH˙ implies that PhNH2˙+ and PhNH˙ are not the intermediates in the formation of OANIblue. DFT calculations also reveal that apart from the one-electron transfer pathway between aniline and SPS, the two-electron transfer pathway is also likely to occur in the presence of phenol, resulting in the formation of PhNH+/PhN˙˙ without producing PhNH2˙+ and PhNH˙. The produced PhNH+/PhN˙˙ intermediates then couple with aniline, PhNH+, aminophenyl sulfate and its hydrolysate to form dimers, trimers, oligomers, and eventually OANIblue. This study not only describes a novel method to prepare water-soluble OANI, but also gives new insight on the importance of phenol in the production of OANIblue.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 7
·2257-2264
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IF 6.177
Fei Zhang,Chunzheng Wu,Shuibo Wang,Shiwei Wang,Tong Li,Laixi Zou,Hongbo Yu,Hongfeng Yin
Although supported Rh nanoparticles (NPs) are one of the best catalysts for the selective hydrogenation of phenol to cyclohexanol, they still suffer from poor selectivity problems. In this study, we promoted the selectivity of Rh NPs with CoOx through an in situ transformation of the bimetallic RhCo NPs on SiO2. Among the obtained Rh–CoOx/SiO2 catalysts, the one with a Co/Rh molar ratio of 1/3 exhibited the highest phenol conversion (i.e., 98.1%) and the highest selectivity to cyclohexanol (i.e., 99.4%). Our study showed that CoOx promoters modified the electronic states of Rh and created new active sites at their interface, which are beneficial to the activation of phenol and the desorption of cyclohexanol. Excessive coverage of Rh by CoOx, however, would cause deactivation due to the less exposure of the Rh–CoOx interface.
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Green Energy & Environment
·
2022
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IF 12.781
Qi Zhao,Christian Marcus Pedersen,Jiamin Wang,Rui Liu,Yuanli Zhang,Xiuyin Yan,Zhenzhou Zhang,Xianglin Hou,Yingxiong Wang
The component analysis and structure characterization of complex mixtures of biomass conversion remain a challenging work. Hence, developing effective and easy to use techniques is necessary. Diffusion-ordered NMR spectroscopy (DOSY) is a non-selective and non-invasive method capable of achieving pseudo-separation and structure assignments of individual compounds from biomass mixtures by providing diffusion coefficients ( D ) of the components. However, the conventional 1 H DOSY NMR is limited by crowded resonances when analyzing complex mixtures containing similar chemical structure resulting in similar coefficient. Herein we describe the application of an advanced diffusion NMR method, Pure Shift Yielded by CHirp Excitation DOSY (PSYCHE-iDOSY), which can record high-resolution signal diffusion spectra efficiently separating compounds in model and genuine mixture samples from cellulose, hemicellulose and lignin. Complicated sets of isomers ( d -glucose/ d -fructose/ d -mannose and 1,2-/1,5-pentadiol), homologous compounds (ethylene glycol and 1,2-propylene glycol), model compounds of lignin, and a genuine reaction system (furfuryl alcohol hydrogenolysis with ring opening) were successfully separated in the diffusion dimension. The results show that the ultrahigh-resolution DOSY technique is capable of detecting and pseudo-separating the mixture components of C 5 /C 6 sugar conversion products and its derivative hydrogenation/hydrogenolysis from lignocellulose biomass.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yunning Chen,Lu Yang,Yingnan Sun,Renquan Guan,Di Liu,Jie Zhao,Qingkun Shang
A CDs@Cu-HQCA/TiO 2 flower composite photocatalyst (CDs: carbon dots, HQCA : 8-hydroxyquinoline-5-carboxylic acid) was constructed by exploiting the synergy of complex-sensitization, TiO 2 -morphology control, and carbon dot-surface modification. The photocatalytic degradation of phenol, norfloxacin, tetrabromobisphenol A and Cr (VI) by Cu-HQCA/TiO 2 particle, tube, diamond and flower-like show that the Cu-HQCA complex effectively extends the visible light absorption range of composite photocatalysts, and the flower morphology of TiO 2 not only improves the adsorption of pollutants but also enhances the photoelectric response of the composite photocatalyst. In this manner, a CDs@Cu-HQCA/TiO 2 flower catalyst that demonstrates excellent performance for the removal of dexamethasone, which does not degrade well naturally, was prepared, which delivered a rate of degradation of 99.4% and a degree of mineralization of 77.4% for dexamethasone. Possible degradation sites and dexamethasone degradation products were studied by combining computational chemistry with high-resolution mass spectrometry, and a possible mechanism for photogenerated carrier transmission and separation in the CDs@Cu-HQCA/TiO 2 flowers is proposed.
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