JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Tong Liu,Yang Liu,Peng Zhou,Zhaokun Xiong,Heng Zhang,Chuanshu He,Ye Du,Gang Yao,Bo Lai
As one of the most promising advanced oxidation processes , the activation of S(IV) by iron-based materials to produce SO 4 •− has become a hot technology for the degradation of organic pollutants . However, the mechanism of radical chain reactions has not been clearly explored. Herein, we established a novel AOP system based on the combination of zero-valent iron (ZVI) and potassium pyrosulfite (PPS). Combined with the degradation trends of CBZ and the change of DO concentration, the system was proposed to be divided into a slow initiation stage in 5 min and a rapid degradation stage in 5 − 10 min. Through a series of quenching experiments, electron paramagnetic resonance tests and several probe experiments, the mechanisms of two radical chain reactions were proposed between ZVI and PPS: the first one produced O 2 •− and HO • , and the other produced SO 3 •− , SO 5 •− , SO 4 •− and HO • . The two-stage reaction and two radical production paths of the ZVI/PPS system were proposed for the first time, which provided theoretical guidance for the practical application of the ZVI/PPS system. The ZVI/PPS system has been found to have excellent environmental adaptability in the treatment of industrial wastewater .
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高影响因子
COMPOSITES PART B-ENGINEERING
·
2022
·
IF 11.322
Fucheng Wang,Jinfeng Zhang,Kaixin Sun,Liwei Quan,Jing Wang,Naiqin Zhao,Chunsheng Shi,Shijian Zheng
Interfacial bonding is an important factor affecting the mechanical properties of composites. The interface between the in-situ synthesized ceramic phase and the metal matrix is considered ideal, so little attention is paid to the interfacial modification. In this work, we found that interfacial segregation affects the growth of the MgAlB 4 whisker and the interface of reinforcement and matrix in the composites. Systematic experiments and theoretical calculations indicate Fe solute prefer to segregate at the MgAlB 4 - { 10 1 ‾ 0 } /Al interfaces in in-situ synthesized MgAlB 4 /Al composites, which is helpful to reduce system free energy. On the one hand, Fe segregation induces the whisker coarsening and the formation of planar defects with a sandwich structure formed by a layer of Fe atoms and two layers of Al atoms in coarse-whiskers, on the other hand, it improves the interfacial strength . Although extra Fe aggravates the whisker coarsening, the synergistic reinforcing effect of the whiskers and the extra Fe is greater than the sum of their individual reinforcing effects. This work demonstrates that interfacial segregation can be used to modulate the size of reinforcements and improve interfacial strength.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Jingdong Yang,Yu Li,Zequn Yang,Kaimin Shih,Guang-Guo Ying,Yong Feng
The presence of 1,4-dioxane in various water streams poses a threat to the health of human beings. In this study, the oxidative combination of ozone with peroxymonosulfate (PMS) was for the first time used to remove 1,4-dioxane from water. Near complete abatement of 1,4-dioxane was achieved by ozone-PMS after reaction of only 15 min and the degradation kinetics was found to be positively correlated with doses of PMS and ozone. Ozone-PMS oxidation had the optimum performance at slight base pH values. Both sulfate radicals and hydroxyl radicals were generated in ozone-PMS oxidation and these radicals resulted in the degradation of 1,4-dioxane. The effects of common water constituents and real water matrices were investigated. It was found that bicarbonate ions with a concentration up to 10 mM had a slight promoting effect, while either chloride ions or natural organic matter inhibited only slightly the degradation. Meanwhile, no obvious difference in the degradation of 1,4-dioxane was found among the real water matrices and deionized water , which demonstrates that ozone-PMS oxidation has high tolerance and stability. The results from this study demonstrate that ozone-PMS may be a promising technology for the removal of 1,4-dioxane from various water matrices.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yujiao Wen,Meng Liu,Shikai Li,Lezhu Su,Yifan Wang,Zhi Zhou,Nan Zhou,Ruilian Li
Antibiotics accumulated in ecosystem can easily enter the agricultural cycle with irrigation water, which brings a huge potential threat to food security. Transition metals are widely utilized in advanced oxidation processes to degrade pollutants, but the poor stability has significantly impeded their application in irrigation water. To solve these problems, the harmless tetrasodium iminodisuccinate is selected to pyrolysis with ferrite and cobalt resources to obtain a composite heterogeneous catalyst composed of porous carbon and Co 3 Fe 7 , CoFe 2 O 4 (IDC@Co 3 Fe 7 /CFO). The catalyst exhibits excellent catalytic performance in peroxydisulfate (PDS) activation and shows a high removal efficiency of sulfamethazine up to 100%. The ESR analysis proves SO 4 • − , •OH and •O 2 – are the main active substances, and sulfamethazine can be gradually degraded until mineralization. More importantly, with the formation of Metal-Metal/Metal-Oxygen bonds and the protection of the IDS derived carbon, the dispersion and stability of the metal can be greatly promoted. The composite can maintain the rate of degrading sulfamethazine above 93.44% after 10 times catalytic reactions , with extremely low detection of Fe or Co leaching. This study not only give a super-stable material for the removal of antibiotics in irrigation water, but also provides a novel stratagem for obtaining stable catalytic structures.
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高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Si-Jia Guan,Peng Zhang,Shen-Jing Ji,Yu Cao,Nian-Tzu Suen
It is well known that the “iron” impurity will influence the oxygen evolution reaction (OER) in an alkaline electrolyte, especially for the Ni-based electrocatalyst. Many research studies have investigated the function of Fe in the OER active phase, such as M(OH)2/MOOH (M = Ni and/or Fe), while, surprisingly, very few studies have examined the function of Fe in the “precatalyst” system. Accordingly, in this work, the Ni3–xFexP (x = 0, 0.5, 1) series as an Ni-based precatalyst was employed to inspect the function of internal and external Fe in the Ni-based precatalyst system. It was realized that the sample with internal Fe (i.e., Ni2.5Fe0.5P and Ni2FeP) exhibits efficient OER activity compared to that of the Fe-free one (i.e., Ni3P) owing to the large amount of active M(OH)2/MOOH formed on the surface. This indicates that the internal Fe in the present system may have the ability to facilitate the phase transformation; it was later rationalized from electronic structural calculations that the d band center of the internal Fe (middle transition metal) and Ni (late transition metal) holds the key for this observation. Adding excessive ferrous chloride tetrahydrate (FeCl2·4H2O) as the external Fe in the electrolyte will greatly improve the OER performances for Ni3P; nevertheless, that the OER activity of Ni2FeP is still much superior than that of Ni3P corroborates the fact that the Fe impurity is not the only reason for the elevated OER activity of Ni2FeP and that internal Fe is also critical to the phase transformation as well as OER performance.
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高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Long Li,Yuhao He,Heyun Fu,Xiaolei Qu,Zhaoyi Xu
Nanoscale zero-valent iron (nZVI) has drawn great interest in the remediation of contaminated waters . In this study, we prepared a novel and stable nZVI embedded in N-doped carbon matrix (nZVI@MOF-CN) using a facile direct carbonization method, in which an iron-containing metal-organic framework (MOF) served as both the iron and carbon sources, and melamine as the nitrogen source. The nZVI@MOF-CN composites were used in the removal of bromate in water, which could be effectively reduced by the surface electrons transferred from nZVI to the carbon encapsulation layer due to the Schottky-Mott effect. Doped nitrogen significantly facilitated the reduction of bromate by nZVI, because it enhanced the nZVI dispersion and bromate adsorption, and modulated the carbon matrix conductivity. The bromate reduction activity of nZVI@MOF-CN was more than 50 times higher that of its un-doped counterpart and a commercial nZVI. Moreover, owing to the protection of carbon encapsulation layer, nZVI@MOF-CN exhibited good stability and reusability. The leached concentration of iron ions of nZVI@MOF-CN was less than 5% of the commercial nZVI under the same reaction conditions. Commercial nZVI almost completely lost its bromate reduction activity after use (3% reduction efficiency in the examined time frame), while nZVI@MOF-CN maintained a reduction efficiency of 61%. The nZVI@MOF-CN could be effectively regenerated by hydrogenation reduction. After five reaction-regeneration cycles, nZVI@MOF-CN still achieved a bromate reduction efficiency of approximately 80%. These results suggest that MOF-derived nZVI materials are highly reactive and stable for the reductive removal of pollutants in water.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jie Ye,Yue Lai,Chao Wang,Raymond Jianxiong Zeng,Changgeng Liu,Hao Lin,Shungui Zhou,Zhen He
Sulfate radical ( SO 4 · - )-based advanced oxidation processes (SR-AOPs) are promising for sludge dewatering. In this work, an electrochemically driven Fe 0 -activated sulfite system (E/Fe/sulfite) was developed and demonstrated for sustainably releasing Fe 2+ to activate sulfite for dewatering waste activated sludge. Under the optimal conditions (sulfite dosage = 40 mg/g dry solids, current density = 30 mA/cm 2 , pH = 6, and time = 60 min), the reduction of capillary suction time and water content of sludge cake were 87.9 ± 2.8 % and 73.1 ± 0.8 %, respectively. The improved dewatering performance was attributed to the degradation of tightly-bound extracellular polymeric substances, along with the decreased live/dead cell ratio and the increased permeability of sludge flocs. The thermal effect (∼21–59 °C) in the E/Fe/sulfite system accelerated the release of intracellular proteins, which could be effectively degraded by the strong oxidizing SO 4 · - . The results also suggested that electrochemical oxidation and thermal effect in the E/Fe/sulfite system had a synergistic impact on improving sludge dewaterability. According to the density functional theory calculation, the hydrophobic amino acids produced from protein degradation were favorable for forming the drainage channels and enhancing sludge dewaterability. This study provides new insights for understanding the SR-AOPs and their applications to sludge treatment.
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高影响因子
WATER RESEARCH
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2022
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IF 13.4
Meng-Fan He,Wen-Qiang Li,Zhi-Hui Xie,Shu-Run Yang,Chuan-Shu He,Zhao-Kun Xiong,Ye Du,Yang Liu,Feng Jiang,Yang Mu,Bo Lai
In this study, mechanically sulfidated microscale zero valent iron (S-ZVI) was found to effectively activate the peracetic acid (PAA) with a result of almost complete degradation of six micropollutants within 10 min under neutral conditions, and > 95% sulfamethoxazole (SMX) removal after six cycles. Reactive oxidized species (ROS) including HO•, carbon-centered radicals, and Fe(IV) were generated in the S-ZVI/PAA system, while HO• was the main contributor towards micropollutants degradation. This study clearly revealed that enhancement of the electron donating ability of ZVI by the formed conductive iron sulfides was crucial for promoted Fe(II) generation and subsequent PAA activation over several cycles, rather than the ability of sulfides to reduce Fe(III) for Fe(II) regeneration as reported previously. Interestingly, it's discovered that co-existence of Fe(III) would dramatically improve the contaminants removal efficiency of the S-ZVI/PAA system; transform the surfaced Fe(II) dominated ROS generation process to aqueous Fe(II) one; enhance the tolerance of the proposed system to water matrix. The promoting effect of predosed Fe(III) on PAA activation by S-ZVI should be mainly associated with: the greater ability of Fe(III) than H 2 O to accept electron from Fe 0 for obtaining more active sites; slower Fe 0 consumption and solid sulfur species release for elevated electron utilization efficiency and PAA activation. Considering the convenient and cost-effective access of Fe(III), the decrease of acute toxicity of treated SMX, excellent stability and good removal of various micropollutants fully demonstrate the superiority of S-ZVI/PAA system for practical application.
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高影响因子
Metals
·
2022
·Vol. 12
·期 6
·1019
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IF 2.695
Shushi Zhang,Peng Hu,Jiating Rao,Zhenyang Wang,Yanbing Zong,Jianliang Zhang
HIsmelt is well suited for smelting vanadium–titanium magnetite due to its flexibility in feedstock selection and tolerance to high viscosity slag, compared with the blast furnace. In this work, the effect of smelting time on the distribution behavior and recovery rates of vanadium and titanium in HIsmelt smelting of vanadium–titanium magnetite was investigated by experiment for the first time. The relationship between slag viscosity and temperature at different smelting times was further revealed by thermodynamic calculations. The experimental results show that extending the smelting time increases the FeO content in the slag, theLVrose from 0.66 to 5.02, theLTideclined from 206.90 to 114.86, the shorter smelting time is favorable for increasing the recovery ratio of vanadium and titanium in metal and slag. In addition, slag viscosity decreases with increasing smelting time. The precipitation of high melting point titania spinel and CaTiO3phases is responsible for the significant increase in slag viscosity at 1300 °C.Keywords:HIsmelt;vanadium titano–magnetite;distribution behavior;recovery;viscosity
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Ke Lei,Jiaming Bao,Xiangyu Zhao,Hao Wang,Deqiu Zou
Due to the advantages of high thermal conductivity, high heat storage density per unit volume and large specific surface area, metal-based microencapsulated phase change material (MEPCM) has a broad application prospect in the field of medium/high-temperature heat storage. However, the problems of thermal expansion and large supercooling seriously restrict its development and application. Our previous research work showed that “double-layer coating, sacrificial inner layer” method can successfully solve the thermal expansion problem of metal-based MEPCM. Based on this method, we aim to further investigate the supercooling suppression of metal-based MEPCM by loading nanoparticles into the core material skillfully when sacrificing the inner layer. Phase change properties of three kinds of MEPCM loaded with different nanoparticles (nano-BN, nano-diamond, and nano-Fe) with the same concentration were compared. It was found that the supercooling suppression effect of nano-Fe was the best. Furthermore, supercooling suppression effect of nano-Fe with different concentrations was compared. The results demonstrated that nano-Fe with a concentration of 0.9% showed the best supercooling suppression effect. In addition, supercooling suppression effect of different particle sizes was compared. The results showed that the supercooling degree of MEPCM decreased by 41.5% and 5.6% when nano-Fe with a particle size of 50 nm and 100 nm was loaded, respectively, indicating that nano-Fe with the particle size of 50 nm is more effective than that of 100 nm. Finally, supercooling suppression effect of different coating methods was compared. The results showed that the supercooling suppression effect of “double-layer coating, sacrificial inner-layer” is much better than that of single-layer coating.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Shiyao Li,Rong Cheng,Jiahao Li,Haobo Hou,Yi Wang,Jiaao Chen,Yuwei Xiang,Min Zhou
The efficient removal of hexavalent chromium from solution is a challenging task, in this paper, the nZVI and nitrogen co-doped magnetic carbon aerogel microsphere composites (nZVI@NCAs) were prepared via the microemulsion polymerization and subsequent carbonization process, and were expected to satisfactory performance in the removal of Cr(VI). From batch experiments, the Cr(VI) removal process by nZVI@NCA900 fitted better with the pseudo-second-order model. The optimal nZVI@NCA900 was superior to that of most magnetic carbon-substrate composites, displaying high Cr(VI) adsorption capacity of 266.79 mg·g −1 at 318 K. Additionally, it was found that Cr(VI) was reduced to the low-toxicity Cr(III) from the results analyzed by XPS, and nZVI@NCA900 exhibited Cr(VI) reduction performance of 33.92% Cr(VI) reduced to Cr(III). The reaction between the nZVI@NCAs and Cr(VI) was pH-dependence, endothermic and spontaneous. Removal mechanisms might involve multiple processes. The nZVI particles on the surface acted as reductants to reduce Cr(VI) to Cr(III) and form Cr(III)/Fe(III) hydroxides to precipitate on nZVI@NCAs. Simulation results by DFT prove that N is an active site and show positive effect in the adsorption system. N atoms were used as active sites to stabilize the interaction with Cr(VI) via adsorption attributed to electrostatic and act as electron donors for reduction of Cr(VI). The nZVI particles encapsulated by carbon aerogels could provide magnetic stability after acid reaction, which was beneficial to the separation of adsorbents after reaction and reuse for many cycles. These results provide a new view for developing magnetic carbon materials to remove Cr(VI) from contaminated water.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xin Liu,Peng Xu,Shiqi Xie,Lei Wang,Zhuoyu Yang,Pengfei Zhu,Jingwei Ma,Qiulai He,John C. Crittenden
Zero-valent copper particles (Cu 0 ) used to degrade pollutant due to its in-site generation and activation of hydrogen peroxide (H 2 O 2 ), while the disproportionation of Cu + limited the efficacy. In this study, spiking chloride ion (Cl − ) into zero-valent copper (Cu 0 ) system (Cl − /Cu 0 system) enhanced greatly acetaminophen degradation. The addition of Cl − not only reduced the dismutation reaction of Cu + , but also helped the comproportionation reaction of Cu 0 and Cu 2+ , leading to much generation of Cu + and H 2 O 2 . Hydroxyl radical ( OH) and reactive chlorine species were identified as the dominant reactive oxidants in the Cl − /Cu 0 system with its contribution ratio of degrading acetaminophen being respectively 73.4 % and 23.8 %. In the Cl − /Cu 0 system, Cu + was released by H + corrosion from Cu 0 , and then Cu + coupled with Cl − forming Cu-Cl complexes; Meanwhile, the reaction of O 2 and the species of Cu + (e. g. Cu-Cl complexes and Cu + ) produced H 2 O 2 and, then the species of Cu + catalyzed H 2 O 2 to form OH; Thereinto, partial OH was shifted by Cl − to reactive chlorine species. Except for fulvic acid , coexisting substrates such as sulphate, nitrate and phosphate ions had no obvious inhibition impact on oxidizing acetaminophen in the Cl − /Cu 0 system. Furthermore, the Cl − /Cu 0 system presented a good removal rate of acetaminophen in three actual water samples. Moreover, three kinds of dyes and painkillers was removed over 78 % in the Cl − /Cu 0 system. The residual total dissolved copper was under II-level of environmental quality standards for surface water in China by alkali precipitation and filtration after reaction. Therefore, the study provided a new idea to enhance Cu 0 for the purification of pollutants.
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