WATER RESEARCH
·
2022
·
IF 13.4
Wenxiao Zheng,Yingkai Chen,Hengyi Fu,Zhang Yan,Zhenchao Lei,Weijian Duan,Chunhua Feng
The generation of chlorinated byproducts during the electrochemical oxidation (EO) of Cl − -laden wastewater is a significant concern. We aim to propose a concept of converting reactive species (e.g., reactive chlorines and HO • resulting from electrolysis) into 1 O 2 via the addition of H 2 O 2 , which substantially alleviates chlorinated organic formation. When phenol was used as a model organic compound, the results showed that the H 2 O 2 -involving EO system outperformed the H 2 O 2 -absent system in terms of higher rate constants (5.95 × 10 −2 min −1 vs. 2.97 × 10 −2 min −1 ) and a much lower accumulation of total organic chlorinated products (1.42 mg L −1 vs. 8.18 mg L −1 ) during a 60 min operation. The rate constants of disappearance of a variety of phenolic compounds were positively correlated with the Hammett constants ( σ ), suggesting that the reactive species preferred oxidizing phenols with electron-rich groups. After the identification of 1 O 2 that was abundant in the bulk solution with the use of electron paramagnetic resonance and computational kinetic simulation, the routes of 1 O 2 generation were revealed. Despite the consensus as to the contribution of reaction between H 2 O 2 and ClO − to 1 O 2 formation, we conclude that the predominant pathway is through H 2 O 2 reaction with electrogenerated HO • or chlorine radicals (Cl • and Cl 2 • − ) to produce O 2 • − , followed by self-combination. Density functional theory calculations theoretically showed the difficulty in forming chlorinated byproducts for the 1 O 2 -initiated phenol oxidation in the presence of Cl − , which, by contrast, easily occurred for the Cl • -or HO • -initiated phenol reaction. The experiments run with real coking wastewater containing high-concentration phenols further demonstrated the superiority of the H 2 O 2 -involving EO system. The findings imply that this unique method for treating Cl − -laden organic wastewater is expected to be widely adopted for generalizing EO technology for environmental applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Defu Yin,Renjie Ji,Fanglin Lv,Long Jiang,Jingyun Zhang,Mingya Liu,Zhen Jia,Shitao Yu,Ruiyang Zhao,Yue Liu
Efficient catalysts are still the key to practical industrial applications. In this work, Pd-based catalyst was modified by doping metal Co to obtain Pd-Co@mSiO 2 bimetallic core–shell catalyst. The modified bimetallic core–shell catalyst was used in the hydrogenation of phenol, and the catalytic results showed that the Co modification effectively improved the catalytic performance of the Pd-based catalyst, especially, it reduced the activation energy of the reaction and greatly improve the conversion of phenol. Combined with characterization, it was found that Co doping reduced the particle size of Pd metal particles and affected the adsorption capacity of substrate phenol on the surface of Pd metal. The conversion of phenol was close to 99.9 % within 1 h at 80 °C, while the selectivity of cyclohexanone reached 95.4 %. In addition, the core–shell structure provided a stable environment for the catalyst, which still maintained high activity after being recycled for 5 times.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Weibin Cai,Haihan Wang,Q. Gary Yang,Tiankun Liu,Yujun Wang
Methyl isobutyl ketone (MIBK) and diisopropyl ether (DIPE) are two commonly used extractants in industry, but their efficiency in extracting phenols , especially polyhydroxyphenols, is low. In the work, a highly-efficient extractant was proposed to extract phenolic compounds, including polyhydroxyphenols. The interactions between three extractants, cyclohexanone (CYC), MIBK and DIPE, and phenols were analyzed by the COSMO-RS method and CYC shows stronger interactions with phenols than MIBK and DIPE. The results of Fourier-transform infrared spectroscopy (FTIR) show that strong hydrogen bonds are formed between CYC and phenolic compounds, in agreement with the results of the COSMO-RS method. The effects of concentration, temperature and pH values on the extractant performance were studied. Results showed that the performance of CYC is the best, followed by MIBK and DIPE, whose performance is the worst. As CYC was used as the extractant, the distribution coefficients of the three phenolic compounds, phenol, resorcinol and phloroglucinol, are 96.7, 47.8, 13.0, respectively. These values are 35%, 263%, and 160% larger than those of phenol, resorcinol and phloroglucinol, respectively, corresponding to MIBK. CYC is a highly-efficient extractant for the extraction of phenolic compounds, including polyhydroxyphenol.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Yuchen Zhang,Peng Zhou,Rongfu Huang,Chenying Zhou,Yang Liu,Heng Zhang,Xiaowei Huo,Jian Zhao,Zhaokun Xiong,Bo Lai
The regeneration of Fe(II) is the rate-limiting step in the Fenton/Fenton-like chain reactions that seriously hinder their scientific progress towards practical application. In this study, we proposed iron boride (FeB) for the first time as a new material to sustainably decompose H 2 O 2 to generate hydroxyl radicals , which can non-selectively degrade a wide array of refractory organic pollutants . Fe(II) can be steadily released by the stepwise oxidation of FeB to stimulate Fenton reaction, meanwhile, B-B bonds as electron donors on the surface of FeB effectively promote the regeneration of Fe(II) from Fe(III) species and significantly accelerate the production of hydroxyl radicals. The low generation of toxic by-products and the high utilization rate of iron species validly avoid the secondary organic/metal pollution in the FeB/H 2 O 2 system. Therefore, FeB mediated Fenton oxidation provides a novel strategy to realize a green and long-lasting environmental remediation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2022
·
IF 9.231
Jiannan Chen,Xiuhua Xia,Peizhen Li,Hang Yu,Yunfei Xie,Yahui Guo,Weirong Yao,He Qian,Yuliang Cheng
Natural N and S co-doped carbon dots (NSCDs) were synthesized via hydrothermal synthesis using food-derived crawfish shells as green precursors. The relationship between quantum yield (QY) and protein content of six crawfish shells treated with different alkalis was investigated. The synthesized NSCDs displayed a large QY of 18.57 %, which was higher than most of the chitin-derived CDs. Due to the oxidation of hydroxyl radicals, adding H 2 O 2 and horseradish peroxidase (HRP) quenched the fluorescence of NSCDs, resulting in a detection limit (LOD) of 1.25 μM for H 2 O 2 . The addition of pentachlorophenol (PCP) was supposed to consume part of the hydroxyl radicals and protect NSCDs from being oxidized. Accordingly, a facile and rapid “off–on” fluorescence sensor was developed to detect PCP with a LOD of 2.30 μM. Further, the method described was successfully used to detect PCP in three real samples.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2022
·Vol. 7
·期 40
·e202203035
·
IF 2.307
Yuxiu Fu,Yaming Pang,Yinan Zheng,Xiaoli Song,Liguo Gao
Graphical Photocatalysts enhance the ability to absorb low-energy photons due to the reduction of the band gap. Through the photocatalytic mechanism, it is known that when there is irradiation with light (hv) energy entering Mg 2+ -Mo 6+ -Al 3+ -MoO 4 2− -Layered double hydroxides (LDHs), highly active hole-electron pairs will be generated, and a large amount of ⋅OH will be generated after the reaction, which can completely oxidize the phenol in water into CO 2 and H 2 O. Mg 2+ -Mo 6+ -Al 3+ -MoO 4 2− -Layered double hydroxides (LDHs) materials were successfully prepared via a hydrothermal method by doping Mo 6+ in hydroxide laminates and inserting MoO 4 2− to replace the interlayer anions of LDHs materials. The samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscope (TEM), Fourier transform infrared spectrometer (FTIRS) and ultraviolet-visible spectrophotometer (UV). The electronic density of states was calculated using the density functional theory (DFT) of Vienna Ab-initio Simulation Package (VASP). The effects of Mo 6+ and MoO 4 2− on the structure, morphology, electronic structure and photocatalytic performance of Mg 2+ -Al 3+ -LDHs were systematically studied. The conditions for phenol degradation by Mg 2+ -Mo 6+ -Al 3+ -MoO 4 2− -LDHs were optimized by single factor analysis and response surface methodology. The results show that the MoO 4 2− anion reduces the band gap width and thus enhances the absorption of low-energy photons. The interaction between cations and anions enhances the photocatalytic performance. When the dosage of Mg 2+ -Mo 6+ -Al 3+ -MoO 4 2− -LDHs was 0.03 g, the temperature was 40 °C and the visible light irradiation was 15 min, the removal rate of phenol reached 94.76 %.
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2022
·Vol. 14
·期 21
·4682
·
IF 4.967
Xianxing Meng,Likun Wang,Hongwei Wang,Fang Zhang,Taying Su,Kunmu Cheng
Sulfonated phenol–formaldehyde (SPF) resin used as a cross-linker for petroleum reservoir conformance control was synthesized under alkaline conditions. The reaction process of SPF resin was evaluated by measuring the solution’s viscosity with respect to phenol–formaldehyde (PF) resin. The molecular structure of SPF resin was characterized by both FTIR and HPLC–MS/MS. The influence of the formaldehyde/phenol molar ratio (F/P) and the sodium formaldehyde sulfoxylate/phenol molar ratio (S/P) on the properties of SPF were analyzed in terms of the storage time, coagulation value, molecular size, and zeta potential. The results indicate that the presence of formaldehyde sodium bisulfite could slow down condensation reaction. Phenol rings were connected by methylene bridges in the position of o–p, and sulfonated SPF resin molecules all had one sulfonate group on the oligomer structure. The storage time decreased from 87 to 6 days, and the zeta potential decreased from −3.02 to −7.70 mV with the increase in F/P (1.2–2.0). Meanwhile, the sedimentation value and the diameter increased from 3.291 × 104to 5.045 × 104mg/L and from 2.7 to 5.3 nm, respectively. Sulfonation could significantly increase the storage time and dispersion stability. With the increase in S/P (0.1–0.35), the storage time increased from 15 to 86 days, the sedimentation value increased from 1.927 × 104to 5.269 × 104mg/L, and the diameter decreased from 6.3 to 3.0 nm. This paper can present new ideas for improving the storage stability and salt tolerance of phenol–formaldehyde resin and further improving the range of its applications, which has essential reference significance.Keywords:phenol–formaldehyde resin;sulfonation;characterization;HPLC–MS/MS
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 26
·7647-7658
·
IF 4.478
Xu Wei,Zhang Jin,Ding Houwen,Ding Yueting,Zou Xue,Yang Min,Zhou Qiang,Liu Zhou,Zheng Ling,Zuo Heping,Ge Dianlong,Zhang Qiangling,Huang Chaoqun,Shen Chengyin,Chu Yannan
Exhaled volatile organic compounds (VOCs) have been widely applied for the study of disease biomarkers. Oral exhalation and nasal exhalation are two of the most common sampling methods. However, VOCs released from food residues and bacteria in the mouth or upper respiratory tract were also sampled and usually mistaken as that produced from body metabolism. In this study, exhalation from deep airway was first directly collected through intubation sampling and analyzed. The exhalation samples of 35 subjects were collected through a catheter, which was inserted into the trachea or bronchus through the mouth and upper respiratory tract. Then, the VOCs in these samples were detected by proton transfer reaction mass spectrometry (PTR-MS). In addition, fast gas chromatography proton transfer reaction mass spectrometry (FGC-PTR-MS) was used to further determine the VOCs with the same mass-to-charge ratios. The results showed that there was methanol, acetonitrile, ethanol, methyl mercaptan, acetone, isoprene, and phenol in the deep airway. Compared with that in oral exhalation, ethanol, methyl mercaptan, and phenol had lower concentrations. In detail, the median concentrations of ethanol, methyl mercaptan, and phenol were 7.3, 0.6, and 23.9 ppbv, while those in the oral exhalation were 80.0, 5.1, and 71.3 ppbv, respectively, which meant the three VOCs mainly originated from the food residues and bacteria in the mouth or upper respiratory tract, rather than body metabolism. The research results in our study can provide references for expiratory VOC research based on oral and nasal exhalation samplings, which are more feasible in clinical practice. Graphical abstract
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL PHYSICS LETTERS
·
2022
·
IF 2.719
Xiaoli Song,Yuxiu Fu,Yaming Pang,Liguo Gao
La and Zn species were used to modify HZSM-5 zeolite, which was used to treat phenol in wastewater. Through the combination of multiple direct tools, La and Zn species were successfully loaded into the HZSM-5 zeolite. La-Zn/HZSM-5 zeolite has a small band gap and the catalyst can produce highly active electrons and electron holes when energy enters. The HZSM-5 zeolite after modification improves activity and stability of the catalyst. Therefore, it has a significant effect in the phenol removal experiment. Adding 1.2 mL of hydrogen peroxide and 0.11 g of catalyst, the removal rate can reach 99.38 % after being irradiation with a mercury lamp at 60 °C for 180 min. La-Zn/HZSM-5 zeolite has great potential in the application of photocatalytic degradation of phenol.
✓ 已验证
产品关联
DOI
高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 15
·2586
·
IF 5.719
Diyong Tang,Li Lu,Zhipeng Luo,Baokun Yang,Jun Ke,Weidong Lei,Hongran Zhen,Yuan Zhuang,Jie Sun,Ke Chen,Jie Sun
Biochars are considered as promising materials in energy storage and environmental remediation because of their unique physicochemical properties and low cost. However, the fabrication of multifunctional biochar materials with a well-developed hierarchical porous structure as well as self-doped functionalities via a facile strategy remains a challenge. Herein, we demonstrate a heteroatom-doped porous biochar, prepared by a hydrothermal pretreatment followed by a molten salt activation route. With the creation of a high specific surface area (1501.9 m2/g), a hierarchical porous structure, and the incorporation of oxygen-/nitrogen-functional groups, the as-prepared biochar (BC-24) exhibits great potential for supercapacitor application and organic pollutant elimination. The assembled biochar electrode delivers a specific capacitance of 378 F/g at 0.2 A/g with a good rate capability of 198 F/g at 10 A/g, and excellent cycling stability with 94.5% capacitance retention after 10,000 recycles. Moreover, BC-24 also exhibits superior catalytic activity for phenol degradation through peroxydisulfate (PDS) activation. The phenol (0.2 mM) can be effectively absorbed and then completely degraded within only 25 min over a wide pH range with low catalyst and PDS dosages. More importantly, TOC analysis indicates 81.7% of the phenol is mineralized within 60 min, confirming the effectiveness of the BC-24/PDS system. Quenching experiments and EPR measurements reveal that SO4·−and ·OH as well as1O2are involved in the phenol degradation, while the non-radical pathway plays the dominant role. This study provides valuable insights into the preparation of cost-effective carbon materials for supercapacitor application and organic contaminant remediation.Keywords:biochar;supercapacitor;organic pollutant;peroxydisulfate;free radicals;non-radical pathway
✓ 已验证
产品关联
DOI
PubMed
高影响因子
POLYMER
·
2022
·
IF 4.432
Zhen Wang,Shu Feng Zhou,Yi Zhi Zhuo,Ao Nan Lai,You Zhong Lu,Xiao Bin Wu
Current anion exchange membranes (AEMs) for fuel cells suffer from low ionic conductivity and poor mechanical property. Herein, we introduce adamantane groups onto the block poly(arylene ether sulfone)s backbone to form the selected comb-shaped structure. The structure-property relationships of the AEMs are investigated by varying the ratio of the hydrophobic to hydrophilic segments. The bulk rigid adamantane group can restrain the swelling of the AEMs thus enhancing the mechanical properties and expand the spacing between the hydrophilic/hydrophobic segments of the polymer chains to promote the formation of microphase separation morphology. Consequently, as characterized by atomic force microscope (AFM) and transmission electron microscopy (TEM), the resulting membranes show well-defined microphase separation between the hydrophilic/hydrophobic segments, resulting in high ionic conductivity range from 27.4 to 90.2 mS cm −1 over a temperature range of 30–80 °C. At the same time, the membranes present ultralow swelling ratio with the levels from 1.6% to 6.1% at 30 °C and from 6.8% to 12.7% at 80 °C, respectively, and thus excellent mechanical properties with the tensile strength as high as 11.52 MPa and elongation at break of 29.28%. The excellent comprehensive properties grant the prepared AEMs bright future for fuel cells.
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Longfei Lei,Yuanyuan Liu,Fengxia Tong,Guangyao Zhai,Honggang Zhang,Caiyun Zhang,Zeyan Wang,Peng Wang,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang
In this work, a Bi-based metal–organic framework (MOF; Bi-MMTAA) with 2-mercapto-4-methyl-5-thiazoleacetic acid (MMTAA) as the organic ligand is synthesized. The crystal structure of Bi-MMTAA was determined by single-crystal X-ray diffraction. Theoretical calculations reveal that Bi-MMTAA is a p-type semiconductor, and electrons can delocalize through the π-conjugation when excited by a photon with an energy higher than the Bi-MMTAA band gap, which is beneficial to charge separation and transfer. The photoelectrical properties suggest that free electrons can be produced over Bi-MMTAA under light irradiation. The photocatalytic results suggest that Bi-MMTAA can decolorize rhodamine B (RhB) and oxidize phenylboronic acid to phenol under visible light (λ > 420 nm), with superoxide radicals being the main reactive oxygen species. Our results enrich the family of Bi-based MOFs and may inspire further exploration of Bi-based MOFs, including both synthesis and potential applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）