WATER RESEARCH
·
2023
·
IF 12.8
Bei Ye,Qian-Yuan Wu,Wen-Long Wang,Hong-Ying Hu
Pharmaceutical and personal care products (PPCPs) are frequently detected in water bodies and have potential risks to human health and the ecosystem. The degradation of eight structurally diverse PPCPs by ammonia/chlorine was systematically investigated in this study. Compared with chlorination, ammonia/chlorine markedly enhanced PPCP degradation, and the degradation efficiencies of most PPCPs were greater than 70%. Tert-butanol strongly suppressed PPCP degradation, while bicarbonate suppressed it moderately, suggesting the importance of ClO⋅and ⋅CO 3 − in PPCP degradation. In neutral conditions, PPCP degradation was mainly attributed to ⋅OH, with its contribution ranging from 74% to 100% at a Cl 2 /N molar ratio of 1.6. Regarding the effect of natural organic matter, atrazine and primidone were inhibited the most, while carbamazepine (CBZ), metoprolol (MTP), and atenolol (ATN) were affected the least. PPCP degradation was suppressed in reclaimed water; the degradation of CBZ, MTP, and ATN was suppressed the least, with degradation efficiencies of 77.1%–85.4%, 75.1%–77.1%, and 64.6%–68.8%, respectively. Furthermore, compared with chlorination, fewer volatile halogenated byproducts were formed in reclaimed water when using the ammonia/chlorine process, and the concentration of each byproduct formed by ammonia/chlorine was less than 10 µg/L. This study suggests the feasibility of using ammonia/chlorine oxidation to degrade PPCPs in reclaimed water.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Maolin Wang,Yaling Wang,Xudong Jing,Jiahui Xu,Min Li,Qing Xie,Xiyun Cai
Iron-activated persulfate (PS) systems commonly suffer from the poor Fe(III)/Fe(II) redox cycle in groundwater and soils, due to the rapid oxidation of Fe(II) by both PS-related and naturally occurring oxidative substances. Maintaining the Fe(III)/Fe(II) redox cycle is necessary to achieve the high efficiency and stability of iron-activated persulfate systems toward aromatic contaminants (e.g., PAHs) in groundwater and soils. Herein, we discover the mixtures of dithionite (DTN) and zerovalent iron (ZVI) to synergistically activate PS, and develop highly efficient, stable DTN-ZVI/PS systems for PAHs removal in groundwater and soils. DTN and intermediates sulfite/thiosulfate initiated reduction of ZVI-derived Fe(III) species in DTN-ZVI/PS systems. This reaction accelerated the Fe(III)/Fe(II) redox cycle and coated ZVI with FeS x , both favoring the generation of HO and SO 4 − . DTN-ZVI/PS exhibited Nap removal of >90% in water during 11 of 15 supplementations of Nap and/or PS, 1.4–2.4 times ZVI/PS. Similarly, 0.47–4.3 fold increments of Nap removal k obs were obtained in five chemical types of groundwater, and 1.3–2.4 fold increments of PAHs removal in soils. This study may provide a technical basis to develop new Fe-activated oxidation systems for groundwater and soil remediation .
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Materials Today Chemistry
·
2023
·
IF 7.3
W. He,M.M. Jiang,J.X. Yu,W. Yan,X.Y. Zhang,R. Jiang,H.F. Zhao,Y. Liu,F. Feng,Q.F. Zhang,C.S. Lu,X.N. Li
In recent years, novel carbon-layer encapsulation strategies have been emerging for the construction of heterogeneous catalysts. However, the mechanism action of thermos-catalytic systems is still unclear. The synergistic effect of metal particle size and carbon layer quantity on catalytic performance has not been reported. The strategy to control the carbon layer quantity and metal particle size is still a big challenge. Here, we proposed a novel idea to design catalysts connecting the performance and the structure via work function. The direct pyrolysis of organometallic coordination polymer is induced to control the carbon layer quantity and metal particle size of the carbon-encapsulated catalyst. The results show that the reduction in the nickel nanoparticle size and the carbon layer quantity were favorable for pumping electrons from the nickel core. There was a corresponding relationship between the work function of the catalyst and its selective hydrogenation performance of halogenated aromatic nitro compounds. With low carbon-halogen bond dissociation energy, a high work function decreased catalytic selectivity. Therefore, the work function can be served as a bridge connecting to the configurational relationship of catalysts.
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ChemSusChem
·
2023
·Vol. 16
·期 14
·e202300180
·
IF 8.4
Yinjian Zheng,Zhiyuan Wang,Peng Chen,Wenbiao Zhang,Qingsheng Gao
Graphical Roughness-dependence of Cu electrodes is for the first time identified in the electro-reductive coupling of nitro and carbonyl compounds. With increased roughness, the selectivity of nitrones decreases, while that of imines increases, thanks to the feasible control over the reduction of nitroarenes to hydroxylamines or amines on Cu I /Cu 0 interfaces. The electro-reductive coupling of nitro and carbonyl compounds enables a facile, environmentally friendly and energy benign transformation toward value-added nitrones or imines, but the selectivity is still challenging. Here, the surface roughness of Cu electrodes is introduced for the first time as the determinant to switch products from nitrones to imines owing to the controllable reduction of nitroarenes to hydroxylamines or amines on tailored Cu I /Cu 0 interfaces. The roughness-dependent selectivity, that is the decrease of nitrones and the increase of imines with enhanced roughness, is visible in the electro-reductive coupling of nitrobenzene and furfural. Thus, the high selectivity of nitrone (98 %) and imine (80 %) can be achieved on a surface smooth Cu foil and the one electrochemically roughened in the presence of I − , respectively. Such roughness-dependence of nitrone/imine selectivity on Cu electrodes is further verified in a wide substrate scope, highlighting the promise of surface/interfacial engineering for electrochemical synthesis.
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ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2023
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IF 3.4
Shichun Weng,Wei Feng,Wenqian Wu,Zichao Guo,Liping Chen,Wanghua Chen
Nitrophenols and corresponding sodium nitrophenolates are the main side products in the production of mononitrobenzene (MNB). These side products are hazardous due to their thermal instability nature. In this article, the thermal decomposition behaviors of nitrophenols and sodium nitrophenolates were first characterized by differential scanning calorimeter and accelerating rate calorimetry techniques. Then, the influence of phenol and sodium phenolate on the thermal decomposition of MNB was studied to clarify the effect of phenolic hydroxyl groups on the thermal stability of nitrophenols. It was found that compared to nitrophenols, the exothermic peaks of sodium nitrophenolates were more intense and presented strongly autocatalytic features. Sodium phenolate could significantly decrease the decomposition temperature of MNB. Aniline was detected as the unique product in the decomposition processes of pure MNB and MNB/sodium phenolate mixtures, and the nitrosobenzene was verified as the intermediate product. It was experimentally proven that sodium phenolate could catalyze the decomposition of nitrosobenzene (the decomposition intermediate of MNB). The violent decomposition of sodium nitrophenols was caused by the intermolecular catalysis effect of phenoxy groups.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yaling Wang,Maolin Wang,Qing Xie,Xiyun Cai
We report new activated persulfate systems with cyclodextrin (CD)-coated Fe 3 O 4 @Fe 0 nanoparticles (Fe 3 O 4 @Fe 0 -CD) that are characterized by both highly activating persulfates and rapidly accessing hydrophobic PAHs. Fe 3 O 4 @Fe 0 -β-CD displays chain-like structure of core–shell Fe 3 O 4 @Fe 0 nanoparticles coated with a CD layer (about 5.9 nm). CD coating stabilizes the polycrystalline structure of Fe 3 O 4 @Fe 0 nanoparticles and accelerates mass transfer of PAHs in water, thereby making Fe 3 O 4 @Fe 0 -β-CD intrinsically stable and reactive. Fe 3 O 4 @Fe 0 -β-CD/PS, featured by high yields of highly reactive Fe(IV), had about 30-fold rate constants of naphthalene (Nap) in water as much as Fe 3 O 4 @Fe 0 /PS. Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in water during 13 of total 18 supplementations of Nap and/or PS, whereas Fe 3 O 4 @Fe 0 /PS completely removed Nap only at the first supplementation of Nap. Likewise, Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in simulated groundwater, and degraded four PAHs in soils by >63%. This study may provide a technical basis for the developments of new PS activators to remove recalcitrant hydrophobic contaminants in water and soils.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Daoguang Teng,Peng Jin,Shiqiao Yang,Wenhuan Guo,Zhuang Zhao,Guoli Zhou,Peng Li,Yijun Cao
Various cost-effective polycyclic aromatic hydrocarbons (PAHs) were used to fabricate hyper-cross-linked polymers (HCLPs) via an external cross-linker knitting method (ECLKM) followed by N-source impregnation modification. Multiple characterization techniques and thorough tests confirmed that the resultant thermally stable materials featured large specific surface areas (up to 2870 m2 g–1), narrow pore distributions (<0.70 nm), and high pore volumes (up to 1.09 cm3/g). Effects of porosities and N-doping modification ways on HCLPs’ CO2 capture capacities have been fully studied via controlling experiments. Remarkably, HCLP 1 prepared using naphthalene without further modification possessed the highest CO2 uptake capacity (up to 3.8 mmol g–1), indicating that porosities dominated the CO2 uptake process of HCLPs compared with N-doping modification. This study offers a facile strategy to construct HCLPs with great CO2 capture performances using PAHs via a simple one-pot ECLKM.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Can Feng,Heng Zhang,Yi Ren,Mengfan Luo,Siying Yu,Zhaokun Xiong,Yang Liu,Peng Zhou,Bo Lai
Zerovalent iron (ZVI)-based Fenton-like processes have been widely applied in degrading organic contaminants . However, the surface oxyhydroxide passivation layer produced during the preparation and oxidation of ZVI hinders its dissolution and Fe(III)/Fe(II) cycling, and restricts the generation of reactive oxygen species (ROS). In this study, copper sulfide (CuS) was found to effectively enhance the degradation of diverse organic pollutants in the ZVI/H 2 O 2 system. Moreover, the degradation performance for the actual industrial wastewater (i.e., dinitrodiazophenol wastewater) in the ZVI/H 2 O 2 system was impressively improved by 41% with CuS addition, and the COD removal efficiency could reach 97% after 2 h of treatment. Mechanism investigation revealed that the introduction of CuS accelerated the sustainable supply of Fe(II) in the ZVI/H 2 O 2 system. Specifically, Cu(I) and reductive sulfur species (i.e., S 2– , S 2 2– , S n 2– and H 2 S (aq)) from CuS directly induced efficient Fe(III)/Fe(II) cycling. The iron-copper synergistic effect between Cu(II) from CuS and ZVI expedited Fe(II) generation from ZVI dissolution and Fe(III) reduction by formed Cu(I). This study not only elucidates the promotion effects of CuS on ZVI dissolution and Fe(III)/Fe(II) cycling in ZVI-based Fenton-like processes, but also provides a sustainable and high-efficiency iron-based oxidation system for removal of organic contaminants.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Lei Yang,Zifei Wei,Zihan Guo,Mengfang Chen,Jingchun Yan,Linbo Qian,Lu Han,Jing Li,Mingyue Gu
CoFe 2 O 4 /hydrochar composites (FeCo@HC) were synthesized via a facile one-step hydrothermal method and utilized to activate peroxymonosulfate (PMS) for simultaneous degradation of monochlorobenzene (MCB) and p-chloroaniline (PCA). Additionally, the effects of humic acid , Cl - , HCO 3 - , H 2 PO 4 -, HPO 4 2- and water matrices were investigated and degradation pathways of MCB and PCA were proposed. The removal efficiencies of MCB and PCA were higher in FeCo@HC140–10/PMS system obtained under hydrothermal temperature of 140 °C than FeCo@HC180–10/PMS and FeCo@HC220–10/PMS systems obtained under higher temperatures. Radical species (i.e., SO 4 • - , •OH) and nonradical pathways (i.e., 1 O 2 , Fe (IV)/Co (IV) and electron transfer through surface FeCo@HC140–10/PMS* complex) co-occurred in the FeCo@HC140–10/PMS system, while radical and nonradical pathways were dominant in degrading MCB and PCA respectively. The surface functional groups (i.e., C-OH and C O) and Fe/Co redox cycles played crucial roles in the PMS activation . MCB degradation was significantly inhibited in the mixed MCB/PCA solution over that in the single MCB solution, whereas PCA degradation was slightly promoted in the mixed MCB/PCA solution. These findings are significant for the provision of a low-cost and environmentally-benign synthesis of bimetal-hydrochar composites and more detailed understanding of the related mechanisms on PMS activation for simultaneous removal of the mixed contaminants in groundwater.
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WATER RESEARCH
·
2022
·
IF 13.4
Chaozhi Kuang,Guoshen Zeng,Yangjian Zhou,Yaoyao Wu,Dexuan Li,Yingfei Wang,Chuanhao Li
Conventional electrocatalytic degradation of pollutants involves either cathodic reduction or anodic oxidation process, which caused the low energy utilization efficiency. In this study, we successfully couple the anodic activation of sulfates with the cathodic H 2 O 2 production/activation to boost the generation of sulfate radical (SO 4 ·− ) and hydroxyl radical (·OH) for the efficient degradation of emerging contaminants. The electrocatalysis reactor is composed of a modified-graphite-felt (GF) cathode, in-situ prepared by the carbonization of polyaniline (PANI) electrodeposited on a GF substrate, and a boron-doped diamond (BDD) anode. In the presence of sulfates, the electrocatalysis system shows superior activities towards the degradation of pharmaceutical and personal care products (PPCPs), with the optimal performance of completely degrading the representative pollutant carbamazepine (CBZ, 0.2 mg L −1 ) within 150 s. Radicals quenching experiments indicated that ·OH and SO 4 ·− act as the main reactive oxygen species for CBZ decomposition. Results from the electron paramagnetic resonance (EPR) and chronoamperometry studies verified that the sulfate ions were oxidized to SO 4 ·− radicals at the anode, while the dissolve oxygen molecules were reduced to H 2 O 2 molecules which were further activated to produce ·OH radicals at the cathode. It was also found that during the catalytic reactions SO 4 ·− radicals could spontaneously convert into peroxydisulfate (PDS) which were subsequently reduced back to SO 4 ·− at the cathodes. The quasi-steady-state concentrations of ·OH and SO 4 ·− were estimated to be 0.51×10 −12 M and 0.56×10 −12 M, respectively. This study provides insight into the synergistic generation of ·OH/SO 4 ·− from the integrated electrochemical anode oxidation of sulfate and cathode reduction of dissolved oxygen, which indicates a potential practical approach to efficiently degrade the emerging organic water contaminants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Peizhen Yang,Yuhan Long,Wenli Huang,Dongfang Liu
Singlet oxygen ( 1 O 2 )-dominated advanced oxidation processes has drawn widespread attention for selective oxidation of organic pollutants in complex water environments. However, the high efficiency and selectivity of 1 O 2 generation remains challenging. Herein, we develop single-atom copper anchored on Ti 3 C 2 T x MXene nanosheets (Cu-SA/MXene) by molten salt etching for the generation of 1 O 2 via peroxymonosulfate (PMS) activation. Particularly, it exhibits a high selectivity of 99.71% toward 1 O 2 generation by activating PMS, which shows outstanding catalytic activity for multiple pollutants, and strong resistance to inorganic anions. Experimental and theoretical results reveal that the Cu single atoms with three oxygen coordination environments (Cu-O 3 ) are more favorable for PMS absorption and selectively adsorb the terminal oxygen of PMS to promote the generation of SO 5 .- , resulting in the generation of 1 O 2 . A continuous-flow wastewater system by dispersing catalysts on poly (vinylidene fluoride) membrane exhibit stable catalytic activity for polycarbonate plant wastewater treatment over 8 h.
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Molecular Catalysis
·
2022
·
IF 5.089
Zichen Zhang,Donglin Yang,Jiaqiang Wang,Chaoting Deng,Hengjun Gai,Meng Xiao,Tingting Huang,Quanhong Zhu,Hongbing Song
Ionic liquids (ILs) are unique substances with unique ionic sites. They are regarded as one of the most promising green solvents and catalysts in the 21st century. In this work, the synthesis of imidazolium-based ILs as metal-free catalysts by molecular design is reported for the first time. By using the ILs as precursors, hyper-crosslinked poly(ionic liquid) (HCPIL) was synthesized by Friedel–Crafts alkylation reaction. These metal-free catalysts can effectively activate ethanolamine for the hydrogenation of nitrobenzene, and they have definite active sites. As the synthesized HCPIL-Cl has a rich porous structure and IL structural units, it could maintain the catalytic activity of ILs and recover them via efficient facile filtration and washing. Density functional theory (DFT) calculation suggested that the imidazolium structure is essential to ethanolamine activation. The calculated results of DFT agree well with the experimental results. The hydrogenation of nitrobenzene has many intermediates whose selectivity can be regulated by different gas atmosphere or alkaline environments. This work provides a promising method for the design of metal-free catalysts.
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