CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lin Zhang,Juanjuan Qi,Haiyang Zhang,Lei Xing,Zhanqi Zhou,Renchan Lei,Bo Li,Hui Liu,Lidong Wang
Dimethylamine (DMA), a widely used organic solvent and famous malodorous volatile organic compound (VOC), is easily released into the atmosphere and harms human health. Here, we designed a bifunctional CoFe/Mg mixed metal oxide (MMO) catalyst for activating peroxymonosulfate (PMS) to degrade aqueous DMA, thereby inhibiting DMA re-emission. The results indicated that the DMA (100 mg/L) degradation efficiency exceeded 90% within 80 min. Moreover, the re-emission of DMA into the atmospheric environment was reduced by 80% after catalysis. Electron paramagnetic resonance (EPR) measurements and quenching tests verified SO 4 •− and • OH as the active oxygen species in the CoFe/Mg MMO–PMS system. Combined characterization and density functional theory (DFT) calculation results confirmed that the Co species served as catalytic sites for PMS activation, and the adjacent Mg species acted as adsorption sites for DMA. The synergy effects between the dual sites could accelerate the PMS activation, facilitate the generation of free radicals, and shorten the migration distance between free radicals and pollutants, to realize the efficient DMA degradation. The degradation mechanism and suppressing re-emission process were proposed. This study will provide distinctive insights into the design of catalysts with dual sites and pioneer an unparalleled approach to the industrial governance of effluvial VOCs treatment.
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MARINE POLLUTION BULLETIN
·
2023
·
IF 5.8
Kunpeng Wang,Liju Tan,Yuewei Zhang,Dongmei Zhang,Na Wang,Jiangtao Wang
P-nitrophenol (4-NP) is the most persistent and highly toxic species among nitrophenol. In this work, a novel fluorescent probe for the detection of 4-NP in aqueous environment was constructed by combining the carbon dots (CQDs) with excellent optical properties and the molecularly imprinted polymer (MIP) with favorable selectivity . The CQDs were synthesized by hydrothermal method using citric acid hydrate as carbon source and o -phenylenediamine as surface modifier, then the molecularly imprinted polymers coating on the CQDs (MIP@CQDs) were obtained by sol-gel imprinting process. The fluorescence quenching of MIP@CQDs is the results of internal filtration effect and dynamic quenching when they encounter with 4-NP. The probe is suitable for the quantitative detection of trace 4-NP in actual aqueous samples, such as tap water , wastewater and seawater, with satisfying recoveries from 95.1 % to 107.8 %, wide detection linear ranges between 0 and 144 μmol/L, low detection limit of 0.41 μmol/L and high selectivity. The detection results are consistent with those of the HPLC method. This work provides a simple, rapid and effective fluorescent detection method for trace 4-NP in aqueous environment.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2023
·
IF 7.8
Peng Xu,Zhuoyu Yang,Xin Liu,Pengfei Zhu
Zero-valent copper (ZVC) coupled with oxygen gas (O 2 ) was extensively studied to degrade refractory contaminant, while the active dismutation reaction and low reactivity of Cu(I) refrained the performance at acid condition. In this study, ferrous ion (Fe(II)) was added to the ZVC/O 2 system (ZVC/Fe(II)/O 2 system) to enhance the degradation ability, the degradation rate of acid orange 7 in the ZVC/Fe(II)/O 2 system was enhanced by 34.8% compared to the ZVC/O 2 system, and the corresponding apparent rate constant was almost three times higher than that of the ZVC/O 2 system. In the reactive species identification experiments, by electron spin resonance experiments and quenching experiments of nitrobenzene , tert butyl alcohol and methanol, hydroxyl radical was proven as primary reactive oxygen species rather than high-valent metal-Cu(III). In addition, the optimum ZVC dosage, Fe(II) concentration, pH and stirring rate were derived based on optimization experiments combined with economic applicability. In the ZVC/Fe(II)/O 2 system, the mechanism was analyzed by detecting the variation of the concentration of H 2 O 2 , Cu(I) and total dissolved copper in the solution. In the degradation process , ZVC was corroded to form Cu(I) by H + , then Cu(I) reacted with O 2 to generate hydrogen peroxide, the generated hydrogen peroxide was induced by Fe(II) and Cu(I) to produce hydroxyl radical, at the same time, ZVC and Cu(I) could reduce Fe(III) to Fe(II). The coexisting substances like carbonate ion , nitrate ion, sulfate ion and phosphate ion did not affect the demineralization of acid orange 7 in the ZVC/Fe(II)/O 2 system, chloride ion remarkably accelerated the degradation rate of acid orange 7, while fulvic acid limited the acid orange 7 removal. The ZVC/Fe(II)/O 2 system also showed excellent degradability in well water, lake water and tap water . Total dissolved copper concentration was controlled within 1 mg/L by the alkali precipitation method, which was within II-level environmental quality criteria in China. These facts suggested that Fe(II)-enhanced ZVC system had great development potential in water treatment .
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jinling Xie,Lingrui Zhang,Xuan Luo,Li Huang,Xiaobo Gong,Jing Tian
Dual heteroatoms doping is an efficient method to improve catalytic activity of carbon materials. In this research, N, S co-doped porous carbon material (S-NPC) was prepared by direct thermal reduction method of metal organic frameworks and proved to be an excellent metal-free heterogeneous Fenton-like catalyst for peroxymonosulfate (PMS) activation. Tetracycline hydrochloride (TC) could be completely degraded in a short time of 20 min with 20 mg S-NPC and 10 mg PMS at 25 °C, attributing that N, S co-doping provided more defects (I D /I G = 0.998) to produce more active sites for PMS activation. Based on the results from radical identification, scavenging tests, density functional theory (DFT) and electrochemical analysis, non-radical pathway based on singlet oxygen ( 1 O 2 ) and electron transfer was proposed to be the dominant way in the S-NPC/PMS system and the contribution rate was about 95.872 %. Three possible pathways of TC degradation were proposed by high resolution liquid chromatography-mass spectrometry (LC-MS) and the toxicity of intermediate products was lower than TC. This study provided a novel strategy to degrade pollutants by preparing efficient co-doping metal-free Fenton-like catalyst.
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ChemistrySelect
·
2022
·Vol. 7
·期 44
·e202203089
·
IF 2.307
Lei He,Tuanhui Li,Xiaoxuan Zhang,Shizhong Luo,Zhisheng Shi,Ruirui Yun
Graphical An embedded Ni-based catalysts have been designed and synthesized by a biopolymer-assistant strategy which followed by calcination under different temperature. Among of them, Ni@PC-900 shows an excellent activity and chemo-selectivity for the hydrogenation of nitroarenes under mild conditions, even in the present of alternative unsaturated groups. Considering of the fact that many of the catalysts reported previously show low selectivity in the hydrogenation reaction. Herein, a series of nickel particles embedded in porous carbon have been synthesized by bio-template strategy. Among of them, Ni@PC-900 (PC: porous carbon; 900: the pyrolysis temperature) shows higher activity and selectivity (conversion>99 % within 30 minutes under room temperature) than that of other catalysts. All of the characterizations of the as-synthesized indicate that the high catalytic activity has a positive correlation with the particle size and distribution of the particles. Moreover, Ni@PC-900 also exhibits excellent durability maybe due to the well core-shell structure protecting the active site from leaching during the catalytic process.
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RSC Advances
·
2023
·Vol. 13
·期 3
·2024-2035
·
IF 3.9
Jiale Wu,Liguo Wang,Shuang Xu,Yan Cao,Ziqiang Han,Huiquan Li
Developing efficient and green catalytic systems is highly desired in the syntheses of alicyclic amines via hydrogenation of nitroaromatics. Herein, we developed Ru–Pd dual active site catalysts in which Ru and Pd species were anchored and highly dispersed on air-exfoliated carbon nitride (Ru–Pd/C3N4-air). As-prepared catalysts were employed in the hydrogenation of nitrobenzene (NB) to cyclohexylamine (CHA). Compared with single Ru or Pd based catalysts, Ru–Pd dual active site catalysts obtained a higher CHA production rate of 26.7 mol CHA mol−1 Ru·Pd h−1 at 80 °C and 3 MPa H2. The activation energy for the hydrogenation of the nitro group and benzene ring was calculated as 26.26 kJ mol−1 and 66.30 kJ mol−1, respectively. Intrinsic kinetic studies demonstrated that Pd was the dominant metal for hydrogenation of nitro group, while Ru was dominant for benzene ring. Thereinto, the corresponding non-dominant metals enhanced activation and dissociation of H2, thereby improving catalytic activity significantly. This excellent performance of Ru–Pd catalysts could be attributed to highly dispersed Ru–Nx and Pd–Nx at a nanoscale distance, which was conducive to metal-assisted hydrogenation. Stability investigation showed that the performance of Ru–Pd catalysts could be essentially maintained at a high level. Additionally, the substrate scope could be successfully extended to hydrogenation of other nitroaromatics with different substituents.
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WATER RESEARCH
·
2023
·
IF 12.8
Jinwen Qiu,Xiaokang Hou,Yuan Ren,Chengshuai Liu,Fangyuan Meng,Jyh-Fu Lee,Yu-Jung Lin,Ziyuan Huang,Huanxin Ma,Zhenqing Shi,Chunhua Feng
The photoinduced transformation of ferrihydrite is an important process that can predict the geochemical cycle of Fe in anoxic environments as well as the fate of trace elements bonded to Fe minerals. We report that the photooxidation of sulfite by UV irradiation produces hydrated electrons (super-reductants), which significantly promote ferrihydrite reduction to Fe(II), and SO 3 •− (a moderate oxidant), enabling its further oxidation to more crystalline Fe(III) products. The experimental results show that the concentration of sulfite was key in influencing the rate and extent of surface-bound Fe(II) formation, which ultimately determined the distribution of individual products. For example, fitting of the Mössbauer spectroscopy data revealed that the relative abundances of mineral species after 8 h of treatment in the UV/sulfite systems were 41.9% lepidocrocite and 58.1% ferrihydrite at 2 mM SO 3 2− ; 41.8% goethite, 28.2% lepidocrocite, and 29.1% ferrihydrite at 5 mM SO 3 2− ; and 100% goethite at 10 mM SO 3 2− . The combined results of the chemical speciation analysis and the Cd K-edge EXAFS characterization provided compelling evidence that Cd was firmly incorporated into the structure of newly formed minerals, particularly at high sulfite concentrations. These findings provide an understanding of the role of UV/sulfite in facilitating ferrihydrite transformation and promoting Cd stabilization in oxygen-deficit soils and aquatic environments.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xin Liu,Peng Xu,Pengfei Zhu,Zhuoyu Yang,Ruoxi Wu,Baolin Hou
Zero-valent copper-triggered hydrogen peroxide (Cu 0 /H 2 O 2 ) process was widely used for the degradation of pollutants, while its oxidation efficacy was restrained by the interaction of Cu + with O 2 as well as the dismutation of Cu + . In this study, both ferric ion (Fe 3+ ) and chloride ion (Cl − ) were introduced into the Cu 0 /H 2 O 2 (Fe 3+ /Cl − /Cu 0 /H 2 O 2 ) system, and the removal of acetaminophen was immensely enhanced. In the Fe 3+ /Cl − /Cu 0 /H 2 O 2 , Fe 3+ was converted to Fe 2+ via the reaction of Fe 3+ with Cu 0 and Cu + , and the reaction between Cu + and Fe 3+ receded the reaction of Cu + with O 2 , promoting the formation of reactive oxygen species; Cl − integrated with Cu + to form the Cu-Cl chelate, and Cl − helped the comproportionation of Cu 0 and Cu 2+ to form CuCl, which decreased the reaction of Cu + with O 2 and promoted the generation of reactive oxygen species. Both the addition of Fe 3+ and Cl − in the Cu 0 /H 2 O 2 process greatly improved the utilization of Cu 0 . •OH, Various reactive oxygen species such as •OH, Fe IV O 2+ and reactive chlorine species were identified in the Fe 3+ /Cl − /Cu 0 /H 2 O 2 process. There into, Fe 2+ stimulated H 2 O 2 to form •OH and Fe IV O 2+ , and Cu + triggered H 2 O 2 to form •OH rather than Cu 3+ , and partial •OH was transferred to reactive chlorine species via the interaction of •OH with Cl − . After increasing the solution pH to > 7.0 and leaching solution, the total copper of reaction solution was below 0.455 mg/L. These results suggested that the Fe 3+ /Cl − /Cu 0 /H 2 O 2 process was feasible, effective and environmentally safe, and the research offered a theory instruction for the application of Fe 3+ and Cl − -enhanced Cu 0 /H 2 O 2 process in pollutants decomposition.
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ACS Applied Polymer Materials
·
2023
·
IF 5
Siyuan Zhang,Jiao He,Xinjian Cheng
Amphiphilic hyperbranched polymers (AHBPs) possess important characteristics, such as high solubility, low viscosity, and multiple functional groups, making them of significant scientific interest. In this work, a chain transfer agent (CTA) with a styrene unit was synthesized at first. Subsequently, the CTA was polymerized with a coumarin derivative containing a −C=C bond through reversible addition-fragmentation chain transfer-self-condensing vinyl polymerization (RAFT-SCVP) to obtain the hyperbranched polymer HP-1. Finally, using HP-1 as a macromolecular CTA, amphiphilic hyperbranched fluorescent probes AHP-2 and AHP-3 were synthesized via RAFT polymerization of hydrophilic monomers poly[oligo(ethylene glycol) methacrylate] (PEGMA) and 2-(dimethylamino)ethyl methacrylate (DMAEMA). The as-prepared AHP-2 and AHP-3 were characterized and confirmed. These macromolecular fluorescent probes enable highly sensitive and specific recognition of 4-nitrophenol (4-NP) with detection limit as 0.59 μM. A unique fluorescence quenching effect, termed “enriching inner filter effect (IFE)”, was revealed through the study of the recognition mechanism of the probes for 4-NP in hyperbranched polymers. This effect has the potential to expand the preparation methods of both fluorescent probes and functional hyperbranched polymers. This work investigates the synthesis methodology of amphiphilic hyperbranched polymers and the performance of fluorescent probes, providing a valuable approach for the development of highly sensitive polymer fluorescent probes in the future.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fengliang Cao,Qingshan Zhao,Debin Kong,Xiaojie Tan,Xinxin Li,Tengfei Liu,Linjie Zhi,Mingbo Wu
Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts show great potential for heterogeneous catalysis. However, recognizing and engineering the microenvironment of M-N x sites to achieve satisfactory catalytic performance remains challenging. Herein, we propose a facile g-C 3 N 4 -assisted template strategy to anchor atomic Fe-N 4 sites on highly nitrogen-doped carbon nanosheets. Through regulating the ratio and type of peripheral nitrogen species by carbonization temperature, the optimal Fe-N-C-800 catalyst showed significantly boosted catalytic activities (overall turnover frequency of 13.43 min −1 and activation energy of 19.44 kJ mol −1 ) for nitroarene reduction with extremely low reductant dosage, exceeding most reported metal catalysts. Experimental and theoretical results reveal appropriate graphitic- and pyrrolic-N dopants surrounding the Fe-N 4 center can tailor the local electronic structure and contribute to obvious upshift of the d-band center, which dramatically promotes the adsorption and conversion of reactant substrates, eventually delivering the unprecedented catalytic performance. This work provides a guide for rational coordination environment regulation of single-atom catalysts for efficient chemical transformations.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Yanan Shao,Xiaodong Li,Longbo Jiang,Xue Wei,Yanlan Zhao,Xuwu Chen,Shuai Li
UV/chlorine as an advanced oxidation process (AOPs) has been employed to treat contaminants. However, current research has primarily focused on drinking water and sewage treatment . This paper investigated the degradation of ciprofloxacin (CIP) by UV/chlorine treatment in hospital urine components that contain a higher concentration of iodine (I − ). The results indicated that the characteristic ions (HCO 3 − , SO 4 2− , and NH 4 + ) and I − in hospital urine inhibited CIP removal. In contrast, the characteristic ion, Cl − ion promoted this degradation reaction. Surprisingly, microgram levels of I − strongly inhibited CIP degradation. The characteristic ions can reduce the contribution of hydroxyl radicals (HO•) and reactive chlorine species (RCS). I − can decrease the contribution rate of HO• while slightly increasing the contribution of other radical oxidation in phosphate buffer solution (PBS) ascribed to the formation of HOI and reactive iodine species (RIS). Three degradation pathways have been proposed based on the main transformation products : hydroxylation , electron transfer , and halogen substitution. The piperazine ring of CIP was the main reactive group, and the N2, C10, C16, and C13 atoms were identified as reaction sites. Preliminary toxicity analysis suggested that the toxicity of hospital hydrolyzed urine containing iodine was higher than that of PBS.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yuanxi Huang,Lingjun Bu,Shumin Zhu,Shiqing Zhou,Zhou Shi,Jianwu Wang
Peracetic acid (PAA) is a potential disinfectant for water treatment due to its high efficiency and the limited formation of disinfection byproducts (DBPs). In PAA process of this study, bromide (Br − ) significantly enhanced the degradation of phenolic compounds , including bisphenol A (BPA), phenol , p -aminophenol, and hydroquinone. The promotion is mainly due to the formation of hypobromous acid (HOBr), which comes from the oxidation of Br − by PAA. A kinetic model of PAA treatment in the presence of Br − was established to explore the degradation mechanism of phenolic compounds with good accuracy. The removal of phenolic compounds is positively related to Br − concentration. The degradation process was pH-dependent and favored at acidic conditions. In the real water matrix, the presence of multiple water matrix components may inhibit the degradation of phenolic compounds by consuming PAA and HOBr. Further, the transformation of BPA mainly involves bromination , hydroxylation, oxidation, bond cleavage, and ring opening, resulting in the formation of organic bromines. Brominated DBPs, such as dibromoacetic acid and tribromomethane were found, suggesting the potential adverse health effects of PAA treatment in the presence of Br − . The acute toxicity of phenolic compounds initially increased and then decreased with the increase of reaction time, indicating that prolonging the reaction time may reduce the environmental risk.
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