Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Kang Deng,Xintong You,Minyi Liu,Yongyi Tan,Yilian Lin,Wei Shu,Feiyan Liu,Shunheng Tu,Yi Yang
Herein, we developed a self-assembly heterostructured BiOI/Bi 4 O 5 Br 2 microcluster with the hydrothermal method . Catalysts were mainly characterized by powder X-ray diffraction, field-emission scanning electron microscopy, transmission electron microscope , energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy and diffuse reflectance spectra. The results showed that due to charge induction, BiOI nanosheets were successfully self-assembled and deposited on Bi 4 O 5 Br 2 , forming a unique heterojunction and achieving strong transient photocurrent response. Performances of catalysts were tested and effects of different initial concentrations of the Methylparaben (MPB), catalyst dosage, initial pH and total organic carbon (TOC) conversion were studied. Results reveal that catalytic activity increased with lower initial concentration of MPB and the best dosage of catalyst is 0.5 g·L -1 . The BiOI/Bi 4 O 5 Br 2 microcluster exhibits excellent photocatalytic activity under visible-light irradiation, which can degrade 97% MPB in 2 h and the TOC value is only 20% of the original. The catalytic degradation process conforms to pseudo-first-order kinetics with a rate constant of 0.030 min -1 . The results of detailed active species detection indicate that the photogenerated holes and •O 2 − radicals play the main role in the photocatalytic system. In addition, photoelectrochemical measurements reveal that the excellent strengthened photocatalytic activity is due to the high separation and transfer efficiency derived from the heterostructure.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
RSC Advances
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2015
·Vol. 5
·期 48
·38373-38381
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IF 3.84
Xin Xiao,Ruiping Hu,Shunheng Tu,Chunxia Zheng,Huan Zhong,Xiaoxi Zuo,Junmin Nan
β-Bi2O3 micro/nanostructures with tunable morphologies were synthesized via a one-pot solvothermal–calcining route, and their photocatalytic activity toward degrading methylparaben (MeP, a widely used preservative with estrogenic activity) was evaluated under visible-light (λ ≥ 420 nm) irradiation. The formation process of β-Bi2O3 catalysts can be described as reduction of Bi3+ through a solvothermal reaction, followed by oxidization of metal Bi via calcination in air. During this process, the organic reductants (single or a mixture of ethylene glycol, D-fructose, and ascorbic acid) play important roles in determining the final morphologies and structures of the materials. Photocatalytic tests reveal that MeP can be effectively degraded and mineralized by using synthetic β-Bi2O3 catalysts, and the reaction rate constant of an optimum sample is more than 25 and 160 times faster than a commercial Bi2O3 and synthetic N-TiO2, respectively. The superior photocatalytic activity of the optimum product is ascribed to its pure beta phase with a narrower band gap, good absorption of visible light, more efficient separation of electrons and holes, relatively higher BET specific surface area, and three-dimensional architectures, which favor more surface active sites and easier mass and photoinduced charge transportations. In addition, the main reactive oxygen species and possible degradation intermediates were detected, and the results suggest that photogenerated holes and superoxide radicals are the predominant species in the photochemical oxidation process.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2022
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IF 5.723
Xixi Xiao,Huiyue Xin,Yuanyuan Qi,Chen Zhao,Peng Wu,Xiaohong Li
Herein, we developed a one-pot tandem catalytic process for the hydrogenation of dimethyl terephthalate (DMT) to 1,4-cyclohexanedimethanol (CHDM) with physically mixed 5 Pd/CMK-3 and Cu-600 catalysts in a batch reactor. The reaction process was systematically studied in order to improve the yield of CHDM. The hydrogenation of the phenyl group of DMT was preferential to the ester groups, mainly owing to strong adsorption of DMT and the high activity of the 5 Pd/CMK-3 catalyst, as confirmed by UV–visible spectra and kinetic studies . Up to 82% yield of CHDM can be achieved under the optimized reaction conditions. The possible reaction pathways were proposed based on the detailed investigations with different reactants and catalysts. Promisingly, the developed method may lay a solid foundation for the one-pot synthesis of CHDM via the hydrogenation of DMT.
研究领域:
化学工程
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催化科学
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高影响因子
GREEN CHEMISTRY
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2024
·Vol. 26
·期 11
·6748-6759
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IF 9.3
Yitian Zhang,Jie Gao,Chao Jiang,Gang Luo,Jiajun Fan,James H. Clark,Shicheng Zhang
Chemical upgrading as a recycling technology for poly(ethylene terephthalate) (PET) waste plastic is an effective way to help solve the current challenges of plastic pollution. Catalytic methanolysis technology enables the depolymerization of PET into high-value dimethyl terephthalate (DMT) monomers under relatively mild conditions, thereby achieving closed-loop recycling of PET waste plastic. In this study, we compared the catalytic efficiency of Cu/SiO2 catalysts prepared by three different methods for the depolymerization of PET to DMT. Cu/SiO2-IM, prepared through the impregnation method, exhibited the highest activity, with PET conversion and DMT selectivity reaching 92.35% and 99.0%, respectively, at 200 °C without any initial gas pressure. The exceptional performance of Cu/SiO2-IM can be attributed to its small metal particles, substantial specific surface area, a high ratio of Brønsted acid sites (BAS) to Lewis acid sites (LAS) and the balance of Cu+ and Cu0 active sites on the catalytic surface. Furthermore, possible reaction mechanisms of Cu-based catalysts in the catalytic methanolysis of PET were investigated: Cu+ initiates the attack on the carbon groups along the long PET chain and enhances the nucleophilic attack during the depolymerization reaction, while Cu0 readily interacts with the hydroxyl group of methanol, leading to the formation of a new ester group between the oxygen atom in the hydroxyl group of methanol and the carbon atom in the CO group of PET polyester. This low-cost and high-efficiency catalytic methanolysis study provides a practical approach to PET waste plastic recycling.
研究领域:
化学工程
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环境科学
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材料科学
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高影响因子
ANALYTICAL CHEMISTRY
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2024
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IF 6.7
Jia-Yi Zheng,Xiao-Yuan Ji,An-Qi Zhao,Fang-Yuan Sun,Li-Fang Liu,Gui-Zhong Xin
Mitochondrial complex activity controls a multitude of physiological processes by regulating the cellular metabolism. Current methods for evaluating mitochondrial complex activity mainly focus on single metabolic reactions within mitochondria. These methods often require fresh samples in large quantities for mitochondria purification or intact mitochondrial membranes for real-time monitoring. Confronting these limitations, we shifted the analytical perspective toward interactive metabolic networks at the whole-cell level to reflect mitochondrial complex activity. To this end, we compiled a panel of mitochondrial respiratory chain-mapped metabolites (MRCMs), whose perturbations theoretically provide an overall reflection on mitochondrial complex activity. By introducing N-dimethyl-p-phenylenediamine and N-methyl-p-phenylenediamine as a pair of mass spectrometry probes, an ultraperformance liquid chromatography-tandem mass spectrometry method with high sensitivity (LLOQ as low as 0.2 fmol) was developed to obtain accurate quantitative data of MRCMs. Machine learning was then combined to capture the relationship between MRCMs and mitochondrial complex activity. Using Complex I as a proof-of-concept, we identified NADH, alanine, and phosphoenolpyruvate as metabolites associated with Complex I activity based on the whole-cell level. The effectiveness of using their concentrations to reflect Complex I activity was further validated in external data sets. Hence, by capturing the relationship between metabolites and mitochondrial complex activity at the whole-cell level, this study explores a novel analytical paradigm for the interrogation of mitochondrial complex activity, offering a favorable complement to existing methods particularly when sample quantities, type, and treatment timeliness pose challenges. More importantly, it shifts the focus from individual metabolic reactions within mitochondria to a more comprehensive view of an interactive metabolic network, which should serve as a promising direction for future research into the functional architecture between mitochondrial complexes and metabolites.
研究领域:
分析化学
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生物化学
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机器学习
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代谢组学
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线粒体生物学
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PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2022
·Vol. 97
·期 7
·1695-1704
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IF 3.709
Bao Guo,Jidong Liu,Shixiong Tang,Yida Liu,Zenan Tian,Jianhua Lv
BACKGROUND Whether waste polyethylene terephthalate (PET) can be effectively recycled is one of the main challenges of the current environmental problems. The hydrolysis of dimethyl terephthalate (DMT) to terephthalic acid (TPA) over Nb-modified HZSM-5 zeolite was studied. Nb/HZSM-5 zeolites with different loadings were prepared and characterized by X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, NH 3 -temperature programmed desorption and pyridine adsorption infrared spectroscopy. The effects of different reaction conditions on the conversion of DMT and TPA yield were investigated. RESULTS The yield of TPA strongly depends on the reaction conditions and the loading of Nb. The niobium phase exists in the form of Nb 2 O 5 on the zeolite and interacts with the surface of HZSM-5 to produce the active site of Brønsted acid. The yield of TPA is closely related to the concentration of Brønsted acid sites. On 0.6Nb/HZSM-5 catalyst, the yield of TPA is highest, at about 94%. CONCLUSION Nb/HZSM-5 catalyst has excellent catalytic activity and high stability for DMT hydrolysis. In addition, the product TPA prepared in this study can be directly applied to the current PET production supply chain, providing a promising catalytic route. © 2022 Society of Chemical Industry (SCI).
研究领域:
环境科学
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催化化学
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2022
·Vol. 139
·期 35
·e52814
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IF 3.057
Meiyuan Ma,Shuai Wang,Yue Liu,Hailong Yu,Shitao Yu,Congcong Ji,Haiyan Li,Genkuo Nie,Shiwei Liu
With concern to sustainable development, it is necessary to establish a recycling process of polyethylene terephthalate (PET). Methanolysis of PET is promising for chemical recovery of PET and the products are mainly dimethyl terephthalate (DMT) and ethylene glycol (EG), but the conditions of state-of-art depolymerization are severe. Here, we synthesized ionic liquid [HO 3 S-(CH 2 ) 3 -NEt 3 ]Cl-[ZnCl 2 ] 0.67 with Brönsted–Lewis di-acid and used it to efficiently catalyze the methanolysis of PET ( m methanol : m PET about 4) at milder temperature of 195°C with yield of DMT about 78.4%. Reaction kinetics was studied and the result indicated the depolymerization of PET was a first-order kinetic reaction with the apparent activation energy of DMT formation about 17.63 kJ mol −1 . Random sampling experiment was also conducted and the results showd that DMT was the product of deep depolymerization of PET and two methanol molecules were needed to form DMT and EG in the depolymerization process. This study provides an efficient method to the recycling use of PET and wais significant to waste recovery and green environment.
研究领域:
化学工程
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环境科学
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材料科学
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DOI
高影响因子
INORGANICA CHIMICA ACTA
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2023
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IF 2.8
Ruiqin Huang,Wei Li,Xiaoling Luo,Zheng Liu,Guo-Cheng Han,Runzhi Wei
2,5-bis(trifluoromethyl)terephthalic acid (H 2 L 1 ) as the main ligand and 1,10′-phenanthroline (L 2 ) as the co-ligand were reacted with manganese chloride tetrahydrate (MnCl 2 ·4H 2 O), nickel sulfate hexahydrate (NiSO 4 ·6H 2 O) and cobalt nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O) by solvothermal reaction to give the manganese complex [Mn 2 (L 1 ) 2 (L 2 ) 2 ] n ( 1 ), the nickel complex {[Ni 3 (L 1 ) 3 (L 2 ) 2 (H 2 O) 4 ]·2DMF} n ( 2 ) and the cobalt complex {[Co 2 (L 1 ) 2 (DMF) 2 ]·H 2 O} n ( 3 ). The structures were characterized and their properties studied by means of single-crystal X-ray diffraction, infrared spectroscopy, elemental analysis, ultraviolet spectroscopy, fluorescence spectroscopy, thermogravimetric analysis. The single-crystal structure analysis showed that the complexes 1 – 3 are infinitely extended three-dimensional network-like structures of space groups P 1 - , P 1 - , P 2 1 / n , respectively. The results of fluorescence analysis and thermogravimetric analysis showed that complexes 1 – 3 have good thermal stability and fluorescence properties, respectively. Complex 3 can also maintain good thermal stability at 230 °C, and the maximum fluorescence emission wavelength is 370 nm.
研究领域:
无机化学
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材料科学
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DOI
高影响因子
Inorganic Chemistry Frontiers
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2024
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IF 6.1
Lu Yan,Yue Shen,Zidan Zou,Xiao Zhang,Zhixin Yu,Guozhong Wang,Chun Chen
Hydrogenation of aromatic rings can be used not only for synthesis fine chemicals, but also for hydrogen storage and transportation using organic hydride. In this paper, yolk-shell structural SiO2@Ru@NC catalyst, which was successfully synthesized by a strategy of combining modified Stöber and vacuum-assisted impregnation, revealed excellent catalytic activity in dimethyl terephthalate (DMT) hydrogenation to dimethyl 1,4-cyclohexanedicarboxylate (DMCD), which is a green chemical reagent and precursor for high-value chemicals. Characterization results showed that highly dispersed Ru NPs with subnanometer size distribution were encapsulated in yolk-shell nanoarchitecture and the mesoporous shell could ensure unhindered diffusion of reactant molecules. Moreover, yolk-shell structure-induced interaction of Ru and carbon shell allowed for tuning electronic structure of Ru species, which in turn could regulate catalytic properties. The yolk-shell nanoarchitecture catalyst offers advantages of low active metal loading, excellent activity and stability, thus can expand application of ultra-low loaded precious metal catalysts in catalytic conversion of aromatic compounds.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yujiao An,Xiaowan Li,Zihao Liu,Zhilan Wang,Xiaoquan Lu
Quinones, widely considered as environmental pollutants in wastewater, have been identified as redox-active substances capable of activating persulfate for decontamination purpose. However, the mechanism of peroxydisulfate (PDS) activation by quinones under alkaline conditions remains elusive. In this study, methyl- p -benzoquinone (MBQ) was chosen as a model quinone to elucidate the intrinsic mechanism of activating PDS. The results showed that MBQ/PDS system can effectively degrade atrazine (ATZ) under alkaline conditions (especially at pH 10.5) and achieve simultaneous removal of MBQ. Derivatization analysis, quenching experiments and electron spin resonance tests revealed that the self-transformation product of MBQ, methyl-semiquinone radical (MSQ − ), played a major role in activating PDS while alkali served as an auxiliary activator. Specifically, MSQ − functioned as a mediator in PDS activation, regulating the generation of sulfate radical (SO 4 − ) and hydroxyl radical ( OH), thereby inducing the degradation of ATZ through free radical pathways. Two degradation pathways of ATZ were proposed based on UPLC-Q-TOF-MS analysis and DFT calculation. ECOSAR evaluation indicated MBQ/PDS system can detoxify ATZ, yet it remains imperative to concern the formation of more toxic by-products. Furthermore, MBQ/PDS system exhibited strong resistance to water matrixes (excluding Cl − ) and favorable degradation capabilities towards diverse contaminants. This work broadened the possibility of applying the persulfate system in actual water bodies with alkaline environments, achieving the dual benefit of degrading target contaminants and simultaneously removing the activator quinones themselves, providing a novel “treating pollution with waste” water treatment strategy.
研究领域:
环境化学
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水处理
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污染物降解
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Jiabao Li,Dongxia Yan,Xiujie Cheng,Chunrui Rong,Jian Feng,Xin Feng,Jiayu Xin,Qing Zhou,Yi Li,Junli Xu,Xingmei Lu
The methanolysis of polyethylene terephthalate (PET) can address the environmental pollution and resource waste caused by waste PET, and the obtained monomer dimethyl terephthalate (DMT) is easy to separate and purify. However, conventional methanolysis of PET usually uses metal-containing catalysts, resulting in metal residues in the degradation products, which affects subsequent high-value utilization. Meantime, the reaction conditions of high temperature and high pressure promotes the occurrence of side reactions and reduces the yield of the main products. Herein, the nonmetallic deep eutectic solvent (DES) 1,5-diazabicyclo [4.3.0]-5-nonene (DBN)/Phenol was employed as a catalyst for PET methanolysis. 100% PET conversion and 95.3% DMT yield were obtained at 130 °C for 1 h. The possible reaction mechanism was investigated by combining NMR, FT-IR, GPC analysis, and DFT calculations. DBN and phenol were connected through N–H–O hydrogen bonding, where the hydrogen atom interacted with the carbonyl oxygen of PET and the oxygen atom activated the hydroxyl group of methanol. Additionally, GPC analysis showed that the dissolution and degradation of PET were simultaneous, which enhanced mass transfer and facilitated the reaction. The kinetic studies showed that PET methanolysis followed the first-order kinetic model with an activation energy of 103.3 kJ/mol, which was lower than the literature-reported value. This research provides an efficient nonmetallic deep eutectic solvent catalyst for PET methanolysis, which solves the problem of metal residues in the degradation products and reduces the reaction temperature. It is of great significance to simplify the purification steps and improve the economy of regeneration.
研究领域:
化学工程
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环境科学
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材料科学
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DOI
高影响因子
GREEN CHEMISTRY
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2023
·Vol. 25
·期 18
·7243-7252
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IF 9.8
Boyong Ye,Ruru Zhou,Zixin Zhong,Songlin Wang,Han Wang,Zhaoyin Hou
Abandoned plastics have become a serious hazard to the environment and ecology both on land and in oceans; among them, waste polyethylene terephthalate (PET) accounts for up to 13.9% of all waste plastics. The recycling of these hazardous materials has attracted the attention of many scientists. In this work, an efficient strategy of catalytic upcycling of waste PET to dimethyl terephthalate (DMT) was performed over environmentally friendly TixSi1−xO2 solid acids. Characterization studies disclosed that Lewis acid sites in TixSi1−xO2 catalysts were extremely active for the alcoholysis of PET with methanol under mild conditions. In particular, the yield of DMT over Ti0.5Si0.5O2 (2.5 wt% added PET) reached 98.2% with complete degradation of PET in 2 h at 160 °C. Ti0.5Si0.5O2 could be recycled at least five times without obvious loss of activity. The best specific activity of each acid site in Ti0.5Si0.5O2 reached 708.3 h−1, and it was also capable of upcycling waste bottles and polyester yarn. The degradation mechanism of PET over Ti0.5Si0.5O2 was validated via matrix-assisted laser desorption/ionization time-of-flight mass spectrometry, scanning electron microscopy and gel permeation chromatography. The Ti0.5Si0.5O2-catalyzed alcoholysis method provides a green pathway for upcycling waste PET.
研究领域:
化学工程
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环境科学
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材料科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）