Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 8
·1085-1095
·
IF 4.5
Qi Yi,Zeng Xuezhi,Xiong Lingyingzi,Lin Xuliang,Liu Bowen,Qin Yanlin
The aromatic properties of lignin make it a promising source of valuable chemicals and fuels. Developing efficient and stable catalysts to effectively convert lignin into high-value chemicals is challenging. In this work, MnFe 2 O 4 spinel catalysts with oxygen-rich vacancies and porous distribution were synthesized by a simple solvothermal process and used to catalyze the depolymerization of lignin in an isopropanol solvent system. The specific surface area was 110.5 m 2 ·g −1 , which substantially increased the active sites for lignin depolymerization compared to Fe 3 O 4 . The conversion of lignin reached 94%, and the selectivity of alkylphenols exceeded 90% after 5 h at 250 °C. Underpinned by characterizations, products, and density functional theory analysis, the results showed that the catalytic performance of MnFe 2 O 4 was attributed to the composition of Mn and Fe with strong Mn-O-Fe synergy. In addition, the cycling experiments and characterization showed that the depolymerized lignin on MnFe 2 O 4 has excellent cycling stability. Thus, our work provides valuable insights into the mechanism of lignin catalytic depolymerization and paves the way for the industrial-scale application of this process.
研究领域:
化学工程
·
材料科学
·
可再生能源
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
ShiJun Chen,Jianshan Li,Tingsong Xiong,Biao Liu
Lignin, an aromatic biopolymer produced in large quantities as a byproduct of biorefineries, has garnered significant attention for its potential to be valorized into valuable compounds. This demands for the development of an efficient catalyst. This study is the first evaluate the catalytic efficiency of a synthesized Mo-loaded CeO 2 (5Mo/CeO 2 -syn) catalyst for an in-situ upgradation of lignin oil. The 5Mo/CeO 2 -syn catalyst demonstrated exceptional performance, achieving a high lignin liquefaction yield of 66.7 wt%, compared to 48.1 wt% for 5Mo/CeO 2 -com and 35.5 wt% for the non-catalytic (N-cat) reaction. The effects of varying metal loadings and different alcoholic solvents were systematically investigated for kraft lignin (KL) depolymerization. The results of GC–MS and elemental analysis for the bio-oils revealed a significant increase in calorific value (36 MJ/kg, 5Mo/CeO 2 -syn), attributed to the efficient removal of oxygenates. The N-cat bio-oil contained a high proportion of guaiacyl (G-type) phenols (73.4 %), which were significantly reduced during catalytic reactions as they were transformed into alkyl (H-type) phenols. The GPC analysis also evaluated for the lignin and optimum bio-oils, to confirm the breakage of the macro-polymeric structure of lignin into respective monomeric compounds. Moreover, the 5Mo/CeO 2 -syn catalyst was further evaluated across four catalytic cycles, demonstrating its stability and reusability.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Peixun Yang,Senwei Jiang,Zhen Wu,Daodong Pan,Hangzhen Lan
Metal-organic frameworks (MOFs) hold significant potential for sample preparation, but single-MOF materials often face limitations in selectivity and extraction efficiency. To overcome these, a mesoporous MIL-53(Al)–NH 2 @UiO-66 composites with a core–shell structure was synthesized using an epitaxial growth strategy. This composite leverages the complementary properties of both MOFs, offering enhanced active sites and interaction forces for analytes. The structure and integration of the composite were characterized using Fourier-transform infrared spectroscopy, scanning electron microscopy, and X-ray diffraction, confirming their successful integration. To address the challenge of detecting alkylphenols (APs) in food matrices, known for their endocrine-disrupting properties and low concentrations, a new solid-phase microextraction (SPME) Arrow was fabricated using the MIL-53(Al)–NH 2 @UiO-66 composite combined with polyacrylonitrile as a binder. APs were detected using ultra-performance liquid chromatography and quadrupole time-of-flight tandem mass spectrometry (UPLC-ESI-Q-ToF/MS). The developed SPME Arrow-UPLC-ESI-Q-ToF/MS method exhibits good linearity (R 2 ≥ 0.9958), wide linear range (0.01–1000 μg L –1 ), and high sensitivity (limits of detection ranging from 0.005 to 0.01 μg L –1 ) for APs determination. This method was validated for determining nine APs in milk samples from various packing materials, with spiked recoveries ranging from 85.2 % to 115 % and relative standard deviations from 3.4 % to 13.6 %. This study demonstrates the potential of MOF-on-MOF composites in enhancing the performance of adsorbents for SPME pretreatment, offering a promising approach for improving analytical methodologies in food safety.
研究领域:
分析化学
·
食品安全
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Haoquan Guo,Xinyu Lu,Yue Yang,Jinhe Wei,Lizhi Wu,Li Tan,Yu Tang,Xiaoli Gu
Alkyl phenol is an essential chemical intermediate that is in high demand in the chemical industry. The synthesis of alkyl phenols from lignin-derived molecules is one of the most promising routes for utilizing biomass resources. Herein, we report the catalytic hydrodeoxygenation (HDO) of dihydroeugenol (DHE) to alkyl phenols over a highly dispersed Pd/α-MoC catalyst with a substrate conversion of 98% and a selectivity of 96% to alkyl phenols. The Pd/α-MoC catalyst prepared by co-precipitation and temperature-programmed carbonization exhibits exceptional HDO activity under mild conditions with a low H 2 pressure (1–10 bars). The characterizations of the catalyst suggest that Pd are highly dispersed on the α-MoC matrix. The reaction mechanism was investigated using the substrate scope experiments. Under ambient pressure, the abundant oxygen vacancies and acidity sites on Pd/α-MoC enable the selective hydrodeoxygenation of lignin monomers.
研究领域:
化学工程
·
生物质利用
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2016
·
IF 3.926
Yuqian Jia,Hao Su,Y.-L. Elaine Wong,Xiangfeng Chen,T.-W. Dominic Chan
In this work, the thermo-responsive polymer PNIPAM tethered to Fe 3 O 4 @SiO 2 @MOF core-shell magnetic microspheres was first synthesized by a surface-selective post-synthetic strategy and underwent highly efficient magnetic solid-phase extraction (MSPE) of alkylphenols from aqueous samples. Alkylphenols, including 4- tert -octylphenol (OP) and 4- n -nonylphenol (NP), were selected as target compounds. The sample quantification was carried out using LC–MS/MS in multiple reaction monitor (MRM) mode. Under optimal working conditions, the developed method showed good linearity in the range of 5–1000 ng L −1 , a low limit of detection (1.5 ng L −1 ), and good repeatability (relative standard deviation, <8%, n = 5) for NP and OP. Owning to the hydrophilic/hydrophobic switchable properties of the nanocomposite, high recoveries (78.7–104.3%) of alkylphenols were obtained under different extraction conditions. The levels of OP and NP in environmental samples collected from local river, lake and pond waters were analyzed using the developed method. It was believed that the synthesized material with the thermo-responsive coating, large surface areas and magnetic properties should have great potential in the extraction and removal of alkylphenols from environmental samples.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Jiajun Li,Shaoqi Kong,Guochao Yan,Xuanlai Chen
The serious hazards posed by inhalable coal dust to the safety, air purity, and health of coal miners can be effectively alleviated through the use of appropriate dust suppressants. The wetting enhancement capabilities of two dust suppressants, octylphenol polyoxyethylene ether (OP-10) and nonylphenol polyoxyethylene ether (NP-10), were examined in this study through experimental and simulation methods. Macroscopic experiments (surface tension, contact angle, coal dust settling time, and water retention) indicate that the shorter the alkyl chain attached to the benzene ring in the surfactant and the lower the surface tension, the more conducive it is to improving the fluidity and suspension stability of anthracite particles in the wetting solution and further improving the interfacial properties and wetting effect between coal dust and the liquid medium. Mesoscopic experiments (laser particle size, FTIR, XPS, UV–visible spectroscopy, BET, and SEM) showed that the relevant properties of APEO-modified coals were greatly changed, especially the anthracite modified with short-chain alkyl groups of OP-10, which exhibited a stronger aggregation effect on the coal dust particles and increased the pore structure and specific surface area of the coal dust. Additionally, the hydrophilic functional groups are augmented, leading to a notable enhancement in the adsorption capacity of OP-10 on the coal surface. Microscopic simulations (Density Functional Theory calculations, Molecular Dynamics simulations) reveal that APEO surfactants with longer alkyl side chains attached to benzene rings hinder the π-π interactions between the coal's aromatic ring structures and the benzene rings in the surfactants. The surface polarity of coal modified with OP-10 is significantly enhanced, resulting in a more pronounced improvement in wetting performance and an increased water retention capability. The study systematically explores surfactant microstructure effects on anthracite wetting, laying essential groundwork for advanced dust suppression system development.
研究领域:
环境科学
·
材料科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Dan Wang,Ruofei Zhu,Jiangfei Lou,Jiugang Yuan,Jin Xu,Xuerong Fan
Alkylphenol polyethoxylate (APEO n ) is an emerging contaminant mainly referred to nonylphenol polyethoxylate (NPEO n ) and octylphenol polyethoxylate (OPEO n ). A novel multiscale rough composite photocatalyst (CuO@Cu-H 3 BTC) with marigold-flower nanosheets and sub-micron flakes was successfully constructed for photodegradation of OPEO n and NPEO n under visible light. Several technologies (such as SEM , EDS, FTIR, XRD, XPS and EPR) were utilized to characterize the structures and properties of the as-obtained sample. The effect of OPEO n and NPEO n removal by CuO@Cu-H 3 BTC MOF and the influence of reaction conditions on the removal efficiency were explored. It was found that 96% of OPEO n and 79% of NPEO n were removed under the action of adsorption in darkness and degradation in visible light irradiation within 120 min when treating 25 mg/L OPEO n and NPEO n solution with 1.6 g/L of CuO@Cu-H 3 BTC MOF composite. The corresponding OPEO n and NPEO n removal efficiency could still achieve almost 72% and 51% after the CuO@Cu-H 3 BTC MOF was recycled five times, respectively. The degradation mechanism of APEO n investigation revealed that the free radicals and holes generated in the CuO@Cu-H 3 BTC MOF degraded APEO n , and the existence of holes was confirmed to play the major role through quenching experiment. In summary, this facile and novel CuO@Cu-H 3 BTC MOFs composite photocatalyst boosts the application platform in wastewater treatment .
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 4
·1-13
·
IF 5.3
Yang Peixun,Zhu Xiaoyan,Lan Hangzhen,Wu Yichun,Pan Daodong
A solid-phase microextraction (SPME) Arrow and high-performance liquid chromatography-UV detector (HPLC-UV, detection at 225 nm) based method was developed for the selective determination of nine alkylphenols (APs) in milk. The functionalized mesoporous UiO-66 (4-meso-UiO-66) was utilized as the new coating material, which was synthesized by post-modification of pore-expanded UiO-66-NH 2 by an esterification reaction with 4-pentylbenzoic acid. It was fully characterized by X-ray photoelectron spectroscopy (XPS), fourier transformation infrared spectrometry, nitrogen sorption-desorption test, scanning electron microscopy, transmission electron microscopy, and X-ray diffractometer. The characterization results showed the ester groups and benzene rings were introduced into the 4-meso-UiO-66, and the mesoporous structure was predominant in the 4-meso-UiO-66. The extraction mechanism of 4-meso-UiO-66 to APs is the synergistic effect of Zr-O electrostatic interaction and the size exclusion effect resulting from XPS, selectivity test, and nitrogen sorption-desorption test. The electrospinning technique was utilized to fabricate the 4-meso-UiO-66 coated SPME Arrow and polyacrylonitrile (PAN) was used as the adhesive. The mass rate of 4-meso-UiO-66 to PAN and the electrospinning time were evaluated. The extraction and desorption parameters were also studied. The linear range of this method was 0.2–1000 μg L –1 with a coefficient of determination greater than 0.9989 under the optimal conditions. The detection limits were 0.05–1 μg L –1 , the inter-day and intra-day precision (RSD) were 2.8–11.5%, and the recovery was 83.6%–112%. The reusability study showed that the extraction performance of this new SPME Arrow could be maintained after 80 adsorption-desorption cycles. This method showed excellent applicability for the selective determination of APs in milk. Graphical abstract
研究领域:
分析化学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
ATMOSPHERIC ENVIRONMENT
·
2023
·
IF 5
Fangjie Wang,Xiaoning Chen,Huichen Li,Bowen Huang,Yu He,Zongwei Cai
The interest in the contaminants in PM 2.5 1 (PMs with a diameter of <2.5 μm) has increased because of its potential adverse effects on human health. In this study, seven alkylphenols (APs), which are a typical endocrine-disrupting chemicals (EDCs), were measured by atmospheric pressure gas chromatography-tandem mass spectrometry (APGC-MS/MS). The methods were successfully applied to analyze the PM 2.5 samples collected from Taiyuan and Guangzhou. The total concentration of seven APs was 700.58 pg m −3 in Guangzhou and 916.12 pg m −3 in Taiyuan. The dominant PM 2.5 -bound APs were 4-pentylphenol (4-PeP), 4-nonylphenol (4-NP), and 2-6-di-tert-butyl-4-(hydroxymethyl)phenol (BHT-OH). Meanwhile, a higher concentration of APs was observed in Taiyuan during spring and winter, according with obvious seasonal variation. The presence of APs in air samples from Guangzhou was primarily attributed to human activities. Furthermore, estimated daily intakes (EDIs) of APs via ambient inhalation were calculated for different age groups to evaluate human exposure risk, which revealed that the worst-case EDI for children was 61.29 pg kg bw −1 day −1 , indicating that the presence of APs in the atmospheric environment should not be underestimated.
研究领域:
环境科学
·
公共卫生
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Fuhang Mai,Zhe Wen,Yunfei Bai,Zewei Ma,Kai Cui,Kai Wu,Fei Yan,Hong Chen,Yongdan Li
A WO3/γ-Al2O3 catalyst prepared by an incipient-wetness impregnation method is employed in the selective conversion of enzymatic hydrolysis lignin (EHL) into various alkylphenols in supercritical ethanol. In the reaction, EHL is completely dissolved and converted into aliphatic and aromatic compounds with a total yield of 363.4 mg/g lignin at 320 °C for 8 h. The yield of aromatic compounds is 315.8 mg/g lignin, accounting for 86.9% of the total yield of the products, and the overall selectivity of alkylphenols reaches 67.5%. Compared to WO3 and H2WO4, the WO3/γ-Al2O3 shows a higher activity for the conversion of EHL in supercritical ethanol. Besides, ethanol is found to be the most effective solvent for the depolymerization of EHL with the WO3/γ-Al2O3 catalyst. The WO3/γ-Al2O3 keeps the high catalytic activity in three reuses.
研究领域:
生物化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Jing Li,Yalin Wu,Huahua Bai,Xiangli Wen,Qingxiang Zhou,Yongyong Yuan,Yongli Liu,Chunmao Chen,Libing Guo
The influence of alkylphenols to environment cannot be ignored, as they are common product from chemical industries and potential threat to human health. Some alkylphenols are listed as persistent toxic substances (PTS) by the United Nations Environment Programme (UNEP). In this study, the optimized magnetic reduced graphene oxide (MrGO) was synthesized by a facile solvothermal method, and investigated for adsorption of three typical alkylphenols. In neutral condition, MrGO showed extremely high adsorption capacity of three typical alkylphenols, 4-heptylphenol (4-HP), 4- tert -octylphenol (4-OP), and 4-nonylphenol (4-NP), which could reach 938.9 mg g −1 (40 °C), 987.8 mg g −1 (40 °C), and 989.7 mg g −1 (20 °C), respectively. This study revealed that the adsorption process was a heterogeneous multi-layer physical adsorption, and the adsorption rates were related to the number of unoccupied vacancies on the adsorbent surface. From batch experiments and density functional theory (DFT) calculations, the main adsorption interactions between MrGO and alkylphenols were deduced to be π–π, hydrogen-bond, and hydrophobic interactions. What's more, the different affinities of MrGO towards different targets were further distinguished and explained in detail. The wonderful stability and recyclability of MrGO made it a promising cost-effective remediation candidate.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ANALYTICAL LETTERS
·
2015
·
IF 1.03
Yuehuang Jiang,Xiaolei Zhang,Tingting Tang,Tianshu Zhou,Guoyue Shi
Using single-drop microextraction followed by high performance liquid chromatography, an effective method for the rapid extraction for endocrine disruptors, including estrogens and alkylphenols, was developed. Factors that influenced the extraction efficiency, such as hydrogen bonding, hydrophobic property, polarity, and van der Waals forces, were evaluated in detail. The results indicated that bisphenol A and estrogens were extracted effectively by the solvents with hydrogen bond acceptors and higher polarity; alkylphenols preferred solvents that could supply strong van der Waals forces or possessed π-π stacking structures and superior hydrophobicity. The optimum extraction conditions were determined, including extraction time, pH, and salt effects. Under the optimized conditions, high extraction factors (≥147) were achieved. Limits of detection for the endocrine disruptors were between 0.33 and 0.67 µg L−1. The method strategy is well suited for the determination of trace levels of endocrine disruptors in environmental water.
研究领域:
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）