INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Xiaodan Wu,Changjun Cai,Qingjing Cen,Guiming Fu,Xuan Lu,Hongli Zheng,Qi Zhang,Xian Cui,Yuhuan Liu
Laccase is a green catalyst that can efficiently catalyze phenolic pollutants, and its catalytic efficiency is closely related to the interaction between enzyme and substrates. To investigate the binding effects between enzyme and phenolic pollutants, phenol, p-chlorophenol, and bisphenol A were used as substrates in this study. We focused on the removal and catalytic mechanism of these pollutants in water using yellow laccase derived from Coriolopsis gallica . The enzymatic catalytic products were characterized using Ultraviolet-Visible Absorption Spectroscopy (UV–Vis), Fourier Transform Infrared Spectroscopy (FTIR), and High-Resolution Mass Spectrometry (HRMS), and the catalytic mechanism of laccase on phenolic pollutants was further explored by molecular docking. Based on the structural characterization and molecular docking results, the possible polymerization pathways of these phenolic compounds were speculated. Laccase catalyzed phenol to produce phenolic hydroxyl radicals, their para-radicals, and ortho-radicals, which polymerized to form oligomers linked by benzene‑oxygen-benzene and benzene-benzene. P-chlorophenol produced phenolic hydroxyl radicals and their ortho-radicals, polymerizing to form oligomers connected by benzene‑oxygen-benzene or benzene-benzene. The C C bond of the isopropyl group of bisphenol A broke to formed an intermediate product, which was further polymerized to formed a benzene‑oxygen-benzene linked oligomer.
研究领域:
环境生物学
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酶催化
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污染治理
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DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Shuyu Chen,Zhengkai Wu,Xueying Cheng,Lu Chen,Yunning Chen,Yingna Guo,Changhua Wang,Qingkun Shang
In this work, we used a simple hydrothermal method to in-situ grow Zn 3 In 2 S 6 on MIL-100(Fe) octahedra, and obtained a MIL-100(Fe)@Zn 3 In 2 S 6 Z-scheme heterojunction photocatalyst. We systematically studied its performance in degrading phenol and p-nitrophenol (PNP) under visible light. MIL-ZIS 6 -2 can remove 89.1 % of phenol within 120 min and nearly 100 % of PNP within 60 min. Its photocatalytic activity to the degradation of phenol is 30.7 times and 1.7 times higher than that of MIL-100(Fe) and Zn 3 In 2 S 6 , respectively. And the photocatalytic activity to degrade PNP is 18.2 times and 1.4 times higher than MIL-100(Fe) and Zn 3 In 2 S 6 . Further research was conducted on its band structure and photocatalytic response mechanism through photoelectric performance, ultraviolet photo-electron spectroscopy, and electron spin resonance spectrometer testing. The results showed that the formation of Z-scheme heterojunction not only increased the specific surface area of the composite photocatalyst, enabling it to provide more reaction sites, but also effectively suppressed the recombination of photogenerated holes and electrons, improving the redox ability of the photocatalyst. This work provides a new perspective for constructing efficient Zn 3 In 2 S 6 -based composite photocatalysts and addressing environmental issues.
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
ACS ES&T Engineering
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2021
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IF 0
Cong Wang,Shao-Yi Jia,You Han,Yang Li,Yong Liu,Hai-Tao Ren,Song-Hai Wu,Xu Han
Enzymatic polymerization of phenolic contaminants to polyphenolics by H2O2 is an effective method to turn phenolic wastes to useful polymers. However, the sensitivities and the high costs of enzymes always limit their applications in the long-run treatment of industrial wastewater. In this study, a highly efficient CuO-persulfate (PS) system is reported to be a promising candidate for enzyme–H2O2 and shows high reactivity to polymerize various phenolic contaminants to polymers under alkaline conditions with the ratio of PS/phenolics less than 2.0. Compared with the generally accepted mechanism that the oxidizing species of SO4•– and ·OH generated during PS activation primarily contribute to the oxidation of various organic contaminants, quenching experiments, EPR (electron paramagnetic resonance) analysis and DFT calculations in this study indicate that PS is activated on CuO via a nonradical pathway under alkaline conditions, and the O–O bond in PS is moderately elongated from 1.45 to 1.58 Å. The inversely linear relationship between log kobs and BDEO–H values of various phenolics in the Hammett plot confirms H-abstraction from various phenolics under alkaline conditions. DFT calculations further reveal the formation of phenolic radicals after the activated PS abstracts H from phenolic −OH, followed by subsequent polymerization of phenoxyl radicals to polyphenolics. Characterizations of the oxidation products confirm that more than 80% phenolic contaminants have been transformed to polyphenolics. This study provides a new alternative for recovering various phenolic contaminants from industrial wastewater.
研究领域:
环境科学
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化学工程
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DOI
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zhao Song,Yu Zhang,Peiru He,Xuesong Liu,Nanqi Ren,Yidi Chen
Phenolic pollutants are highly toxic and can affect the growth and reproduction of aquatic organisms, as well as contaminate drinking water resources, posing a significant threat to both ecological and human health. However, conventional biological treatment processes are constrained in treating high salinity organic wastewaters due to the potentially lethal effects of high concentrations of dissolved salts on microorganisms. While advanced oxidation processes have shown promise in removing phenolic contaminants from high-saline wastewater, their widespread application is always limited by the high costs associated with energy and chemical usage. In this study, we explored the potential application of directly introducing peroxymonosulfate (PMS) and peracetic acid (PAA) to high-salinity water for the removal of nine phenolic contaminants. By establishing a correlation between the degradation rate constants in the PMS/Cl – ( k PMS ) and PAA/Cl – ( k PAA ) systems and various molecule descriptors, two multiple linear regression models were developed to predict the degradation rate constants under investigation. Additionally, we selected bisphenol A (BPA) as the target contaminant and investigated the impact of common ions found in natural water, such as HCO 3 – , NO 3 – , and humic acid, on the removal of BPA using two systems. Finally, we conducted experiments using tap water and sewage water to demonstrate the practical application and performance of the two systems. These experiments aimed to provide valuable insights into the influence of background chloride on PMS and PAA activation, as well as the potential of direct PMS/PAA introduction for eliminating phenolic micropollutants from high-saline wastewaters.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Shunyao Li,Dan Hong,Wenjun Chen,Jun Wang,Kai Sun
Humification processes of phenolic pollutants may play a profound role in environment purification and plant growth. However, little literature is performed to explore exoenzyme-driven humification to polymerize 17 β -estradiol (E2) and humic constituents (HCs), and the effects of their polymeric precipitates on plant growth are usually overlooked. Herein, E2 conversion and radish ( Raphanus sativus L.) growth were systematically investigated under humification mediated by extracellular laccase (EL) of Trametes versicolor . Results disclosed that EL-assisted humification achieved a wonderful E2 conversion efficiency (>99%) within 2-h, but the presence of HCs such as humic acid (HA), vanillic acid (VA), and ferulic acid (FA) impeded E2 elimination significantly. Compared with HC-free, the kinetics constants declined by 2.84-, 5.72-, and 5.22-fold with HA, VA, and FA present, respectively. Intriguingly, three close-knit self/cross-linked precipitates ( i.e. , E2-HA, E2-VA, and E2-FA hybrid precipitates) in dark gray, dark brown, and deep yellow were created after a continuous humification by phenolic radical-initiated polymerization mechanisms. The formation of these humified precipitates was extremely effective on circumventing phytotoxicity caused by monomeric E2, VA, or FA. Furthermore, they acted as humic-like organic fertilizers , accelerating seed germination, root elongation, and enhancing NaCl-tolerance of radish through the combination of oxygen-contained functional components and auxin structural analogues with unstable and stubborn carbon skeletons. This is the first study reporting the pollution purification and plant growth promotion in EL-activated humification. Our findings frame valuable perspectives regarding the natural detoxification and carbon sequestration of phenolic pollutants and the application of their polymeric precipitates in global crop production.
研究领域:
环境科学
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植物学
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生物化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Haotian Liu,Chuang Wang,Yi Yang,Minghui Gao,Aifang Xue,Hao Chen,Xing Ding
The preferential degradation of specific harmful organic pollutants in photocatalytic processes is critically important, yet remains a significant challenge due to the uncontrolled nature of reactive species, particularly those with high oxidation potentials such as •OH and h + . In this work, we designed an iodine-doped Bi 2 MoO 6 semiconductor to establish a system for photo-induced H 2 O 2 generation. The incorporation of iodine led to a steady enhancement in the selective photo-degradation of para -substituted phenolic pollutants, known precursors to carcinogenic p-benzoquinones, facilitated by the activation of iodine radicals through H 2 O 2 . This system exhibited impressive photo-degradation (96 %) and mineralization efficiency for acetaminophen (APAP), along with superior environmental applicability. It also demonstrated selectivity in degrading phenols with para -substitutions. The in-situ generation and activation of H 2 O 2 and •I were identified as the crucial pathways in this photocatalytic system. This work provides a novel modification path to accomplish the simultaneous generation and utilization of H 2 O 2 in the photocatalytic system and ultimately makes a remarkable performance for the targeted remediation of environmental pollutants.
研究领域:
环境科学
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光催化材料
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污染治理
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Pan Yang,Jinlan Tang,Zhuorui Ding,Yiqun Chen,Zizheng Liu,Jianping Yuan,Yuhua Zhu,Pengchao Xie
Carbocatalysts, widely regarded as eco-friendly catalysts in the field of peroxymonosulfate (PMS) activation for pollutant removal, exhibit significant variations in performance depending on the type of carbon atom hybridization. Notably, the novel graphdiyne (GDY), characterized by its sp-hybridized carbon (sp-C), has recently garnered significant attention. However, the precise mechanistic role of sp-C on PMS activation remains unclear. Herein, we elucidate the role of sp-C on PMS activation and the corresponding mechanism behind enhanced phenolic pollutant degradation over the GDY catalyst. GDY demonstrates exceptional phenolic removal efficiency (97 %), which far exceeds that of traditional sp 2 -hybridized graphene (2 %). The GDY facilitates pollutant oxidation via a catalyst-mediated electron transfer mechanism. The sp-C provides additional sites for PMS adsorption and donates significantly more electrons from GDY to PMS (0.51 e more than graphene), effectively facilitating PMS activation, intermediate species conversion, and reaction kinetics during phenolic pollutant degradation. By integrating the monolithic GDY catalyst into a flow-through device for continuous phenolic pollutant removal, long-lasting phenolic removal was maintained for over 80 hours, with a removal rate exceeding 85 %. This work highlights that sp-C in GDY effectively enhances PMS activation, providing a pathway for efficient organic pollutant degradation in advanced oxidation processes.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Yanyang Liu,Liqing Li,Zheshan Duan,Qingliang You,Guiying Liao,Dongsheng Wang
In this work, a chitosan modified nitrogen-doped porous carbon composite (CS-NPC) with abundant micropore and mesopore was prepared by the hydrothermal carbonization combined with chemical activation, and used as an adsorbent for phenolic pollutants removal. The CS-NPC composite were characterized by the field emission scanning electron microscopy (FE-SEM), N 2 adsorption-desorption curves, X-ray photoelectron spectrum (XPS), X-ray diffraction (XRD) and Raman. It was found that the resulting carbon material owned large specific surface areas (2189.88 m 2 g −1 ) and total pore volume (1.123 cm 3 g −1 ), and its micropore and mesopore volume was 0.494 and 0.629 cm 3 g −1 , respectively. Batch adsorption experiments were carried out to study the impact of various factors like solution pH value, contact time and ionic intensity. The adsorption process can be described by the pseudo-second-order kinetic model and Langmuir adsorption isotherm model. And at 298 K, the adsorption capability of the CS-NPC composite for phenol, BPA and 2,4-DCP was 254.45, 675.68 and 892.86 mg g −1 , respectively, which was much higher than that of previously reported carbon-based materials due to its own high specific surface areas, abundant functional groups ( NH 2 , −OH) and porous structure. The adsorbent still remained excellent regeneration after five cycles. And the CS-NPC composite can be regarded as a broad-spectrum adsorbent toward other organic pollutants including methyl orange, methylene blue and tetracycline. This study developed a novel, low-cost and green porous carbon composite which was combined with the advantage of both phenolic resin and CS, and the CS-NPC would be an outstanding adsorbent for the removal of various organic contaminants from wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xiaoyan Chen,Jiangdong Cui,Xinyu Yang,Taoyue Yuan,Jiacheng Ge,Mengtao Ma,Shunke Ding,Wenhai Chu
The core bottleneck in water decontamination lies in trigging the selective removal of trace contaminants in the presence of complex water matrices, overcoming the inevitable consumption of oxidants and energy input by the water matrix. Here, the selective removal of phenolic contaminants with permanganate (PM) oxidation mediated by 2,2,6,6-tetramethylpiperidinooxy (TEMPO)-functionalized silica (SiO 2 @TEMPO) was firstly reported. SiO 2 @TEMPO was synthesized by covalently bonding 4-oxo-2,2,6,6-tetramethylpiperidinooxy onto SiO 2 through a 3-aminopropyltriethoxysilane bridge. The loading capacity of Wt% for nitrogen element in SiO 2 @TEMPO are 1.01–1.27 %. The degradation rate of tetracycline (around 1.50 min −1 ) with SiO 2 @TEMPO/PM are around 15 folds higher than that with PM, attributed to the formation of the reactive N-oxoammonium cation via single-electron transfer during PM oxidation. SiO 2 @TEMPO exhibited excellent stability and recyclability after five consecutive cycles of tetracycline degradation. Three transformation pathways (hydroxylation, demethylation, and dehydration) for tetracycline degradation by SiO 2 @TEMPO/PM were proposed based on the identification of 36 transformation products using HPLC/Q-Orbitrap HRMS. Thereinto, the attack of the N-oxoammonium cation in SiO 2 @TEMPO on the phenolic hydroxyl group to form corresponding hydroxylation and quinylation products accounted for the dominant degradation pathway. SiO 2 @TEMPO/PM also demonstrated remarkable adaptability across a wide pH range of 5.0–9.0, indicating its potential for practical applications. The significant resistance to the inhibitory effects of co-existing water matrix components (humic acid, cations and anions), along with the marked differences in degradation efficiency between phenolic and non-phenolic contaminants, demonstrate the selectivity of SiO 2 @TEMPO/PM towards phenolic contaminants. These results offer new insights into the selective removal of phenolic contaminants and pave the way for the development of efficient and sustainable strategies for water remediation.
研究领域:
环境科学
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化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Yuge Wang,Huiyu Duan,Hao Li,Jianzheng Zhen,Weiyang Lv
The application of MoS 2 as an emerging cocatalyst in wastewater treatment is of great significance, but the efficiency of cocatalyst is often limited due to its easy agglomeration and insufficient interaction with the catalyst. Here, we used layered double hydroxide (LDH) as the catalyst and the growth template of MoS 2 to achieve an efficient combination of catalyst and cocatalyst in the removal of organic pollutants by peroxymonosulfate (PMS) activation. The outcomes showed that the MoS 2 intercalated LDH composite samples (MLDH) owned excellent phenol degradation performance, reaching nearly 100% removal within 10 min, and the calculated apparent rate constants were 2.3, 5.6, 17.7 and 19.8 times higher than that of the samples of directly growing MoS 2 on the LDH (M@LDH), physically blended MoS 2 and LDH samples, LDH and MoS 2 , respectively. Based on the results of electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS), SO 4 •- had a major impact on the elimination of phenol, Mo(Ⅳ) in MoS 2 also participated in and encouraged the Fe(Ⅲ)/Fe(Ⅱ) redox cycle, providing the driving force for the further activation of PMS . Moreover, the effects of pH value, anions, cations and water environment of MLDH during the activation of PMS were also determined, and it was found that under various catalytic environments, MLDH always maintained a high removal rate of phenol and showed strong anti-interference ability. Collectively, the results of this research would offer more possibilities and suggestions for creating highly effective catalysts for wastewater cleanup.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 10
·3402-3410
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IF 6.119
Xiaojian Xu,Jinghui Wang,Renliang Huang,Wei Qi,Rongxin Su,Zhimin He
The construction of a nanozyme that mimics a natural enzyme is a promising strategy to obtain a highly stable catalyst. Laccases are members of copper-containing oxidases, as environmental catalysts, and show significant potential in biotechnology and environmental remediation. In this study, inspired by the active site and electron transfer of laccase, a new laccase mimic (defined as CA-Cu) was synthesized via the coordination of copper with a cysteine (Cys)–aspartic acid (Asp) dipeptide. The as-prepared CA-Cu nanozyme exhibits significant laccase-like activity and catalytic oxidation of a wide range of phenolic pollutants, such as 2,4-dichlorophenol, phenol, p-chlorophenol, 2,6-dimethoxyphenol, hydroquinone, o-nitrophenol and o-aminophenol hydroquinone. It has a similar Km (Michaelis constant), a higher vmax (maximum rate) and better recyclability than laccase at the same mass concentration. In addition, the CA-Cu nanozyme is robust in a broad temperature range (0–100 °C), at extreme pH and under long-term storage. Surprisingly, the catalytic performance of the CA-Cu nanozyme was enhanced under high-salt conditions or at high concentrations of heavy metal ions, which lead to severe loss in the catalytic activity of laccase. We believe that this nanozyme is a promising environmental catalyst for the treatment of phenolic pollutants under high-salt or heavy metal ion conditions.
研究领域:
环境科学
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生物化学
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材料科学
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DOI
高影响因子
CHEMOSPHERE
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2020
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IF 5.778
Hailu Demissie,Guangyu An,Ruyuan Jiao,Gefei Ma,Libing Liu,Hongyan Sun,Dongsheng Wang
Recent water treatment plants require multi-process techniques to remove contaminants from aqua media. In this study, we investigate the novel, in situ coated sodium dodecylsulphate (SDS), on kegging Al 30 nanocluster as a single water treatment alternative for the removal of phenolic contaminants and suspension. FTIR, TEM-EDX and Zeta potential analysis characterized the nanocluster decoration. The resulting property was examined by emission (λ-max) of the molecular probe, the online aggregate image of fluorescence microscopy, and mixing isochrone, fat-soluble dye solubilization . The coated media was examined as nearly resembling the hydrophobicity of 1-octanol. The elemental line scanning and mapping showed different morphologies of floc depending on the SDS concentration. The material was found to follow Brownian motion to enmesh suspended particles like a ladder, and served as entrapper for small organic contaminants by the sorbed SDS aggregate, based on their log K O/W . About 85% and ≥95% removal archived for contaminants with the least and highest K O/W value, respectively. The residual solutes in the supernatant were well decomposed by using a bacterial agent. One-step removal (less footprint) and ease of operation make this approach an environmentally compatible and cost-effective alternative for the large-scale treatment process.
研究领域:
环境科学
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材料科学
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生物学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）