JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Rongzheng Zhang,Lei Wang,Juan Han,Jiacong Wu,Chunmei Li,Liang Ni,Yun Wang
Enhancing the catalytic activity and stability of enzymes is of great importance in the development of green chemical and cost-effective application, with removal of bisphenol A (BPA) as a prominent example. Engineering immobilization carriers and immobilization methods of enzymes endows great potential to achieve above goal. Until now, these reports have focused on employing the metal-organic frameworks (MOFs) to increase the stability and reusability of enzymes, an enhancement in its catalytic activity has yet to be addressed. This work introduced a biomimetic mineralization process for facile synthesis of laccase@HKUST-1 biocomposite under mild condition. By exploiting the activity of laccase@HKUST-1, we demonstrated, for the first time, that the integration of laccase and HKUST-1 containing cofactor Cu 2+ ions leaded to 1.5-fold enhancement in the catalytic activity compared with free laccase, which was due to the synergistic enhancement of substrate oxidation. Indeed, the laccase@HKUST-1 biocomposite could function as active biocatalysts under biologically challenging conditions, such as acidic condition, high temperature, organic solvent, and continuous operation. The oxidation of phenols, such as BPA, with laccase@HKUST-1 reached higher catalytic performance than free laccase, and gave 100% degradation efficiency within 4 h. This study provides a feasible method to improve the activity and stability of laccase, which enable completely remove of BPA from the environment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Mantang Chen,Nan Wang,Lihua Zhu
Single-atom catalysts with a maximum atomic utilization are promising in wastewater treatment. Herein, a single-atom dispersed Co-N-C catalyst was prepared by a calcination-acid treatment method. The obtained Co-N-C was confirmed to possess excellent performances of both adsorption and catalytic ability of activating peroxymonosulfate (PMS). It was found that the adsorption performance was related to the surface area and pore volume and the removal of bisphenol A (BPA) was determined by the defect density of the catalyst. It was observed that a calcination temperature of 900 °C yielded the best Co-N-C catalyst named Co-N-C-900. All the added BPA (80 mg L −1 ) was completely degraded in 3 min by using 0.5 g L −1 Co-N-C-900 and 0.3 g L −1 PMS with a degradation rate constant ( k ) of as high as 2.81 min −1 . In this single-atom catalytic system, the main reactive species were confirmed to be singlet oxygen. A mechanism study suggested that the fast and efficient degradation of BPA was attributed to the synergistic effect between fast adsorption of mesoporous carbon and efficient catalysis of single-atom Co-N x complex.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Zhong-Shuai Zhu,Xiao-Jie Yu,Jin Qu,Ya-Qiong Jing,Yasmine Abdelkrim,Zhong-Zhen Yu
Low crystalline flowerlike cobalt silicate hydroxide (Co 3 (Si 2 O 5 ) 2 (OH) 2 , CoSiO x ) is synthesized by a one-pot hydrothermal approach. Abundant highly active Co OH + is preformed on the surface of CoSiO x , while the low crystallinity of CoSiO x leads to the formation of active 1 O 2 caused by the generation of oxygen vacancy in the valence change cycle between Co 2+ and Co 3+ . The optimal CoSiO x with a high specific surface area of 665.2 m 2 g −1 could expose surface Co OH + , thus rapidly activate peroxymonosulfate (PMS) and accelerate catalytic efficiencies. As a result, at least 11 kinds of organic pollutants could be degraded with 33–242% higher efficiencies than reported. In addition to the common SO 4 - and OH, large amounts of active 1 O 2 endow the CoSiO x /PMS system with superb catalytic performances in diverse conditions, suggesting the excellent adaptability for practical usage. This work provides a new protocol to advance the PMS activation process for high-performance cobalt based heterogeneous catalysts.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Junqin Liu,Pingxiao Wu,ShanShan Yang,Saeed Rehman,Zubair Ahmed,Nengwu Zhu,Zhi Dang,Zehua Liu
This work presents a novel strategy for peroxydisulfate (PDS) activation under controlled non-radical/radical mechanism, which is based on a photo-switch over layered CuFe oxide (CFO). The non-radical mechanism is attained by CFO under dark environment, and the radical mechanism is achieved through the visible light irradiation. Electron paramagnetic resonance (EPR) and density functional theory (DFT) studies demonstrate the non-radical activation mechanism is conducted by the polarization effect of CFO to PDS molecule. The radical mechanism could be elucidated by the one-electron reduction of the PDS by excited electrons on conduction band of CFO. Products analyses based on HPLC-MS and Fukui functions suggest that the non-radical degradation pathway could decrease the generation of halide intermediates, whereas the radical pathway may not be observed with this property. Quantitative structure-activity relationships (QSARs) were established between the observed pseudo-first-order rates of various phenolic pollutants and the classical descriptors (i.e., Hammett constant, Pka, E HOMO and E LUMO ) in the non-radical and radical systems, respectively, to give instructions of pathway choice for different pollutants. Considering the non-radical/radical pathway both have their own unique strengths (e.g., non-radical pathway has high selectivity to pollutants and high utilization efficiency of oxidant, and radical pathway has considerable degradation rate and strong mineralization ability), these pathways should be chosen wisely for pollutant degradation according to reality conditions.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jiawei Lin,Yongyou Hu,Luxiang Wang,Donghui Liang,Xian Ruan,Sicheng Shao
In this study, we synthesized a typical iron-based metal-organic framework, MIL-88B (Fe), and constructed a MIL-88B (Fe)/persulfate/visible light (M88/PS/Vis) system for photocatalytic degradation of bisphenol A (BPA) in aqueous solution. The removal efficiency, environmental factors, and degradation mechanism and pathways were explored. The results showed that there were synergistic effects in the M88/PS/Vis system: BPA (10 mg/L) could be removed completely within 25 min with 0.6 g/L M88 and 2 mM PS under visible light, while the removal rates with individual M88/Vis or M88/PS was only 26.0% and 34.1%, respectively. In addition, the BPA degradation rate in the M88/PS/Vis system (0.107 min −1 ) was 4.7 times higher than that in the M88/PS system (0.023 min −1 ) and 8.9 times higher than that in the M88/Vis system (0.012 min −1 ), respectively. Additionally, environmental factors could strongly impact the degradation of BPA in the studied system in which O 2 − and SO 4 − played a dominant role. More importantly, risk assessment in the BPA/M88/PS/Vis system was, for the first time, estimated in our study via the “ecological structure activity relationships” program at three trophic levels and Cell Counting Kit-8 method. Although there were some intermediates with higher biological toxicity than BPA and increased the toxicity of solution, most intermediates were one or more level less toxic than BPA. In most cases, the toxicity of solutions were lower than the initial samples, which demonstrated the effectiveness of M88/PS/Vis system in the reduction of toxicity of BPA, and the toxicity hazard in general could be effectively avoided by prolonging the duration of light exposure. This research provides a profound understanding of the potential application of PS activation by photocatalyst for both BPA removal and toxicity shift under visible light.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2019
·
IF 5.026
Peng Mei,Huihui Wang,Han Guo,Ning Zhang,Sailun Ji,Yapeng Ma,Jiaqi Xu,Ying Li,Hamed Alsulami,Mohammed Sh Alhodaly,Tasawar Hayat,Yubing Sun
A new photocatalyst of TiO 2 /C 3 N 4 composite (TiO 2 /g-C 3 N 4 ) was synthesized by the hydrothermal method. The characterization showed that TiO 2 /g-C 3 N 4 extended absorption light range and enhanced generation efficiency of photo-induced electron. Under the simulated solar irradiation, the photodegradation rate of bisphenol A (BPA) by TiO 2 /g-C 3 N 4 was twice as fast as that of g-C 3 N 4 . Furthermore, TiO 2 /g-C 3 N 4 presented the good stability and excellent selectivity for BPA degradation. The high degradation rate of BPA by TiO 2 /g-C 3 N 4 was demonstrated to be superoxide radical (·O 2 − ) and singlet oxygen ( 1 O 2 ) by radical quenching experiment, which was further evidenced by EPR, XPS, DRS and PL analysis. These findings revealed that TiO 2 /g-C 3 N 4 can be used as a potential photocatalyst for removing organic pollutants in actual environmental remediation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Bao-Cheng Huang,Gui-Xiang Huang,Jun Jiang,Wu-Jun Liu,Han-Qing Yu
Carbon-based materials are recognized as promising candidates for pollutant degradation because of their environmental benignity. Massive and cost-effective production and efficient recovery of carbon-based catalysts are crucial to apply this technology. However, various nanostructured carbons with different dimensions are usually utilized as precursors while not considering their complex preparation procedures and the high costs of ingredients. Moreover, catalyst separation and recovery are not given sufficient attention. In this work, a calcium salt-assisted pyrolysis strategy is proposed to tune the catalytic site formation of carbon-based catalysts. Results show that blending equal amounts of Ca2+ (calcium chloride) and organic precursors could greatly improve the catalytic activity of the carbonated product to activate peroxymonosulfate for pollutant degradation. In addition, the proposed synthetic strategy is universal to most of the readily accessed and cost-effective organic precursors. Singlet oxygen is identified as the main reactive oxidant for pollutant removal in the catalytic reaction. By cross-linking calcium ions and alginate as a hydrogel to immobilize the catalyst, the carbon material could be readily recovered. Furthermore, a long-term continuous-flow reactor test is conducted to validate the effectiveness of applying the immobilized catalyst to treat a synthetic wastewater with 0.5 mM bisphenol A. As a result, a green synthesis and immobilization strategy for persulfate catalysts is successfully established, and the prepared catalyst might be applied for wastewater treatment through using calcium salt in two purposes.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 44
·期 4
·1245-1252
·
IF 3.069
Shi-Wen Lv,Jing-Min Liu,Ning Zhao,Chun-Yang Li,Zhi-Hao Wang,Shuo Wang
The issue of environmental pollution is currently more and more serious, and developing an effective method with universal applicability for removing various contaminants is pretty necessary. Herein, a novel photocatalyst denoted as Co-doped MIL-53-NH2(Fe : Co 4 : 1) was constructed via a feasible solvothermal method, which served as an efficient mediator to activate peroxydisulfate for degrading various organic pollutants. Results from the current work indicated that doping Co with an appropriate proportion could enhance the optical absorption intensity of MIL-53-NH2 and reduce the band gap. Furthermore, a Co ion acting as a mediator could facilitate the charge transfer through a Co3+/Co2+ redox pathway, and thereby suppress the recombination of photogenerated electron–hole pairs. More interestingly, the Co-doped MIL-53-NH2 exhibited excellent and extensive degradation abilities for various organic pollutants including bisphenol A (BPA), antibiotics and organic dyes in the presence of peroxydisulfate (PS) under visible light irradiation. It was also found that ˙OH and SO4−˙ were the major contributors to the catalytic process. Total organic carbon (TOC) analysis indicated that the majority of the contaminants were degraded into CO2 and H2O. Even in the real samples, the developed Co-doped MIL-53-NH2/PS/solar system still possessed excellent performance for the degradation of BPA. Possible photocatalytic mechanisms and the kinetics were also investigated. Besides, the Co-doped MIL-53-NH2 had good catalytic reusability and stability. To sum up, this study provides a promising approach for removing organic pollutants from wastewater.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SEPARATION SCIENCE
·
2019
·Vol. 42
·期 22
·3451-3458
·
IF 2.516
Lili Lian,Xinhao Jiang,Jinyi Lv,Fengkun Bai,Bo Zhu,Dawei Lou
Glucose-derived carbon-decorated magnetic microspheres were synthesized by an easy hydrothermal carbonization method and used as a high-efficiency adsorbent to extract bisphenols in water and tea drinks. The as-prepared carbon-decorated magnetic microspheres had a well-defined core–shell structure with a shell thickness of about 5 nm. The microspheres possessed high saturation magnetization at 60.8 emu/g and excellent chemical stability in aqueous solution. The experimental parameters affecting the extraction efficiency, including extraction time, pH, adsorbent dosage, desorption solvents, desorption time, and solution volume were evaluated. Electrostatic and π–π interactions were the major driving forces during extraction. Overall, a new magnetic solid-phase extraction method of determining bisphenols was developed on the basis of as-prepared magnetic microspheres. The method had a wide linear range, low limits of detection (0.03–0.10 µg/L), and high recoveries (85.4–104.6%).
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Dongli Wei,Jiachen Li,Zhongshan Chen,Lijun Liang,Junping Ma,Mingzhi Wei,Yuejie Ai,Xiangke Wang
A kind of magnetic covalent organic frameworks (Fe 3 O 4 @TpND) is successful synthesized by the solvothermal method . The synthesis process involves two steps, where the first step corresponding to the synthesis and amino- modification of magnetic particles (Fe 3 O 4 -NH 2 ) and the second step launched with COF polymerization outside Fe 3 O 4 -NH 2 . This kind of novel materials (Fe 3 O 4 @TpND) could inherit the physicochemical superiority of COF plane and the easy recoverability of Fe 3 O 4 . The experimental results confirm that Fe 3 O 4 @TpND possessed a favorable adsorption capacity (114.97 mg L − 1 , at 298 K and pH 6.0), rapidly uptake rate, a broad pH range, and superior renewability on the removal of bisphenol-A (BPA). To shed more light on the sorption mechanism, both of static density functional theory (DFT) calculation and molecular dynamic (MD) simulation are introduced to portray the molecular-scale interaction between TpND and BPA. By exploring the geometric structures, as well as the energetic and electronic properties of the complex, the phenolic aldehyde groups in TpND were found to exert significant contribution to capture BPA molecules via the hydrogen bonding effects. From the perspective of dynamic MD simulation, the size of BPA cluster and physical pore structure of the adsorbent also possess a remarkable aggregating effect on the sorption process. Accordingly, this study provides crucial fundamental and valuable knowledge of COF materials applied in the field of water purification .
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2019
·
IF 3.858
Lili Lian,Xinhao Jiang,Junjiao Guan,Zhifu Qiu,Xiyue Wang,Dawei Lou
The migration of bisphenols (BPs) can take place from plastic packaging materials into freshly cooked takeaway food, especially at high temperatures. In this study, cetyltrimethylammonium bromide - intercalated zinc oxide (ZnO@CTAB) was developed and used to extract the migration of BPs (bisphenol A and bisphenol AF) from disposable plastic materials to contained food simulates. Several experimental parameters that influence extraction efficiency were investigated. Under optimal conditions, a sensitive dispersive solid-phase extraction method based on ZnO@CTAB was proposed for the analysis of BPs coupled with ultra-high performance liquid chromatography and time-of-flight mass spectrometry. The method exhibited good linearity of calibration, high recovery (97.63–109.33%), low limits of detection 0.027–0.030 μg L −1 , and acceptable precisions. The developed method was used to carry out a migration test from two disposable plastic bags and a disposable plastic container, using distilled water at 100 °C as a hot liquid food simulant. The migration concentrations of bisphenol AF was found to be 0.42 μg L −1 and 0.86 μg L −1 for the two types of disposable plastic bags, and the concentration of bisphenol A was 0.49 μg L −1 for disposable plastic container. The proposed method was also applied to investigate the migration of BPAF from the disposable plastic bags to different food simulants, revealing that the release of BPAF levels depended on the polarity of the liquid food components.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Jiajun Long,Longqian Xu,Linghui Zhao,Huaqiang Chu,Yunfeng Mao,Deli Wu
In this study, Cu(0) was synthesized with NaBH 4 as a reducing agent for Cu(II) and used to activate dissolved molecular oxygen (O 2 ) under acidic conditions. The Cu(0) synthesized had much higher activity than the purchased. The roles of Cu was clarified and the formation of reactive oxygen species was discussed through direct detection for the first time. By detecting the valence change of Cu in a CuO system, Bisphenol A (BPA) was found to accelerate the transformation of Cu(II) to Cu(I). Besides, the evidence from electron spin resonance (ESR) studies and scavenging tests revealed the new roles of Cu(0) that Cu(0) could not only convert O 2 to produce ·O 2 − , but also catalyze H 2 O 2 to ·OH. The results from this study offer evidence of new reaction pathways in Cu-activated O 2 systems and deepen understanding of the reaction between Cu species and O 2 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）