CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Zhiyue Dong,Liang Zhang,Jiang Gong,Qiang Zhao
Covalent organic frameworks (COFs) nanostructures capable of efficient visible light absorption, complete holes-electrons separation, and reactant enrichment remain a synthetic challenge for advanced photocatalysts. Herein, we rationally design a novel Cu-coordinated terpyridyl-based, 2D lamellar COF-909(Cu) nanorods. The coordinated single Cu sites not only dramatically enhance the visible light absorption and achieve the complete electrons-holes separation, but also provide the specific binding sites to enrich N/O-containing organic toxicants. The laminar arrangement and 1D nanochannel of COF-909(Cu) nanorods shorten the transfer distance of electrons to the active sites. As a proof of concept, it shows excellent performance in the photocatalytic degradation of sulfamethoxazole, which surpasses the-state-of-art photocatalysts. Density functional theory calculations confirm the structure-function relationship between the single Cu sites and the complete electrons-holes separation as well as strong binding sites for target molecules.
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高影响因子
Colloid and Interface Science Communications
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2020
·
IF 2.831
Ziyang He,Qiang Huang,Liucheng Mao,Hongye Huang,Meiying Liu,Junyu Chen,Fengjie Deng,Naigen Zhou,Xiaoyong Zhang,Yen Wei
In this study, we developed a rapid microwave-assisted Diels-Alder reaction to prepare hydroxylated ND; then the ionic copolymers functionalized ND composites were obtained through direct surface-initiated Ce(IV)/HNO 3 redox polymerization by utilization of the hydroxyl groups and the resultant ND based composites were utilized for adsorptive removal of copper ions. The results demonstrated the Pseudo-second-order model can well describe the adsorption kinetic of ND-poly(AA -co- MPC) and it has been confirmed that the adsorption behavior is initiative and endothermic and related thermodynamic parameters (△G, △H, △S). The Langmuir isotherm model is better to describe the adsorption isotherms and the temperature experiment results show the best pH environment is pH 7–9. The results above demonstrated the ND-poly(AA -co- MPC) prepared by Ce(IV)/HNO 3 redox polymerization shows great potential in environmental treatment and remediation and the easy, mild, hydrous polymerization strategy can be exampled in the field of material surface modification.
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CHROMATOGRAPHIA
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2020
·Vol. 83
·期 8
·927-932
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IF 1.596
Liu Xiaobo,Zhang Ying,Shang Meijie,Zhu Liping,Yu Min
The effects of furoic acid and furfuryl alcohol on the detection of furfural in transformer oil were studied using the traditional liquid–liquid extraction combined with high-performance liquid chromatography (LLE-HPLC) technology, in which, the methanol used as extraction agent and the C18 column and ultraviolet−visible detector were used as the separation and detection units for the determination of the furfural. The results show that the presence of furfuryl alcohol or furoic acid increases the extraction efficiency of furfural from 42.07 to 73.21% and 65.33%, respectively. The extraction efficiency of furfural decreases when the concentrations of furfuryl alcohol increase from 0.2 to 0.6 mg L −1 , but the extraction efficiency of furfural increases with the concentrations of furoic acid from 0.2 to 0.6 mg L −1 . This indicated that the accuracy of detection and extraction efficiency of furfural in transformer oil by LLE-HPLC technology may be affected by the furfuryl alcohol or furoic acid dissolved in transformer oil.
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Molecular Catalysis
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2020
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IF 3.687
Yang Zhong,Bo Zhou,Lijun Wang
Fe/FeO x embedded in LDH was prepared by reducing the pre-synthesized [Fe(C 2 O 4 ) 3 ] 3− anions intercalated LDH and used as a multi-functional catalyst for synthesis of C7-C9 compound via transfer hydrogenation between furfural (C5) and short-chain alcohols (C2-C4) and a subsequent aldol reaction of furfural with intermediate short-chain aldehydes in the absence of a homogeneous base with furfuryl alcohol as a byproduct. Screening reaction conditions, evaluation and improvement of the cyclic catalytic performance, and determination of catalytically active components were performed, and the results demonstrated that both high conversion and high selectivity to the C C bond forming product can be obtained under a non-oxidizing atmosphere of Ar or H 2 /Ar mixed gas, a reaction temperature of 140 °C and a reaction time of 4 h; the catalyst was easily deactivated during the cycle experiments, however, its catalytic stability can be effectively improved by depositing Ni with weak reducibility on the surface of Fe nanoparticles at the cost of reducing partial catalytic activity. Fe/FeO x together with LDH as a whole proved to be effective in catalyzing the transfer hydrogenation reaction and the support LDH imparted basic catalytic function to the composite realizing the aldol reaction in the absence of a homogeneous base.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Meesam Ali,Muhammad Danish,Muhammad Tariq,Ayyaz Ahmad,Khurram Shahzad Ayub,Shuguang Lyu
This study demonstrated a novel approach for prolonged benefits in groundwater remediation schemes utilizing PVA coated nano calcium peroxide (PVA@nCP) activated by Fe(II)/nFeS or Fe(III)/nFeS. Various techniques (SEM, TEM, XRD, EDS, FTIR, and BET) were used to characterize the synthesized nFeS and the prepared PVA@nCP. Trichloroethylene (TCE) was chosen as the target pollutant and its degradation performance was assessed in both Fe(II)/nFeS and Fe(III)/nFeS activated PVA@nCP systems, and the second-order reaction kinetics were determined. The effect of nFeS dose revealed its dominant role in Fe(III)/nFeS system by providing a surface platform, and at the same time, it also enhanced TCE removal in Fe(II)/nFeS system·H 2 O 2 release behavior, the participation of Fe(II) in both solution and surface, and the generated (free and surface-bound) active species (HO , O 2 − & 1 O 2 ) determined the insights of synergistic mechanisms. Electron spin resonance (ESR) identified the active species initially, which correspondingly confirmed by quenching tests. Moreover, X-ray photoelectron spectroscopy (XPS) investigated the surface reaction mechanism, showing the dominant role of S(-II) as an efficient converter of iron species as Fe(II) increased from 35% to 45% and 45.5% and Fe(III) decreased from 65% to 55% and 54.5% in Fe(II)/nFeS and Fe(III)/nFeS systems respectively. The effects of initial solution pH and common anions (Cl − , HCO 3 − , NO 3 − , & SO 4 2− ) on TCE removal were further examined, and recycling use of nFeS was investigated for its reusability in both systems. The findings of this work suggest that both systems, i.e., PVA@nCP/Fe(II)/nFeS and PVA@nCP/Fe(III)/nFeS, are novel processes and possessing potential applicability in TCE contaminated groundwater remediation.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Hai Guo,Huai-Yuan Niu,Chao Liang,Cheng-Gang Niu,Yu Liu,Ning Tang,Yang Yang,Hui-Yun Liu,Ya-Ya Yang,Wen-Jun Wang
In this work, electron-withdrawing groups functionalized few layer graphitic carbon nitride (FCN-12) nanosheet was prepared and utilized for photocatalytic activation of peroxymonosulfate (PMS). Experimental characterization and density functional theory (DFT) calculation reveals that the electronic structure of FCN-12 is efficiently adjusted by forming an upward band bending, as the functionalized carbonyl (C=O) and carboxyl (-COOH) groups can withdraw the electron from the C-N=C skeleton. With the addition of PMS, FCN-12 displays superb photocatalytic activity for chlortetracycline hydrochloride (CTC) degradation, where 83.4% CTC can be degraded within 120 min under visible light irradiation, much higher than that of bulk g-C 3 N 4 (34.3%). Besides, even under the different pH condition and co-existed anions environment, FCN-12/PMS/vis system still exhibits favorable applicability. The boosted catalytic performance is resulted from the collective effect of the few-layer feature and the energy band bending, which leads to the effective migration of photogenerated electron from FCN-12 to PMS via C=O and -COOH groups. This work not only provides an exhaustive insight into the role of energy band bending in electron-withdrawing group functionalized g-C 3 N 4 , but also paves the avenue for the development of metal-free photocatalyst-mediated environmental remediation based on PMS activation.
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CHINESE JOURNAL OF CATALYSIS
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2020
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IF 6.146
Qianqian Guo,Fan Yang,Xiaohui Liu,Mengqing Sun,Yong Guo,Yanqin Wang
Silicoaluminophosphate-34 (SAPO-34) molecular sieves have important applications in the petrochemical industry as a result of their shape selectivity and suitable acidity. In this work, nanoaggregate SAPO-34 with a large external surface area was obtained by dissolving pseudoboehmite and tetraethylorthosilicate in an aqueous solution of tetraethylammonium hydroxide and subsequently adding phosphoric acid . After hydrolysis in an alkaline solution, the aluminum and silicon precursors exist as Al(OH) 4 − and SiO 2 (OH) − , respectively; this is beneficial for rapid nucleation and the formation of nanoaggregates in the following crystallization process. Additionally, to study the effect of the external surface area and pore size on the catalytic performance of different SAPO-34 structures, the alcoholysis of furfuryl alcohol to ethyl levulinate (EL) was chosen as a model reaction. In a comparison with the traditional cube-like SAPO-34, nanoaggregate SAPO-34 generated a higher yield of 74.1% of EL, whereas that with cube-like SAPO-34 was only 19.9%. Moreover, the stability was remarkably enhanced for nanoaggregate SAPO-34. The greater external surface area and larger number of external surface acid sites are helpful in improving the catalytic performance and avoiding coke deposition.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2019
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IF 3.261
Qiwen Du,Weichen Jia,Jingyu Dai,Chao Du,Aiyun Shao,Rongmin Zhang,Yuefei Ji
Natural organic matter (NOM) contains a large number of aromatic ketones and quinones, which can produce reactive oxygen species (ROS), such as 1 O 2 and HO·, through photosensitization. These ROS play important roles in the attenuation of organic pollutants in sunlit surface water. The NOM components fractionated with XAD-8 resin at different pH influence the photo-generation of ROS, which may be related to the degree of dissociation of functional groups. In this study, probe chemicals were used to investigate the effect of dissociation degree (p K a ) of NOM model compounds on ROS production under 254 nm UV irradiation. Experimental results showed that six model compounds with similar molecular weights and structures but different p K a values have different ROS production abilities in a pH 7.0 reaction system. The ability for DHB 2,5 (2.97), DHB 3,4 (4.48), and GUA (9.99) to photo-generate 1 O 2 increased with increasing dissociation. The ability for DHB 3,4 and GUA to photo-generate HO· followed the same trend. The correlation between NOM dissociation constant and ROS generation is preliminary established, which explains the influence of functional groups. Our results may provide some basic information for understanding the correlation between NOM structural features and ROS generation.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 3
·864-875
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IF 5.721
Yang Li,Didi Li,Shisuo Fan,Ting Yang,Qi Zhou
In this work, novel dumbbell-like Mn2O3 was prepared using a low-cost and environmentally friendly template (gelatin) and applied to activate peroxymonosulfate (PMS) for pollutant degradation. The characterization results showed that dumbbell-like microstructures were formed by the self-assembly of tiny nanoparticles. Mn2O3-G (gelatin as the template) as a heterogeneous catalyst for PMS activation could effectively degrade various pollutants and exhibited an excellent degradation rate of rhodamine B (0.2333 min−1, in 30 min) for PMS activation compared to Mn2O3-C (carboxymethyl cellulose as the template), Mn2O3-N (without a template), and MnO2. The superior catalytic performance of Mn2O3-G was ascribed to its high oxygen vacancy content. The radical scavenging and EPR experiments revealed that SO4˙−, OH˙, O2˙−, and 1O2 were identified as reactive species generated from PMS activation. The oxygen vacancies participated in the generation of the reactive species. Thus, a facile and environmentally friendly method is provided for the synthesis of dumbbell-like Mn2O3 as a high-efficiency catalyst for PMS activation. Furthermore, this study shows a new mechanistic insight into PMS activation on Mn2O3.
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GREEN CHEMISTRY
·
2020
·Vol. 22
·期 3
·850-859
·
IF 9.48
Yang Qian,Ze-Jun Li,Xian-Long Du,Qi Zhang,Yi Zhao,Yong-Mei Liu,Yong Cao
Development of a highly efficient and robust catalyst with reduced usage of noble metals is extremely desirable for selective hydrogenations of furan-containing bio-based feedstocks, which represents an attractive and sustainable alternative to petrochemical resources. Herein, we describe a new type of well-dispersed Ru subnanoclusters (ca. 0.50 wt%) supported on commercial P25 TiO2 material obtained from a facile and effective amino acid-assisted deposition–precipitation strategy. The as-synthesized catalyst exhibits superior catalytic activity and selectivity for direct hydrogenation of industrially important furfural as well as a range of structurally diverse bio-based furanic compounds to their corresponding fully hydrogenated derivatives. An average turnover frequency (ATOF) value as high as 367 h−1 at 80 °C and 4 MPa H2 is obtained, which is the highest reported value. This catalyst also shows stable furfural total hydrogenation in 5 reaction cycles conducted at 80 °C (52 mmol-scale, turnover number up to 12 500). In terms of the kinetic and structural characterizations, the key performances of the ultrasmall Ru clusters are proposed to mainly originate from an enhanced number of unsaturated surface Ru atoms and change in local coordination environment. Our work highlights the importance of the subnanometric size of Ru clusters in the advancement of efficient and affordable approaches towards bio-based chemical production.
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Molecular Catalysis
·
2019
·
IF 2.938
Chenglong Dong,Hongtao Wang,Haochen Du,Jiebang Peng,Yang Cai,Shuai Guo,Jianli Zhang,Chanatip Samart,Mingyue Ding
Furfurylamine converted from biomass-based platform molecules furfural was proven a significant intermediate in the synthesis of different valuable compounds. The combination of Ruthenium with HZSM-5 was acted as an excellent selective and reusable catalyst for the reduction amination of furfural with environmentally friendly ammonia and hydrogen. Incorporation of Ru species into HZSM-5 had a significant enhancement to the acid sites of Ru/HZSM-5. The Ru/HZSM-5(46) catalyst with optimized acid sites and interaction of the Ru-O-Al bond displayed an excellent catalytic performance, producing 76 % yield of furfurylamine at only 15 min, and could be recycled five times without loss of performance. Synergistic effect between RuO 2 and metallic Ru in the Ru/HZSM-5 catalyst facilitated the reduction amination of furfural.
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APPLIED SURFACE SCIENCE
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2019
·
IF 5.155
Jingquan Wang,Hongguang Guo,Yang Liu,Wei Li,Bo Yang
In this study, porous BiFeO 3 (BFO) was successfully synthesized by sol-gel method and employed as an activator for peroxymonosulfate (PMS) to degrade bisphenol AF (BPAF), an emerging contaminant in the water. Porous BFO were prepared and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and oxygen temperature programmed desorption (O 2 -TPD). Compared to the raw BFO, large improvement of BPAF removal was observed when using porous BFO to activate PMS. The influences of selected activating systems, PMS dosage, catalysts loading, initial pH and water matrix on the degradation efficiency were examined. The role of reactive oxygen species produced in the degradation process of BPAF were identified through chemical quenching experiments and electron spin resonance (ESR), which demonstrated that high performance of porous BFO/PMS on BPAF removal was ascribed to the co-oxidation of radicals (sulfate radical and hydroxyl radical) and non-radical reactive oxygen species (singlet oxygen). Based on the XPS and ESR results, this study proved that lattice oxygen on the surface of BFO participated in the formation of singlet oxygen and the oxygen vacancies were propitious for the catalytic degradation. The reaction pathways and the mechanism of BPAF degradation via the BFO/PMS system were also proposed.
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