JOURNAL OF MOLECULAR STRUCTURE
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2019
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IF 2.12
Maocai Yan,Zhen Zhang,Jinhui Zhou,Wei Li,Chunyan Zhang,Jingchang Zhang,Huannan Wang,Xuelu Yang,Shuai Fan,Zhaoyong Yang
Maleimide skeleton distributes widely in a great many substances, and maleimides are very useful building blocks in organic synthesis and many related disciplines, like bioconjugation . As an excellent leaving group, tosyloxy (-OTs) group are very popular in organic synthesis; however, reports on use of -OTs group on maleimide scaffold are very rare. In this study, 3-tosyloxymaleimide was prepared from l -tartaric acid and used to react with various phenols or naphthols under PTC condition to give 3-aryloxymaleimides through nucleophilic substitutions. Yields of the reaction were not high due to a competitive transesterification reaction; however, this reaction would be practical if the side-reaction could be suppressed by appropriate reaction conditions. The reaction mechanism was investigated by theoretical computation. The intermediates and transition states of the reaction, as well as the potential barrier and reaction free energy , were calculated using density functional theory (DFT), and influencing factors of the reaction were discussed. Theoretical computations showed that this nucleophilic substitution is favorable both kinetically and thermodynamically, while electron-withdrawing groups on phenols are harmful to such reactions. This study will provide new knowledge and insights on the chemical properties of maleimide and tosyloxy group, as well as the related chemical reactions.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2019
·
IF 4.784
Jing Qin,Hui-yang Wang,Dan Zhuang,Fan-cheng Meng,Xing Zhang,He Huang,Guang-ping Lv
A neutral polysaccharide (ALP-1) and an acidic polysaccharide (ALP-3) were purified from Atractylodes lancea (Thunb.) DC. ALP-1 exhibited a linear backbone composed of (2 → 1)-linked β - d -fructofuranose. The backbone of ALP-3 was elucidated as →4)-GalA p -(1 → 3,4)-Rha p -(1→, and with branch chain substituted at O-3 position of →3,4)-Rha p -(1→. The branch chain consists of →3,5)-Ara f -(1→, →5)-Ara f -(1→, and Ara f -(1→. Particularly, ALP-3 could significantly stimulate macrophage proliferation in a dose-dependent manner, and stimulate phagocytic, NO and cytokines production than ALP-1 on RAW264.7 cells. Besides, both ALP-1 and ALP-3 could activate T-cells in Peyer's patch cells and enhance the production of colony stimulation factors. While the ALP-3 also showed better intestinal immune system modulating activity than ALP-1. The result of this study indicated that the structure diversity of polysaccharide is crucial for its bioactivity. And also provided evidence for that carbohydrate polymers in A. lancea definitely contributed to its pharmaceutical effects.
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Environmental Chemistry Letters
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2019
·Vol. 17
·期 4
·1831-1837
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IF 4.617
Wang Shengli,Yan Linlin,Guan Xiaohui,Jia Yanping,Song Lianfa,Zhang Haifeng
Hydroxyl radicals are commonly produced either by metal activation or by using external energy. However, the application of these methods is limited by low working pH and secondary contamination with metal ions. Alternatively, the reaction between hydrogen peroxide (H 2 O 2 ) and hydroxylamine is an environmentally friendly process that generates active radicals, but the reaction rate is slow. To improve this, we report here a novel and efficient activator for the H 2 O 2 /hydroxylamine system that uses sulfate ions ( \({\text{SO}}_{4}^{2 - }\) ). We tested the effects of different systems, concentrations of H 2 O 2 , hydroxylamine and \({\text{SO}}_{4}^{2 - }\) , and pH on the degradation of Rhodamine B. The mechanism was also investigated by kinetic calculation, a radical scavenging experiment, and anions comparison. Results show that the addition of \({\text{SO}}_{4}^{2 - }\) effectively improved Rhodamine B degradation and widened the working pH. The hydroxyl radical was found to be the primary radical responsible for dye degradation. Moreover, only \({\text{SO}}_{4}^{2 - }\) shows an enhanced effect under the same ionic strength conditions. Overall, our findings reveal a new method for water purification at acidic and near-neutral pH, especially for sulfate-rich wastewater treatment.
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ANALYTICA CHIMICA ACTA
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2019
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IF 5.256
Chuyi Ni,Junlong Huang,Xintong Xie,Yueru Shi,Juan Zheng,Gangfeng Ouyang
Ordered mesoporous carbons (OMCs) are a kind of remarkable adsorbents in environment area due to high surface area, controllable pore size and superior stability. However, the inherent hydrophobicity and strong π-π interaction make OMCs have an advantage for the adsorption of nonpolar pollutants, leading to great demands for the development of new-type OMCs with outstanding adsorption efficiencies towards polar pollutants. The zirconium and nitrogen co-doped ordered mesoporous carbon (Zr/N-OMC) was obtained by directly carbonizing the composites of phenolic resin and UiO-66-NH 2 , with uniform mesopore structure, large surface area (583 m 2 g −1 ) and widely dispersed heteroatoms . Due to these prominent properties, the Zr/N-OMC was fabricated as high-performance solid phase microextraction coating. The results proved that the doping zirconium and nitrogen could act as active sites to interact with polar pollutants, resulting in fast adsorption rate and enhanced adsorption capacity. Therefore, the high-performance Zr/N-OMC-coated fiber was coupled with gas chromatography-mass spectrometry to establish sensitive analytical method for the detection of trace phenols from real water samples. This work would open up a new avenue for simple and efficient modification of OMC with enhanced adsorption performance to expand applications.
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JOURNAL OF POROUS MATERIALS
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2018
·Vol. 26
·期 3
·819-828
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IF 1.858
Tao Jianli,Liu Lujuan,Zhu Peihong,Zhai Kang,Ma Qian,Zhang Danning,Ma Jie,Zhai Yunpu,Liu Yonggang,Zhang Ruiqin
A Ni-based cage-like C–SiO 2 –Al 2 O 3 (Ni/CL-CSA) catalyst was synthesized successfully via a facile dual-templating method and used for the hydrotreatment of phenol. The catalyst was characterized by SEM, TEM, XRD, TG and N 2 adsorption techniques. Results show that Ni/CL-CSA has three-dimensional connected macroporous structure with pore size of about 100 nm and ordered mesoporous windows with average pore size of approximately 3.8 nm. Size of nickel particle is 6.1 nm. BET surface area of the catalyst is 212 m 2 /g and pore volume is 0.24 cm 3 /g. Hydrogenation and the stability performance of the catalyst was studied for bio-oil model compound phenol. Results reveal that adding macropores into Ni-based mesoporous C–SiO 2 –Al 2 O 3 (Ni/MP-CSA) can improve the mass transfer rate and reduce the particles growth, thus improve the catalytic activities in the hydrotreatment of phenol, reducing catalyst sintering at high temperature and improving the stability of the catalyst.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Ming Zhu,Jie Miao,Xiaoguang Duan,Daqin Guan,Yijun Zhong,Shaobin Wang,Wei Zhou,Zongping Shao
The deployment of an efficient catalyst is critical for successful application of peroxymonosulfate-based advanced oxidation processes to the rapid degradation of retardant organics in wastewater. Considering the rich properties of perovskite oxides and their drawbacks of low specific area and easy cation leaching, we reported a facile postsynthesis hydrothermal treatment method for preparing SrCo0.6Ti0.4O3−δ@CoOOH (SCT@CoOOH) nanocomposite as an efficient catalyst for PMS activation here. Surprisingly, CoOOH nanosheets were grown in situ over the surface of SCT substrate, resulting in a significantly increased surface area (22.1 m2 g–1), enhanced charge transfer capability, more generated surface oxygen defects and a strongly synergistic effect created between the bulk SCT and CoOOH surface layer. Remarkably, SCT@CoOOH exhibited higher (1.7 times) catalytic activity (0.84 mg L–1 min–1) for phenol degradation than SCT. Additionally, suppressed cobalt leaching was demonstrated in the SCT@CoOOH/PMS system. Notably, singlet oxygen as additional oxidative species were formed to accelerate phenol degradation in the radical-based SCT@CoOOH/PMS system due to the surface oxygen defects. The beneficial effect of higher pH value and different influence of foreign anions on the reation rate were also investigated. As a universal method, it may be also useful for the development of innovative functional materials for other various applications.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2018
·
IF 4.61
Tao Zeng,Shuqi Li,Jianan Hua,Zhiqiao He,Xiaole Zhang,Hongru Feng,Shuang Song
Nanocarbon materials are emerging as alternative activators of peroxymonosulfate (PMS) for organics decomposition. However, the relatively low activity and complex syntheses hindered their practical application and innovation with respect to rational design of carbocatalysts is highly desired. Herein, an in situ replication and transformation strategy was employed to facilely convert porous Fe 3 O 4 microspheres into novel Fe/N codoped large-pore mesoporous carbon spheres (M‑Fe/NC) as Fenton-like catalysts for PMS activation . Benefiting from the abundance of active sites induced by dual heteroatom doping, the enhanced active site exposure due to the unique mesoporous structure, and the high stability of carbon component, the derived M‑Fe/NC was superior to the pristine Fe 3 O 4 for PMS activation to degrade various organics and was efficient over a wide pH range (2–9). Compared with the proposed mechanisms of previous reports, both radical (surface-bound SO 4 − and OH) and nonradical ( 1 O 2 and direct oxidation) pathways are involved in the M‑Fe/NC/PMS system. Furthermore, experimental observations in combination with DFT calculations reveal that graphitic N and Fe N 4 sites serve as dual reaction centers in the catalysis. This research opened an avenue for development of novel multi-doped carbocatalysts used to activate PMS for sustainable remediation.
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CHEMICAL ENGINEERING JOURNAL
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2018
·
IF 6.735
Ying Liu,Xiaoyan Chen,Yulin Yang,Yong Feng,Deli Wu,Shun Mao
Cobalt-based nanostructures have shown a great potential for radical production by activating persulfate (PS). Here, we report a facile strategy to synthesize nitrogen-doped porous Co@C nanoboxes (Co@NC) by pyrolysis of zeolitic imidazolate frameworks (ZIF-67), followed by partially etching away the metallic cobalt. With a nitrogen-enriched hollow porous carbon nanobox and embedded Co nanoparticles, the Co@NC shows high efficiency in PS activation for p-Chloroaniline (PCA) removal. The degradation study shows that a complete removal of high concentration PCA is done within two minutes, which is superior to most of the reported PCA removals with PS-based advanced oxidation processes (AOPs). More importantly, the Co@NC exhibits high catalytic activities in a wide range of pH from 5 to 9. The Co@NC also shows very limited Co 2+ release with a dissolution proportion of 0.28%, much lower than previously reported Co-based catalysts, and remains high efficiency after five successive reaction cycles. A heterogeneous activation mechanism though surface reaction is proposed, in which PCA firstly absorbs on the carbon nanobox surface, then being oxidized by generated radicals and non-radical species. The unique structure and outstanding performance of Co@NC catalysts present new insights in catalyst design for PS-based advanced oxidation for organic pollutants removal in waste water.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2018
·
IF 4.61
Ruikun Wang,Qianqian Ma,Xuemin Ye,Chunxi Li,Zhenghui Zhao
Coking wastewater is used to prepare coal slurry, which can be used as combustion and gasification fuel. This promising technology simultaneously achieves resource utilization and wastewater management . Slurrying properties are essential to the industrial application of coal slurry. These properties are considerably influenced by coal surface properties and the adsorption of an additive by coal. In this study, the effects of the internal components (e.g., phenol, ammonia nitrogen, and metal ions) of coking wastewater on the adsorption of an additive by coal and on coal surface properties were measured. Results showed that the competitive adsorption between phenol and the additive reduced the amount of additive adsorbed on coal. However, phenol acted as an additive to improve the wettability of coal particles. Cations (Ca 2+ , NH 4 + , and Na + ) adversely affected the slurrying because they weakened the negative charges of coal. Furthermore, a large amount of water was adsorbed due to the ionic bonding effects, thereby reducing the free water in the coal slurry system. The maximum slurrying concentration of CWCS was 0.8 percentage points higher than that of CWS, suggesting that coking wastewater enhanced the slurrying capability of the coal slurry by integrating the various effects induced by the different internal components.
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ENERGY & FUELS
·
2018
·
IF 3.024
Youan Ji,Yucui Hou,Shuhang Ren,Congfei Yao,Weize Wu
Phenols have wide applications and much commercial value, and they are obtained from oil mixtures by separation. However, the previous separation agents have low separation efficiency or corrosive halide ions or are difficult to be regenerated. In this work, we designed several tetraethylammonium amino acid (TAAA) ionic liquids (ILs) without corrosive halide ions and found that the ILs could separate phenols from oil mixtures with much higher extraction efficiency and could be regenerated using CO2. The effects of separation time, initial phenol content, TAAA type, water content in TAAA, and phenol type on separation were investigated. It has been found that TAAA can separate phenols with high separation efficiencies, and the maximum separation efficiency of phenol can reach up to 99.0% at a TAAA:phenol mole ratio of 0.60. Meanwhile, ultimate phenol contents can reach as low as 1.40 g/dm3. The initial phenol content almost has no influence on the ultimate phenol contents. For real coal tar oil mixtures, the separation efficiency of phenols can reach up to 98.6%. The TAAAs can be regenerated and reused without significant decreases in separation efficiency of phenols. The separation mechanism has also been proposed based on chemical reactions.
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SCIENCE AND ENGINEERING OF COMPOSITE MATERIALS
·
2019
·Vol. 26
·期 1
·261-269
·
IF 0.705
Xiazhi Zhou,Wei Zhou,Dianchun Ju,Yinxian Peng,Lei Zhou,Sheng Tang,Jing Wang
In this work, hierarchical porous resins (PRs) are fabricated and applied as novel adsorbent for removal of oily substance. The oil/water (o/w) high internal phase emulsions (HIPEs), stabilized by phenolic resin precursor and tween 80, were used as the template for simultaneous polymerization of aqueous phase, methenamine, sodium persulfate and liquid paraffin. Subsequently, dopamine hydrochloride, 1-dodecanethiol and Fe 3 O 4 particles are grafted onto the interface of PRs via adhesion of dopamine and Markel addition reaction between quinone groups on dopamine and sulfhydryl groups on 1-dodecanethiol. The as-prepared composites possessed hydrophobicity and magnetic property (HPRs). The physical and chemical properties, morphology and adsorption properties of HPRs are characterized by XRD, FT-IR, TGA, SEM, N 2 adsorption-desorption isotherms. The as-synthesized HPRs composites had a typical hierarchical porous structure, and the resulted macropores with a well-defined open-cell and interconnecting pore throat structure could be controlled via the composition of the aqueous phase of emulsion. The hierarchical porous structure of HPRs contained macropores ranging from 0.3 μm to 4 μm and mesopores of 11.26 nm. HPRs have rough and hydrophobic surface (water contact angle of 130 ∘ ) with specific surface area of 15.06 m 2 /g and pore volume of 0.0349 cm 3 /g. The oil adsorption rate and the oil retention rate for toluene are 11.765 g/g and 86.43%, respectively. The oil adsorption rate in the first minute can reach more than 80% of the highest oil adsorption rate. The oil adsorption rate of HPRs after three recycling experiments can still reach 87.32%of the first-time oil adsorption rate.
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Soft Matter
·
2019
·Vol. 15
·期 31
·6411-6417
·
IF 3.399
Xun Tong,Yuan Qiu,Xiaoyu Zhao,Bijin Xiong,Rongzhen Liao,Haiyan Peng,Yonggui Liao,Xiaolin Xie
Photoresponsive supramolecular gels have aroused continuous attention because of their extensive applications; however, most studies utilize UV light, which inevitably brings about some health and environmental issues. The halogen bond is an important driving force for constructing supramolecules due to its high directionality, tunable strength, good hydrophobicity, and large size of the halogen atoms. Yet, it still remains a formidable challenge to utilize halogen bonds as a driving force to fabricate a visible light responsive gel. In this work, to fabricate such a gel, azopyridine-containing Azopy-Cn (n = 8, 10, 12) was selected as a halogen bond acceptor, while 1,2-bis(2,3,5,6-tetrafluoro-4-iodophenyl)diazene (BTFIPD) was chosen as both the halogen bond donor and visible light responsive moiety. The visible light response of BTFIPD resulted from the significant separation of n–π* energy levels between trans and cis isomers due to the introduction of an electron-withdrawing group (fluorine) to azobenzene at the ortho-position. Interestingly, the gel exhibited a good gel-to-sol transition behavior upon green light irradiation. At the same time, the morphologies varied from uniform narrow flakes to broad sheets with increasing illumination time. We provide an environmentally-friendly visible light-triggered method to regulate the phase transition of supramolecular materials in applications ranging from energy conversion to information storage.
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