SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Xiaoyan Zhang,Yunning Chen,Qingkun Shang,Yingna Guo
A novel photocatalyst (Cu-TiO 2 @HQ) had been synthesized by combining Cu-doped TiO 2 nanoparticles with 8-Hydroxyquinoline (HQ) via hydrothermal method. The photocatalytic activities of Cu-TiO 2 @HQ were investigated by using phenol and tetrabromobisphenol A (TBBPA) as target pollutants, respectively. The results indicated that the degradation efficiencies of phenol and TBBPA by Cu-TiO 2 @HQ were 99.2% (in 30 min) and 99.4% (in 10 min) under visible light irradiation. Both of them were much better than that of pure TiO 2 (8.63% in 30 min) and Cu-TiO 2 (14.74% in 30 min). When phenol or TBBPA were degraded together with the reduction of Cr (VI), the reaction rate of each pollutant was significantly increased, and the cyclic stability of photocatalyst Cu-TiO 2 @HQ was greatly improved. Based on the spectroscopic and photoelectric characteristic analysis we found that in the mixture of phenol-Cr (VI) or TBBPA-Cr (VI) both photo-generated electrons and holes can be consumed simultaneously, thus preventing their recombination. The possible degradation products of phenol and TBBPA including its degradation path way were also analyzed by high resolution liquid chromatography-mass spectrometry-mass spectrometry.
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MACROMOLECULES
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2020
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IF 5.918
Qiong Li,Songqi Ma,Sheng Wang,Yanlin Liu,Muhammad Abu Taher,Binbo Wang,Kaifeng Huang,Xiwei Xu,Yingying Han,Jin Zhu
Recycling thermosets have become extremely important due to their ecological and economic benefits. The development of thermosets that undergo reversible polymerization provides a solution to the end-life disposal issue of thermosetting materials. However, the synthesis and recycling of the current chemically recyclable thermosets are harsh, complex, and energy-intensive, and their stability is often low. Here, we designed asymmetric acetal-containing thermosets (PRCs) from general phenolic resin and 1,4-cyclohexanedimethanol divinyl ether through one-step “click” cross-linking without using catalysts and solvents and without releasing small-molecule byproducts. PRCs exhibited conspicuous stress relaxation via a dissociative mechanism, corresponding to the superior malleability and reprocess recyclability. Importantly, PRCs presented excellent creep resistance even at 100 °C. In addition, PRCs could be readily and highly efficiently recovered to original phenolic resin via hydrolysis under specific mild acidic conditions but possessed high chemical stability under neutral conditions and even weak acidic conditions or acidic conditions in the absence of organic solvents with outstanding wettability and swellability toward the samples. Thermosets with different properties could be easily achieved via regulating raw materials. This work provides a promising dynamic covalent motif and a practical method to produce readily dual-recyclable (reprocess recyclable and chemically recyclable) thermosets with superior performance and stability.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Huanfang Zhou,Limin Chen,Shuting Li,Songqing Huang,Yingying Sun,Yanhong Chen,Zhao Wang,Wei Liu,Xinchun Li
A facile and green method for preparation of gold/palladium (Au/Pd) bimetallic nanoparticles interleaved reduced graphene oxide (rGO) composite was presented. One-step electroreduction of Au/Pd precursors and graphene oxide synergistically produced a multilayered and well-structured nanohybrid on glassy carbon electrode, which was explored as a highly efficient electrocatalyst . This operation is easy and controllable, as compared with time-consuming and procedure-tedious hydrothermal synthesis . The morphology and chemical constituents were meticulously characterized. The remarkable electrocatalytic performance of the prepared nanohybrid was demonstrated by detection of a high-risk carcinogen pollutant, hydrazine. By optimizing the preparation condition and investigating the electrochemical behavior, we achieved the sensitive analysis of hydrazine with ultralow oxidation overpotential. Amperometry was employed for constructing the quantitative calibration curve ; the steady-state current originating from hydrazine oxidation was proportional to the analytical concentration ranging from 0.1 μM to 200 μM, with the detection limit of 16 nM. Moreover, the nanohybrid displayed considerable anti-interfering ability with respect to hydrazine detection, as a variety of potentially coexisting substances produced negligible electrochemical response in the given analytical condition. Advantages including easy-to-preparation, high sensitivity and favorable selectivity , as well as broad linear response make the present method feasible for monitoring of hydrazine in water environment.
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Journal of Energy Chemistry
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2020
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IF 7.216
Huimin Liu,Yidan Zhang,Jingshan Luo
Ammonia synthesis by electrocatalytic nitrogen reduction reaction (NRR) is considered as a promising alternative to the Haber−Bosch process. However, due to the extremely low ammonia yield and easily accessible extraneous contamination in the laboratory, NRR study always suffers from fluctuation and variability. Finding and eliminating all kinds of possible extraneous contamination is crucial to evaluate the performance of electrocatalytic ammonia synthesis accurately. In this work, we systematically explored two factors that affect NRR results but are easy to be ignored: the selection of membrane for NRR and the unconscious N-source in NRR catalysts. After series of experiments, we proposed a low-cost and almost pollution-free Celgard 3501 membrane as the separator for NRR to avoid the adsorption and release of ammonia by the membrane. In addition, we proposed a pre-reduction strategy to remove residual or adsorbed NO x contaminants in catalysts. These two solutions will help the community to evaluate the NRR activity more accurately.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Fu Yang,Liuzhu Zhou,Shuying Gao,Xuyu Wang,Jin Chen,Aihua Yuan,Edison Huixiang Ang
Combining different active states of metal species together in special configuration might trigger interesting synergetic effect for catalytic process. As a proof-of-concept, the present study has developed an ingenious approach to reach functional mesoporous molecular sieve which in-situ encapsulates two different states of highly-active FeOx inside centered core and nano-tunnel of mesoporous silica , respectively. The α-Fe 2 O 3 in-situ immobilized nanoneedles coated by the porous silica afford ∼5 nm diameter, plus highly-dispersed Fe 2 O 3 cluster-like species attachment in confined mesopore, which synergistically contributes to high activity and stabilization of catalyst. The combined iron oxides in special configuration deliver an appreciable catalytic activity in phenol hydroxylation (46.4% conversion, 87.9% benzenediol selectivity) during multiple catalytic cycles, compared to some reported results, which benefited from accelerating production of oxidative free radicals from H 2 O 2 and the tailored micrpopore (∼1.4 nm) which could enhance the catalytic selectivity of targeted products. Furthermore, the photocatalytic antimicrobial effect of Fe catalyst against Escherichia coli was also demonstrated via the constructed synergy of two FeOx nanospecies with assistance of light.
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Food Analytical Methods
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2020
·Vol. 13
·期 10
·1842-1851
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IF 2.667
Qu Fei,Sun Yang,Guo Shuxian,Yan Hang,You Jinmao
2,4-Dichlorophenoxyacetic acid (2,4-D) is a typical chlorinated aromatic herbicide which is widely used because of its low cost. Herein, a new fluorescent assay for 2,4-D is developed based on covalent organic frameworks (COFs) and MnO 2 nanosheets. The fluorescence of COFs is quenched effectively by MnO 2 nanosheets. Ascorbic acid 2-phosphate (AAP) is hydrolyzed by alkaline phosphatase (ALP) to produce ascorbic acid (AA), which reduces MnO 2 nanosheets into Mn 2+ , so the quenched fluorescence recovers. Additionally, 2,4-D can inhibit the catalytic activity of ALP. Therefore, the addition of 2,4-D quenches the fluorescence of COF-MnO 2 system again. Under the optimum conditions, this assay displays a wide linear range of 2,4-D from 1 to 150,000 ng/mL with a limit of detection of 0.36 ng/mL. Then, this method is successfully used to measure 2,4-D in rice, millet, and cucumber samples with satisfactory recoveries. Compared with other probes for 2,4-D detection, both of COFs and MnO 2 nanosheets are stable, cost-effective, and easily prepared. The sensitivity and linear range of 2,4-D in this strategy are superior to most reported works. This is the first time that a novel sensing platform using fluorescent COFs and MnO 2 nanosheets is developed for 2,4-D.
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ACS Nano
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2020
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IF 14.588
Kuo Zhang,Pei-Pei Yang,Ping-Ping He,Shi-Fang Wen,Xiao-Ran Zou,Yu Fan,Zi-Ming Chen,Hui Cao,Zhou Yang,Kai Yue,Xinxin Zhang,Hua Zhang,Lei Wang,Hao Wang
Cancer therapeutic strategies based on angiogenesis attract great attention from fundamental and clinical research. Blocking oxygen and nutrition supply to tumor cells could inhibit the growth of tumors based on occlusion of blood vessels in the tumor. Herein, we report a dual-responsive peptide-based nanoparticle, mimicking the laminin fibrillogenesis specifically and highly efficiently in tumor vessels, resulting in the blockage of tumor vessels and the growth inhibition of tumors. The laminin mimic peptide (LMMP) is designed with a fibrillation sequence, a pH-responsive sequence, and a targeting sequence. The LMMP in nanoformulations is delivered to blood vessels in the tumors, where the microenvironment (pH and microthrombus) enable LMMP to process laminin fibrillogenesis, constructing fibrous networks. The laminin-like fibrous networks capture red blood cells etc., forming occlusion specifically in the tumor blood vessels to inhibit the growth of the tumor.
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Environmental Science and Ecotechnology
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2020
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IF 0
Jing Ding,Lingjun Bu,Bingxin Cui,Guanshu Zhao,Qingwei Gao,Liangliang Wei,Qingliang Zhao,Dionysios D. Dionysiou
Bisphenol (BP) analogues in wastewater effluent and groundwater pose a potential threat to human health due to their ability to disrupt steroidogenesis. A new solar-assisted electrochemical process (SECP) was developed and evaluated for the degradation of BP analogues. The effects of quenchers, current density, initial pH, supporting electrolyte, and aqueous matrix on the removal kinetics of bisphenol AF (BPAF) and bisphenol A (BPA) were investigated. The kinetic constants of BPAF, BPA, and bisphenol S (BPS) in the SECP with irradiation intensity of 500 mW cm −2 were 0.017 ± 0.002 min −1 , 0.022 ± 0.002 min −1 , and 0.012 ± 0.001 min −1 , respectively. The changes in the degradation rates of BPAF, BPA, and BPS in the presence of quenchers indicated the relative contribution of hydroxyl radical ( ● OH) oxidation, anodic electrolysis, and singlet ( 1 O 2 ) oxygenation in the degradation of BPs in the SECP. The enhanced rate of generation of ● OH and 1 O 2 was observed in the SECP compared with those in the conventional electrochemical system. The identification of the transformation products (TPs) of BPAF demonstrated that hydroxylation, ring cleavage, β-scission, and defluorination were the major processes during the oxidation in the SECP. The conversion to fluoride ions (76%) and mineralization of total organic carbon (72%) in the SECP indicated further degradation of TPs. The results from this study improved our understanding of the degradation of BP analogues in the electrooxidation irradiated by solar light and help to establish the application potential of the SECP for the effective degradation of emerging contaminants in wastewater.
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RSC Advances
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2020
·Vol. 10
·期 32
·18572-18580
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IF 3.119
Jiao Wang,Ting Wang,Xiaohui Liu,Yan Lu,Jingjing Geng
Multiple-responsive supramolecular vesicles have been successfully fabricated by the complexation between β-cyclodextrin (β-CD) and a pH/photo dual-responsive amphiphile 4-(4-(hexyloxy)phenylazo)benzoate sodium (HPB) with azobenzene and carboxylate groups. When mixing β-CD with HPB to reach a host/guest molar ratio of 1 : 1, the azobenzene group of HPB could be spontaneously included by β-CD molecules. Then, the formed inclusion complexes (HPB@β-CD) could self-assemble into vesicles, which was driven by the hydrophobic interaction of the alkyl chain of HPB and the hydrogen bonds between neighboring β-CDs. The reversible assembly/disassembly of the vesicles could be simply regulated under UV or visible light irradiation. The reversible phase transformation between vesicles and microbelts could also be realized by adjusting the pH values of the sample. Adding both competitive guest molecules (1-adamantane carboxylic acid sodium (ADA)) and α-amylase would result in the phase transformation from vesicles to micelles. Moreover, the vesicles would be destroyed when β-CD was continuously added until the ratio of host/guest reached 2 : 1. Such an interesting quintuple-responsive vesicle system reported here not only has potential applications in various fields such as controlled release or drug delivery, but also provides a reference for the design and construction of multiple responsive systems.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Hang Li,Yi Zhai,Xubin Zhang,Guojun Lv,Yu Shen,Xuqing Wang,Tao Jiang,Yuzhou Wu
Hierarchical iron-containing TS-1 zeolites (FTS) were successfully synthesized via post-treatment desilication over microporous Fe-TS-1, which were prepared through a one-step hydrothermal synthesis. The prepared samples were characterized by X-ray diffraction, N2 adsorption–desorption, field-emission scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, ultraviolet visible spectroscopy, and X-ray fluorescence spectrometry. The experimental results illustrated that the MFI structure of all the FTS samples remained unchanged after NaOH desilication and acid treatment. The newly created mesopores can be controlled by changing the amount of framework Fe, as the extraction of Si could be affected because of the inhibitory effect of iron species during the desilication process. The catalytic performance of the prepared samples in phenol hydroxylation with H2O2 was investigated. Among all the samples, FTS-50-D showed a highest phenol conversion of 45.2% and a dihydroxybenzene selectivity of 95.2%. Besides, FTS-50-D also showed good reusability for five recycling tests.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Shaoqi Yang,Guangming Cai,Xingmei Lu,Chenguang Wang,Mi Feng,Junli Xu,Qing Zhou,Jiayu Xin,Longlong Ma
Hydrodeoxygenation (HDO) of lignin-derived phenols and dimeric ethers to biofuels has great significance for advanced utilization of renewable lignocelluloses and the future biobased economy. Herein, we find that the deoxygenation process during the lignin-derived model compound HDO process could efficiently be catalyzed by low-cost protic ionic liquids under mild conditions. 2-Hydroxy-N-(2-hydroxyethyl)-N-methylethanaminium trifluoromethanesulfonate ([BHEM]CF3SO3) shows the highest catalytic activity for the deoxygenation reaction during the lignin-derived compound HDO process with Rh/C as the hydrogenation catalyst. The conversion of phenol is 100% under 4 MPa H2 at 130 °C for 6 h, and the yield of cyclohexane is 93.3%. Furthermore, the catalytic system with [BHEM]CF3SO3 as the deoxygenation catalyst and Rh/C as the hydrogenation catalyst demonstrates efficient catalytic activity for various lignin-derived phenols and dimeric ethers with ≥99.0% conversion and >90.0% selectivity. The catalytic system is reused five times for HDO of phenol to test its stability.
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RSC Advances
·
2020
·Vol. 10
·期 14
·8558-8567
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IF 3.119
Jindong Wang,Wenzhi Li,Huizhen Wang,Ajibola Temitope Ogunbiyi,Xiaomeng Dou,Qiaozhi Ma
To improve the utilization of lignin, much effort has been devoted to lignin depolymerization with the aim to decrease waste and enhance profitability. Here, a dual property (acid and base) catalyst, namely S2O82−–K2O/TiO2, was carefully researched. Upon loading S2O82− and K2O onto TiO2, acid and base sites emerged, and S2O82− and K2O mutually enhanced the acid and base strengths of the catalyst enormously; this indeed facilitated lignin depolymerization. Under appropriate conditions, the yields of liquid product, petroleum ether soluble (PE-soluble) product and total monomer products were 83.76%, 50.4% and 28.96%, respectively. The constituents of the PE-soluble fraction, which are mainly monomers and dimers, can be used as liquid fuels or additives. In addition, after the catalyst was modified by Ni, better results were obtained. Surprisingly, it was found that the Ni enhanced not only the hydrogenation capacity but also the acidity. The highest high heating value (HHV) of the liquid product (33.6 MJ kg−1) was obtained, and the yield of PE-soluble product increased from 50.4 to 56.4%. The product can be utilized as a fuel additive or be converted to bio-fuel. This catalysis system has significant potential in the conversion of lignin to bio-fuel.
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