JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
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IF 5.091
Junyan Kuang,Zipeng Xing,Junwei Yin,Zhenzi Li,Qi Zhu,Wei Zhou
Ti 3+ self-doped single-crystalline SrTiO 3−x nanocubes acting as molecular bricks are successfully assembled onto Ti 3+ self-doping single-crystalline TiO 2−x (B) nanorods through an effortless two-step hydrothermal process coupled with an in situ solid-state chemical reduction method. SrTiO 3−x nanocubes act as molecular bricks, which are uniformly assembled onto the surface of TiO 2−x (B) nanorods due to lattice matching. The band gap of the resultant SrTiO 3−x /TiO 2−x (B) sample is ∼2.97 eV, which exhibits excellent photocatalytic performance for the reduction of Cr(VI) and hydrogen production under visible light. The apparent rate constant k value for the photocatalytic reaction of SrTiO 3−x /TiO 2−x (B) for Cr(VI) reduction is ∼8 times higher than that of white TiO 2 (B). The photocatalytic hydrogen production rate for SrTiO 3−x /TiO 2−x (B) is ∼160.2 μmol g −1 h −1 , which is ∼5 times higher than that of white TiO 2 (B). The enhanced photocatalytic activity can be considered to be caused by a synergetic effect of heterojunction formation and the introduction of Ti 3+ self-doping, which can not only facilitate the separation of photogenerated charge carriers between TiO 2−x (B) and SrTiO 3−x , but also broaden the photoresponse from the UV to visible-light region.
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FUEL PROCESSING TECHNOLOGY
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2018
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IF 3.956
Riyang Shu,Biqin Lin,Jingtao Zhang,Chao Wang,Zhi Yang,Ying Chen
Upgrading of bio-oils to value-added products through simple and cost-efficient catalytic routes is always a big challenge in the energy utilization field. Herein, we prepared a highly dispersed 2 wt% Ru/TiO 2 catalyst using a simple and novel photochemical method at room temperature . The synthetic catalyst exhibited an efficient performance on the HDO of phenolic compounds and real bio-oil, owing to its high Ru dispersion. Guaiacol could be converted into cyclohexane with 91.3% selectivity at 260 °C under 1 MPa H 2 atmosphere. Other typical phenolic monomers (phenol, anisole , etc.) and dimers (α-O-4, 4-O-4, etc.) were transformed into cycloalkanes with most yield close to 100%. Results showed that the cleavage of ether bonds and the HDO step can be realized in one pot. This catalytic system was also effective on the upgrade of bio-oil derived from the pyrolysis of cotton straw. A upgraded product composed of 32.4% hydrocarbons and 57.6% alkylphenols was achieved at 280 °C, which can be used as fuels and chemicals respectively. The enhanced reaction temperature (300 °C) enabled hydrocarbon contents increased to 41.4%, leaving the other oxygenated compounds only 4.2%. This work provides a promising reference for the valorization of raw bio-oil.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Jiali Ge,Xinghao Wang,Chenguang Li,Siyuan Wang,Lianhong Wang,Ruijuan Qu,Zunyao Wang
Polychlorinated diphenyl sulfides (PCDPSs) are a group of dioxin-like compounds that have been widely used in agricultural and industrial productions. Here, we systematically investigated the photochemical behaviors of 2,2′,3′,4,5-pentachlorodiphenyl sulfide (2,2′,3′,4,5-PCDPS) on the surface of silica gel (SG) in an aqueous environment. Under the simulated sunlight irradiation, 2,2′,3′,4,5-PCDPS adsorbed on SG (0.11 mg/g) was found to be degraded with time, giving a removal rate of 68.5% within 16 h at pH 7.0. Environmental factors like pH and humic acid can also affect the removal rate. Results showed that the removal rate of 2,2′,3′,4,5-PCDPS in alkaline conditions (75.6% at pH 11) was higher than that in acidic conditions (46.7% at pH 3). Moreover, the addition of (1–5 mg/L) humic acid can promote the degradation rate compared to control group. In our study, it was found that SG can act as photocatalyst to generate reactive oxygen species (ROS) for the degradation of PCDPSs, and UV light contributed much more than visible light (>420 nm). According to electron paramagnetic resonance (EPR) technology and radicals quenching experiments, hydroxyl radical ( OH), single oxygen ( 1 O 2 ), and superoxide radical ( O 2 − ) participated in the removal of the contaminant. Based on the identified intermediate products via LC–MS, two main pathways, i.e., the hydroxyl-substituted reaction of the benzene ring and the oxidation of the sulfur atom, were proposed for the photodegradation of 2,2′,3′,4,5-PCDPS. Then, the density functional theory (DFT) was employed to confirm these reaction pathways. This study would enhance the understanding of the photochemical transformation and environmental fate of PCDPSs on the surface of solids in natural waters.
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ENERGY & FUELS
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2018
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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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RSC Advances
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2018
·Vol. 8
·期 46
·26371-26376
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IF 2.936
Qiu Li,Qun Li,Zhihui Hao,Xucai Zheng,Wei He
We report a novel water-soluble polysaccharide from Rhizoma panacis japonica, namely, PJ-1 with anti-inflammatory activity. We first obtained a polysaccharide from this herb by eluting with water. After fully characterizing PJ-1 with a series of chromatographic technologies, we evaluated its biological activity by stimulating Raw 264.7 cells to express inflammatory cytokines and found that PJ-1 effectively enhanced the production of anti-inflammatory factors such as IL-10. We further identified its anti-inflammatory effect in a mouse model of sepsis induced by a lipopolysaccharide. The treatment of PJ-1 evidently suppressed the secretion of major inflammatory cytokines and increased the survival rate of mice. Particularly, we verified the STAT3 signal pathway responsible for the anti-inflammatory activity. Thus, PJ-1, which has remarkable anti-inflammatory effect and mechanism of action, may be a promising candidate as an anti-inflammatory agent.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2018
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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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BIOCONJUGATE CHEMISTRY
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2018
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IF 4.485
Dongzhi Yang,Xinyue Yao,Jingjing Dong,Na Wang,Yan Du,Shian Sun,Liping Gao,Yuanyuan Zhong,Chuntong Qian,Hao Hong
Due to the excellent photoluminescent properties and singlet oxygen (1O2) generating efficiency, graphene quantum dots (GQDs) with maximal emission in near-infrared region (NIR) exhibited great potential in cancer imaging and therapy. However, GQDs can be cleared quickly via the renal system in vivo because of their ultrasmall size, which leads to the compromised cancer cell killing efficacy. Here, we report a hybrid nanoplatform, where GQDs were incorporated into the cavity of hollow mesoporous silica nanoparticles (hMSN) to form GQDs@hMSN-PEG nanoparticles (NPs). Optical characterization indicated that GQDs@hMSN-PEG NPs still maintained good absorption and emission properties from GQDs, and the composite NPs still possessed similar 1O2 generating efficiency. GQDs@hMSN-PEG NPs exhibited good biocompatibility in vitro and in vivo. High cargo-loading efficiency was achieved for doxorubicin (DOX), and the formed GQDs@hMSN(DOX)-PEG NPs showed the feasibility of tumor-oriented drug delivery. The extended retention time in tumor and good drug loading efficacy confirmed that GQDs@hMSN-PEG could serve as one promising candidate for combinational cancer treatment where photodynamic therapy and chemotherapy modules can be integrated into one system.
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ACS Applied Materials & Interfaces
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2018
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IF 8.097
Jing Li,Jiantao Yu,Yishun Huang,Haoran Zhao,Leilei Tian
Oligonucleotide-stabilized silver nanoclusters (AgNCs) show promising applications in bioimaging and bio-/chemo-sensing. However, their unsatisfactory photostability limits their practical applications. In this work, fluorescent AgNCs were synthesized in situ in a DNA hydrogel, consisting of cross-linked enzymatically amplified polymeric DNAs with cytosine-rich sequences in the presence of Ag+. The fluorescence property of the resultant AgNCs was optimized by a rational design of the DNA sequences to cover a broad spectrum with comparable green and red emissions. Under the protection of the DNA hydrogel, the AgNCs showed significantly improved photostability in an ambient oxygen environment, as well as low cytotoxicity even at a high concentration. Therefore, these properties show the rolling-circle-amplification-stabilized AgNCs to be a promising possible fluorescent probe for the detection of reactive oxygen/nitrogen species (ROS/RNS) in live cells because red-emitting species are susceptible to oxidation and consequently convert to green-emitting species. Finally, the as-prepared AgNCs were demonstrated to be a sensitive and specific probe for cellular imaging and the monitoring of ROS/RNS levels, which broadens the applications of AgNCs and provides a new tool for related biological investigations.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2018
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IF 2.88
Huanhuan Fan,Guo Qiang Xiang,Yule Wang,Heng Zhang,Keke Ning,Junyue Duan,Lijun He,Xiuming Jiang,Wenjie Zhao
In the present work, a selective and sensitive method for detecting TNP using manganese doped carbon quantum dots (Mn-CDs) was developed. The Mn-CDs were prepared via a simple hydrothermal method using 1-(2-pyridinylazo)-2-naohthalenol naohthalenol (PAN) and MnCl 2 as precursors. The as-prepared Mn-CDs have UV emission with high quantum yield (83.2%). Because of the strong characteristic absorption of TNP at 356 nm, which has good spectral overlap with the emission peak of Mn-CDs, the fluorescence intensity of Mn-CDs at 360 nm is linearly quenched in the presence of TNP in the concentration range of 0.1–200 μM. The developing assay based on an inner filter effect (IFE) mechanism for detecting TNP is selective, convenient, and shows that the as-prepared Mn-CDs have application prospects for simple and specific analytical chemistry .
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FUEL
·
2018
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IF 4.908
Youan Ji,Yucui Hou,Shuhang Ren,Congfei Yao,Weize Wu
Phenolic compounds, which are widely used in producing synthetic fibers, engineering plastics, and other industrial organic chemicals, can be obtained from oil mixtures before further processing or applications by separation. Based on Lewis/Brønsted acid-base theory, we proposed the separation of phenolic compounds from oil mixtures using some environmentally benign biological reagents (BRs, including 1,3-dimethylxanthine-DMX, isonicotinamide-INA, and L-lysine-LYS). The effects of stirring time, temperature, initial phenol concentration, and BR:phenol mole ratio on phenol removal were studied in detail. LYS, INA and DMX show phenol removal efficiencies of 98.4%, 82.2%, and 66.6% from toluene at BR:phenol mole ratios of 1.6, 1.4, and 0.4, respectively, and those of 99.1%, 91.8%, and 74.6% from n -hexane at BR:phenol mole ratios of 2.20, 1.60, and 0.80, respectively, at room temperature. The BRs were regenerated with an anti-extraction method for four cycles without significant changes in separation efficiency and their properties. In addition, it is found that there is little toluene entrained in the biological reagents, which is as low as 2.3 wt% of separated phenol, indicating high purities of products. These BRs show the advantages of easy biodegradation, no corrosion to the equipment and containers, and no pollution to the environment.
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ANALYTICAL SCIENCES
·
2018
·Vol. 35
·期 2
·147-152
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IF 1.355
Ju Yan Jun,Li Na,Liu Shi Gang,Fan Yu Zhu,Ling Yu,Xiao Na,Luo Hong Qun,Li Nian Bing
A fluorescence method for the determination of picric acid (PA) using phosphorus-doped carbon dots (P-CDs), synthesized from β-cyclodextrin and sodium pyrophosphate, is described. The P-CDs are very uniform and monodisperse with a diameter of about 2.8 nm. Under an excitation of 350 nm, the P-CDs emit bright blue fluorescence with an emission peak at 440 nm. The as-synthesized P-CDs serve as a sensitive, selective, and label-free fluorescent probe for the detection of PA. Based on an inner filter effect between PA and P-CDs, a linear response is obtained for PA from 0.1 to 10 μM with a detection limit of 82 nM. Finally, this sensing system has been demonstrated to have practicability for PA detection in the environmental water samples.
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Polymers
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2018
·Vol. 10
·期 12
·1329
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IF 2.935
Lingyu Liu,Xudong Zhu,Yanbo Zeng,Hailong Wang,Yixia Lu,Jian Zhang,Zhengzhi Yin,Zhidong Chen,Yiwen Yang,Lei Li
In this paper, we report a new composite of reduced graphene oxide/Fe3O4-ionic liquid based molecularly imprinted polymer (RGO/Fe3O4-IL-MIP) fabricated for diphenylamine (DPA) detection. RGO/Fe3O4-IL-MIP was prepared with RGO/Fe3O4as supporter, ionic liquid 1-vinyl-3-butylimidazolium hexafluorophosphate ([VC4mim][PF6]) as functional monomer, ionic liquid 1,4-butanediyl-3,3’-bis-l-vinylimidazolium dihexafluorophosphate ([V2C4(mim)2][(PF6)2]) as cross-linker, and diphenylamine (DPA) as template molecule. Fourier transform infrared spectroscopy, thermal gravimetric analysis, scanning electron microscopy, and vibrating sample magnetometer were employed to characterize the RGO/Fe3O4-IL-MIP composite. RGO/Fe3O4-IL-MIP was then drop-cast onto a glassy carbon electrode to construct an electrochemical sensor for DPA. The differential pulse voltammetry (DPV) peak current response for 20 μM DPA of RGO/Fe3O4-IL-MIP modified glassy carbon electrode (GCE) was 3.24 and 1.68 times that of RGO/Fe3O4-IL-NIP and RGO/Fe3O4-EGDMA-MIP modified GCEs, respectively, indicating the advantage of RGO/Fe3O4-IL-MIP based on ionic liquid (IL) as a cross-linker. The RGO/Fe3O4-IL-MIP sensor demonstrated good recognition for DPA. Under the optimized conditions, the RGO/Fe3O4-IL-MIP sensor exhibited a DPA detection limit of 0.05 μM (S/N = 3) with a linear range of 0.1–30 μM. Moreover, the new RGO/Fe3O4-IL-MIP based sensor detected DPA in real samples with satisfactory results.Keywords:reduced graphene oxide;Fe3O4;molecularly imprinted polymer;ionic liquid cross-linker;electrochemical sensor;diphenylamine
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