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Journal of Biobased Materials and Bioenergy · 2020 ·Vol. 14 ·期 1 ·20-28 · IF 1.126

The Changing Structure of Residual Lignin in the Unbleached Bagasse Pulp During Chlorine Dioxide Delignification

Lei Ming,Luo Bin,Zhang Qingtong,Guo Chenyan,Chi Mingchao,Yun Xiaojing,Min Douyong,Wang Shuangfei

Herein, residual lignin was extracted from unbleached sugarcane bagasse pulp via the sequential enzymatic-weak acid hydrolysis method. Subsequently, chlorine dioxide delignification was applied to the extracted lignin. The structural changes of lignin during chlorine dioxide delignification were characterized by Fourier transform infrared spectroscopy (FT-IR), 13C-nuclear magnetic resonance (13C NMR), 1H-13C heteronuclear single quantum coherence (2D HSQC), and quantitative 31P-nuclear magnetic resonance (31P-NMR) spectroscopy. The degradation products of lignin dissolved in the simulated bleaching liquor, extracted, and quantified via gas chromatography-mass spectrometry (GC-MS). Lignin was significantly degraded during the delignification process, showing cleavage of the aromatic ring, removal of the methoxyl group, and cleavage of major interunit linkages. However, the carboxylic acid content increased and GC-MS analysis indicated that lignin was degraded into several organic substances dissolved in the liquor. However, only a few absorbable organic halides (AOX) were generated, confirming that chlorine dioxide bleaching is an ideal bleaching method.

研究领域: 植物化学 · 制浆造纸工程
✓ 已验证 DOI 高影响因子
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INORGANICA CHIMICA ACTA · 2022 · IF 3.118

Use chloride to assist in constructing of penta- and nano-nucleus mixed-valent Cu(I/II) clusters and their photo-thermal properties

Jing-Wen Zhang,Ling-Xiao Wang,Xun Cheng,Lin-Lin Hou,Jing-Zhe Li,Chun-Feng Wang,Xiao-Wei Yan,Kuan-Guan Liu

To prepare new series of mixed-valence polynuclear Cu(I/II) clusters, chloride ions are introduced to construct two mixed-valence polynuclear Cu(I/II) clusters for evaluating their photothermal conversion performance. X-ray single-crystal structural analysis reveals their molecular formula are {Cu II [Cu I (Cy 3 P)] 4 (BTA) 4 Cl 2 }·5DMF (I·5DMF, Cy 3 P = triscyclohexylphosphine, BTA = benzotriazole, DMF = N, N -Dimethylformamide) and {(Cu II ) 3 [Cu I (PPh 2 Py)] 6 (BTA) 8 Cl 4 }·6DMF (II· 6 DMF, Ph 2 PyP = diphenyl-2-pyridylphosphine), respectively. X-ray Photoelectron Spectroscopy (XPS) and Electrospray Ionization Mass Spectrometry (ESI-MS) confirm their chemical composition and charge state. The reported two mixed-valence Cu I /Cu II clusters have different nucleus (penta-nucleus for I and nano-nucleus for II) and different proportion of valence state (1/4 for I vs 1/2 for II). The thermogravimetric analysis (TGA) reveals the thermal stability of both clusters is less than our previously reported penta-nucleus mixed-valence Cu I /Cu II clusters. Contrastively studies of their optical absorption properties by the solid-state ultraviolet diffuse reflection spectra indicate high-nucleus mixed-valence Cu I /Cu II cluster with higher proportion of Cu II is superior to those penta-nucleus mixed-valent Cu(I/II) clusters. With the introduction of chloride ions to the structures of mixed-valence Cu I /Cu II clusters have not remarkably changed their photothermal conversion performance. This study provides a practicable way to construct new mixed-valence Cu I /Cu II clusters with different photothermal conversion performance.

研究领域: 化学 · 材料科学
✓ 已验证 DOI 高影响因子
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ACS Sensors · 2020 · IF 7.333

Molecular Fluorescent Probes for Imaging and Evaluation of Hypochlorite Fluctuations during Diagnosis and Therapy of Osteoarthritis in Cells and in a Mouse Model

Ji-Ting Hou,Bingya Wang,Yuxia Zou,Peiwen Fan,Xueping Chang,Xinhua Cao,Shan Wang,Fabiao Yu

The early diagnosis of osteoarthritis (OA) can halt or delay the progression of the disease, and it is essentially beneficial to its treatment. However, biomarkers with sufficient sensitivity for dynamically identifying early OA are still yet to be determined. The overproduced hypochlorous acid (HOCl) has been proposed as an obvious symptom in early OA. Herein, based on the oxidation reaction of the sulfur atom in phenothiazine into sulfoxide, we design and synthesize a phenothiazine-derived coumarin fluorescent probe PDC for the detection of ClO– in cells and in an OA mouse model. The probe PDC exhibits excellent selectivity and sensitivity for ClO– detection with a limit of detection as low as 16.1 nM. Taking advantage of the probe PDC, we visualize and evaluate the level changes of ClO– in macrophage cells, which is stimulated by various inflammatory factors. The anti-inflammatory and therapeutic effects of selenocysteine and methotrexate in inflamed cells are also confirmed. Finally, with in vivo imaging of ClO– concentration changes in OA BALB/c mouse models, we successfully inspected the relationship between OA phenotypes and the burst of ClO–. We suggest that abnormal changes in HOCl concentration may be considered as a new biomarker for the early OA diagnosis.

研究领域: 生物化学 · 医学影像 · 风湿病学
✓ 已验证 DOI PubMed 高影响因子
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CERAMICS INTERNATIONAL · 2017 · IF 2.986

Chloride flux growth of crystalline strontium niobates and nitridation to perovskite SrNbO2N

Yue Li,Feng-Qiang Xiong,Ruiling Ou,Lipeng Wan,Congling Yin,Ruxin Che,Minghui Yang

Highly crystalline (110) layered perovskite Sr 2 Nb 2 O 7 , (111) layered perovskite Sr 5 Nb 4 O 15 and complex perovskite Sr 4 Nb 2 O 9 were prepared by NaCl-KCl flux growth method from SrCO 3 and Nb 2 O 5 . This flux synthesis achieves single strontium niobate phase in contrast to mixed niobates from the solid state reaction with the same heating parameters. A little excess of Sr source was found to be required for the synthesis of Sr 5 Nb 4 O 15 and Sr 4 Nb 2 O 9 at elevated temperature due to slight evaporation. The three strontium niobates were converted to perovskite SrNbO 2 N via thermal ammonolysis under NH 3 flow at 900   °C. Post-wash treatment was performed to remove the byproduct SrO. This makes additional nanopores in SrNbO 2 N in the cases of Sr 5 Nb 4 O 15 and Sr 4 Nb 2 O 9 , and results in increasing surface areas of SrNbO 2 N with Sr:Nb ratios in the precursors (from 9.9 to 19.8 and 35.5   m 2 /g). On the other hand, the UV–Vis diffusion reflectance spectra reveal decreasing light absorption by defects in SrNbO 2 N in this order. This suggests fewer low-valent Nb defects in SrNbO 2 N prepared from precursor with higher Sr:Nb ratio. SrNbO 2 N prepared from Sr 4 Nb 2 O 9 would be advantageous for applications that require high surface area and low defect density of the material.

研究领域: 材料科学 · 化学工程
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING RESEARCH & DESIGN · 2022 · IF 4.119

Simultaneous Fe(OH)3 formation and silicon adsorption removal from reverse osmosis brine wastewater

Jingjing Sun,Shangqing Chen,Junfeng Wang,Yi Nie

The reduce of the silicon concentration to low level (<5 mg·L −1 ) from the reverse osmosis brine wastewater is challenging and desirable for the maintain the membrane life and performance, as well as the wastewater treatment costs. This work focuses on the removal of silicon from the reverse osmosis brine wastewater by adding FeCl 3 into the plant wastewater for simultaneous Fe(OH) 3 formation and silicon adsorption. The effects of pH, FeCl 3 dosing concentration, reaction time, and temperature on the silicon removal ratio were investigated. It was demonstrated that the silicon removal ratio could reach up to 94% and its residual concentration was 3.2 mg·L −1 , which met the require of water quality in the reverse osmosis system. These results showed that Fe(OH) 3 could effectively be formed by adding FeCl 3 and realize the efficient silicon removal from the reverse osmosis brine wastewater, even when chloride ion (Cl - ), sulfate anion ( S O 4 2 - ) and nitrate ion ( N O 3 - ) were present. Moreover, the adsorption thermodynamics, kinetics and isotherms during the process of the adsorption of silicon from the wastewater by Fe(OH) 3 were studied. The calculated adsorption capacity of silicon could reach 612.74 mg·g −1 , which was much larger than those of reported adsorbents. These results showed that the silicon removal process was spontaneously exothermic and mainly controlled by the physical adsorption and the monomolecular layer adsorption. This simple and cost-effective method could be used for the silicon removal from different kinds of Si-containing wastewater.

研究领域: 环境科学 · 废水处理
✓ 已验证 DOI 高影响因子
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ACS Catalysis · 2020 · IF 12.35

Hydrogenative Ring-Rearrangement of Biobased Furanic Aldehydes to Cyclopentanone Compounds over Pd/Pyrochlore by Introducing Oxygen Vacancies

Qiang Deng,Rui Gao,Xiang Li,Jun Wang,Zheling Zeng,Ji-Jun Zou,Shuguang Deng

Upgrading furanic aldehydes (such as furfural or 5-hydroxymethyl furfural) to cyclopentanone compounds (such as cyclopentanone or 3-hydroxymethyl cyclopentanone) is of great significance for the synthesis of high-value chemicals and biomass utilization. Developing an efficient reduced metal/acidic support with Lewis acidity is the key to facilitating the carbonyl hydrogenation and hydrolysis steps in the hydrogenative ring-rearrangement reaction. Herein, three pure Lewis acidic pyrochlore supports of the form A2B2O7 (La2Sn2O7, Y2Sn2O7, and Y2(Sn0.7Ce0.3)2O7-δ) with the same crystal structures and different metals are synthesized. The Lewis acidity and the surface properties of the pyrochlore can be tuned by inserting different kinds of A and B site metals. After impregnation, Pd nanoparticles with appropriate particle sizes are uniformly loaded on the surface of pyrochlore. For the reaction of the furanic aldehydes, all of these pyrochlore-based catalysts exhibit hydrogenation and hydrolysis rates that are both faster than those of traditional support-based catalysts due to the oxygen vacancy and pure Lewis acidity of the support. Among these pyrochlore-based catalysts, Pd/Y2Sn2O7 exhibits activity and selectivity that are higher than those of Pd/La2Sn2O7. Moreover, the Y2Sn2O7-based catalyst partially substituted by Ce3+ ions at the B site is more efficient, with the highest cyclopentanone yield and 3-hydroxymethyl cyclopentanone yield of 95.0% and 92.5%, respectively. Furthermore, the catalyst can still maintain an effective activity and stability after 4 runs. This study not only presents an efficient biobased route for the production of cyclopentanone compounds but also focuses on the acid catalytic performance of pyrochlore based on its pure Lewis acidity.

研究领域: 催化化学 · 生物质利用 · 材料科学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Formation of halogenated by-products during chemical cleaning of humic acid-fouled UF membrane by sodium hypochlorite solution

Zongping Wang,Jiaqi Ding,Pengchao Xie,Yiqun Chen,Ying Wan,Songlin Wang

Sodium hypochlorite (NaClO) solution has been widely used to restore the flux of fouled membrane. The test of membrane flux herein also suggests that humic acid-fouled membranes could be efficiently cleaned by blending in NaClO solution at off-line mode. However, toxic halogenated by-products were found to form during the chemical cleaning of membrane fouling by NaClO solution. All the halogenated by-products except TCE and MCAA rose significantly with the increase of HA concentration. With prolonged chemical-cleaning time, the concentrations of formed chloral hydrate (CH) and trichloroacetic acid (TCAA) rose monotonically, while chloroform (TCM), trichloroacetonitrile (TCAN), trichloroethylene (TCE), trichloronitromethane (TCNM) followed an obvious increasing and then decreasing pattern. The formed TCM, TCAA and 1,1-dichloro-2-propanone (1,1-DCP) show obvious positive dependences on NaClO concentration, which was contrary to the formation of dichloroacetonitrile (DCAN) and 1,1,1-trichloro-2-propanone (TCP). With increasing the blending pH, both TCM and CH increased apparently, while haloacetic acids (HAAs) and haloacetonitriles (HANs) decreased continuously. Overall, the relatively stable halogenated by-products were favored at higher temperature compared to the unstable ones in the temperature range of 15–35   °C. 1,1-DCP, TCNM, TCM and TCAA were found to be easier to form when using the membranes with medium molecular weight cutoff (3   kDa and 5   kDa). The presence of calcium ions (Ca 2+ ) also affected the formation of halogenated by-products as   a result that lots of them were significantly reduced at a Ca 2+ concentration of 10   mg/L. This study suggests that the remained NaClO solution after treatment of fouled membrane would contain some toxic by-products and should be carefully treated.

研究领域: 环境科学 · 水处理工程
✓ 已验证 DOI 高影响因子
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GREEN CHEMISTRY · 2020 ·Vol. 22 ·期 18 ·5984-5988 · IF 9.48

Direct conversion of biomass derived L-rhamnose to 5-methylfurfural in water in high yield

Yunchao Feng,Zheng Li,Sishi Long,Yong Sun,Xing Tang,Xianhai Zeng,Lu Lin

We report here that L-rhamnose, a less popular renewable and commercially available carbohydrate, can be used as a potential raw material to generate 5-methylfurfural (MF). In particular, nearly 100% yield of MF was achieved over 7 consecutive cycles in NaCl solution containing AlCl3 within 30 min, thus providing an alternative and industrializable way for the production of the potential bio-platform compound MF.

研究领域: 生物化学 · 可再生能源化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Chlorine-assisted synthesis of CuCo2S4@(Cu,Co)2Cl(OH)3 heterostructures with an efficient nanointerface for electrocatalytic oxygen evolution

Haitao Xu,Dianhua Song,Jiao Li,Yan Zhao,Ruijie Yang,Jingzhe Zhao

The demand for sustainable energy sources urges the development of efficient and earth-abundant electrocatalysts . Herein, chlorine assisted ion-exchange and in-situ sulfurization processes were combined to construct CuCo 2 S 4 @(Cu,Co) 2 Cl(OH) 3 heterostructures from Cu(OH) 2 nanoarrays. Chlorine element in the cobalt source stimulated the formation of (Cu,Co) 2 Cl(OH) 3 precursor, and further facilitated partial transformation of the precursor to CuCo 2 S 4 on the surface to achieve composite structure. The mixed valences of Co element (Co 3+ in CuCo 2 S 4 and Co 2+ in (Cu,Co) 2 Cl(OH) 3 ) and O S interpenetrated nanointerface in the composite catalysts provided low electron transfer resistance for good alkaline oxygen evolution reaction (OER) activities. In 1 mol L −1 KOH electrolyte, the overpotentials of the optimal composite catalyst reached 253 and 290 mV respectively at the current density of 20 and 50 mA cm −2 , which is comparable to the activity of commercial Ir/C (281 mV@20 mA cm −2 ). These findings could provide opportunities for designing effective and inexpensive composite electrocatalysts through nanointerface engineering strategy.

研究领域: 材料科学 · 电化学 · 能源转换与存储
✓ 已验证 DOI PubMed 高影响因子
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

Activated carbon adsorption coupled with ozonation regeneration for efficient removal of chlorobenzene

Mingzhu Ren,Jing Wang,Zhengyang Wang,Sihan Sun,Jiakai Qiu,Yanchun Shi,Zhou-jun Wang,Yongbing Xie

Chlorobenzene is a typical toxic and persistent organic pollutant in wastewater and site polluted groundwater. In this study, powdered activated carbon (AC) was used for the adsorption of chlorobenzene from simulated wastewater, and it showed high adsorption capacity in a wide range of pH. Pseudo-second-order kinetic model and Langmuir isothermal adsorption model are suitable to describe the adsorption process . Furthermore, the adsorption mechanism is clarified by correlating the adsorption rate constants with the molecular descriptor by theory calculating. Chlorobenzene adsorption on AC was mainly controlled by π-π interaction and hydrophobicity , external mass transfer and intraparticle diffusion. Ozonation was adopted to regenerate the adsorption saturated AC and simultaneously avoid secondary solid waste. After three cycles of adsorption-ozonation, the adsorption capacity of AC even increased from 80 to 215 mg/g due to the increase of oxygen-containing functional groups on the AC surface. This mode can also be used for granular AC column adsorption, and ozonation partially restored the adsorption capacity. The work provides a better alternative way to deal with chlorobenzene polluted wastewater and groundwater.

研究领域: 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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CELLULOSE · 2020 ·Vol. 27 ·期 5 ·2737-2756 · IF 4.21

Porous SBA-15/cellulose membrane with prolonged anti-microbial drug release characteristics for potential wound dressing application

Shen Zhi,Cai Ning,Xue Yanan,Yu Bo,Wang Jianzhi,Song Hao,Deng Hang,Yu Faquan

Abstract A sustained release of anti-infection drugs is beneficial for the reduction of required dressing change times and the protection of the granulation tissue against further infection. In this work, the strategy of encapsulating mesoporous SBA-15 particles in a permeable cellulose membrane (CM) was used in the preparation of antibacterial cellulose based composite membranes to depot store and deliver drugs with prolonged anti-microbial drug release characteristics. It was found that SBA-15 with the protection of phosphate buffered saline prefilled in SBA-15 mesoporous channel could resist strong alkali environment during composite membranes preparation and its mesoporous structure remained intact, which was verified by SEM, TEM and BET results. The resultant cellulose based composite membrane containing 30 wt% SBA-15 (denoted as P-CM-SBA (30%)) had achieved 3.6 wt% drug loading and demonstrated the sustained release of chloramphenicol for 250 h, which was resulted from SBA-15/cellulose structure-inducing two-stage release behavior. Strong antibacterial activity of P-CM-SBA (30%) against S. aureus and E. coli . could last 144 h. In addition, the tensile strength, water vapor transmission rate and swelling properties of P-CM-SBA (30%) conformed to the primary requirements of wound dressing materials. Therefore, cellulose based composite membrane with 30 wt% SBA-15 particles possesses the potential for the application of wound healing. Graphic abstract

研究领域: 材料科学 · 生物医学工程 · 药剂学
✓ 已验证 DOI 高影响因子
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Frontiers in Pharmacology · 2020 · IF 4.225

Inhibition of Tyrosinase by Mercury Chloride: Spectroscopic and Docking Studies

Chen Jianmin,Ye Yaling,Ran Mengnan,Li Qinglian,Ruan Zhipeng,Jin Nan

Inorganic mercury compounds have been used in skin-lightening products since ancient times. Although a previous study demonstrated that mercury impeded the transfer of Cu2+ to the apotyrosinase, the effect of mercury on tyrosinase is still unclear. In the present study, the mechanism of mercury chloride (HgCl2) induced inactivation of tyrosinase was investigated for the first time. The IC50 values were 29.97 and 77.93 μmol/L for monophenolase and diphenolase, respectively. A kinetic analysis revealed that HgCl2 inhibited tyrosinase activity in an irreversible non-competitive manner. The strong intrinsic fluorescence quenching suggested that the formation of the HgCl2-tyrosinase complex induced conformational changes of the enzyme, and HgCl2 had only one single binding site or a single class of binding site on tyrosinase. The molecular docking and further experiments demonstrated that HgCl2 bound to the amino residuals (His) in the catalytic center of tyrosinase. To our knowledge, these findings presented in this paper were the first evidence of the direct interactions between HgCl2 and tyrosinase, which provided a deep understanding of the inhibition mechanism of mercury on tyrosinase.

研究领域: 生物化学 · 毒理学
✓ 已验证 DOI PubMed 高影响因子
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