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Purification and characterization of Al_(13) species in coagulant polyaluminum chloride

Journal of Environmental Sciences 2009年第1期21卷 18-22页

作者： GAO Baoyu CHU Yongbao yue qinyan WANG Yan School of Environmental Science and Engineering Shondong University Jinan 250100 China. School of Environment and Safety Engineering Qingdong University of Science and Technology Qingdao 266042 China Key Laboratory of Colloid and Interface Chemistry Minstry of Education Shandong University Jinan 250100 China

Nano-Al13 was separated and purified by four methods to investigate its characteristic, and was analyzed by Al-Ferron timed complexation spectrophotometer, ^27Al-NMR （nuclear magnetic resonance）, and transmission electron microscopy （TEM）. Coagulation efficiency of nano-Al13, polyaluminum chloride （PAC）, and AlCl3 in synthetic water were also investigated by jar test. The dynamic process and aggregation state of kaolin suspensions coagulating with nano-Al13, PAC, and AlCl3 were also investigated. The experimental results indicated that the efficiency of gel column chromatography method was the highest for separating PAC solution with low Al concentration. Ethanol and acetone method was simple and could separated PAC solution with different Al concentrations, while silicon alkylation white block column chromatography method could separate PAC solution only with low Al concentration. The SO4^2-/Ba^2＋ displacement method could separate PAC solution with high Al concentration, but extra inorganic cation and anion could be introduced into the solution during the separation. The coagulation efficiency and dynamic experimental results showed that nano- Al13 with a high positive-charged species was the main species of electric neutralization in coagulation process, and it could reduce the turbidity and increase the effective particles collision rate efficiently in coagulation process. Its coagulation speed and the particle size of coagulant formed were of greatest value in this study.

关键词： nano-Al13 separation and purification coagulation dynamic processes

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Investigation of dynamic processing on aluminum floc aggregation:Cyclic shearing recovery and effect of sulfate ion

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Science China Chemistry 2008年第4期51卷 386-392页

作者： CHU YongBao GAO BaoYu yue qinyan WANG Yan School of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042China School of Environmental Science and Engineering Shandong UniversityJinan 250100China

The floc formation and re-aggregation potential and the effects of sulfate on coagulation by AlCl3, polyaluminum chloride (PAC), and Al13 species using a photometric dispersion analyzer (PDA) are in- vestigated. It is found that the recovery level from shearing is the highest for the Al13 species. This is likely a result of increased collision efficiency due to more effective charge neutralization. The ex- perimental results show that sulfate has a significant effect on coagulation and promoting aggregation of hydrolyzed species for the Al13 species. It results in significant improvement of the coagulation effi- ciency through an electrostatic patch effect. The results further indicate that zeta potential of the parti- cle suspension is not the only indicator for the coagulant efficiency when precipitate formation sig- nificantly improves coagulation.

关键词： Al13 species coagulation dynamics polyaluminum chloride (PAC) sulfate

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Separating method and dynamic processes of Nano-Al_(13)

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Frontiers of Environmental Science & Engineering 2007年第3期1卷 368-373页

作者： GAO Baoyu CHU Yongbao yue qinyan KONG Chunyan WANG Xiaona School of Environmental Science and Engineering Shandong UniversityJinan 250100China College of Material and Environment Qingdao University of Science and TechnologyQingdao 266042China Department of Chemistry Dezhou UniversityDezhou 253023China

In order to investigate the characteristics of pure Nano-Al_(13) ,Nano-Al_(13) was separated and purified from a series of poly-aluminum chloride(PAC)solutions which had the same Al_(13) percentage but different total Al concentrations,by using column chromatography,ethanol-acetone resolving and SO_(4)^(2−)/Ba^(2+)displacement.The Al_(13) species yield was characterized by Al-ferron timed complexation spectropho-tometry and 27Al-NMR(nuclear magnetic resonance).The coagulation efficiency of Nano-Al_(13) ,PAC and AlCl_(3) in synthetic water was also investigated by Jar tests.The dynamic process and aggregation state of kaolin suspensions coagulating with Nano-Al_(13) ,PAC and AlC_(13) were similarly investigated using a photometric dispersion analyzer 2000(PDA2000).The experimental results indicated that the ethanol-acetone resolving method was simple and could separate the PAC solution at different concentrations,while column chromatography could separate PAC solutions at low concentrations.The SO_(4)^(2−)/Ba^(2+)displacement method could separate PAC solutions at high concentrations.However,extra inorganic cation and anion could be added in the solution during separation.The coagulation efficiency and dynamic experimental results showed that Nano-Al_(13) with high positive-charged species was effective in removing turbidity and color.The dynamic process results showed that Nano-Al_(13) also had the best recovery capability after shearing compared with PAC and AlCl3 because the Nano-Al_(13) conformation is more effective in charge neutralization.

关键词： Nano-Al_(13) separation and purification coagula-tion dynamic processes

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Carbon-based single atom catalyst: Synthesis, characterization, DFT calculations

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Chinese Chemical Letters 2022年第2期33卷 663-673页

作者： Yanan Shang Xiaoguang Duan Shaobin Wang qinyan yue Baoyu Gao Xing Xu Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityJi’nan 250100China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia

Carbon-based single-atom catalysts(SACs) with atomic sizes of active sites have become the promising candidates for a variety of catalytic systems because of their high atom utilization, and unique electronic structures. Different types of single-atom sites can be fabricated via multiple preparation strategies, which would demonstrate distinct different coordination configurations and electronic features, and ultimately affected the structure-catalysis relationship of SACs in targeted reactions. As a result, it is necessary to identify the active sites of SACs and understand the structure-catalysis relationship of SACs at the atomic scale. In this review, a variety of preparation strategies of carbon-based SACs were documented. Then, the recent development on versatile characterization techniques and computational achievements were summarized regarding in understanding the electronic and geometric characteristics of carbon-based SACs.Finally, major challenges and development directions concerning single-atom sites identification and advanced tools development are discussed to shed light on future research of carbon-based SACs.

关键词： Single atom Synthesis DFT calculations Characterization Catalysis

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Insights into properties of activated carbons prepared from different raw precursors by pyrophosphoric acid activation

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Journal of Environmental Sciences 2016年第3期28卷 235-243页

作者： Yuan Gao qinyan yue Baoyu Gao Shandong Provincial Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong University

Low-cost activated carbons（ACs） were prepared from four kinds of solid wastes：petroleum coke,Enteromorpha prolifera,lignin from papermaking black liquid and hair,by pyrophosphoric acid（H_4P_2O_7） activation.Thermo-gravimetric analysis of the pyrolysis of H_4P_2O_7-precursor mixtures implied that H_4P_2O_7 had different influences on the pyrolysis behavior of the four raw materials.N_2 adsorption/desorption isotherms,scanning electron microscopy,Fourier transform infrared spectroscopy and adsorption capacities for dyes were used to characterize the prepared activated carbons.AC derived from E.prolifera exhibited the highest surface area（1094 m^2/g） and maximum monolayer adsorption capacity for malachite green（1250 mg/g）.Kinetic studies showed that the experimental data were in agreement with the pseudo-second-order model.The adsorption isotherms were well described by the Langmuir isotherm model,indicating the adsorption of dye onto the ACs proceeded by monolayers.

关键词： Solid waste Pyrophosphoric acid Low-cost adsorbent Dye Adsorption

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Synchronous removal of CuO nanoparticles and Cu2+ by polyaluminum chloride-Enteromorpha polysaccharides: Effect of Al species and pH

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Journal of Environmental Sciences 2020年第2期32卷 1-11页

作者： Yuanxia Luo Baoyu Gao Jie Wang qinyan yue Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong University266000 QingdaoChina

Copper oxide nanomaterials have been extensively applied and can have serious impacts when discharged into the aquatic environment, especially when complexed with humic acid(HA) to form composite contaminants.As an innovative recycled coagulant aid,Enteromorpha polysaccharides(Ep) were associated with polyaluminum chloride(PACl)(denoted as PACl-Ep) to simultaneously remove CuO nanoparticles, Cu2+and HA in this study.The influence of different Al species coagulants(AlCl3, PAClb and PAClc) and water pH on coagulation performance, floc properties and reaction mechanisms was investigated in detail.Results showed that in the three PACl-Ep systems, PAClb-Ep gave the highest removal efficiencies for turbidity and Cu2+, and the best UV254 removal effect was reached by using PAClc-Ep.Higher contents of Alb and Alc contributed to great coagulation performance because of their stronger bridging and sweeping effects.For all the Al species coagulants, alkalescent conditions were more conducive to removing Cu and HA compared to acidic conditions.Additionally, smaller and more agminated flocs with great recovery ability were formed by PAClb-Ep and PAClc-Ep systems(bridging and enmeshment effects cooperated with the chelated reticular structure formed by the Ep and Al species).Similarly,due to the increased hydrolysis and hydroxide precipitates, flocs formed under the condition of alkalescence were smaller, denser and stronger compared with weakly acidic conditions.

关键词： Al species Enteromorpha polysaccharides Polyaluminum chloride 27Al nuclear magnetic resonance Simultaneous removal

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Facile one-step synthesis of functionalized biochar from sustainable prolifera-green-tide source for enhanced adsorption of copper ions

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Journal of Environmental Sciences 2018年第11期30卷 185-194页

作者： Yuan Gao Xiuzhen Zhu qinyan yue Baoyu Gao Shandong Provincial Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and Engineering Shandong University Jinan 250100 China Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education) School of Environmental Science and Technology Dalian University of Technology Linggong Road 2 Dalian 116024 China

The use of biochars formed by hydrothermal carbonization for the treatment of contaminated water has been greatly limited, due to their poorly developed porosity and low content of surface functional groups. Also, the most common modification routes inevitably require post-treatment processes, which are time-consuming and energy-wasting. Hence, the objective of this research was to produce a cost-effective biochar with improved performance for the treatment of heavy metal pollution through a facile one-step hydrothermal carbonization process coupled with ammonium phosphate, thiocarbamide, ammonium chloride or urea, without any posttreatment. The effects of various operational parameters, including type of modification reagent, time and temperature of hydrothermal treatment, and ratio of modification reagent to precursor during impregnation, on the copper ion adsorption were examined. The adsorption data fit the Langmuir adsorption isotherm model quite well. The maximum adsorption capacities （mg/g） of the biochars towards copper ions followed the order of 40-8h-1.0-APBC （95.24）〉 140-Sh-O-BC （12.52）〉 140-8h-1.0-TUBC （12.08）〉 140-Sh-1.0-ACBC （7.440）〉 140-Sh-1.0-URBC （5.277）. The results indicated that biochars modified with ammonium phosphate displayed excellent adsorption performance toward copper ions, which was 7.6-fold higher than that of the pristine biochar. EDX and FT-IR analyses before and after adsorption demonstrated that the main removal mechanism involved complexation between the phosphate groups on the surface of the modified biochars and copper ions.

关键词： Hydrothermal carbonization Functionalized biochar Adsorption Heavy metal

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Effect of viscosity,basicity and organic content of composite flocculant on the decolorization performance and mechanism for reactive dyeing wastewater

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Journal of Environmental Sciences 2011年第10期23卷 1626-1633页

作者： Yuanfang Wang Baoyu Gao qinyan yue Yan Wang Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and Engineering Shandong University Jinan 250100 China

A coagulation/flocculation process using the composite flocculant polyaluminum chloride-epichlorohydrin dimethylamine （PAC- EPI-DMA） was employed for the treatment of an anionic azo dye （Reactive Brilliant Red K-2BP dye）. The effect of viscosity 01）, basicity （B = [OH]/[Al]） and organic content （Wp） on the flocculation performance as well as the mechanism of PAC-EPI-DMA flocculant were investigated. The η was the key factor affecting the dye removal efficiency of PAC-EPI-DMA. PAC-EPI-DMA with an intermediate η （2400 mPa.sec） gave higher decolorization efficiency by adsorption bridging and charge neutralization due to the co-effect of PAC and EPI-DMA polymers. The Wp of the composite flocculant was a minor important factor for the flocculation. The adsorption bridging of PAC-EPI-DMA with η of 300 or 4300 mPa.sec played an important role with the increase of Wp, whereas the charge neutralization of them was weaker with the increase of Wp. There was interaction between Wp and B on the removal of reactive dye. The composite flocculant with intermediate viscosity and organic content was effective for the treatment of reactive dyeing wastewater, which could achieve high reactive dye removal efficiency with low organic dosage.

关键词： composite flocculant reactive dye removal flocculation mechanism decolorization efficiency

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Characterization of dissolved organic matter and membrane fouling in coagulation-ultrafiltration process treating micro-polluted surface water

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Journal of Environmental Sciences 2019年第1期31卷 318-324页

作者： Fan Bu Baoyu Gao qinyan yue Xue Shen Wenyu Wang Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and Engineering Shandong University

Coagulation–ultrafiltration(C–UF) is widely used for surface water treatment. With the removal of pollutants, the characteristics of organic matter change and affect the final treatment efficiency and the development of membrane fouling. In this study, we built a dynamic C–UF set-up to carry out the treatment of micro-polluted surface water, to investigate the characteristics of dissolved organic matter from different units. The influences of poly aluminum chloride and poly dimethyldiallylammonium chloride(PDMDAAC) on removal efficiency and membrane fouling were also investigated. Results showed that the dosage of PDMDAAC evidently increased the UV254 and dissolved organic carbon removal efficiencies,and thereby alleviated membrane fouling in the C–UF process. Most hydrophobic bases(HoB)and hydrophobic neutral fractions could be removed by coagulation. Similarly, UF was good at removing HoB compared to hydrophilic substances(HiS) and hydrophobic acid(HoA)fractions. HiS and HoA fractions with low molecule weight accumulated on the surface of the membrane, causing the increase of transmembrane pressure(TMP). Membrane fouling was mainly caused by a removable cake layer, and mechanical cleaning was an efficient way to decrease the TMP.

关键词： Coagulation Ultrafiltration Dissolved organic matter Membrane fouling

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Fractionation of residual Al in natural water treatment from reservoir with poly-aluminum-silicate-chloride (PASiC): Effect of OH/Al, Si/Al molar ratios and initial pH

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Journal of Environmental Sciences 2012年第11期24卷 1908-1916页

作者： Zhonglian Yang Baoyu Gao Yan Wang Yaqin Zhao qinyan yue Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityJi'nan 250100China

An aluminum fractionation study was conducted for a surface reservoir water treatment to understand the performance of poly- aluminum-silicate-chloride （PASiC） in terms of the residual A1 fractions as a function of initial pH. The coagulation performance expressed as turbidity and organic matter removal was established as supporting data. Some extra data were evaluated in terms of the residual A1 ratio of the composite PASiC coagulant. The main residual A1 sources were the A1 fractions derived from the use of PASiC. The turbidity and organic matter removal ability was optimal at initial pH 6.00-7.00, while the concentrations of various residual A1 species and the residual A1 ratio of PASiC were minimal at an initial pH range of 7.00-8.00. Under the conditions of OH/AI molar ratio = 2.00 and Si/A1 molar ratio = 0.05, PASiC had superior coagulation performance and comparatively low residual A1 concentrations. The A1 fraction in the composite PASiC coagulant seldom remained under such conditions. Experimental data also indicated that the suspended （filterable） AI fraction was the dominant species, and organic-bound or organo-A1 complex A1 was considered to be the major species of dissolved A1 in water treated by PASiC coagulation. Additionally, the dissolved inorganic monomeric A1 species dominated the dissolved monomeric A1 fraction.

关键词： coagulation performance OH/A1 and Si/AI molar ratio poly-aluminum-silicate-chloride （PAniC） resi0ual AI speclataon residual A1 ratio

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