Lingjun Kong

Preparation and characterization of a hierarchical porous char from sewage sludge with superior adsorption capacity for toluene by a new two-step pore-fabricating process

A kind of hierarchical porous char (SCCA/Zn) was prepared from sewage sludge by a new two-step pore-fabricating process coupling citric acid (CA) with ZnCl2 in a pyrolysis process. The char was characterized by element analysis, N2-adsorption and mercury intrusion measurement etc. It is found that coupling CA and ZnCl2 can synergistically fabricate pores in the pyrolysis process, resulting in a hierarchical porous char, SCCA/Zn, with the largest SBET of 867.6 m(2) g(-1) due to the fact that the former contributes to the fabrication of macro-pores, which provides more space for fabricating meso- and micro-pores by ZnCl2 activation. Although the SBET of SCCA/Zn was 15% less than that of activated carbon fiber (ACF, SBET=999.5 m(2) g(-1)), SCCA/Zn had a higher toluene adsorption capacity (0.83 g g(-1)) than ACF. The inconsistence between their SBET and adsorption capacity can be ascribed to the strong hydrophobic property of SCCA/Zn.

Catalytic wet air oxidation of 2-chlorophenol over sewage sludge-derived carbon-based catalysts.

A sewage sludge derived carbon-supported iron oxide catalyst (FeSC) was prepared and used in the Catalytic Wet Air Oxidation (CWAO) of 2-chlorophenol (2-CP). The catalysts were characterized in terms of elemental composition, surface area, pHPZC, XRD and SEM. The performances of the FeSC catalyst in the CWAO of 2-CP was assessed in a batch reactor operated at 120°C under 0.9MPa oxygen partial pressure. Complete decomposition of 2-CP was achieved within 5h and 90% Total Organic Carbon (TOC) was removed after 24h of reaction. Quite a straight correlation was observed between the 2-CP conversion, the amount of iron leached in solution and the pH of the reaction mixture at a given reaction time, indicating a strong predominance of the homogeneous catalysis contribution. The iron leaching could be efficiently prevented when the pH of the solution was maintained at values higher than 4.5, while the catalytic activity was only slightly reduced. Upon four successive batch CWAO experiments, using the same FeSC catalyst recovered by filtration after pH adjustment, only a very minor catalyst deactivation was observed. Finally, based on all the identified intermediates, a simplified reaction pathway was proposed for the CWAO of 2-CP over the FeSC catalyst.

Simultaneous reduction and adsorption for immobilization of uranium from aqueous solution by nano-flake Fe-SC

Uranium containing radioactive wastewater is seriously hazardous to the natural environment if it is being discharged directly. Herein, nano-flake like Fe loaded sludge carbon (Fe-SC) is synthesized by carbothermal process from Fe-rich sludge waste and applied in the immobilization of uranium in aqueous. Batch isotherm and kinetic adsorption experiments are adopted to investigate the adsorption behavior of Fe-SC to uranium in aqueous. XPS analyses were conducted to evaluate the immobilized mechanism. It was found that the carbonized temperature played significant role in the characteristics and immobilization ability of the resulted Fe-SC. The Fe-SC-800 carbonized at 800°C takes more advantageous ability in immobilization of uranium from aqueous than the commercial available AC and powder zero valent iron. The adsorption behavior could be fitted well with the Langmuir isotherm adsorption model and pseudo-second order model. The equilibrium adsorption amount and rate for Fe-SC-800 is high to 148.99mgg-1 and 0.015gmg-1min-1, respectively. Both reductive precipitation and physical adsorption are the main mechanisms of immobilization of uranium from aqueous by Fe-SC-800.

Sorption Performance and Mechanism of a Sludge-Derived Char as Porous Carbon-Based Hybrid Adsorbent for Benzene Derivatives in Aqueous Solution

A porous sludge-derived char was prepared by a new one-step pyrolytic process with citric acid-ZnCl2 mixed fabricating-pore agents. The sludge-derived char was confirmed to be a hierarchically porous hybrid adsorbent containing-elemental carbon, -highly carbonized organic species and -inorganic ash with a great surface area of 792.4m(2)g(-1). It was used as a carbon-based hybrid adsorbent for four benzene derivatives including 4-chlorophenol, phenol, benzoic acid and 4-hydroxylbenzoic acid in aqueous solution. Results showed that their sorption isotherms were nonlinear at low concentrations and linear at high concentrations. The sorption performance could be described by a multiple sorption model (QT=QA+KPCe). The order of these partition sorption coefficients (KP) of these benzene derivatives was consistent with their octanol-water partition coefficients (logKow), but those saturated amounts (QA) were inconsistent with their logKow. The inconstancy was found to be considerably dependent on the preferential interaction of benzoic acid with SiO2 in the sludge-derived char. Quantum theoretical calculation confirmed that the preferential interaction was attributed to the formation of hydrogen bonds (1.61 and 1.69Å) and new Si-O bonds (1.83 and 1.87Å) between the carboxyl of benzoic acid and the SiO2 surface in the sorption process.

Performance and Mechanism of Piezo-Catalytic Degradation of 4-Chlorophenol: Finding of Effective Piezo-Dechlorination

Piezo-catalysis was first used to degrade a nondye pollutant, 4-chlorophenol (4-CP). In this process, hydrothermally synthesized tetragonal BaTiO3 nano/micrometer-sized particles were used as the piezo-catalyst, and the ultrasonic irradiation with low frequency was selected as the vibration energy to cause the deformation of tetragonal BaTiO3. It was found that the piezoelectric potential from the deformation could not only successfully degrade 4-chlorophenol but also effectively dechlorinate it at the same time, and five kinds of dechlorinated intermediates, hydroquinone, benzoquinone, phenol, cyclohexanone, and cyclohexanol, were determined. This is the first sample of piezo-dechlorination. Although various active species, including h+, e-, •H, •OH, •O2-, 1O2, and H2O2, were generated in the piezoelectric process, it was confirmed by ESR, scavenger studies, and LC-MS that the degradation and dechlorination were mainly attributed to •OH radicals. These •OH radicals were chiefly derived from the electron reduction of O2, partly from the hole oxidation of H2O. These results indicated that the piezo-catalysis was an emerging and effective advanced oxidation technology for degradation and dechlorination of organic pollutants.

Adsorption of phosphorus by calcium-flour biochar: Isotherm, kinetic and transformation studies

Discharging phosphorus (P)-contaminated water directly into the aquatic environment leads to resource loss and eutrophication. Thus, removing P from waste streams is imperative. In this study, calcium-decorated biochar (Ca-BC) in different mass ratios of Ca to BC was designed to effectively adsorb P from solution. Ca-BC was characterized through X-ray diffraction (XRD) analysis, followed by isotherm and kinetic adsorption experiments. The decorated Ca on the BC surface was found to have preferred P adsorption ability. A design of calcium hydroxide (Ca(OH)2) to flour in a mass ratio of 2:1 was found to have a maximum adsorption capacity of 314.22 mg g-1 for P. The Langmuir and pseudo-second-order models fit the sorption process adequately. XRD analysis indicated that the preferable adsorption ability to P was due to the reaction of Ca(OH)2 and PO43-, forming the hydroxylapatite (Ca5(PO4)3(OH)) crystal. The P in solution was transformed to the crystal. Thus, Ca-BC is an environmental friendly and low-cost sorbent for P removal.

Preparation and adsorption behavior of new hollow-like spherical sludge chars for methylene blue

A new pyrolytic process was successfully used to prepare hollow-like spherical sludge chars (HSC). In the process, pre-formed cotton spheres with a low density were firstly coated by a layer of sludge paste containing ZnCl2 to form cotton fiber@sludge spheres and then pyrolyzed at 500 °C for 2 h. The resulting HSC possessed a diameter of about 3 mm, a low density of 0.1008 g cm−3 and a high surface area of 1008 m2 g−1. The column adsorption behavior showed that the adsorption capacity and rate constant of HSC for methylene blue reached 186.4 mg g−1 and 0.232 mL min−1 mg−1. The adsorption capacity is about 8.4 and 12 fold of the adsorption capacities of GAC (22.28 mg g−1) and SC (15.26 mg g−1), respectively, and the adsorption rate constant is about 1.3 fold of that of GAC and SC. The great adsorption capacity and rate constant can be considerably dependent on the special hollow-like spherical structure of HSC.

Incorporation of Cadmium and Nickel into Ferrite Spinel Solid Solution: X-ray Diffraction and X-ray Absorption Fine Structure Analyses

The feasibility of incorporating Cd and Ni in hematite was studied by investigating the interaction mechanism for the formation of CdxNi1-xFe2O4 solid solutions (CNFs) from CdO, NiO, and α-Fe2O3. X-ray diffraction results showed that the CNFs crystallized into spinel structures with increasing lattice parameters as the Cd content in the precursors was increased. Cd2+ ions were found to occupy the tetrahedral sites, as evidenced by Rietveld refinement and extended X-ray absorption fine structure analyses. The incorporation of Cd and Ni into ferrite spinel solid solution strongly relied on the processing parameters. The incorporation of Cd and Ni into the CNFs was greater at high x values (0.7 < x ≤ 1.0) than at low x values (0.0 ≤ x ≤ 0.7). A feasible treatment technique based on the investigated mechanism of CNF formation was developed, involving thermal treatment of waste sludge containing Cd and Ni. Both of these metals in the waste sludge were successfully incorporated into a ferrite spinel solid solution, and the concentrations of leached Cd and Ni from this solid solution were substantially reduced, stabilizing at low levels. This research offers a highly promising approach for treating the Cd and Ni content frequently encountered in electronic waste and its treatment residues.

Facile synthesis of highly reactive and stable Fe-doped g-C 3 N 4 composites for peroxymonosulfate activation: A novel nonradical oxidation process

Ferrous ions (Fe2+) are environmentally friendly materials but show extremely inefficient persulfate activation. Polymeric graphitic carbon nitride (g-C3N4) has recently shown potential to activate persulfates, but the process requires intense light irradiation. To overcome these drawbacks, we designed an innovative heterogeneous iron catalyst by doping Fe into g-C3N4 (Fe-g-C3N4) and used it to activate peroxymonosulfate (PMS) for degradation of pollutant phenol. The catalysts synthesized were fully characterized with various techniques, such as X-ray diffraction, Mössbauer spectroscopy, and X-ray photoelectron spectroscopy. Fe was found to be coordinated with the framework of g-C3N4. Approximately 100% degradation of phenol was achieved with Fe-g-C3N4 after 20 min of reaction, whereas less than 5% degradation of phenol was achieved with Fe2+. Fe-g-C3N4-PMS had a wide effective pH range, and its reactivity was nearly independent of natural illumination. In contrast to the previously proposed radical mechanisms, quenching experiments revealed that nonradical oxidation contributed to the observed degradation. The OO bond in the activated PMS likely underwent heterolysis, producing high-valence iron species (FeIVO) as the primary active species. These findings have important implications for the development of a selective heterogeneous nonradical-oxidation process.

Coupling template nanocasting and self-activation for fabrication of nanoporous carbon

Hierarchical nanoporous carbon (NPC) with great surface area and developed pore size distribution has been intently concerned. Herein, we report a facile method coupling template nanocasting and self-activation to fabricate nanoporous carbon with continuous micro, meso and macro pores, in which CaCO3 acted as template and activation reagent while the flour was the carbon precursor. Effects of mass ratio of CaCO3 to flour and carbonized temperature on the pore structures of NPC were investigated by nitrogen adsorption-desorption isotherms and SEM analysis. Another kind of carbon was prepared by directly mixed powder CaCO3 with flour carbonized at 800 °C (NPC-p) to comparatively investigate the pore fabricating mechanism. Results shown that carbonized at 800 °C was favorable to fabricate the continuous macro, meso and micro pores. The resulted NPC in a mass ratio of 1 to 2 had the considerable SBET and VT of 575.4 m2/g and 0.704 cm3/g, respectively. Only surface activation was observed for NPC-p. Nanocasting of the powder CaCO3 contributed to fabricate macropores and the CO2 activation contributed to meso- and micropores. Coupling activation and nanocasting effect due to the decomposition of CaCO3 template into CO2 and CaO was ascribed to synthesize the nanoporous carbon.