Elemental mercury (Hg0) removal from coal syngas using magnetic tea-biochar: Experimental and theoretical insights.

Mercury is ranked 3rd as a global pollutant because of its long persistence in the environment. Approximately 65% of its anthropogenic emission (Hg0) to the atmosphere is from coal-thermal power plants. Thus, the Hg0 emission control from coal-thermal power plants is inevitable. Therefore, multiple sorbent materials were synthesized using a one-step pyrolysis method to capture the Hg0 from simulated coal syngas. Results showed, the Hg0 removal performance of the sorbents increased by the citric acid/ultrasonic application. T5CUF0.3 demonstrated the highest Hg0 capturing performance with an adsorption capacity of 106.81 µg/g within 60 min at 200 °C under complex simulated syngas mixture (20% CO, 20% H2, 10 ppmV HCl, 6% H2O, and 400 ppmV H2S). The Hg0 removal mechanism was proposed, revealing that the chemisorption governs the Hg0 removal process. Besides, the active Hg0 removal performance is attributed to the high dispersion of valence Fe3O4 and lattice oxygen (α) contents over the T5CUF0.3 surface. In addition, the temperature programmed desorption (TPD) and XPS analysis confirmed that H2S/HCl gases generate active sites over the sorbent surface, facilitating high Hg0 adsorption from syngas. This work represented a facile and practical pathway for utilizing cheap and eco-friendly tea waste to control the Hg0 emission.

Effect of Sonochemical Treatment on Thermal Stability, Elemental Mercury (Hg0) Removal, and Regenerable Performance of Magnetic Tea Biochar.

Elemental mercury (Hg0) removal from a hot gas is still challenging since high temperature influences the Hg0 removal and regenerable performance of the sorbent. In this work, a facile yet innovative sonochemical method was developed to synthesize a thermally stable magnetic tea biochar to capture the Hg0 from syngas. A sonochemically synthesized magnetic sorbent (TUF0.46) exhibited a more prodigious surface area with developed pore structures, ultra-paramagnetic properties, and high dispersion of Fe3O4/γ-Fe2O3 particles than a simply synthesized magnetic sorbent (TF0.46). The results showed that TUF0.46 demonstrated strong thermostability and attained a high Hg0 removal performance (∼98.6%) at 200 °C. After the 10th adsorption/regeneration cycle, the Hg0 removal efficiency of TUF0.46 was 19% higher than that of TF0.46. Besides, at 23.1% Hg0 breakthrough, TUF0.46 achieved an average Hg0 adsorption capacity of 16.58 mg/g within 24 h under complex syngas (20% CO, 20% H2, 5% H2O, and 400 ppm H2S). In addition, XPS results revealed that surface-active components (Fe+, O2-, O*, C=O) were the key factor for high Hg0 removal performance over TUF0.46 from syngas. Hence, sonochemistry is a promising practical tool for improving the surface morphology, thermal resistance, renewability, and Hg0 removal efficiency of a sorbent.

Study on the Pretreatment Process and Removal Rules of Sulfur-Containing Compounds for Medium- and Low-Temperature Coal Tar.

The heteroatoms (sulfur and nitrogen) and metals (ferrum and calcium) in coal tar can easily cause the corrosion of hydrogenation equipment, catalyst poisoning, and environmental pollution. These should be removed before coal tar is hydrogenated. In this study, with the acid refining method, the effects of three polyether demulsifiers (i.e., PD1, PD2, and PD3), polyamine carboxylate demetallizers (i.e., PCD1, PCD2, and PCD3), and separation temperature on the removal of ferrum, calcium, sulfur, and nitrogen in medium- and low-temperature coal tar were determined. PD2 was selected, and the added amount was 200 µg·g-1. When the PD2 demulsifier was added alone or PD2 demulsifier with various demetallization agents was added, heteroatoms in coal tar could be effectively removed. For the experiments and analysis, the pretreatment conditions of coal tar were as follows: the addition amount of the PD2 demulsifier was 200 µg·g-1, the addition amount of the PCD3-type demetallization agent was 400 µg·g-1, and the stirring temperature was 80 °C. Before and after pretreatment, the methods of inductively coupled plasma-atomic emission spectrometer, gas chromatography-mass spectrometry (MS), and Fourier transform-ion cyclotron resonance MS were used in the present study to explore and analyze the distribution, occurrence form, and removal law of sulfur in coal tar. As revealed from the results, sulfur compounds in coal tar <360 °C fraction (light coal tar fraction, LF) before being pretreated had a lower content, which existed as benzothiophene and dibenzothiophene largely. Sulfur compounds S1 and S2 achieved the maximum relative abundance in >360 °C fraction (heavy coal tar fraction, HF). After the compounds were pretreated, the sulfur removal rate reached 40.0% in LF, and the sulfur compounds were primarily removed. For HF, the sulfur removal rate reached 20.1%. In addition, S1 compounds within the dibenzothiophene derivatives exhibiting more side chains and a larger condensation degree were basically removed. S2 compounds, mainly linked to several quinolines or more aromatic rings and thioether-aliphatic amine sulfur compounds exhibiting small molecular weight and simple structures, were relatively easy to remove. The SO class (e.g., the sulfones and thiophene-ketone group) was more difficult to remove.