SO_4~(2-)/ZrO_2固体酸催化神华煤直接液化反应性研究

通过间歇式加氢液化实验,考察了THN溶剂中液化温度、液化时间、氢气初压以及催化剂用量等反应条件对SO42-/ZrO2固体酸催化神华煤液化性能的影响,并基于产物分布和IR光谱表征,探讨了SO42-/ZrO2固体酸催化神华煤液化反应性及催化作用。结果表明,提高液化温度有利于煤催化加氢裂解,提高转化率和油气收率;增大氢气压力能够促进煤向沥青烯与前沥青烯等中间产物转化,但不利于生成液化油气;延长反应时间有利于前沥青烯加氢裂解,提高液化油气收率;SO42-/ZrO2固体酸的催化作用主要表现为对煤大分子结构的催化裂解,转化率和油气收率随催化剂用量增加而增大。此外,提高液化温度和氢气初压有利于含氧结构转化。

Study on the direct liquefaction reactivity of Shenhua coal catalyzed by SO 4 2- /ZrO 2 solid acid

Effects of liquefaction conditions, including temperature, time, initial hydrogen pressure, and catalyst dosage on direct liquefaction were investigated by batch hydro-liquefaction of Shenhua coal catalyzed by SO₄^2-/ZrO₂ solid acid. The mechanism and catalysis of Shenhua coal liquefaction catalyzed by SO₄^2-/ZrO₂ solid acid were also discussed by distribution and IR analysis of the products. The results indicate that increase in temperature is favorable for catalytic hydrocracking of coal, an increase in liquefaction conversion, and yields of oil plus gas. Raising the initial hydrogen pressure facilitates coal conversion into asphaltene and preasphaltene, but depresses the formation of oil and gas. The increase of liquefaction time is beneficial to the hydrocracking of preasphaltene with an increase in yields of oil plus gas. SO₄^2-/ZrO₂ solid acid mainly catalyzes the hydrocracking of coal macromolecular structure so that the conversion and yields of oil plus gas increase with increasing catalyst dosage. In addition, the conversion of the oxygen-containing structures such as hydroxyl needs high liquefaction temperature and initial hydrogen pressure.