文档介绍：摘要本文的主要研究内容足采用不同的催化刹制备技术制备二氧化碳与甲醇在常压条件下合成碳酸二甲酯的催化剂,并用XRD、BET、TPD、TPR和原位红外等技术对相应催化剂的晶相结构、比表面平J{、孔径、表面酸碱性能、C02和 CH30H在催化剂上的吸附行为等催化性能进行了表征。用浸渍沉淀法结合微波和超卢波技术制备负载型Zr02/A1203催化剂,并用 MgO、La203、Ce02等氧化物对ZrOe/A1203催化剂进行掺杂和崩K20,M003, 和V:05等对ZrO:/A1203催化剂进行表面改性。结果表明,在ZrO:/A1203催化剂中掺杂MgO,La203,和Ce02等氧化物,能有效地阻止Zr02的团聚,减小Zr02 的粒径,催化剂的比表面积增大,表面酸、碱中心数和强度得到了~定的调控。其【1J,在Zr02/A1203复合载体l|1掺入CeO!能增加催化剂表面碱性中心数,催化剂活性较高,%,碳酸二甲酯的选择性为100%。用K20, M003,和V205等对Zr02/A1203催化剂进行表新改性,对Zr02的晶相结构、比表面积和孔径影响不明显,但能有效调控催化剂的表面的酸、碱中心数和强度。其rflM003和V205能使Zr02/A1203催化剂表面的酸性巾一tL,数增加,表现出较好的催化活性。在Zr02/A1203催化剂中Zr02作为活性组分,在以■氧化碳与甲醇为原料常压条件下合成碳酸二甲酯具有一定的催化活性和高选择性,在此基础上,以Zr02 ,,La203,和Ce02氧化物。结果表明,掺杂氧化物能稳定t-Zr02的结构,提高催化剂的比表而积和表衙碱性中心强度,掺杂氧化物能促进CH30H. 和C02在各催化剂表面发生解离吸附,, %,碳酸二甲酯的选择性为100%。采用尿素均匀沉淀法、, 考察了不同制备方法和不同锆铈比对催化剂的催化性能影响。结果表明,尿素均匀沉淀法制备的催化剂表面具有较多的酸性位和金属位,表现山较好的催化性能。NiO—,NiO由较好还原性能,催化剂表面同时具有的酸性位和碱性位,催化剂能有效吸附活化CH30H和C02,%,碳酸二甲酯的选择性为100%。关键词:碳酸二甲酯,甲醇,二氧化碳,氧化锆,掺杂氧化物 Abstract This dissertation consists of the following parts:different method was applied tO prepare thecatalysts,and thesynthesis ofdimethyl carbonatefrom carbon dioxide and methanol was chosen toinvestigate the catalytic properties of the catalysts. The crystal structure,surface area,pore diameter and acid center properties ofthe catalysts were characterized by X—raydiffraction(XRD),BET volume method (BET),Fourier transformation infra-red(FToIR),and temperature—programmed desorption(TPD),et The impregnation—precipitation method,microwave and supercritical was applied to prepare thesupported Zr02/ MgO、La203 and Ce02 were doped inthe Zr02/A1203 andtheZr02/A1203 was modified byK20、M003 and results indicated thatthedoping oxides blocked theintegrating oftheZr02 grain sizeoftheZr02 was decreased and the surface area ofthecatalysts was existence of the Ce02 incre