石油学报(石油加工)
石油學報(石油加工)
석유학보(석유가공)
ACTA PETROLEI SINICA(PETROLEUM PROCESSING SECTION)
2010年
2期
201-207
,共7页
王声洁%沈本贤%肖卫国%宋庆雷
王聲潔%瀋本賢%肖衛國%宋慶雷
왕성길%침본현%초위국%송경뢰
Au(en)_2Cl_3%乙炔%氢氯化%金
Au(en)_2Cl_3%乙炔%氫氯化%金
Au(en)_2Cl_3%을결%경록화%금
Au(en)_2Cl_3%acetylene%hydrochlorination%gold
采用Au(en)_2Cl_3作前驱体,制备了用于乙炔氢氯化反应的载Au催化剂,并采用N_2-吸附、XRD、TEM进行了表征.在常压固定床反应器中考察了Au的价态、载体、Au负载量、碱金属助剂对Au催化剂活性的影响.结果表明,催化乙炔氢氯化反应的载Au催化剂的活性组分主要以离子态Au~n存在.采用椰壳质活性炭(AC~s)为载体、KCl为助剂、Au负载量为1%(质量分数)时,载Au催化剂Au-K/AC~s具有较高分散度,平均粒径为2.3 nm.以Au-K/AC~3作为催化剂,在温度180℃、空速240 h~(-1)、y(HCl)/V(C_2H_2)=1.1时,乙炔氢氯化反应的转化率可达98%以上,氯乙烯选择性不低于99.5%;在空速为2000 h~(-1)时,该催化剂仍具有较好的稳定性.
採用Au(en)_2Cl_3作前驅體,製備瞭用于乙炔氫氯化反應的載Au催化劑,併採用N_2-吸附、XRD、TEM進行瞭錶徵.在常壓固定床反應器中攷察瞭Au的價態、載體、Au負載量、堿金屬助劑對Au催化劑活性的影響.結果錶明,催化乙炔氫氯化反應的載Au催化劑的活性組分主要以離子態Au~n存在.採用椰殼質活性炭(AC~s)為載體、KCl為助劑、Au負載量為1%(質量分數)時,載Au催化劑Au-K/AC~s具有較高分散度,平均粒徑為2.3 nm.以Au-K/AC~3作為催化劑,在溫度180℃、空速240 h~(-1)、y(HCl)/V(C_2H_2)=1.1時,乙炔氫氯化反應的轉化率可達98%以上,氯乙烯選擇性不低于99.5%;在空速為2000 h~(-1)時,該催化劑仍具有較好的穩定性.
채용Au(en)_2Cl_3작전구체,제비료용우을결경록화반응적재Au최화제,병채용N_2-흡부、XRD、TEM진행료표정.재상압고정상반응기중고찰료Au적개태、재체、Au부재량、감금속조제대Au최화제활성적영향.결과표명,최화을결경록화반응적재Au최화제적활성조분주요이리자태Au~n존재.채용야각질활성탄(AC~s)위재체、KCl위조제、Au부재량위1%(질량분수)시,재Au최화제Au-K/AC~s구유교고분산도,평균립경위2.3 nm.이Au-K/AC~3작위최화제,재온도180℃、공속240 h~(-1)、y(HCl)/V(C_2H_2)=1.1시,을결경록화반응적전화솔가체98%이상,록을희선택성불저우99.5%;재공속위2000 h~(-1)시,해최화제잉구유교호적은정성.
Gold-supported catalysts for acetylene hydrochlorination were prepared with Au(en)_2Cl_3 as precursor and analyzed by the characterization methods of N_2-adsorption, XRD and TEM. Effects of gold valence, support, Au loading and alkali metals on the catalytic performances of gold-supported catalysts were studied in detail at an atmospheric fixed bed reactor. The results indicated that the active constituents of gold-supported catalysts for hydrochlorination of acetylene were ionic Au~(n+). With activated carbon derived from coconut shell(AC~s) as the support, KCl as the promoter and Au loading of 1%, gold-supported catalyst Au-K/AC~s was of high dispersity and high catalytic activity for acetylene hydrochlorination. Under the reaction conditions of temperature 180℃, total gas hourly space velocity (GHSV) 240 h~(-1), feed volume ratio V(HCl)/V(C_2H_2)= 1.1, the conversion of acetylene was up to 98% and the selectivity to vinyl chloride was more than 99.5%. In addition, the stability of Au-K/AC~s catalyst was still favorable, even the GHSV was up to 2000 h~(-1).