工业催化
工業催化
공업최화
INDUSTRIAL CATALYSIS
2015年
6期
469-475
,共7页
精细化学工程%二氧化碳%环加成%SBA - 15 分子筛%石墨相氮化碳
精細化學工程%二氧化碳%環加成%SBA - 15 分子篩%石墨相氮化碳
정세화학공정%이양화탄%배가성%SBA - 15 분자사%석묵상담화탄
fine chemical engineering%carbon dioxide%cycloaddition%SBA-15 molecular sieve%graphitic carbon nitride
二氧化碳的催化活化是其作为 C1资源利用的关键。为了开发高效二氧化碳活化催化剂，将二聚氰胺通过浸渍法负载到介孔分子筛 SBA -15孔道中，高温焙烧后，得到 SBA -15负载的石墨相氮化碳 g - C3 N4催化剂。采用透射电镜、X 射线衍射、N2吸附和 X 射线光电子能谱对催化剂进行表征。结果表明，负载 g - C3 N4后，SBA -15分子筛的介孔结构未发生明显变化，g - C3 N4以纳米态分布于 SBA -15分子筛的孔道中。将 g - C3 N4/ SBA -15催化剂用于催化二氧化碳与环氧化合物环加成反应制备环状碳酸酯，考察催化剂组成和反应条件对催化性能的影响。结果表明， g - C3 N4/ SBA -15催化剂有效催化二氧化碳与环氧化合物环加成反应。以 g - C3 N4/ SBA -15为催化剂，在反应温度140℃、反应压力3.5 MPa、反应时间4 h、ZnBr2物质的量分数为1.0%和二聚氰胺负载质量分数为20%条件下，环状碳酸酯产率达91.6%，g - C3 N4/ SBA -15催化剂制备工艺简单，原料价廉，催化性能优异。
二氧化碳的催化活化是其作為 C1資源利用的關鍵。為瞭開髮高效二氧化碳活化催化劑，將二聚氰胺通過浸漬法負載到介孔分子篩 SBA -15孔道中，高溫焙燒後，得到 SBA -15負載的石墨相氮化碳 g - C3 N4催化劑。採用透射電鏡、X 射線衍射、N2吸附和 X 射線光電子能譜對催化劑進行錶徵。結果錶明，負載 g - C3 N4後，SBA -15分子篩的介孔結構未髮生明顯變化，g - C3 N4以納米態分佈于 SBA -15分子篩的孔道中。將 g - C3 N4/ SBA -15催化劑用于催化二氧化碳與環氧化閤物環加成反應製備環狀碳痠酯，攷察催化劑組成和反應條件對催化性能的影響。結果錶明， g - C3 N4/ SBA -15催化劑有效催化二氧化碳與環氧化閤物環加成反應。以 g - C3 N4/ SBA -15為催化劑，在反應溫度140℃、反應壓力3.5 MPa、反應時間4 h、ZnBr2物質的量分數為1.0%和二聚氰胺負載質量分數為20%條件下，環狀碳痠酯產率達91.6%，g - C3 N4/ SBA -15催化劑製備工藝簡單，原料價廉，催化性能優異。
이양화탄적최화활화시기작위 C1자원이용적관건。위료개발고효이양화탄활화최화제，장이취청알통과침지법부재도개공분자사 SBA -15공도중，고온배소후，득도 SBA -15부재적석묵상담화탄 g - C3 N4최화제。채용투사전경、X 사선연사、N2흡부화 X 사선광전자능보대최화제진행표정。결과표명，부재 g - C3 N4후，SBA -15분자사적개공결구미발생명현변화，g - C3 N4이납미태분포우 SBA -15분자사적공도중。장 g - C3 N4/ SBA -15최화제용우최화이양화탄여배양화합물배가성반응제비배상탄산지，고찰최화제조성화반응조건대최화성능적영향。결과표명， g - C3 N4/ SBA -15최화제유효최화이양화탄여배양화합물배가성반응。이 g - C3 N4/ SBA -15위최화제，재반응온도140℃、반응압력3.5 MPa、반응시간4 h、ZnBr2물질적량분수위1.0%화이취청알부재질량분수위20%조건하，배상탄산지산솔체91.6%，g - C3 N4/ SBA -15최화제제비공예간단，원료개렴，최화성능우이。
The catalytic activation of carbon dioxide is the key for its utilization as C1 resource. In order to develop efficient catalysts for the activation of carbon dioxide,dicyandiamide was loaded on the mesochannels of SBA-15 molecular sieve by impregnation method,and then after calcination,SBA-15 loaded graphitic carbon nitride(g-C3 N4 )catalysts were obtained. The catalysts were characterized by transmission electron microscopy,X-ray diffraction,N2 adsorption and X-ray photoelectron spectroscopy. The results showed that the mesoporous structure of SBA-15 molecular sieve had not changed significantly after loading g-C3 N4 . g-C3 N4 nanophases were dispersed in the channels of SBA-15 molecular sieve. g-C3 N4 / SBA-15 catalyst was employed for the catalytic synthesis of cyclic carbonate from cycloaddition of carbon dioxide with epoxide. The effects of catalyst composition and the reaction conditions on catalytic performance were investigated. The results showed that g-C3N4 / SBA-15 catalyst could effectively catalyze the cycloaddition of carbon dioxide with epoxide. Under the condition of reaction temperature 140 ℃,reaction pressure 3.5 MPa, reaction time 4 h,ZnBr2 amount 1. 0mol% ,dicyandiamide mass fraction 20% and g-C3 N4 / SBA-15 as the catalyst,cyclic carbonate yield reached 91. 6% . g-C3 N4 / SBA-15 catalyst had the advantages of simple preparation process,cheap raw materials and excellent catalytic performance.
