天然气化工
天然氣化工
천연기화공
NATURAL GAS CHEMICAL INDUSTRY
2013年
4期
24-28
,共5页
张四方%刘建春%任跃红%王振国%李军
張四方%劉建春%任躍紅%王振國%李軍
장사방%류건춘%임약홍%왕진국%리군
碳酸二甲酯%气相合成%二氧化碳%甲醇%负载型Cu-Zn催化剂%介孔碳材料%酚醛树脂
碳痠二甲酯%氣相閤成%二氧化碳%甲醇%負載型Cu-Zn催化劑%介孔碳材料%酚醛樹脂
탄산이갑지%기상합성%이양화탄%갑순%부재형Cu-Zn최화제%개공탄재료%분철수지
dimethyl carbonate%gas phase synthesis%carbon dioxide%methanol%supported Cu-Zn catalyst%mesoporous carbon material%phenol-formaldehyde resin
以新制备的酚醛树脂为炭前驱体,加入不同Cu/Zn比例的硝酸铜-硫酸锌溶液混合,煅烧制备了酚醛树脂基介孔碳材料负载Cu-Zn催化剂,用XRD、XPS、N2吸附/脱附等手段对其进行了表征,并在固定床反应器中考察了其催化二氧化碳和甲醇气相直接合成碳酸二甲酯的性能。结果表明:n(Cu)/n( Zn)=2的Cu-Zn/PF催化剂具有最好的催化性能,其比表面积达459m2· g-1,平均孔径3.44nm,催化剂活性组分均匀地分散在载体上且与载体有明显的强相互作用;该催化剂在反应温度为320℃,反应压力为3.2MPa时,甲醇转化率达98.11%,碳酸二甲酯选择性为95.05%,并有较好的稳定性。
以新製備的酚醛樹脂為炭前驅體,加入不同Cu/Zn比例的硝痠銅-硫痠鋅溶液混閤,煅燒製備瞭酚醛樹脂基介孔碳材料負載Cu-Zn催化劑,用XRD、XPS、N2吸附/脫附等手段對其進行瞭錶徵,併在固定床反應器中攷察瞭其催化二氧化碳和甲醇氣相直接閤成碳痠二甲酯的性能。結果錶明:n(Cu)/n( Zn)=2的Cu-Zn/PF催化劑具有最好的催化性能,其比錶麵積達459m2· g-1,平均孔徑3.44nm,催化劑活性組分均勻地分散在載體上且與載體有明顯的彊相互作用;該催化劑在反應溫度為320℃,反應壓力為3.2MPa時,甲醇轉化率達98.11%,碳痠二甲酯選擇性為95.05%,併有較好的穩定性。
이신제비적분철수지위탄전구체,가입불동Cu/Zn비례적초산동-류산자용액혼합,단소제비료분철수지기개공탄재료부재Cu-Zn최화제,용XRD、XPS、N2흡부/탈부등수단대기진행료표정,병재고정상반응기중고찰료기최화이양화탄화갑순기상직접합성탄산이갑지적성능。결과표명:n(Cu)/n( Zn)=2적Cu-Zn/PF최화제구유최호적최화성능,기비표면적체459m2· g-1,평균공경3.44nm,최화제활성조분균균지분산재재체상차여재체유명현적강상호작용;해최화제재반응온도위320℃,반응압력위3.2MPa시,갑순전화솔체98.11%,탄산이갑지선택성위95.05%,병유교호적은정성。
Mesoporous carbon-supported Cu-Zn catalysts were prepared by adding the aqueous solutions of copper nitrate and zinc sulphate with different Cu/Zn atomic ratios to the new prepared phenol-formaldehyde resin and calcination. The catalysts were characterized by XRD, XPS and N2 adsorption/desorption, and their catalytic behaviors in the direct gas phase synthesis of dimethyl carbonate from CO2 and methanol were evaluated in a flow fixed-bed reactor. The results showed that the Cu-Zn/PF catalyst with a Cu/Zn atomic ratio of 2 exhibited the best catalytic performance, the specific surface area and average pore size of which were 459m2·g-1 and 3.44nm, respectively, and the active component Cu was well dispersed on the surface of the support, and further more, there was a strong interaction between the active component and the support;over the optimized catalyst, under reaction temperature of 320℃ and pressure of 3.2MPa, the conversion of methanol was up to 98.11% with a selectivity to dimethyl carbonate of 95.05%;and the catalyst showed good stability.