CO_(2)氧化1-丁烯脱氢制1,3-丁二烯多孔碳球负载铁基催化剂

Iron-based catalyst loaded on porous carbon spheres for oxidative dehydrogenation of 1-butene to 1,3-butadiene with CO_(2)

采用腔径11.6 nm、孔径3.4 nm的ZIF-8作为分子尺度的笼子用于分离和封装乙酰丙酮铁(分子直径约9.7 nm),并对其热解制备出掺氮多孔碳球锚定的高分散Fe-NC催化剂,利用紫外可见吸收光谱仪、N2物理吸附仪、X射线衍射仪、扫描电子显微镜、透射电子显微镜等仪器表征了催化剂的物理化学性质,并考察了其催化CO2氧化1-丁烯脱氢制1,3-丁二烯的反应性能。结果表明:Fe-NC催化剂是具有较大比表面积、一定酸碱性位的多孔多面体结构的碳材料,铁在碳材料上高度分散;其在催化CO_(2)氧化1-丁烯脱氢制1,3-丁二烯反应时具有优良的催化活性及稳定性,高分散Fe(0.01)-NC催化剂的1,3-丁二烯初始转换频率高达0.0377 s-1。

ZIF-8(the cavity diameter was 11.6 nm,and pore size 3.4 nm)was used as molecular scale cages to separate and encapsulate iron acetylacetone(the molecule diameter was about 9.7 nm),and the high-dispersed iron anchored on N-doped porous carbon spheres(Fe-NC catalyst)were obtained through high-temperature pyrolysis.The physical and chemical properties of the catalyst were characterized by UV-vis,N2 adsorption,XRD,SEM and TEM,and the catalytic performance for the reaction of oxidative dehydrogenation of 1-butene to 1,3-butadiene with CO2 was evaluated.The results showed that the Fe-NC catalyst was a porous polyhedral carbon material with a large specific surface area and adjustable acid-base sites,and the iron species were highly dispersed over the carbon material.The Fe-NC catalyst had showed good catalytic activity and stability in the reaction of oxidative dehydrogenation of 1-butene to 1,3-butadiene with CO_(2).The TOF of the highly dispersed Fe(0.01)-NC catalyst for 1,3-butadiene could reach up to 0.0377 s-1.