Xue Mei, Chitrakar Ramesh, Sakane Kohji, Hirotsu Takahiro, Ooi Kenta, Yoshimura Yuji, Toba Makoto, Feng Qi
Health Technology Research Center, National Institute of Advanced Industrial Science and Technology (AIST), 2217-14 Hayashi, Takamatsu 761-0395, Japan.
J Colloid Interface Sci. 2006 Jun 15;298(2):535-42. doi: 10.1016/j.jcis.2005.12.051. Epub 2006 Feb 3.
Ce(IV)-loaded Y-zeolites (CeY) were prepared for selective removal of the trace amount of organic sulfur compounds from hydrodesulfurization (HDS)-treated diesel oil. The CeY samples can be obtained from NH4-Y-zeolite (NH4Y) using liquid-phase ion-exchange and solid-state ion-exchange methods. The ion-exchange reactions, structures, and selective adsorptions of organic sulfur compounds of the CeY samples were investigated using XRD, IR, XPS, TEM, and GC sulfur analyzer. The organic sulfur compound uptakes strongly depend on the amount and the valency of Ce in the zeolite structure. Ce(IV) shows much higher adsorptive ability than Ce(III). A CeY-S sample prepared by solid-state ion-exchange reaction of NH4Y and Ce(NO3)3 with Ce/NH4 mole ratio of 0.63 at 250 degrees C showed a maximum sulfur uptake from a model solution of HDS-treated gasoline containing thiophene [S = 5 ppm (ppm = mg/L)]. A desulfurization from a HDS-treated diesel oil containing organic sulfur compounds (S = 1.87 ppm) and H2S (S = 0.73 ppm) was investigated with a combination of the CeY-S and a CuO adsorbent for removal of H2S by a batch method. The sulfur content was reduced to below 0.01 ppm for the first time. This method provides a promising desulfurization process to prepare a clean fuel for fuel cells.
制备了负载铈(IV)的Y型沸石(CeY),用于从加氢脱硫(HDS)处理后的柴油中选择性去除痕量有机硫化合物。CeY样品可通过液相离子交换和固态离子交换方法从NH4-Y型沸石(NH4Y)获得。使用XRD、IR、XPS、TEM和GC硫分析仪研究了CeY样品的离子交换反应、结构以及有机硫化合物的选择性吸附。有机硫化合物的吸附量强烈依赖于沸石结构中铈的含量和价态。Ce(IV)的吸附能力比Ce(III)高得多。通过在250℃下将NH4Y与Ce(NO3)3进行固态离子交换反应制备的CeY-S样品,Ce/NH4摩尔比为0.63,从含噻吩的HDS处理汽油模型溶液[S = 5 ppm(ppm = mg/L)]中显示出最大的硫吸附量。采用CeY-S和CuO吸附剂组合通过间歇法研究了从含有机硫化合物(S = 1.87 ppm)和H2S(S = 0.73 ppm)的HDS处理柴油中脱硫。硫含量首次降至0.01 ppm以下。该方法为制备用于燃料电池的清洁燃料提供了一种有前景的脱硫工艺。