Bifunctionalized hollow nanospheres for the one-pot synthesis of methyl isobutyl ketone from acetone.
Bifunctionalized hollow nanospheres for the one-pot synthesis of methyl isobutyl ketone from acetone.
复制标题
DOI：
10.1002/cssc.201200383
复制
发表时间：
2012-12
期刊：
影响因子：
8.4
通讯作者：
Peng Wang;Shiyang Bai;Jiao Zhao;Panpan Su;Qihua Yang;Can Li
中科院分区：
文献类型：
--
作者：
Peng Wang;Shiyang Bai;Jiao Zhao;Panpan Su;Qihua Yang;Can Li
Pd掺杂丙磺酸功能化空心微球是丙酮和氢气一锅法合成甲基异丁基酮(MIBK)的高效双官能化催化剂。这些空心纳米球表现出比它们的体相介孔对应物(SBA-15或FDU-12)更高的活性，这主要是由于空心纳米球的短扩散阻力。具有二氧化硅骨架的空心纳米球比具有乙烷桥联骨架的空心纳米球具有更高的活性和选择性，这表明具有亲水性的空心纳米球有利于MIBK的形成。这可能是由于亲水表面对丙酮的亲和力增加，而对MIBK的亲和力降低，从而阻止了MIBK与丙酮的深度缩合。在最佳反应条件下，MIBK的选择性可达90%，丙酮转化率可达43%。这一结果是迄今为止对介孔二氧化硅催化剂报道得最好的结果之一。控制和微调催化剂的形貌和表面性质为提高固体催化剂的催化性能提供了一种有效的策略。
Pd-doped propyl sulfonic acid-functionalized hollow nanospheres proved to be efficient bifunctionalized catalysts for the one-pot synthesis of methyl isobutyl ketone (MIBK) from acetone and hydrogen in liquid phase. These hollow nanospheres exhibited a higher activity than their bulk mesoporous counterparts (SBA-15 or FDU-12), mainly due to the short diffusion resistance of hollow nanospheres. Hollow nanospheres with silica frameworks showed higher activity and selectivity for MIBK than those with ethane-bridged frameworks, suggesting that hollow nanospheres with hydrophilic surface properties favor the formation of MIBK. This is probably due to the increased affinity of the hydrophilic surface towards acetone and its decreased affinity towards MIBK, which precludes deep condensation of MIBK with acetone. Under optimal conditions, up to 90 % selectivity for MIBK can be obtained with conversions of acetone as high as 43 %. This result is among the best reported so far for mesoporous silica-based catalysts. The control/fine-tuning of morphology and surface properties provides an efficient strategy for improving the catalytic performance of solid catalysts.