Immobilization of H3PMo12O40 catalyst on the nitrogen-containing mesoporous carbon and its application to the vapor-phase 2-propanol conversion reaction
Immobilization of H3PMo12O40 catalyst on the nitrogen-containing mesoporous carbon and its application to the vapor-phase 2-propanol conversion reaction
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DOI：
10.1007/s11814-008-0041-2
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发表时间：
2008-04
影响因子：
2.7
通讯作者：
Heesoo Kim;J. Jung;D. Park;Joohyung Lee;K. Cho;Sunyoung Park;Sang Hee Lee;I. Song
中科院分区：
文献类型：
--
作者：
Heesoo Kim;J. Jung;D. Park;Joohyung Lee;K. Cho;Sunyoung Park;Sang Hee Lee;I. Song
采用模板法合成了高表面积（= 1115 m2/g）、大孔体积（=1.18 cm3/g）的含氮介孔碳（N-MC）。然后修饰N-MC表面形成正电荷，从而为[PMo12O40]3−的固定化提供位点。利用[PMo12O40]3−的整体负电荷，H3PMo12O40（PMo12）作为电荷匹配组分被化学固定在N-MC载体上。结果表明，PMo12/N-MC在固定PMo12后，仍能保持较高的比表面积（=687 m2/g）和较大的孔体积（=0.67 cm3/g）。通过化学固定，pmo12在N-MC载体上被精细地分散。在气相2-丙醇转化反应中，PMo12/N-MC的转化率高于未负载的PMo12。此外，与未负载的PMo12相比，PMo12/N-MC具有增强的氧化催化活性和抑制的酸催化活性。PMo12/N-MC的这种催化行为是由于PMo12在牺牲质子的化学固定化形成的N-MC载体上的分子分散。
Nitrogen-containing mesoporous carbon (N-MC) with high surface area (=1,115 m2/g) and large pore volume (=1.18 cm3/g) was synthesized by a templating method. The surface of N-MC was then modified to form a positive charge, and thus, to provide sites for the immobilization of [PMo12O40]3−. By taking advantage of the overall negative charge of [PMo12O40]3−, H3PMo12O40(PMo12) was chemically immobilized on the N-MC support as a charge matching component. It was found that the PMo12/N-MC still retained relatively high surface area (=687 m2/g) and large pore volume (=0.67 cm3/g) even after the immobilization of PMo12. It was also revealed that PMo12species were finely and molecularly dispersed on the N-MC support via chemical immobilization. In the vapor-phase 2-propanol conversion reaction, the PMo12/N-MC showed a higher conversion than the unsupported PMo12. Furthermore, the PMo12/N-MC showed an enhanced oxidation catalytic activity and a suppressed acid catalytic activity compared to the unsupported PMo12. This catalytic behavior of PMo12/N-MC was due to the molecular dispersion of PMo12on the N-MC support formed via chemical immobilization by sacrificing the proton.