Enhanced catalytic hydrogenation of aqueous bromate over Pd/mesoporous carbon nitride

Enhanced catalytic hydrogenation of aqueous bromate over Pd/mesoporous carbon nitride
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DOI:
10.1016/j.cej.2013.08.111
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发表时间:
2013-12
影响因子:
15.1
通讯作者:
Peng Zhang;Fang Jiang;Huan Chen
Peng Zhang;Fang Jiang;Huan Chen
中科院分区:
工程技术1区
文献类型:
--
作者:
Peng Zhang;Fang Jiang;Huan Chen

文献摘要

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合成了介孔氮化碳(MCN)负载钯催化剂,并对溴酸盐的液相催化加氢进行了研究。表征结果表明,Pd/MCN催化剂具有较大的BET表面积、较高的等电点(IEP)、有序的介孔结构和良好的分散在MCN孔中的Pd颗粒。与Pd/活性炭(Pd/AC)和Pd/有序介孔碳(Pd/CMK-3)相比,由于其介孔结构和较高的IEP, Pd/MCN具有更高的溴酸盐还原催化活性。溴酸盐在Pd/MCN上的加氢过程符合Langmuir-Hinshelwood模型,反映了吸附控制反应机理。ph -催化活性的连锁关系与催化剂的吸附能力有关。发现表面Pd位点的翻转频率(TOFs)与Pd粒度有关。共存的阴离子抑制了溴酸盐的还原。结果表明,Pd/MCN是一种很有前景的溴酸盐加氢催化剂。
Pd catalysts supported on mesoporous carbon nitride (MCN) were synthesized and the liquid phase catalytic hydrogenation of bromate was investigated. Characterization results showed that the Pd/MCN catalysts had large BET surface area, high isoelectric point (IEP), ordered mesoporous structure and well dispersed Pd particles in the pores of MCN. Compared with Pd/active carbon (Pd/AC) and Pd/ordered mesoporous carbon (Pd/CMK-3), Pd/MCN displayed higher catalytic activity for bromate reduction, due to its mesoporous structure and high IEP. The bromate hydrogenation process over Pd/MCN followed the Langmuir–Hinshelwood model, reflecting an adsorption controlling reaction mechanism. The pH-catalytic activity linked relationship was related to the adsorption ability of catalysts. Turn over frequencies (TOFs) of the surface Pd sites were found to be dependent on Pd particle size. The coexisting anions suppressed the reduction of bromate. The present results demonstrated that Pd/MCN could be a promising catalyst for the application on bromate hydrogenation.