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Two-dimensional covalent-organic-framework-derived nitrogen-rich carbon nanosheets modified with small Pd nanoparticles for the hydrodechlorination of chlorophenols and hydrogenation of phenol
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2018-09-30 , DOI: 10.1016/j.apcata.2018.09.028
Mengying Fan , Yu Long , Yangyang Zhu , Xiwei Hu , Zhengping Dong

Heteroatom-doped carbon materials have attracted immense attention for heterogeneous catalysis applications because of their excellent physicochemical properties. In this work, we prepared a cost-effective triazinyl-containing two-dimension COFs (2D-COFs), and then the 2D-COFs was self-templated carbonized to fabricate 2D nitrogen-doped carbon nanosheets (NCNs). NCNs were modified with highly dispersed small palladium nanoparticles (Pd NPs), affording the Pd/NCNs catalyst. The as-prepared NCNs and Pd/NCNs exhibited a smoke-like morphology, a large specific surface area, and mesoporous and macroporous structures, which can enhance reactants diffusion and mass transfer. The obtained Pd/NCNs catalyst exhibited excellent activity, stability, and recyclability in the aqueous-phase hydrodechlorination (HDC) of organic hazardous substances chlorophenols (CPs). Meanwhile, outstanding activity and high selectivity were observed for the subsequent hydrogenation of the HDC product phenol to cyclohexanone. The excellent activity of the Pd/NCNs catalyst was related to the synergistic effect of Pd NPs and the nitrogen atoms doped in the NCNs. Thus, this study offers a novel, facile route for fabrication heteroatom-doped carbon materials derived from cost-effective COFs materials to prepare highly dispersed small noble-metal-NP-modified catalysts for various catalytic applications.



中文翻译:

二维共价有机框架衍生的富含Pd纳米粒子的富氮碳纳米片,用于氯酚的加氢脱氯和苯酚的加氢

杂原子掺杂的碳材料由于其优异的理化性质而在非均相催化应用中引起了极大的关注。在这项工作中,我们制备了具有成本效益的含三嗪基的二维COF(2D-COF),然后将2D-COF进行自我模板碳化,以制造2D氮掺杂碳纳米片(NCN)。NCN用高度分散的小钯纳米粒子(Pd NPs)改性,得到Pd / NCNs催化剂。所制备的NCN和Pd / NCN表现出烟状形态,较大的比表面积以及中孔和大孔结构,可增强反应物的扩散和传质。所得的Pd / NCNs催化剂表现出优异的活性,稳定性,有机有害物质氯酚(CPs)在水相加氢氯化(HDC)中的可回收性。同时,对于随后的HDC产物苯酚加氢为环己酮,观察到优异的活性和高选择性。Pd / NCNs催化剂的优异活性与Pd NP和NCN中掺杂的氮原子的协同作用有关。因此,这项研究提供了一种新颖,简便的方法,可用于制造由经济高效的COFs材料制成的杂原子掺杂碳材料,以制备高度分散的小型贵金属NP改性催化剂,以用于各种催化应用。Pd / NCNs催化剂的优异活性与Pd NPs和NCNs中掺杂的氮原子的协同作用有关。因此,这项研究提供了一种新颖,简便的方法,可用于制造由经济高效的COFs材料制成的杂原子掺杂碳材料,以制备高度分散的小型贵金属NP改性催化剂,以用于各种催化应用。Pd / NCNs催化剂的优异活性与Pd NPs和NCNs中掺杂的氮原子的协同作用有关。因此,这项研究提供了一种新颖,简便的方法,可用于制造由经济高效的COFs材料制成的杂原子掺杂碳材料,以制备高度分散的小型贵金属NP改性催化剂,以用于各种催化应用。

更新日期:2018-09-30
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