Tandem Nitrogen Functionalization of Porous Carbon: Toward Immobilizing Highly Active Palladium Nanoclusters for Dehydrogenation of Formic Acid

Tandem Nitrogen Functionalization of Porous Carbon: Toward Immobilizing Highly Active Palladium Nanoclusters for Dehydrogenation of Formic Acid
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DOI:
10.1021/acscatal.7b00053
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发表时间:
2017-04-01
期刊:
影响因子:
12.9
通讯作者:
Xu, Qiang
Xu, Qiang
中科院分区:
化学1区
文献类型:
--
作者:
Li, Zhangpeng;Yang, Xinchun;Xu, Qiang

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通过湿化学还原法合成了氮(N)功能化多孔碳载体(N-MSC-30)固定的高度分散的钯纳米团簇(Pd NC),其中通过串联低温热处理方法制备的N-MSC-30被证明是稳定Pd NC的独特载体。所制备的Pd/N-MSC-30对甲酸(FA)脱氢表现出极高的催化活性和可回收性,在333 K下具有最高的周转频率(TOF = 8414 h(-1)),远高于一步法制备的N-MSC-30负载的Pd催化剂。这种串联热处理策略为将超细金属纳米颗粒固定在N功能化碳材料上提供了一种简便有效的合成方法,在各种催化领域具有巨大的应用前景。
Highly dispersed palladium nanoclusters (Pd NCs) immobilized by a nitrogen (N)-functionalized porous carbon support (N-MSC-30) are synthesized by a wet chemical reduction method, wherein the N-MSC-30 prepared by a tandem low temperature heat-treatment approach proved to be a distinct support for stabilizing the Pd NCs. The prepared Pd/N-MSC-30 shows extremely high catalytic activity and recyclability for the dehydrogenation of formic acid (FA), affording the highest turnover frequency (TOF = 8414 h(-1)) at 333 K, which is much higher than that of the Pd catalyst supported on the N-MSC-30 prepared via a one-step process. This tandem heat treatment strategy provides a facile and effective synthetic methodology to immobilize ultrafine metal NPs on N-functionalized carbon materials, which have tremendous application prospects in various catalytic fields.