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Nitrogen-fixing of ultrasmall Pd-based bimetallic nanoclusters on carbon supports
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-06-12 , DOI: 10.1016/j.jcat.2020.06.003
Lei Wang , Peng Yin , Le-Le Zhang , Shan-Cheng Shen , Shi-Long Xu , Ping Chen , Hai-Wei Liang

Synthesis of supported Pd-based bimetallic catalysts is of great importance in the heterogeneous catalysis field owing to their optimal geometric and electronic effects. Downsizing active metals to ultrasmall nanocluster (<2 nm), which is mandatory for maximizing the metal atom utilization, however remains as formidable synthesis challenges. Here, we present a general synthetic approach to sub-2 nm Pd-based bimetallic nanoclusters on porous nitrogen-doped carbon supports, in which the strong chemical interaction between metal and nitrogen largely suppresses the metal aggregation during the H2-reduction at 400–500 °C. Through the nitrogen-fixing strategy, we prepare 9 sub-2 nm Pd-based bimetallic nanocluster catalysts by conventional impregnation process. The prepared supported bimetallic Pd-Pb nanocluster catalyst exhibit a high turnover frequency of 1092 h−1 for the semihydrogenation of phenylacetylene under a mild condition (30 °C, 5 bar H2), along with a high selectivity of >93% to styrene, demonstrating the alloying and small-size effects in the bimetallic nanocluster catalysts.



中文翻译:

碳载体上超小型Pd基双金属纳米团簇的固氮作用

负载型Pd基双金属催化剂的合成由于其最佳的几何和电子效应而在多相催化领域中具有重要意义。将活性金属小型化为超小型纳米簇(<2 nm),这对于最大限度地利用金属原子是必不可少的,但是仍然面临着巨大的合成挑战。在这里,我们提出了一种通用的合成方法,用于在多孔氮掺杂碳载体上的亚2 nm Pd基双金属纳米团簇,其中金属和氮之间的强化学相互作用在很大程度上抑制了H 2期间的金属聚集-在400–500°C下还原。通过固氮策略,我们通过常规浸渍工艺制备了9个亚2 nm Pd基双金属纳米簇催化剂。制备的负载型双金属Pd-Pb纳米簇催化剂在温和条件下(30°C,5 bar H 2)对苯乙炔进行半氢化反应显示出1092 h -1的高周转频率,并且对苯乙烯的选择性高> 93% ,证明了双金属纳米簇催化剂的合金化和小尺寸效应。

更新日期:2020-06-29
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