Jie Zhou, Yuanyuan Wu, Yonghong Liu, Na Li, Zhen Yang, Jiadi Ying, Xiaorong Ren, Tao Zhang, Wei Xu, Jinyang Chen, Xingzhong Cao, Runsheng Yu, Minfeng Zeng
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引用次数: 0
摘要
掺杂 N 的多孔碳具有高孔隙率、大比表面积、丰富的活性位点以及与催化活性金属物种的强螯合作用,因此在异质支撑领域具有巨大潜力。在这里,我们通过简单的碳化和活化过程,成功地制备了由不同质量比的海藻酸盐/三聚氰胺混合物衍生的新型 N 掺杂多孔碳。通过扫描电镜、电子显微镜和 N2 吸附表征,确认了衍生 N 掺杂碳的分层多孔结构。经过 Na2PdCl4 溶液浸渍和进一步还原处理后,Pd0 纳米粒子被均匀地固定在 SMCNC 载体上,生成了新型 Pd@SAMNC 催化剂。优化后的 Pd@SAMNC-0.6 具有较高的 N 含量(5.13%)、Pd 含量(5.90%)和较大的 BET 比表面积(1884.5 m2/g)。多孔碳材料的正电子湮没寿命光谱(PALS)研究提供了亚纳米级微孔信息,证明 Pd@SAMNC-0.6 比商用 Pd@AC 能够为反应提供更多的活性位点。Pd@SAMNC-0.6 催化剂在芳香卤化物与烯烃的赫克偶联反应中表现出卓越的催化效率,并且可以循环使用 17 次而不会显著降低催化效率。
Pd nanoparticle supported on N‐doped carbon derived from sodium alginate/melamine blends as efficient heterogeneous catalyst for Heck reactions
N‐doped porous carbon shows great potential in the field of heterogenous supports due to its high porosity, large surface area, rich active sites, and strong chelation with catalytic active metals species. Here, we successfully fabricated novel N‐doped porous carbon derived from alginate/melamine blends with different mass ratio by simple carbonization and activation process. Hierarchical porous structure of the derived N‐doped carbon has been confirmed with the SEM, TEM and N2 adsorption characterization. After Na2PdCl4 solution impregnation and further reduction process, Pd0 nanoparticles have been uniformly immobilized on the SMCNC support to produce novel Pd@SAMNC catalyst. The optimated Pd@SAMNC‐0.6 possesses a high N content (5.13%), Pd content (5.90%), large BET specific surface area of 1884.5 m2/g. Positron annihilation lifetime spectroscopy (PALS) investigation of the porous carbon materials provided the sub‐nano level microporous information proofs of Pd@SAMNC‐0.6 had the capability to provide more active sites for reactions than commercial Pd@AC. Pd@SAMNC‐0.6 catalyst showed superior catalytic efficiency in Heck coupling reaction between aromatic halides and alkenes and can be recycled for 17 runs without significant decrease in catalytic efficiency.
期刊介绍:
With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.