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Sustainable direct H2O2 synthesis over Pd catalyst supported on mesoporous carbon: The effect of surface nitrogen functionality
Catalysis Today ( IF 5.3 ) Pub Date : 2021-01-13 , DOI: 10.1016/j.cattod.2020.12.036
Xiang Ji , Dongdong Chen , Lin Peng , Francesco Frison , Chiara Dalla Valle , Cristina Tubaro , Marco Zecca , Paolo Centom , Daiqi Ye , Peirong Chen

We employed oxygen- and nitrogen-functionalized mesoporous carbons (OMC and N-OMC) as supports for Pd nanoparticles pre-formed via a modified colloidal method. In the direct synthesis of hydrogen peroxide (H2O2) from H2 and O2, the prepared Pd/OMC catalyst outperformed a commercial Pd catalyst supported on activated carbon (Pd/AC) and a Pd catalyst on oxygen-functionalized carbon nanotubes (Pd/OCNT) in terms of H2O2 productivity, emphasizing the advantage of mesoporous carbon support. An even higher H2O2 productivity was obtained over Pd catalyst supported on N-OMC with 2.72 at.% nitrogen on the surface. However, a further increase of surface nitrogen content to 13.26 at.%, as the case of mesoporous carbon directly grown using N-containing carbon precursor (NMC), led to increased activity (in terms of H2 consumption) but poor H2O2 productivity. X-ray photoelectron spectroscopy analyses of the Pd/MC catalysts suggest that a suitable amount of N groups (ca. 2.72 at.%) on the MC surface led to a high fraction of Pd2+ in the Pd/MC catalyst, which is believed to be important for achieving high selectivity in direct H2O2 synthesis. These results highlight that tuning the surface properties of carbon supports is a versatile approach to fabricate highly selective supported Pd catalysts for the sustainable direct synthesis of H2O2 from H2 and O2.



中文翻译:

在介孔碳上负载的 Pd 催化剂上可持续的直接 H 2 O 2合成:表面氮官能度的影响

我们采用氧和氮功能化的介孔碳(OMC 和 N-OMC)作为通过改良胶体方法预先形成的 Pd 纳米颗粒的载体。在由 H 2和 O 2直接合成过氧化氢 (H 2 O 2 ) 中,制备的 Pd/OMC 催化剂的性能优于负载在活性炭上的商用 Pd 催化剂 (Pd/AC) 和氧官能化碳纳米管上的 Pd 催化剂(Pd/OCNT) 在 H 2 O 2生产率方面,强调介孔碳载体的优势。更高的 H 2 O 2在 N-OMC 上负载的 Pd 催化剂上获得了生产率,表面有 2.72 at.% 的氮。然而,表面氮含量进一步增加至 13.26 at.%,如使用含氮碳前体 (NMC) 直接生长的介孔碳,导致活性增加(就 H 2消耗而言)但 H 2 O较差2生产力。Pd/MC 催化剂的 X 射线光电子能谱分析表明,MC 表面上适量的 N 基团(约 2.72 at.%)导致Pd/MC 催化剂中 Pd 2+ 的比例高,这是据信对于在直接 H 2 O 2 中实现高选择性很重要合成。这些结果突出显示调谐碳载体的表面性能是制造高度选择性的负载的Pd催化剂H的可持续直接合成一种通用方法2 ö 2选自H 2和O 2

更新日期:2021-01-13
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