催化作用
介孔材料
化学
氮气
X射线光电子能谱
材料科学
碳纤维
氧气
无机化学
化学工程
有机化学
复合数
工程类
复合材料
作者
Xiang Ji,Dongdong Chen,Lin Peng,Francesco Frison,Chiara Dalla Valle,Cristina Tubaro,Marco Zecca,Paolo Centomo,Daiqi Ye,Peirong Chen
标识
DOI:10.1016/j.cattod.2020.12.036
摘要
• Mesoporous carbon supports are beneficial for H 2 O 2 CDS reaction over Pd catalysts. • Surface oxygen groups led to increased selectivity but depressed activity of Pd catalysts. • Surface nitrogen groups led to increased activity but depressed selectivity of Pd catalysts. • The presence of 2.7 at.% surface nitrogen on carbon improves the H 2 O 2 productivity of Pd catalyst. • Co-existence of Pd 2+ and Pd 0 is crucial for selective H 2 O 2 formation over Pd catalyst. 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 (H 2 O 2 ) from H 2 and O 2 , 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 H 2 O 2 productivity, emphasizing the advantage of mesoporous carbon support. An even higher H 2 O 2 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 H 2 consumption) but poor H 2 O 2 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 Pd 2+ in the Pd/MC catalyst, which is believed to be important for achieving high selectivity in direct H 2 O 2 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 H 2 O 2 from H 2 and O 2 .
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