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Direct synthesis of hydrogen peroxide over palladium catalysts supported on glucose-derived amorphous carbons
Korean Journal of Chemical Engineering ( IF 2.9 ) Pub Date : 2021-05-31 , DOI: 10.1007/s11814-021-0748-x
Hang Thi Thuy Vu , Viet Le Nam Vo , Young-Min Chung

Untreated and sulfonated biomass-derived amorphous carbons were prepared by the pyrolysis of D-glucose at different temperatures, followed by sulfonation. Not only the surface functional group concentration but also the structure of polyaromatic carbon sheets was significantly affected by the carbonization temperature and sulfonation. More importantly, the carbonization temperature played a crucial role in determining the size of Pd nanoparticles (NPs) on glucose-derived carbons (GCx) and thereby affected the catalytic performance of Pd/GCx for the direct synthesis of hydrogen peroxide (DSHP). The volcano-shaped dependency between the Pd NP size and the carbonization temperature of GCx agrees well with the reverse relationship between the Pd NP size and the catalytic activity of Pd/GCx. The flexible polyaromatic carbon sheet structure of the GCx was beneficial in increasing the sulfonic acid group content on the carbon surface and, therefore, H2O2 selectivity was improved in the presence of the Pd/S-GC2 catalyst (Pd supported on the sulfonated glucose-derived carbon pyrolyzed at 723 K). However, both H2 conversion and H2O2 productivity decreased over the same catalyst, possibly due to the decreased number of active sites on the clustered or single-site Pd. Reducing the catalyst resulted in a decrease in H2O2 selectivity by significantly lowering the Pd2+/Pd0 ratio and increasing the Pd NP size. These results clearly demonstrate that fine control of the physicochemical properties of the active metal and GCx support and their synergistic combination is essential to realize an efficient Pd catalyst supported on GCx for the DSHP reaction.



中文翻译:

葡萄糖衍生无定形碳负载钯催化剂直接合成过氧化氢

通过在不同温度下热解 D-葡萄糖,然后进行磺化,制备了未经处理和磺化的生物质衍生的无定形碳。碳化温度和磺化反应不仅对表面官能团浓度有显着影响,而且对多环芳烃碳片的结构也有显着影响。更重要的是,碳化温度在决定葡萄糖衍生碳 (GCx) 上 Pd 纳米粒子 (NPs) 的尺寸方面起着至关重要的作用,从而影响 Pd/GCx 直接合成过氧化氢 (DSHP) 的催化性能。Pd NP 尺寸与 GCx 碳化温度之间的火山形依赖性与 Pd NP 尺寸与 Pd/GCx 催化活性之间的反向关系非常吻合。在 Pd/S-GC2 催化剂(负载在磺化葡萄糖衍生碳上的 Pd 在 723 K 下热解)存在下,2 O 2选择性得到改善。然而,H 2转化率和H 2 O 2生产率在相同的催化剂上均下降,这可能是由于簇状或单中心Pd 上活性位点数量的减少。通过显着降低 Pd 2+ /Pd 0减少催化剂导致 H 2 O 2选择性降低比率并增加 Pd NP 尺寸。这些结果清楚地表明,精细控制活性金属和 GCx 载体的物理化学性质及其协同组合对于实现负载在 GCx 上用于 DSHP 反应的高效 Pd 催化剂至关重要。

更新日期:2021-06-01
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