当前位置: X-MOL 学术J. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Transformation of reduced graphene aerogel-supported atomically dispersed iridium into stable clusters approximated as Ir6 during ethylene hydrogenation catalysis
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-05-07 , DOI: 10.1016/j.jcat.2022.04.028
Samira F. Kurtoğlu-Öztulum 1, 2 , KaanYalçın 1, 2 , Yuxin Zhao 1, 2 , Hatice Pelin Çağlayan 1, 2 , Adam S. Hoffman 3 , Bruce C. Gates 4 , Simon R. Bare 3 , Uğur Ünal 2, 5, 6 , Alper Uzun 1, 2, 6
Affiliation  

Transformation of atomically dispersed reduced graphene aerogel (rGA)-supported complexes, IrI(C2H4)2+, with an iridium loading of 9.9 wt%, to form low-nuclearity clusters was investigated during ethylene hydrogenation catalysis. Continuous-scan X-ray absorption spectra demonstrate the formation of clusters well approximated as Ir4 during reaction at 100 °C in flowing equimolar ethylene and H2. The Ir4 clusters transformed into clusters well approximated as Ir6 when the feed molar ratio was switched to H2:C2H4 = 2 and remained stable in pure H2 at 100 °C. Catalyst performance data show that hydrogenation activity increased with metal nuclearity in the order of atomically dispersed iridium/rGA≪ Ir4/rGA < Ir6/rGA. Continuous scan X-ray absorption data, complemented with aberration-corrected scanning transmission electron microscopy images, demonstrate that the supported clusters approximated as Ir6 are stable even in H2 at atmospheric pressure and 100 °C. These supported iridium clusters are among the ones having the highest metal loadings reported for a supported metal cluster catalyst.



中文翻译:

乙烯加氢催化过程中还原石墨烯气凝胶负载的原子分散铱转化为近似于 Ir6 的稳定簇

研究了在乙烯加氢催化过程中原子分散的还原石墨烯气凝胶 (rGA) 负载的配合物 Ir I (C 2 H 4 ) 2 +的转化,铱负载量为 9.9 wt%,以形成低核团簇。连续扫描 X 射线吸收光谱表明,在 100 °C 下,在流动的等摩尔乙烯和 H 2的反应过程中,簇的形成非常接近于 Ir 4。当进料摩尔比切换为 H 2 :C 2 H 4时,Ir 4簇转变为非常近似于 Ir 6的簇= 2 并在 100 °C 下 在纯 H 2中保持稳定。催化剂性能数据表明,加氢活性随着金属核的增加而增加,其顺序为原子分散的铱/rGA≪ Ir 4 /rGA < Ir 6 /rGA。连续扫描 X 射线吸收数据,辅以像差校正的扫描透射电子显微镜图像,表明近似为 Ir 6的受支持簇即使在大气压和 100 °C的 H 2中也是稳定的。这些负载型铱簇属于负载型金属簇催化剂所报道的具有最高金属负载量的那些。

更新日期:2022-05-07
down
wechat
bug