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Hydrogen dissociation and CO2 activation in cascade CO2 fixation on PdIn/TiO2 catalyst
Chem Catalysis ( IF 11.5 ) Pub Date : 2024-11-21 , DOI: 10.1016/j.checat.2024.101116
Leilei Zhou, Ying Wang, Yinze Yang, Liyan Zhang, Jingrong Li, Tingting Xiao, Peikai Luo, Xinluona Su, Haiyang Cheng, Fengyu Zhao

Reduction of CO2 emissions and conversion of CO2 to valuable chemicals is an urgent mission, as it is vital to the global environment and sustainable development. The activation of CO2 is always considered to be the key step for its transformation. Herein, we verified that the activation and dissociation behavior of H2 was the controlling step for CO2 reduction. PdIn alloy was an active center and played a pivotal role in CO2 hydrogenation to the methyl reagent of HCOO∗. H2 split to active Hδ− species on PdIn alloy sites. Strong nucleophilic Hδ− reacted with the CO2 adsorbed on oxygen defects to form ∗HCOO in situ. A high yield of up to 99% was achieved for the cascade fixation of CO2 to valuable amines. The new insights into the activation of CO2 and H2 and their contributions to CO2 conversion that we present will attract the attention of researchers in catalysis, synthesis, surface, and interface chemistry.

中文翻译:


PdIn/TiO2 催化剂上级联 CO2 固定中的氢解离和 CO2 活化



减少 CO2 排放并将 CO2 转化为有价值的化学品是一项紧迫的任务,因为它对全球环境和可持续发展至关重要。CO2 的活化始终被认为是其转化的关键步骤。在此,我们验证了 H2 的激活和解离行为是 CO2 还原的控制步骤。PdIn 合金是一个活性中心,在 CO2 加氢成 HCOO∗ 甲基试剂中起关键作用。H2 在 PdIn 合金位点上分裂成活性 Hδ− 物质。强亲核 Hδ− 与吸附在氧缺陷上的 CO2 反应,位形成 ∗HCOO。将 CO2 级联固定到有价值的胺上实现了高达 99% 的高产率。我们提出的关于 CO2 和 H2 活化及其对 CO2 转化贡献的新见解将引起催化、合成、表面和界面化学研究人员的注意。
更新日期:2024-11-21
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