CeO2 supported Pd dimers boosting CO2 hydrogenation to ethanol

被引：139

作者：

Lou, Yang ^{[1
,2
]}

Jiang, Feng ^{[1
]}

Zhu, Wen ^{[3
]}

Wang, Li ^{[1
]}

Yao, Tingyi ^{[1
,2
]}

Wang, Shanshan ^{[1
]}

Yang, Bo ^{[3
]}

Yang, Bing ^{[4
]}

Zhu, Yongfa ^{[1
,2
,5
]}

Liu, Xiaohao ^{[1
]}

机构：

[1] Jiangnan Univ, Sch Chem & Mat Engn, Key Lab Synthet & Biol Colloids, Minist Educ, Wuxi 214122, Jiangsu, Peoples R China

[2] Jiangnan Univ, Int Joint Res Ctr Photorespons Mol & Mat, Wuxi 214122, Jiangsu, Peoples R China

[3] ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai 201210, Peoples R China

[4] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China

[5] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2021年 / 291卷

基金：

中国国家自然科学基金;

关键词：

CO2; hydrogenation; Pd dimer; Ethanol; CeO2; INITIO MOLECULAR-DYNAMICS; CU BIMETALLIC CATALYSTS; SINGLE-ATOM CATALYST; SELECTIVE HYDROGENATION; HETEROGENEOUS CATALYSIS; METHANOL SYNTHESIS; PREFERENTIAL OXIDATION; PROMOTION; OXIDE; PALLADIUM;

D O I：

10.1016/j.apcatb.2021.120122

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Hydrogenation of CO2 into valuable chemicals is of great significance but very challenging due to its chemical inertness and selectivity controlling. Here, we report that CeO2 supported Pd dimers can efficiently convert CO2 to ethanol with significantly higher activity and selectivity compared to those in literatures, which gives a selectivity of 99.2 % to ethanol with a space-time yield of 45.6 g(ethanol) g(Pd)(-1) h(-1). The Pd dimers possessing unique Pd2O4 configuration and high homogeneity enables to directly dissociate CO2 to CO, trigger C-C coupling but appropriately inhibit further C2+ coupling, which benefits to selectively form ethanol. The Pd2O4 configuration can strongly bind CO on Pd-2/CeO2, which prevents CO desorption and promotes the coupling between CO and CH3 intermediates to form the precursor of ethanol. The strategy of constructing atom-precision active sites reported in this work opens new avenues to develop highly selective catalysts for CO2/CO hydrogenation reactions.

引用

页数：7

共 71 条

[1] Pd/ZnO catalysts for direct CO2 hydrogenation to methanol [J].