ZrO2-x modified Cu nanocatalysts with synergistic catalysis towards carbon-oxygen bond hydrogenation

doi:10.1016/j.apcatb.2020.119406

IHEP OpenIR > 北京同步辐射装置

	ZrO2-x modified Cu nanocatalysts with synergistic catalysis towards carbon-oxygen bond hydrogenation
	BSRF用户
	2021
发表期刊	APPLIED CATALYSIS B-ENVIRONMENTAL (IF:9.446[JCR-2016],8.87[5-Year])
ISSN	0926-3373
EISSN	1873-3883
卷号	280 页码:119406
条目编号	BSRF00155
文章类型	Article
摘要	Carbon-oxygen bond hydrogenation serves as a versatile fundamental reaction extensively applied in chemicals synthesis, but rational design of heterogeneous catalysts with satisfactory catalytic performance and stability remains a big challenge. Herein, a ZrO2-x modified Cu nanocatalyst with unique interfacial structure Cu-O-Zr3+ - Vo (Vo denotes oxygen vacancy), was elaborately designed and prepared via a facile in situ structural transformation from layered double hydroxide precursors, confirmed by a comprehensive study including HADDF-STEM, in situ EXAFS and quasi in situ XPS measurements. The optimized catalyst (Cu/ZrO2-x-S3) exhibits an extremely high catalytic performance toward dimethyl oxalate (DMO) hydrogenation to ethylene glycol (EG), with a yield of 99.5 %. Notably, the turnover frequency (TOF) value and space time yield of EG reach up to 42.4 h(-1) and 1.05 g(EG).g(cat)(-1)-h(-1), respectively. This is, to the best of our knowledge, the highest level compared with previously reported Cu-based catalysts under similar conditions. In addition, the in situ investigations (in situ DMO-FTIR, in situ DMO-EXAFS) and catalytic evaluations substantiate interfacial sites serve as active center: the Zr3+- Vo facilitates adsorption and activation of C=O/C-O groups; whilst H-2 molecule undergoes dissociation at the interfacial Cu species, followed by hydrogen spillover onto Cu-O-Zr for hydrogenation of activated C=O/C-O bonds. This interfacial synergistic catalysis offers a new reaction pathway with decreased activation energy, accounting for the resulting superior catalytic performance, which can be extended to other carbon-oxygen bonds hydrogenation systems.
DOI	10.1016/j.apcatb.2020.119406
收录类别	SCI ; ADS
语种	英语
WOS研究方向	Chemistry ; Engineering
WOS类目	Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS记录号	WOS:000572391700008
ADS Bibcode	2021AppCB.28019406C
ADS URL	https://ui.adsabs.harvard.edu/abs/2021AppCB.28019406C
ADS引文	https://ui.adsabs.harvard.edu/abs/2021AppCB.28019406C/citations
线站	1W1B
引用统计	正在获取... 被引频次：14 [ADS]
文献类型	期刊论文
条目标识符	https://ir.ihep.ac.cn/handle/311005/292923
专题	北京同步辐射装置
推荐引用方式 GB/T 7714	BSRF用户. ZrO2-x modified Cu nanocatalysts with synergistic catalysis towards carbon-oxygen bond hydrogenation[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2021,280:119406.
APA	BSRF用户.(2021).ZrO2-x modified Cu nanocatalysts with synergistic catalysis towards carbon-oxygen bond hydrogenation.APPLIED CATALYSIS B-ENVIRONMENTAL,280,119406.
MLA	BSRF用户."ZrO2-x modified Cu nanocatalysts with synergistic catalysis towards carbon-oxygen bond hydrogenation".APPLIED CATALYSIS B-ENVIRONMENTAL 280(2021):119406.