Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst

	Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst
	Huang, Yanqiang 2; Wang, Xinkui 3; Miao, Shu 2; Li, Lin 2; Yang, Xiaofeng 2; Liu, Qinggang 2,3; Zhang, Tao 2; Li, Yanqin 3; Li, Yong 1,4
刊名	NATURE COMMUNICATIONS
	2017-11-10
卷号	8
英文摘要	Catalytic transformation of CO2 to formate is generally realized through bicarbonate hydrogenation in an alkaline environment, while it suffers from a thermodynamic sink due to the considerable thermodynamic stability of the bicarbonate intermediate. Here, we devise a route for the direct catalytic conversion of CO2 over a Schiff-base-modified gold nanocatalyst that is comparable to the fastest known nanocatalysts, with a turnover number (TON) of up to 14,470 over 12 h at 90 degrees C. Theoretical calculations and spectral analysis results demonstrate that the activation of CO2 can be achieved through a weakly bonded carbamate zwitterion intermediate derived from a simple Lewis base adduct of CO2. However, this can only occur with a hydrogen lacking Lewis base center in a polar solvent. This finding offers a promising avenue for the direct activation of CO2 and is likely to have considerable implications in the fields of CO2 conversion and gold catalytic chemistry.
WOS标题词	Science & Technology
类目[WOS]	Multidisciplinary Sciences
研究领域[WOS]	Science & Technology - Other Topics
关键词[WOS]	CARBON-DIOXIDE ; FORMIC-ACID ; CARBAMATE FORMATION ; ROOM-TEMPERATURE ; KINETICS ; IDENTIFICATION ; CONVERSION ; MOLECULES ; MECHANISM ; METHANOL
收录类别	SCI
语种	英语
WOS记录号	WOS:000414869200006
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/149716]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
作者单位	1.Univ Bremen, Ctr Environm Res & Sustainable Technol, D-28359 Bremen, Germany 2.Chinese Acad Sci, Collaborat Innovat Ctr Chem Energy Mat, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 3.Dalian Univ Technol, Sch Chem, State Key Lab Fine Chem, Dalian 116024, Peoples R China 4.Univ Bremen, Inst Appl & Phys Chem, D-28359 Bremen, Germany
推荐引用方式 GB/T 7714	Huang, Yanqiang,Wang, Xinkui,Miao, Shu,et al. Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst[J]. NATURE COMMUNICATIONS,2017,8.
APA	Huang, Yanqiang.,Wang, Xinkui.,Miao, Shu.,Li, Lin.,Yang, Xiaofeng.,...&Li, Yong.(2017).Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst.NATURE COMMUNICATIONS,8.
MLA	Huang, Yanqiang,et al."Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst".NATURE COMMUNICATIONS 8(2017).