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Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst
Liu, Qinggang1,2; Yang, Xiaofeng2; Li, Lin2; Miao, Shu2; Li, Yong3,4; Li, Yanqin1; Wang, Xinkui1; Huang, Yanqiang2; Zhang, Tao2
刊名NATURE COMMUNICATIONS
2017-11-10
DOI10.1038/s41467-017-01673-3
8
收录类别SCI
文章类型Article
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
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.
语种英语
WOS记录号WOS:000414869200006
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/149716
专题中国科学院大连化学物理研究所
作者单位1.Dalian Univ Technol, Sch Chem, State Key Lab Fine Chem, Dalian 116024, Peoples R China
2.Chinese Acad Sci, Collaborat Innovat Ctr Chem Energy Mat, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
3.Univ Bremen, Inst Appl & Phys Chem, D-28359 Bremen, Germany
4.Univ Bremen, Ctr Environm Res & Sustainable Technol, D-28359 Bremen, Germany
推荐引用方式
GB/T 7714
Liu, Qinggang,Yang, Xiaofeng,Li, Lin,et al. Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst[J]. NATURE COMMUNICATIONS,2017,8.
APA Liu, Qinggang.,Yang, Xiaofeng.,Li, Lin.,Miao, Shu.,Li, Yong.,...&Zhang, Tao.(2017).Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst.NATURE COMMUNICATIONS,8.
MLA Liu, Qinggang,et al."Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst".NATURE COMMUNICATIONS 8(2017).
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