Perspectives on the Active Sites and Catalyst Design for the Hydrogenation of Dimethyl Oxalate

Ye，Run Ping1,2,3; Lin，Ling1; Wang，Lu Cun4; Ding，Dong4; Zhou，Zhangfeng1; Pan，Pengbin1; Xu，Zhenghe5; Liu，Jian3,6; Adidharma，Hertanto2; Radosz，MacIej2; Fan，Maohong2,7,8; Yao，Yuan Gen1

2020-04-17

10.1021/acscatal.9b05477

ACS Catalysis   影响因子和分区

2155-5435

2155-5435

What should people do with the huge amount of CO captured? CO to CO is a promising way for using carbon resources because CO is one component of syngas for the production of many important synthesis intermediates such as dimethyl oxalate (DMO). Hydrogenation of DMO provides an economical and eco-friendly approach for the synthesis of methyl glycolate, ethylene glycol (EG), and ethanol, which is often determined by the reaction conditions and catalysts with different active sites. Thus, DMO or EG is also an important carbon carrier or CO utilization product. Also, DMO hydrogenation is a representative reaction for studying the structure-activity relationship in C═O/C-O bond hydrogenation. Therefore, this work provides a comprehensive review of the progress in DMO hydrogenation from the perspective of constructing and stabilizing the active sites. The silver and copper based catalysts with different structures and morphologies used for DMO hydrogenation have been discussed with regard to their catalytic performance and reaction mechanism. The synergy of Cu and Cu in DMO hydrogenation has been questioned, and new active sites are proposed with more experimental evidence. New reaction routes, hybrid active sites, and the effect of catalyst structure on the active sites for DMO hydrogenation have been achieved and reviewed. Moreover, a strategy of introducing organic additives to improve EG yield and stabilize copper species has been described. This work may help advance the understanding of active sites in DMO hydrogenation and guide the future rational design and fabrication of highly stable and low-cost DMO hydrogenation catalysts.

active sites Cu based catalysts dimethyl oxalate ethanol ethylene glycol heterogeneous catalysis hydrogenation reaction structure-activity relationship

SCI ; EI

英语

其他

National Key R&D Program of China[2017YFB0307301][2017YFA0206802] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDA21020800] ; Science and Technology Service Network Initiative[KFJ-STS-QYZD-048] ; Science Foundation of Guizhou Province[[2018]2193] ; NSF of China[21703247] ; NSF of Fujian Province[2018J05029][2019J05156] ; China Postdoctoral Science Foundation[2019M661143] ; Idaho National Laboratory Directed Research and Development Program under DOE Idaho Operations Office[DE-AC07-05ID14517] ; Fujian industrial guide project[2019H0053]

Chemistry

Chemistry, Physical

WOS:000543700400002

AMER CHEMICAL SOC

20202008665399

Additives ; Carbon ; Catalysis ; Catalyst activity ; Copper ; Carbon dioxide ; Oxalic acid ; Ethanol ; Ethylene ; Hydrogenation ; Polyols

Copper:544.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2

2-s2.0-85084602097

Scopus

1.Key Laboratory of Coal to Ethylene Glycol and Its Related Technology,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou, Fujian,350002,China
2.Departments of Chemical and Petroleum Engineering,University of Wyoming,Laramie,82071,United States
3.State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian, Liaoning,116023,China
4.Idaho National Laboratory,Idaho Falls,83415,United States
5.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen, Guangdong,518055,China
6.DICP-Surrey Joint Centre for Future Materials,Department of Chemical and Process Engineering,Advanced Technology Institute,University of Surrey,Guilford, Surrey,GU2 7XH,United Kingdom
7.School of Energy Resources,University of Wyoming,Laramie,82071,United States
8.School of Civil and Environmental Engineering,Georgia Institute of Technology,Atlanta,30332,United States

Ye，Run Ping,Lin，Ling,Wang，Lu Cun,et al. Perspectives on the Active Sites and Catalyst Design for the Hydrogenation of Dimethyl Oxalate[J]. ACS Catalysis,2020,10(8):4465-4490.

Ye，Run Ping.,Lin，Ling.,Wang，Lu Cun.,Ding，Dong.,Zhou，Zhangfeng.,...&Yao，Yuan Gen.(2020).Perspectives on the Active Sites and Catalyst Design for the Hydrogenation of Dimethyl Oxalate.ACS Catalysis,10(8),4465-4490.

Ye，Run Ping,et al."Perspectives on the Active Sites and Catalyst Design for the Hydrogenation of Dimethyl Oxalate".ACS Catalysis 10.8(2020):4465-4490.