| Freezing copper as a noble metal-like catalyst for preliminary hydrogenation | |
| Sun, Jian1; Yu, Jiafeng1; Ma, Qingxiang2; Meng, Fanqiong1; Wei, Xiaoxuan3; Sun, Yannan1,4; Tsubaki, Noritatsu5 | |
| 刊名 | Science advances
 |
| 2018-12-01 | |
| 卷号 | 4期号:12页码:10 |
| ISSN号 | 2375-2548 |
| DOI | 10.1126/sciadv.aau3275 |
| 通讯作者 | Sun, jian(sunj@dicp.ac.cn) ; Wei, xiaoxuan(xxwei@zjnu.edu.cn) |
| 英文摘要 | The control of product distribution in a multistep catalytic selective hydrogenation reaction is challenging. for instance, the deep hydrogenation of dimethyl oxalate (dmo) is inclined to proceed over cu/sio2 catalysts because of inevitable coexistence of cu+ and cu-0, leading to hard acquisition of the preliminary hydrogenation product, methyl glycolate (mg). here, the oriented dmo hydrogenation into mg is achieved over the sputtering (sp) cu/sio2 catalysts with a selectivity of more than 87% via freezing cu in a zero-valence state. our density functional theory calculation results revealed that cu-0 is the active site of the preliminary hydrogenation step, selectively converting dmo to mg via center dot h addition, while cu+ is a key factor for deep hydrogenation. the prominent coster-kronig transition enhancement is observed over sp-cu/sio2 from auger spectra, indicating that the electron density of inner shells in cu atoms is enhanced by high-energy argon plasma bombardment during the sp process. thus, the "penetration effect" of outermost electrons could also be enhanced, making these cu nanoparticles exhibit high oxidation resistance ability and present noble metal-like behaviors as au or ag. therefore, the regulation of cu chemical properties by changing the electron structure is a feasible strategy to control the hydrogenation products, inspiring the rational design of selective hydrogenation catalysts. |
| WOS关键词 | SURFACE-PLASMON RESONANCE ; DIMETHYL OXALATE ; CU/SIO2 CATALYSTS ; CHEMOSELECTIVE SYNTHESIS ; SELECTIVE HYDROGENATION ; GOLD NANOPARTICLES ; METHYL GLYCOLATE ; ETHYLENE-GLYCOL ; HMS CATALYST ; PERFORMANCE |
| WOS研究方向 | Science & Technology - Other Topics |
| WOS类目 | Multidisciplinary Sciences |
| 语种 | 英语 |
| 出版者 | AMER ASSOC ADVANCEMENT SCIENCE |
| WOS记录号 | WOS:000454369600023 |
| 内容类型 | 期刊论文 |
| URI标识 | http://www.corc.org.cn/handle/1471x/2372934 |
| 专题 | 大连化学物理研究所 |
| 通讯作者 | Sun, Jian; Wei, Xiaoxuan |
| 作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, Dalian 116023, Peoples R China 2.Ningxia Univ, State Key Lab High Efficiency Utilizat Coal & Gre, Yinchuan 750021, Peoples R China 3.Zhejiang Normal Univ, Coll Geog & Environm Sci, Yingbin Ave 688, Jinhua 321004, Peoples R China 4.Dalian Univ Technol, Sch Chem, Dalian 116023, Peoples R China 5.Univ Toyama, Dept Appl Chem, Grad Sch Engn, Toyama 9308555, Japan |
| 推荐引用方式 GB/T 7714 | Sun, Jian,Yu, Jiafeng,Ma, Qingxiang,et al. Freezing copper as a noble metal-like catalyst for preliminary hydrogenation[J]. Science advances,2018,4(12):10. |
| APA | Sun, Jian.,Yu, Jiafeng.,Ma, Qingxiang.,Meng, Fanqiong.,Wei, Xiaoxuan.,...&Tsubaki, Noritatsu.(2018).Freezing copper as a noble metal-like catalyst for preliminary hydrogenation.Science advances,4(12),10. |
| MLA | Sun, Jian,et al."Freezing copper as a noble metal-like catalyst for preliminary hydrogenation".Science advances 4.12(2018):10. |
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