Ultrathin and Vacancy-Rich CoAl-Layered Double Hydroxide/Graphite Oxide Catalysts: Promotional Effect of Cobalt Vacancies and Oxygen Vacancies in Alcohol Oxidation
文献类型：期刊论文
| 作者 | Chen, LF; Guan, SL; Zhang, X; Wang, B; Cao, XZ ; Yu, Z; He, YF; Evans, DG; Feng, JT; Li, DQ
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| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2018 |
| 卷号 | 8期号:4页码:3104-3115 |
| 关键词 | exfoliation ultrathin layered double hydroxides vacancy selective alcohol oxidation |
| ISSN号 | 2155-5435 |
| DOI | 10.1021/acscatal.7b03655 |
| 文献子类 | Article |
| 英文摘要 | Co-containing layered double hydroxides (LDHs) are potential non-noble-metal catalysts for the aerobic oxidation of alcohols. However, the intrinsic activity of bulk LDHs is relatively low. In this work, we fabricated ultrathin and vacancy-rich nanosheets by exfoliating bulk CoAI-LDHs, which were then assembled with graphite oxide (GO) to afford a hybrid CoAI-ELDH/GO catalyst. TEM, AFM, and positron annihilation spectrometry indicate that the thickness of the exfoliated LDH platelets is about 3 rim, with a large number of vacancies in the host layers. Fourier transformed XAFS functions show that the Co-O and Co center dot center dot center dot center dot Co coordination numbers (5.5 and 2.8, respectively) in the hybrid CoAI-ELDH/GO material are significantly lower than the corresponding values in bulk CoAI-LDHs (6.0 and 3.8, respectively). Furthermore, in addition to the oxygen vacancies (V-O) and cobalt vacancies (V-Co), CoAI-ELDH/GO also contains negatively charged V-Co-Co-OH delta- sites and exposed lattice oxygen sites. CoAI-ELDH/GO shows excellent performance as a catalyst for the aerobic oxidation of benzyl alcohol, with a TOF of 1.14 h(-1); this is nearly five times that of the unexfoliated bulk CoAI-LDHs (0.23 h(-1)) precursor. O-2-TPD and DRIFT spectroscopy declare that the oxygen storage capacity and mobility are facilitated by the oxygen vacancies and surface lattice oxygen sites. Meanwhile, DFT calculations of adsorption energy show that benzyl alcohol is strongly adsorbed on the oxygen vacancies and negatively charged V-Co-Co-OH delta- sites. A kinetic isotope effect study further illustrates that the vacancy-rich CoAI-ELDH/GO catalyst accelerates the cleavage of the O-H bond in benzyl alcohol. Finally, we show that the hybrid CoAI-ELDH/GO material exhibits excellent catalytic activity and selectivity in the oxidation of a range of other benzylic and unsaturated alcohols. |
| WOS关键词 | SUPPORTED GOLD NANOPARTICLES ; LOW-TEMPERATURE OXIDATION ; AEROBIC OXIDATION ; BENZYL ALCOHOL ; SELECTIVE OXIDATION ; MOLECULAR-OXYGEN ; DOUBLE HYDROXIDES ; CO3O4 NANORODS ; ACTIVE-SITES ; METAL-OXIDES |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000430154100055 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/285911]  |
| 专题 | 高能物理研究所_多学科研究中心 |
| 作者单位 | 中国科学院高能物理研究所 |
| 推荐引用方式 GB/T 7714 | Chen, LF,Guan, SL,Zhang, X,et al. Ultrathin and Vacancy-Rich CoAl-Layered Double Hydroxide/Graphite Oxide Catalysts: Promotional Effect of Cobalt Vacancies and Oxygen Vacancies in Alcohol Oxidation[J]. ACS CATALYSIS,2018,8(4):3104-3115. |
| APA | Chen, LF.,Guan, SL.,Zhang, X.,Wang, B.,Cao, XZ.,...&Wang, Q.(2018).Ultrathin and Vacancy-Rich CoAl-Layered Double Hydroxide/Graphite Oxide Catalysts: Promotional Effect of Cobalt Vacancies and Oxygen Vacancies in Alcohol Oxidation.ACS CATALYSIS,8(4),3104-3115. |
| MLA | Chen, LF,et al."Ultrathin and Vacancy-Rich CoAl-Layered Double Hydroxide/Graphite Oxide Catalysts: Promotional Effect of Cobalt Vacancies and Oxygen Vacancies in Alcohol Oxidation".ACS CATALYSIS 8.4(2018):3104-3115. |
入库方式： OAI收割
来源：高能物理研究所
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