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Ultrathin and vacancy-rich coal-layered double hydroxide/graphite oxide catalysts: promotional effect of cobalt vacancies and oxygen vacancies in alcohol oxidation
Wang, Qian1,2; Chen, Lifang1; Guan, Shaoliang3; Zhang, Xin1; Wang, Bin4; Cao, Xingzhong5; Yu, Zhi1; He, Yufei1,2; Evans, David G.1; Feng, Junting1,2
刊名Acs catalysis
2018-04-01
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
DOI10.1021/acscata1.7b03655
通讯作者Feng, junting(fengjt@mail.buct.edu.cn) ; Li, dianqing()
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
WOS类目Chemistry, Physical
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000430154100055
内容类型期刊论文
URI标识http://www.corc.org.cn/handle/1471x/2177524
专题高能物理研究所
通讯作者Feng, Junting; Li, Dianqing
作者单位1.Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
2.Beijing Univ Chem Technol, Beijing Engn Ctr Hierarch Catalysts, Beijing 100029, Peoples R China
3.Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Cardiff CF10 3AT, S Glam, Wales
4.Sinopec Beijing Res Inst Chem Ind, Beijing 100013, Peoples R China
5.Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714
Wang, Qian,Chen, Lifang,Guan, Shaoliang,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 Wang, Qian.,Chen, Lifang.,Guan, Shaoliang.,Zhang, Xin.,Wang, Bin.,...&Li, Dianqing.(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 Wang, Qian,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.
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