Tailoring the morphology of Pd nanoparticles on CNTs by nitrogen and oxygen functionalization

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	Tailoring the morphology of Pd nanoparticles on CNTs by nitrogen and oxygen functionalization
	R. Arrigo; S. Wrabetz; M. E. Schuster; D. Wang; A. Villa; D. Rosenthal; F. Girsgdies; G. Weinberg; L. Prati; R. Schlogl; D. S. Su
	2012
发表期刊	Physical Chemistry Chemical Physics
ISSN	1463-9076
卷号	14 期号:30 页码:10523-10532
摘要	The influence of N and O functionalization of CNT on the morphology of supported Pd-PVA nanoparticles is studied with respect to the catalytic activity in the liquid phase oxidation of benzyl alcohol to benzaldehyde. The impact of specific N and O sites on the carbon surface induced by the high temperature N-functionalization in the temperature range 673-873 K was observed by HRTEM as increased nanoparticles dispersion and enhanced metal wetting at the carbon surface. Those small nanoparticles that stabilized at the N-CNTs surface are beneficial for improving catalytic performance. The interaction of O-2 with the metal surface was studied by microcalorimetry. At 353 K, the PVA shell hinders the dissociative oxygen chemisorption at the surface of the fresh catalyst. Differently, a very high (maximum for Pd/N-CNT873K 750 kJ mol(-1)) and oscillating exothermic differential heat is registered for the washed samples. Such high differential heat on the "washed'' sample is due to the sum of oxygen chemisorption and PVA oxidation. Thereby, it is demonstrated that the PVA overlayer suppresses the total combustion reaction pathway. This contribution has highlighted the impact of the dynamic change of morphology of these Pd nanoparticles under the reaction conditions on the catalytic performance and how this is modulated by the nature of the support as well as the PVA. The support with its varying ability to strongly bind Pd regulates the morphology of the nanoparticles on which the sub-surface penetration of O, H, C from the reactants depends, all modulating the electronic structure and thus the reactivity.
部门归属	[arrigo, rosa; wrabetz, sabine; schuster, manfred e.; wang, di; rosenthal, dirk; girsgdies, frank; weinberg, gisela; schloegl, robert; su, dang sheng] fritz haber inst max planck gesell, dept anorgan chem, d-14195 berlin, germany. [wang, di] karlsruhe inst technol, d-76344 eggenstein leopoldshafen, germany. [villa, alberto; prati, laura] univ milan, dept inorgan chem l malatesta, i-20133 milan, italy. chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china.;arrigo, r (reprint author), fritz haber inst max planck gesell, dept anorgan chem, faradayweg 4-6, d-14195 berlin, germany.;arrigo@fhi-berlin.mpg.de; dangsheng@fhi-berlin.mpg.de
关键词	Liquid-phase Oxidation In-situ Xps Alcohol Oxidation Benzyl Alcohol Catalytic-activity Pd(111) Oxidation Carbon Nanotubes Au Nanoparticles Oxide Formation Gold Particles
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文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/59886
专题	中国科学院金属研究所
推荐引用方式 GB/T 7714	R. Arrigo,S. Wrabetz,M. E. Schuster,et al. Tailoring the morphology of Pd nanoparticles on CNTs by nitrogen and oxygen functionalization[J]. Physical Chemistry Chemical Physics,2012,14(30):10523-10532.
APA	R. Arrigo.,S. Wrabetz.,M. E. Schuster.,D. Wang.,A. Villa.,...&D. S. Su.(2012).Tailoring the morphology of Pd nanoparticles on CNTs by nitrogen and oxygen functionalization.Physical Chemistry Chemical Physics,14(30),10523-10532.
MLA	R. Arrigo,et al."Tailoring the morphology of Pd nanoparticles on CNTs by nitrogen and oxygen functionalization".Physical Chemistry Chemical Physics 14.30(2012):10523-10532.