루테늄이 도입된 티타네이트 나노시트의 합성 및 산화 촉매 활성 연구

이윤희; 권기영; Yoonhee Lee; Ki-Young Kwon

Applied Chemistry for Engineering, Vol.28, No.5, 593-596, October, 2017

DOI10.14478/ace.2017.1056 Export Citation

루테늄이 도입된 티타네이트 나노시트의 합성 및 산화 촉매 활성 연구

Synthesis and Oxidative Catalytic Property of Ruthenium-doped Titanate Nanosheets

이윤희, 권기영^†

경상대학교 화학과

Yoonhee Lee, and Ki-Young Kwon^†

Department of chemistry and RINS, Gyeongsang National University, Jinju 52828, South Korea

E-mail:

초록

본 연구에서는 염기조건에서 수열합성법으로 소듐 티타네이트 나노시트를 합성하였다. 합성한 소듐 티타네이트 나노 시트를 RuCl3 수용액에서 자외선을 조사하여 루테늄을 소듐 티타네이트 나노시트의 표면에 도입하였다. X-선 회절 분석과 투과전자현미경 및 에너지 분산형 분광기 실험을 통하여 샘플의 결정성과 형태를 분석하였고, 그 결과 루테늄 원자가 소듐 티타네이트 표면에 균일하게 흡착되어 있는 것을 확인할 수 있었다. 또한 유도결합플라즈마 발광분광 분석법을 통하여 소듐 티타네이트 나노시트에 도입된 루테늄을 정량하였다. 루테늄이 도입된 소듐 티타네이트 나노시트의 경우 산소를 산화제로 이용한 알코올 산화반응에 응용하였으며, 특히 루테늄이 7% 도입된 소듐 티타네이트 나노시트는 105 ℃, 1기압 상에서 벤질 알코올을 다른 부산물 없이 벤즈알데하이드로 산화시키는 데 있어서 turnover frequency가 2.1 h-1인 촉매활성을 보였다.

Sodium titanate nanosheets were prepared by a hydrothermal synthesis method under basic conditions. Ruthenium was introduced on the surface of sodium titanate nanosheets through an UV irradiation in the aqueous RuCl3 solution. The crystal phase and morphology of synthesized samples were analyzed by X-ray diffraction, transmission electron microscopy and energy dispersive spectroscopy. In addition, the content of Ru was evaluated by inductively coupled plasma. It was proposed that a monomeric form of ruthenium was incorporated on the surface of sodium titanate. Ruthenium incorporated sodium titanates were applied to alcohol oxidation using molecular oxygen as an oxidant. The sample with 7% ruthenium showed a catalytic activity with a turnover frequency value of 2.1 h-1 in oxidizing benzyl alcohol to benzaldehyde without any other byproducts at 105 ℃ and 1 atmosphere.

Keywords:titanate nanosheet;alcohol oxidation;ruthenium

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[1] O’Regan B, Gratzel M, Nature, 353, 737 (1991)

[2] Joo JB, Lee I, Dahl M, Moon GD, Zaera F, Yin Y, Adv. Funct. Mater., 23, 4246 (2013)

[3] Kuo HL, Kuo CY, Liu CH, Chao JH, Lin CH, Catal. Lett., 113(1-2), 7 (2007)

[4] Li N, Zhang LD, Chen YZ, Fang M, Zhang JX, Wang HM, Adv. Funct. Mater., 22(4), 835 (2012)

[5] Vaaramaa K, Lehto J, Desalination, 155(2), 157 (2003)

[6] Sylvester P, Clearfield A, Sep. Sci. Technol., 34(13), 2539 (1999)

[7] Kokubo T, Mater. Sci. Eng. C-Biomimetic Supramol. Syst., 25, 97 (2005)

[8] Ramirez-Salgdo J, Djurado E, Fabry P, J. Eur. Ceram. Soc., 24, 2477 (2004)

[9] Huang J, Cao Y, Deng Z, Tong H, J. Solid State Chem., 184, 712 (2011)

[10] Bennett MA, Matheson TW, Compr. Organomet. Chem., 4, 931 (2006)

[11] Owston NA, Parker AJ, Williams JMJ, Chem. Commun., 8, 624 (2008)

[12] Liu J, He S, Li C, Wang F, Wei M, Evans DG, Duan X, J. Mater. Chem., 2, 7570 (2014)

[13] Horiuchi Y, Kamei G, Saito M, Matsuoka M, Chem. Lett., 42(10), 1282 (2013)

[14] Yoon H, Zou J, Park S, Sammes NM, Chung JS, ECS Trans., 57, 1655 (2013)

[15] Anand NK, Carreira EM, J. Am. Ceram. Soc., 123, 9687 (2001)

[16] Northrup AB, MacMillan DWC, J. Am. Chem. Soc., 124(24), 6798 (2002)

[17] Sheldon RA, Arends IWCE, Dijksman A, Catal. Today, 57(1-2), 157 (2000)

[18] Sheldon RA, Arends IWCE, Brink GJT, Acc. Chem. Res., 35, 774 (2002)

[19] Opre Z, Ferri D, Krumeich F, Mallat T, Baiker A, J. Catal., 241(2), 287 (2006)

[20] Stuchinskaya TL, Kozhevnikov IV, Catal. Commun., 4, 609 (2003)