Strong metal-support interaction boosting the catalytic activity of Au/TiO2 in chemoselective hydrogenation

doi:10.1016/S1872-2067(20)63763-9

Abstract

Abstract:

Gold catalysts have been reported as highly effective catalysts in various oxidation reactions. However, for chemoselective hydrogenation reactions, gold-based catalysts normally show much lower catalytic activity than platinum group metals, even though their selectivities are excellent. Here, we report that the chemoselective hydrogenation activity of 3-nitrostyrene to 3-vinylaniline over Au/TiO₂ can be enhanced up to 3.3 times through the hydrogen reduction strategy. It is revealed that strong metal-support interaction, between gold nanoparticles (NPs) and TiO₂ support, is introduced through hydrogen reduction, resulting in partial dispersion of reduced TiO_x on the Au surface. The partially covered Au not only increases the perimeter of the interface between the gold NPs and the support, but also benefits H₂ activation. Reaction kinetic analysis and H₂-D₂ exchange reaction show that H₂ activation is the critical step in the hydrogenation of 3-nitrostyrene to 3-vinylaniline. Density functional theory calculations verify that hydrogen dissociation and hydrogen transfer are favored at the interface of gold NPs and TiO₂ over the hydrogen-reduced Au/TiO₂. This study provides insights for fabricating highly active gold-based catalysts for chemoselective hydrogenation reactions.

Key words: Gold catalysis, Strong metal support interaction, Interface, 3-Nitrostyrene chemoselective hydrogenation, Boosting activity

Feng Hong, Shengyang Wang, Junying Zhang, Junhong Fu, Qike Jiang, Keju Sun, Jiahui Huang. Strong metal-support interaction boosting the catalytic activity of Au/TiO₂ in chemoselective hydrogenation[J]. Chinese Journal of Catalysis, 2021, 42(9): 1530-1537.

×
share this article

Add to citation manager EndNote|Ris|BibTeX

URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63763-9

https://www.cjcatal.com/EN/Y2021/V42/I9/1530

Figures/Tables 4

Fig. 1. Conversion of 3-NS and selectivity of 3-VA versus time over Au/TiO2 catalysts calcined under different conditions. Gold catalysts were calcined at (a) 400 or (b) 500 °C. Reaction conditions: 3-NS (1.2 mmol); Au catalyst (6 × 10-3 mmol Au); H2 pressure (2 MPa); stirring rate: 1200 rpm, temperature: 60 °C.

Fig. 2. (a) TOF values of 3-NS hydrogenation over Au/TiO2-500H and Au/TiO2-500O. Conditions: 3-NS (1.2 mmol); Au catalyst (6 × 10-3 mmol Au). (b) Arrhenius plots for 3-NS chemoselective hydrogenation over Au/TiO2-500H and Au/TiO2-500O. Conversion of 3-NS is in the range 10%-20%. Reaction conditions: 3-NS (0.2 mmol); Au catalyst (1 × 10-3 mmol Au); H2 pressure (2 MPa); stirring rate: 1200 rpm; temperature: 40, 50, 60 and 70 °C.

Fig. 3. (a) 3-NS conversion versus time over Au/TiO2 catalyst calcined under different gaseous atmospheres; (b) EPR spectra of the gold catalysts calcined at 500 °C under different gases; HAADF-STEM images and EELS spectra of (c,d) Au/TiO2-500O and (e,f) Au/TiO2-500H.

Fig. 4. H2-D2 exchange reaction over Au/TiO2-500H (a) and Au/TiO2-500O (b). This reaction was performed in a fixed bed at a temperature range of 30-200 °C. Conditions: 30 mL·min of 50% H2 and 50% D2 (space velocity = 36000 mL·gcat-1·h-1); temperature range: 30-200 °C; pressure: 0.1 MPa. (c) The reaction paths for the H2-D2 exchange reaction on Au/TiO2-x (representing Au/TiO2-500H) and Au/TiO2 (on behalf of Au/TiO2-500O). (d) The energy changes of hydrogen transfer on Au/TiO2 and Au/TiO2-x. The red, blue, yellow, and pink balls represent oxygen, titanium, gold, and hydrogen or deuterium, respectively.

References

[1]	M. Haruta, T. Kobayashi, H. Sano, N. Yamada, Chem. Lett., 1987, 405-408.
[2]	G. J. Hutchings, J. Catal., 1985,96, 292-295.
[3]	A. U. Nilekar, S. Alayoglu, B. Eichhorn, M. Mavrikakis, J. Am. Chem. Soc., 2010,132, 7418-7428.
[4]	T. Hayashi, K. Tanaka, M. Haruta, J. Catal., 1998,178, 566-575.
[5]	K. Suzuki, T. Yamaguchi, K. Matsushita, C. Iitsuka, J. Miura, T. Akaogi, H. Ishida, ACS Catal., 2013,3, 1845-1849.
[6]	A. Corma, P. Serna, Science, 2006,313, 332-334.
[7]	N. Yang, H. Cheng, X. Liu, Q. Yun, Y. Chen, B. Li, B. Chen, Z. Zhang, X. Chen, Q. Lu, J. Huang, Y. Huang, Y. Zong, Y. Yang, L. Gu, H. Zhang, Adv. Mater., 2018,30, e1803234.
[8]	S. Jian, Y. Li, Chin. J. Catal., 2016,37, 91-97.
[9]	A. Corma, P. Concepcion, P. Serna, Angew. Chem. Int. Ed., 2007,46, 7266-7269.
[10]	Y. Matsushima, R. Nishiyabu, N. Takanashi, M. Haruta, H. Kimura, Y. Kubo, J. Mater. Chem., 2012,22, 24124-24131.
[11]	H. Wei, X. Wei, X. Yang, G. Yin, A. Wang, X. Liu, Y. Huang, T. Zhang, Chin. J. Catal., 2015,36, 160-167.
[12]	B. Hammer, J. K. Norskov, Nature, 1995,376, 238-240.
[13]	C. Mohr, H. Hofmeister, J. Radnik, P. Claus, J. Am. Chem. Soc., 2003,125, 1905-11.
[14]	E. Bus, J. A. van Bokhoven, Phys. Chem. Chem. Phys., 2007,9, 2894-2902.
[15]	E. Bus, J. T. Miller, J. A. van Bokhoven, J. Phys. Chem. B, 2005,109, 14581-14587.
[16]	T. Fujitani, I. Nakamura, T. Akita, M. Okumura, M. Haruta, Angew. Chem. Int. Ed., 2009,48, 9515-8.
[17]	S. Baishya, R. C. Deka, Comput. Theor. Chem., 2012,1002, 1-8.
[18]	H. W. Ghebriel, A. Kshirsagar, J. Chem. Phys., 2007,126, 244705.
[19]	M. Chen, Y. Cai, Z. Yan, D. W. Goodman, J. Am. Chem. Soc., 2006,128, 6341-6346.
[20]	S. Yao, X. Zhang, W. Zhou, R. Gao, W. Xu, Y. Ye, L. Lin, X. Wen, P. Liu, B. Chen, E. Crumlin, J. Guo, Z. Zuo, W. Li, J. Xie, L. Lu, C. J. Kiely, L. Gu, C. Shi, J. A. Rodriguez, D. Ma, Science, 2017,357, 389-393.
[21]	Y. Wei, J. Liu, Z. Zhao, A. Duan, G. Jiang, J. Catal., 2012,287, 13-29.
[22]	N. M. Schweitzer, J. A. Schaidle, O. K. Ezekoye, X. Pan, S. Linic, L. T. Thompson, J. Am. Chem. Soc., 2011,133, 2378-2381.
[23]	S. J. Tauster, S. C. Fung, R. T. K. Baker, J. A. Horsley, Science, 1981,211, 1121-1125.
[24]	S. J. Tauster, Acc. Chem. Res., 1987,20, 389-394.
[25]	J. C. Matsubu, S. Zhang, L. DeRita, N. S. Marinkovic, J. G. Chen, G. W. Graham, X. Pan, P. Christopher, Nat. Chem., 2017,9, 120-127.
[26]	X. Liu, M.-H. Liu, Y.-C. Luo, C.-Y. Mou, S. D. Lin, H. Cheng, J.-M. Chen, J.-F. Lee, T.-S. Lin, J. Am. Chem. Soc., 2012,134, 10251-10258.
[27]	P. Hu, Z. Huang, Z. Amghouz, M. Makkee, F. Xu, F. Kapteijn, A. Dikhtiarenko, Y. Chen, X. Gu, X. Tang, Angew. Chem. Int. Ed., 2014,53, 3418-3421.
[28]	A. Bruix, J. A. Rodriguez, P. J. Ramirez, S. D. Senanayake, J. Evans, J. B. Park, D. Stacchiola, P. Liu, J. Hrbek, F. Illas, J. Am. Chem. Soc., 2012,134, 8968-8974.
[29]	H. Tang, F. Liu, J. Wei, B. Qiao, K. Zhao, Y. Su, C. Jin, L. Li, J. J. Liu, J. Wang, T. Zhang, Angew. Chem. Int. Ed., 2016,55, 10606-10611.
[30]	H. Tang, J. Wei, F. Liu, B. Qiao, X. Pan, L. Li, J. Liu, J. Wang, T. Zhang, J. Am. Chem. Soc., 2016,138, 56-59.
[31]	Z. Qiao, H. Feng, J. Zhou, Phase Transit, 2014,87, 59-70.
[32]	S. J. Tauster, S. C. Fung, R. L. Garten, J. Am. Chem. Soc., 1978,100, 170-175.
[33]	A. Kumar, V. Ramani, ACS Catal., 2014,4, 1516-1525.
[34]	M. Macino, A. J. Barnes, S. M. Althahban, R. Qu, E. K. Gibson, D. J. Morgan, S. J. Freakley, N. Dimitratos, C. J. Kiely, X. Gao, A. M. Beale, D. Bethell, Q. He, M. Sankar, G. J. Hutchings, Nat. Catal., 2019,2, 873-881.
[35]	A. L. Nuzhdin, S. I. Reshetnikov, G. A. Bukhtiyarova, B. L. Moroz, E. Y. Gerasimov, P. A. Pyrjaev, V. I. Bukhtiyarov, Catal. Lett., 2017,147, 572-580.
[36]	R. Zanella, S. Giorgio, C. R. Henry, C. Louis, J. Phys. Chem. B, 2002,106, 7634-7642.
[37]	S. Wang, Y. Gao, S. Miao, T. Liu, L. Mu, R. Li, F. Fan, C. Li, J. Am. Chem. Soc., 2017,139, 11771-11778.
[38]	K. Sun, M. Kohyama, S. Tanaka, S. Takeda, J. Phys. Chem. C, 2014,118, 1611-1617.
[39]	X. Song, K. Sun, X. Hao, H. Y. Su, X. Ma, Y. Xu, J. Phys. Chem. C, 2019,123, 26324-26337.
[40]	V. Subramanian, E. E. Wolf, P. V. Kamat, J. Am. Chem. Soc., 2004,126, 4943-4950.
[41]	M. Murdoch, G. I. N. Waterhouse, M. A. Nadeem, J. B. Metson, M. A. Keane, R. F. Howe, J. Llorca, H. Idriss, Nat. Chem., 2011,3, 489-492.
[42]	X. Wang, Y. Li, J. Mol. Catal. A, 2016,420, 56-65.
[43]	Y. Tan, X. Y. Liu, L. Zhang, A. Wang, L. Li, X. Pan, S. Miao, M. Haruta, H. Wei, H. Wang, F. Wang, X. Wang, T. Zhang, Angew. Chem. Int. Ed., 2017,56, 2709-2713.
[44]	Y. Tan, X. Y. Liu, L. Li, L. Kang, A. Wang, T. Zhang, J. Catal., 2018,364, 174-182.
[45]	F. Zuo, L. Wang, T. Wu, Z. Zhang, D. Borchardt, P. Feng, J. Am. Chem. Soc., 2010,132, 11856-11857.
[46]	N. Liu, M. Xu, Y. Yang, S. Zhang, J. Zhang, W. Wang, L. Zheng, S. Hong, M. Wei, ACS Catal., 2019,9, 2707-2717.
[47]	H. Tang, Y. Su, B. Zhang, A. F. Lee, M. A. Isaacs, K. Wilson, L. Li, Y. Ren, J. Huang, M. Haruta, B. Qiao, X. Liu, C. Jin, D. Su, J. Wang, T. Zhang, Sci. Adv., 2017,3, e1700231.
[48]	G. Li, N. M. Dimitrijevic, L. Chen, J. M. Nichols, T. Rajh, K. A. Gray, J. Am. Chem. Soc., 2008,130, 5402-5403.
[49]	J. C. Conesa, P. Malet, G. Munuera, J. Sanz, J. Soria, J. Phys. Chem., 1984,88, 2986-2992.
[50]	M. Okumura, J. M. Coronado, J. Soria, M. Haruta, J. C. Conesa, J. Catal., 2001,203, 168-174.
[51]	M. Comotti, W. C. Li, B. Spliethoff, F. Schuth, J. Am. Chem. Soc., 2006,128, 917-924.
[52]	J. Guzman, B. C. Gates, J. Am. Chem. Soc., 2004,126, 2672-2673.
[53]	A. Lewera, L. Timperman, A. Roguska, N. Alonso-Vante, J. Phys. Chem. C, 2011,115, 20153-20159.
[54]	L. R. Baker, G. Kennedy, M. Van Spronsen, A. Hervier, X. Cai, S. Chen, L.-W. Wang, G. A. Somorjai, J. Am. Chem. Soc., 2012,134, 14208-14216.

Strong metal-support interaction boosting the catalytic activity of Au/TiO₂ in chemoselective hydrogenation

RichHTML

PDF (PC)

Knowledge

Supporting Information

Abstract

Cite this article

share this article

share this article

Figures/Tables 4

References

Related Articles 15

Recommended Articles

Metrics

[1]	Yong Liu, Xiaoli Zhao, Chang Long, Xiaoyan Wang, Bangwei Deng, Kanglu Li, Yanjuan Sun, Fan Dong. In situ constructed dynamic Cu/Ce(OH)_x interface for nitrate reduction to ammonia with high activity, selectivity and stability [J]. Chinese Journal of Catalysis, 2023, 52(9): 196-206.
[2]	Xuan Li, Xingxing Jiang, Yan Kong, Jianju Sun, Qi Hu, Xiaoyan Chai, Hengpan Yang, Chuanxin He. Interface engineering of a GaN/In₂O₃ heterostructure for highly efficient electrocatalytic CO₂ reduction to formate [J]. Chinese Journal of Catalysis, 2023, 50(7): 314-323.
[3]	Si-Yuan Xia, Qi-Yuan Li, Shi-Nan Zhang, Dong Xu, Xiu Lin, Lu-Han Sun, Jingsan Xu, Jie-Sheng Chen, Guo-Dong Li, Xin-Hao Li. Size-dependent electronic interface effect of Pd nanocube-based heterojunctions on universally boosting phenol hydrogenation reactions [J]. Chinese Journal of Catalysis, 2023, 49(6): 180-187.
[4]	Dan-Qing Liu, Bingxing Zhang, Guoqiang Zhao, Jian Chen, Hongge Pan, Wenping Sun. Advanced in-situ electrochemical scanning probe microscopies in electrocatalysis [J]. Chinese Journal of Catalysis, 2023, 47(4): 93-120.
[5]	Qi Xue, Zhe Wang, Yu Ding, Fumin Li, Yu Chen. Chemical functionalized noble metal nanocrystals for electrocatalysis [J]. Chinese Journal of Catalysis, 2023, 45(2): 6-16.
[6]	Yu Gu, Lei Wang, Bo-Qing Xu, Hui Shi. Recent advances in the molecular-level understanding of catalytic hydrogenation and oxidation reactions at metal-aqueous interfaces [J]. Chinese Journal of Catalysis, 2023, 54(11): 1-55.
[7]	Yuyan Qiao, Yanqiu Pan, Jiangwei Zhang, Bin Wang, Tingting Wu, Wenjun Fan, Yucheng Cao, Rashid Mehmood, Fei Zhang, Fuxiang Zhang. Multiple carbon interface engineering to boost oxygen evolution of NiFe nanocomposite electrocatalyst [J]. Chinese Journal of Catalysis, 2022, 43(9): 2354-2362.
[8]	Xugang Yang, Zonghui Liu, Guoliang Wei, Yu Gu, Hui Shi. A critical assessment of the roles of water molecules and solvated ions in acid-base-catalyzed reactions at solid-water interfaces [J]. Chinese Journal of Catalysis, 2022, 43(8): 1964-1990.
[9]	Xianwen Zhang, Zheng Li, Taifeng Liu, Mingrun Li, Chaobin Zeng, Hiroaki Matsumoto, Hongxian Han. Water oxidation sites located at the interface of Pt/SrTiO₃ for photocatalytic overall water splitting [J]. Chinese Journal of Catalysis, 2022, 43(8): 2223-2230.
[10]	Jiang Zhang, Zijian Wang, Mugeng Chen, Yifeng Zhu, Yongmei Liu, Heyong He, Yong Cao, Xinhe Bao. N-doped carbon layer-coated Au nanocatalyst for H₂-free conversion of 5-hydroxymethylfurfural to 5-methylfurfural [J]. Chinese Journal of Catalysis, 2022, 43(8): 2212-2222.
[11]	Jinman Yang, Xingwang Zhu, Qing Yu, Minqiang He, Wei Zhang, Zhao Mo, Junjie Yuan, Yuanbin She, Hui Xu, Huaming Li. Multidimensional In₂O₃/In₂S₃ heterojunction with lattice distortion for CO₂ photoconversion [J]. Chinese Journal of Catalysis, 2022, 43(5): 1286-1294.
[12]	Dan Zhang, Hongfu Miao, Xueke Wu, Zuochao Wang, Huan Zhao, Yue Shi, Xilei Chen, Zhenyu Xiao, Jianping Lai, Lei Wang. Scalable synthesis of ultra-small Ru₂P@Ru/CNT for efficient seawater splitting [J]. Chinese Journal of Catalysis, 2022, 43(4): 1148-1155.
[13]	Liang Jian, Huizhen Zhang, Bing Liu, Chengsi Pan, Yuming Dong, Guangli Wang, Jun Zhong, Yongjie Zheng, Yongfa Zhu. Monodisperse Ni-clusters anchored on carbon nitride for efficient photocatalytic hydrogen evolution [J]. Chinese Journal of Catalysis, 2022, 43(2): 536-545.
[14]	Junxian Bai, Rongchen Shen, Zhimin Jiang, Peng Zhang, Youji Li, Xin Li. Integration of 2D layered CdS/WO₃ S-scheme heterojunctions and metallic Ti₃C₂ MXene-based Ohmic junctions for effective photocatalytic H₂ generation [J]. Chinese Journal of Catalysis, 2022, 43(2): 359-369.
[15]	Qi Hao, Yongmeng Wu, Cuibo Liu, Yanmei Shi, Bin Zhang. Unveiling subsurface hydrogen inhibition for promoting electrochemical transfer semihydrogenation of alkynes with water [J]. Chinese Journal of Catalysis, 2022, 43(12): 3095-3100.