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Nano Research 2023, 16(7): 9059-9064 https://doi.org/10.1007/s12274-023-5684-0
Research Article | Issue | Published: 18 May 2023

Effects of water adsorption on active site-dependent H2 activation over MgO nanoflakes

Show Author's Information Aiyi Dong1,2,§,  Kun Li1,2,§,  Rentao Mu2( ),  Conghui Liu2,  Rongtan Li2,  Haoran Jia2,  Le Lin2,  Qiang Fu2,3( )
School of Science, Dalian Maritime University, Dalian 116026, China
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

§ Aiyi Dong and Kun Li contributed equally to this work.

Keywords:
MgO, hydride, hydroxyl, H2O, H2 activation
Topics:
Nanocatalysts
Cite this article:
Dong A, Li K, Mu R, et al. Effects of water adsorption on active site-dependent H2 activation over MgO nanoflakes. Nano Research, 2023, 16(7): 9059-9064. https://doi.org/10.1007/s12274-023-5684-0
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Abstract Full text Electronic supplementary material About this article

Understanding the effect of H2O adsorption on reactant activation is of great importance in heterogeneous catalysis, which remains a grand challenge particularly in oxide catalyst systems with structural complexity. Herein, the effect of D2O adsorption on D2 activation over MgO nanocatalysts at different temperatures has been investigated by transmission Fourier transform infrared (FT-IR) and temperature-programmed desorption (TPD). Two sets of hydride and hydroxyl species produced from D2 dissociation at more active and less active Mg-O pairs can be observed by FT-IR, which all desorb via the product of D2 as confirmed by TPD experiments. We find that the physically adsorbed D2O overlayer does not affect the dissociation of D2 since D2 may pass through the molecular layer and access the surface-active sites. When D2O is partially dissociated on the MgO surface, D2 can only dissociate at the remaining active sites until that dissociated -ODw groups from D2O occupy all active sites. These findings provide a fundamental understanding of the effect of water adsorption on D2 activation on oxide catalysts.


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About this article

Effects of water adsorption on active site-dependent H2 activation over MgO nanoflakes

Show Author's information Aiyi Dong1,2,§, Kun Li1,2,§, Rentao Mu2( ), Conghui Liu2, Rongtan Li2, Haoran Jia2, Le Lin2, Qiang Fu2,3( )
School of Science, Dalian Maritime University, Dalian 116026, China
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

§ Aiyi Dong and Kun Li contributed equally to this work.

Abstract

Understanding the effect of H2O adsorption on reactant activation is of great importance in heterogeneous catalysis, which remains a grand challenge particularly in oxide catalyst systems with structural complexity. Herein, the effect of D2O adsorption on D2 activation over MgO nanocatalysts at different temperatures has been investigated by transmission Fourier transform infrared (FT-IR) and temperature-programmed desorption (TPD). Two sets of hydride and hydroxyl species produced from D2 dissociation at more active and less active Mg-O pairs can be observed by FT-IR, which all desorb via the product of D2 as confirmed by TPD experiments. We find that the physically adsorbed D2O overlayer does not affect the dissociation of D2 since D2 may pass through the molecular layer and access the surface-active sites. When D2O is partially dissociated on the MgO surface, D2 can only dissociate at the remaining active sites until that dissociated -ODw groups from D2O occupy all active sites. These findings provide a fundamental understanding of the effect of water adsorption on D2 activation on oxide catalysts.

Keywords: MgO, hydride, hydroxyl, H2O, H2 activation

References(48)

[1]

Larese, J. Z.; Arnold, T.; Frazier, L.; Hinde, R. J.; Ramirez-Cuesta, A. J. Direct observation of H2 binding to a metal oxide surface. Phys. Rev. Lett. 2008, 101, 165302.
DOI Google Scholar
[2]

Rodriguez, J. A.; Hanson, J. C.; Frenkel, A. I.; Kim, J. Y.; Pérez, M. Experimental and theoretical studies on the reaction of H2 with NiO: Role of O vacancies and mechanism for oxide reduction. J. Am. Chem. Soc. 2002, 124, 346–354.
DOI Google Scholar
[3]

Chen, H. Y. T.; Giordano, L.; Pacchioni, G. From heterolytic to homolytic H2 dissociation on nanostructured MgO(001) films as a function of the metal support. J. Phys. Chem. C 2013, 117, 10623–10629.
DOI Google Scholar
[4]

Henderson, M. A.; Dahal, A.; Dohnálek, Z.; Lyubinetsky, I. Strong temperature dependence in the reactivity of H2 on RuO2(110). J. Phys. Chem. Lett. 2016, 7, 2967–2970.
DOI Google Scholar
[5]

Li, Z. R.; Werner, K.; Qian, K.; You, R.; Płucienik, A.; Jia, A. P.; Wu, L. H.; Zhang, L. Y.; Pan, H. B.; Kuhlenbeck, H. et al. Oxidation of reduced ceria by incorporation of hydrogen. Angew. Chem., Int. Ed. 2019, 58, 14686–14693.
DOI Google Scholar
[6]

Wang, Y. K.; Zhang, Q. Y.; Lin, Y. W.; Huang, W. J.; Ding, D.; Zheng, Y. P.; Chen, M. S.; Wan, H. L. Insight into the high efficiency of Cu/CeO2(110) catalysts for preferential oxidation of CO from hydrogen rich fuel. Appl. Surf. Sci. 2021, 566, 150707.
DOI Google Scholar
[7]

Copéret, C.; Estes, D. P.; Larmier, K.; Searles, K. Isolated surface hydrides: Formation, structure, and reactivity. Chem. Rev. 2016, 116, 8463–8505.
DOI Google Scholar
[8]

Tsuneoka, H.; Teramura, K.; Shishido, T.; Tanaka, T. Adsorbed species of CO2 and H2 on Ga2O3 for the photocatalytic reduction of CO2. J. Phys. Chem. C 2010, 114, 8892–8898.
DOI Google Scholar
[9]

Wang, G. W.; Hattori, H.; Itoh, H.; Tanabe, K. The formation of adsorbed formaldehyde by the reaction of adsorbed carbon monoxide with hydrogen on magnesium oxide. J. Chem. Soc., Chem. Commun. 1982, 1256–1257.
DOI Google Scholar
[10]

Noto, N.; Isobe, S.; Hashimoto, N. Dehydrogenation properties of hydride-hydroxide systems containing potassium. Int. J. Energy Res. 2021, 45, 18237–18244.
DOI Google Scholar
[11]

Ling, Y. J.; Ran, Y. H.; Shao, W. P.; Li, N.; Jiao, F.; Pan, X. L.; Fu, Q.; Liu, Z.; Yang, F.; Bao, X. H. Probing active species for CO hydrogenation over ZnCr2O4 catalysts. Chin. J. Catal. 2022, 43, 2017–2025.
DOI Google Scholar
[12]

Yang, C. S.; Mu, R. T.; Wang, G. S.; Song, J. M.; Tian, H.; Zhao, Z. J.; Gong, J. L. Hydroxyl-mediated ethanol selectivity of CO2 hydrogenation. Chem. Sci. 2019, 10, 3161–3167.
DOI Google Scholar
[13]

Gao, J.; Teplyakov, A. V. Surface species formed during thermal transformation of ethanol on ZnO powder. J. Catal. 2013, 300, 163–173.
DOI Google Scholar
[14]

Asthana, S.; Samanta, C.; Bhaumik, A.; Banerjee, B.; Voolapalli, R. K.; Saha, B. Direct synthesis of dimethyl ether from syngas over Cu-based catalysts: Enhanced selectivity in the presence of MgO. J. Catal. 2016, 334, 89–101.
DOI Google Scholar
[15]

Yang, M.; Papp, H. CO2 reforming of methane to syngas over highly active and stable Pt/MgO catalysts. Catal. Today 2006, 115, 199–204.
DOI Google Scholar
[16]

Pilarska, A. A.; Klapiszewski, Ł.; Jesionowski, T. Recent development in the synthesis, modification and application of Mg(OH)2 and MgO: A review. Powder Technol. 2017, 319, 373–407.
DOI Google Scholar
[17]

Jafarbegloo, M.; Tarlani, A.; Mesbah, A. W.; Muzart, J.; Sahebdelfar, S. NiO-MgO solid solution prepared by sol-gel method as precursor for Ni/MgO methane dry reforming catalyst: Effect of calcination temperature on catalytic performance. Catal. Lett. 2016, 146, 238–248.
DOI Google Scholar
[18]

Song, Y. D.; Ozdemir, E.; Ramesh, S.; Adishev, A.; Subramanian, S.; Harale, A.; Albuali, M.; Fadhel, B. A.; Jamal, A.; Moon, D. et al. Dry reforming of methane by stable Ni-Mo nanocatalysts on single-crystalline MgO. Science 2020, 367, 777–781.
DOI Google Scholar
[19]

Zeng, F.; Zhang, J.; Xu, R.; Zhang, R. J.; Ge, J. P. Highly dispersed Ni/MgO-mSiO2 catalysts with excellent activity and stability for dry reforming of methane. Nano Res. 2022, 15, 5004–5013.
DOI Google Scholar
[20]

Liao, Q. L.; Liang, M. Y.; Zhang, Z.; Zhang, G. J.; Zhang, Y. Strain-modulation and service behavior of Au-MgO-ZnO ultraviolet photodetector by piezo-phototronic effect. Nano Res. 2015, 8, 3772–3779.
DOI Google Scholar
[21]

Prins, R. Hydrogen spillover. Facts and fiction. Chem. Rev. 2012, 112, 2714–2738.
DOI Google Scholar
[22]

Ealet, B.; Goniakowski, J.; Finocchi, F. Water dissociation on a defective MgO(100) surface: Role of divacancies. Phys. Rev. B 2004, 69, 195413.
DOI Google Scholar
[23]

Hawkins, S.; Kumi, G.; Malyk, S.; Reisler, H.; Wittig, C. Temperature programmed desorption and infrared spectroscopic studies of thin water films on MgO(100). Chem. Phys. Lett. 2005, 404, 19–24.
DOI Google Scholar
[24]

Gribov, E. N.; Bertarione, S.; Scarano, D.; Lamberti, C.; Spoto, G.; Zecchina, A. Vibrational and thermodynamic properties of H2 adsorbed on MgO in the 300−20 K interval. J. Phys. Chem. B 2004, 108, 16174–16186.
DOI Google Scholar
[25]

Knözinger, E.; Jacob, K. H.; Hofmann, P. Adsorption of hydrogen on highly dispersed MgO. J. Chem. Soc., Faraday Trans. 1993, 89, 1101–1107.
DOI Google Scholar
[26]

Cavalleri, M.; Pelmenschikov, A.; Morosi, G.; Gamba, A.; Coluccia, S.; Martra, G. Dissociative adsorption of H2 on defect sites of MgO: A combined IR spectroscopic and quantum chemical study. Stud. Surf. Sci. Catal. 2001, 140, 131–139.
DOI Google Scholar
[27]

Cao, S. F.; Zhao, Y. Y.; Lee, S.; Yang, S.; Liu, J. L.; Giannakakis, G.; Li, M. W.; Ouyang, M. Y.; Wang, D. W.; Sykes, E. C. H. et al. High-loading single Pt atom sites [Pt-O(OH)x] catalyze the CO PROX reaction with high activity and selectivity at mild conditions. Sci. Adv. 2020, 6, eaba3809.
DOI Google Scholar
[28]

Nie, L.; Mei, D. H.; Xiong, H. F.; Peng, B.; Ren, Z. B.; Hernandez, X. I. P.; DeLaRiva, A.; Wang, M.; Engelhard, M. H.; Kovarik, L. et al. Activation of surface lattice oxygen in single-atom Pt/CeO2 for low-temperature CO oxidation. Science 2017, 358, 1419–1423.
DOI Google Scholar
[29]

Huang, Z. G.; Liu, Z. Y.; Zhang, X. L.; Liu, Q. Y. Inhibition effect of H2O on V2O5/AC catalyst for catalytic reduction of NO with NH3 at low temperature. Appl. Catal. B: Environ. 2006, 63, 260–265.
DOI Google Scholar
[30]

Saavedra, J.; Doan, H. A.; Pursell, C. J.; Grabow, L. C.; Chandler, B. D. The critical role of water at the gold-titania interface in catalytic CO oxidation. Science 2014, 345, 1599–1602.
DOI Google Scholar
[31]

Chen, B. H.; Ma, Y. S.; Ding, L. B.; Xu, L. S.; Wu, Z. F.; Yuan, Q.; Huang, W. X. Reactivity of hydroxyls and water on a CeO2(111) thin film surface: The role of oxygen vacancy. J. Phys. Chem. C 2013, 117, 5800–5810.
DOI Google Scholar
[32]

Yu, X.; Schwarz, P.; Nefedov, A.; Meyer, B.; Wang, Y.; Woll, C. Structural evolution of water on ZnO(1010): From isolated monomers via anisotropic H-bonded 2D and 3D structures to isotropic multilayers. Angew. Chem., Int. Ed. 2019, 58, 17751–17757.
DOI Google Scholar
[33]

Kenney, M. J.; Huang, J. E.; Zhu, Y.; Meng, Y. T.; Xu, M. Q.; Zhu, G. Z.; Hung, W. H.; Kuang, Y.; Lin, M. C.; Sun, X. M. et al. An electrodeposition approach to metal/metal oxide heterostructures for active hydrogen evolution catalysts in near-neutral electrolytes. Nano Res. 2019, 12, 1431–1435.
DOI Google Scholar
[34]

Ebbesen, S. D.; Mojet, B. L.; Lefferts, L. In situ ATR-IR study of CO adsorption and oxidation over Pt/Al2O3 in gas and aqueous phase: Promotion effects by water and pH. J. Catal. 2007, 246, 66–73.
DOI Google Scholar
[35]

Bahmanpour, A. M.; Hoadley, A.; Tanksale, A. Formaldehyde production via hydrogenation of carbon monoxide in the aqueous phase. Green Chem. 2015, 17, 3500–3507.
DOI Google Scholar
[36]

Heidberg, J.; Redlich, B.; Wetter, D. Adsorption of water vapor on the MgO(100) single crystal surface. Ber. Bunsenges. Phys. Chem. 1995, 99, 1333–1337.
DOI Google Scholar
[37]

Mu, R. T.; Zhao, Z. J.; Dohnálek, Z.; Gong, J. L. Structural motifs of water on metal oxide surfaces. Chem. Soc. Rev. 2017, 46, 1785–1806.
DOI Google Scholar
[38]

Dong, A. Y.; Lin, L.; Mu, R. T.; Li, R. T.; Li, K.; Wang, C.; Cao, Y. J.; Ling, Y. J.; Chen, Y. X.; Yang, F. et al. Modulating the formation and evolution of surface hydrogen species on ZnO through Cr addition. ACS Catal. 2022, 12, 6255–6264.
DOI Google Scholar
[39]

Liu, P. X.; Abdala, P. M.; Goubert, G.; Willinger, M. G.; Coperet, C. Ultrathin single crystalline MgO(111) nanosheets. Angew. Chem., Int. Ed. 2021, 60, 3254–3260.
DOI Google Scholar
[40]

Li, H. J.; Li, M. J.; Wang, X. F.; Wu, X. G.; Liu, F. D.; Yang, B. H. Synthesis and optical properties of single-crystal MgO nanobelts. Mater. Lett. 2013, 102–103, 80–82.
DOI Google Scholar
[41]

Coluccia, S.; Boccuzzi, F.; Ghiotti, G.; Mirra, C. Evidence for heterolytic dissociation of H2 on the surface of thermally activated MgO powders. Z. Phys. Chem. 1980, 121, 141–143.
DOI Google Scholar
[42]

Noei, H.; Qiu, H. S.; Wang, Y. M.; Muhler, M.; Woll, C. Hydrogen loading of oxide powder particles: A transmission IR study for the case of zinc oxide. ChemPhysChem 2010, 11, 3604–3607.
DOI Google Scholar
[43]

Shi, H.; Yuan, H.; Li, Z.; Wang, W. Y.; Li, Z. Y.; Shao, X. Low-temperature heterolytic adsorption of H2 on ZnO(101̅0) surface. J. Phys. Chem. C 2019, 123, 13283–13287.
DOI Google Scholar
[44]

Liu, P. X.; Zhao, Y.; Qin, R. X.; Mo, S. G.; Chen, G. X.; Gu, L.; Chevrier, D. M.; Zhang, P.; Guo, Q.; Zang, D. D. et al. Photochemical route for synthesizing atomically dispersed palladium catalysts. Science 2016, 352, 797–800.
DOI Google Scholar
[45]

Qin, R. X.; Zhou, L. Y.; Liu, P. X.; Gong, Y.; Liu, K. L.; Xu, C. F.; Zhao, Y.; Gu, L.; Fu, G.; Zheng, N. F. Alkali ions secure hydrides for catalytic hydrogenation. Nat. Catal. 2020, 3, 703–709.
DOI Google Scholar
[46]

Fester, J.; García-Melchor, M.; Walton, A. S.; Bajdich, M.; Li, Z.; Lammich, L.; Vojvodic, A.; Lauritsen, J. V. Edge reactivity and water-assisted dissociation on cobalt oxide nanoislands. Nat. Commun. 2017, 8, 14169.
DOI Google Scholar
[47]

Zhao, S.; Chen, F.; Duan, S. B.; Shao, B.; Li, T. B.; Tang, H. L.; Lin, Q. Q.; Zhang, J. Y.; Li, L.; Huang, J. H. et al. Remarkable active-site dependent H2O promoting effect in CO oxidation. Nat. Commun. 2019, 10, 3824.
DOI Google Scholar
[48]

Saavedra, J.; Whittaker, T.; Chen, Z. F.; Pursell, C. J.; Rioux, R. M.; Chandler, B. D. Controlling activity and selectivity using water in the Au-catalysed preferential oxidation of CO in H2. Nat. Chem. 2016, 8, 584–589.
DOI Google Scholar
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Publication history
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Acknowledgements

Publication history

Received: 27 January 2023
Revised: 09 March 2023
Accepted: 22 March 2023
Published: 18 May 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was financially supported by the National Key R&D Program of China (Nos. 2021YFA1502800, 2022YFA1504800 and 2022YFA1504500), and the National Natural Science Foundation of China (Nos. 91945302, 22272162, 22288201 and 21825203).

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