Abstract
CO2 hydrogenation to methanol is attracting specific interest because of its potential economic and environmental benefits in transforming waste CO2 to value-added hydrocarbons. Copper-based catalysts are documented as efficient and widely applied, whereas insufficient catalytic properties of conventional catalysts hinder their application. Herein, catalysts using Mg-Al hydrotalcite (HT) as the carrier of Cu/ZnO/ZrO2 (CZZ) nanoparticles were prepared to exploit special advantages of hydrotalcite on copper dispersion and catalytic performance. The results show that CZZ nanoparticles can be uniformly dispersed on external surfaces of HT, elevating BET surface areas of CZZ-HT samples by at least 2.5 times compared to pure CZZ. The HT carrier also enriches strong basic sites and hence elevates CO2 adsorption capabilities in the range of reaction temperature. Both copper surface area and copper dispersion of CZZ-HT samples are improved dramatically. A catalyst containing 45.1 wt% of CZZ shows 1.1 times higher copper surface area per gram CZZ and 1.6 times higher copper dispersion than the reference CZZ. Subsequent reactions demonstrate the CZZ-HT samples show remarkably promoted turnover frequency (TOF) for methanol synthesis and retain considerable catalyst stability. The typical catalyst prepared in this research, at the reaction temperature of 523 K and pressure of 3.0 MPa, presents a 68.2% higher methanol STYCu per gram copper and an 117.0% higher SMeOH/SCO ratio than the commercial catalyst. The support HT plays a crucial role for the enhanced catalytic performance physically and chemically. Thus, the as-prepared CZZ-HT catalyst provides a significant improvement for CO2 utilization.
Similar content being viewed by others
References
G. A. Olah, A. Goeppert and G. K. S. Prakash, J. Org. Chem., 74, 487 (2009).
A. Goeppert, M. Czaun, J.-P. Jones, G. K Surya Prakash and G. A. Olah, Chem. Soc. Rev., 43, 7995 (2014).
S. Kar, J. Kothandaraman, A. Goeppert and G. K. S. Prakash, J. CO2Util., 23, 212 (2018).
F. Frusteri, M. Migliori, C. Cannilla, L. Frusteri, E. Catizzone, A. Aloise, G. Giordano and G. Bonura, J. CO2Util., 18, 353 (2017).
F. Jiao, J. Li, X. Pan, J. Xiao, H. Li, H. Ma, M. Wei, Y. Pan, Z. Zhou, M. Li, S. Miao, J. Li, Y. Zhu, D. Xiao, T. He, J. Yang, F. Qi, Q. Fu and X. Bao, Science, 351, 1065 (2016).
Z. Wan, W. Wu, G. (Kevin) Li, C. Wang, H. Yang and D. Zhang, Appl. Catal. A Gen., 523, 312 (2016).
J. M. Thomas and K. D. M. Harris, Energy Environ. Sci., 9, 687 (2016).
M. Kong, Z. Liu, T. Vogt and Y. Lee, Micropor. Mesopor. Mater., 221, 253 (2016).
Y. Men, X. Fang, Q. Gu, R. Singh, F. Wu, D. Danaci, Q. Zhao, P. Xiao and P. A. Webley, Appl. Catal. B Environ., 275, 119067 (2020).
F. Studt, I. Sharafutdinov, F. Abild-Pedersen, C. F. Elkjær, J. S. Hummelshøj, S. Dahl, I. Chorkendorff and J. K. Nørskov, Nat. Chem., 6, 320 (2014).
N. Rui, Z. Wang, K. Sun, J. Ye, Q. Ge and C. Liu, Appl. Catal. B Environ., 218, 488 (2017).
X. Yang, S. Kattel, S. D. Senanayake, J. A. Boscoboinik, X. Nie, J. Graciani, J. A. Rodriguez, P. Liu, D. J. Stacchiola and J. G. Chen, J. Am. Chem. Soc., 137, 10104 (2015).
S. Kattel, P. J. Ramírez, J. G. Chen, J. A. Rodriguez and P. Liu, Science, 355, 1296 (2017).
J. Schumann, T. Lunkenbein, A. Tarasov, N. Thomas, R. Schlögl and M. Behrens, ChemCatChem, 6, 2889 (2014).
G. Bonura, M. Cordaro, C. Cannilla, F. Arena and F. Frusteri, Appl. Catal. B Environ., 152, 152 (2014).
M. K. Koh, Y. J. Wong, S. P. Chai and A. R. Mohamed, J. Ind. Eng. Chem., 62, 156 (2018).
B. Hu, Y. Yin, G. Liu, S. Chen, X. Hong and S. C. E. Tsang, J. Catal., 359, 17 (2018).
J. Xiao, D. Mao, X. Guo and J. Yu, Appl. Surf. Sci., 338, 146 (2015).
M. Tamura, T. Kitanaka, Y. Nakagawa and K. Tomishige, ACS Catal., 6, 376 (2016).
X. An, J. Li, Y. Zuo, Q. Zhang, D. Wang and J. Wang, Catal. Lett., 118, 264 (2007).
L. Liu and A. Corma, Chem. Rev., 118, 4981 (2018).
M. B. Boucher, B. Zugic, G. Cladaras, J. Kammert, M. D. Marcinkowski, T. J. Lawton, E. C. H. Sykes and M. Flytzani-Stephanopoulos, Phys. Chem. Chem. Phys., 15, 12187 (2013).
X. Guo, G. Fang, G. Li, H. Ma, H. Fan, L. Yu, C. Ma, X. Wu, D. Deng, M. Wei, D. Tan, R. Si, S. Zhang, J. Li, L. Sun, Z. Tang, X. Pan and X. Bao, Science, 344, 616 (2014).
M. M.-J. Li, C. Chen, T. Ayvali, H. Suo, J. Zheng, I. Teixeira, L. Ye, H. Zou, D. O’Hare and S. C. E. Tsang, ACS Catal., 8, 4390 (2018).
C. Jeong and Y. W. Suh, Catal. Today, 265, 254 (2016).
Z. Y. Ma, C. Yang, W. Wei, W. H. Li and Y. H. Sun, J. Mol. Catal. A Chem., 231, 75 (2005).
N. J. Venkatesha and S. Ramesh, Ind. Eng. Chem. Res., 57, 1506 (2018).
S. Abelló, F. Medina, D. Tichit, J. Pérez-Ramírez, J. C. Groen, J. E. Sueiras, P. Salagre and Y Cesteros, Chem. — A Eur. J., 11, 728 (2005).
O. Aschenbrenner, P. McGuire, S. Alsamaq, J. Wang, S. Supasitmongkol, B. Al-Duri, P. Styring and J. Wood, Chem. Eng. Res. Des., 89, 1711 (2011).
N. D. Hutson, S. A. Speakman and E. A. Payzant, Chem. Mater., 16, 4135 (2004).
X. Fang, Y. Men, F. Wu, Q. Zhao, R. Singh, P. Xiao, T. Du and P. A. Webley, J. CO2Util., 29, 57 (2019).
S. Saha and S. B. Abd Hamid, RSC Adv., 7, 9914 (2017).
Y. Zhang, C. Chen, X. Lin, D. Li, X. Chen, Y. Zhan and Q. Zheng, Int. J. Hydrogen Energy, 39, 3746 (2014).
X. Guo, D. Mao, G. Lu, S. Wang and G. Wu, Catal. Commun., 12, 1095 (2011).
A. Dandekar and M. A. Vannice, J. Catal., 178, 62 (1998).
F. Arena, G. Italiano, K. Barbera, S. Bordiga, G. Bonura, L. Spadaro and F. Frusteri, Appl. Catal. A Gen., 350, 16 (2008).
Y. Hua, X. Guo, D. Mao, G. Lu, G. L. Rempel and F. T. T. Ng, Appl. Catal. A Gen., 540, 68 (2017).
T. Phongamwong, U. Chantaprasertporn, T. Witoon, T. Numpilai, Y. Poo-arporn, W. Limphirat, W. Donphai, P. Dittanet, M. Chareonpanich and J. Limtrakul, Chem. Eng. J., 316, 692 (2017).
X. Dong, F. Li, N. Zhao, F. Xiao, J. Wang and Y. Tan, Appl. Catal. B Environ., 191, 8 (2016).
N. D. Hutson, S. A. Speakman and E. A. Payzant, Chem. Mater., 16, 4135 (2004).
S. Asthana, C. Samanta, A. Bhaumik, B. Banerjee, R. K. Voolapalli and B. Saha, J. Catal., 334, 89 (2016).
J. Y. Kim, J. A. Rodriguez, J. C. Hanson, A. I. Frenkel and P. L. Lee, J. Am. Chem. Soc., 125, 10684 (2003).
T. Witoon, J. Chalorngtham, P. Dumrongbunditkul, M. Chareonpanich and J. Limtrakul, Chem. Eng. J., 293, 327 (2016).
T. Witoon, N. Kachaban, W. Donphai, P. Kidkhunthod, K. Faungnawakij, M. Chareonpanich and J. Limtrakul, Energy Convers. Manag., 118, 21 (2016).
P. Gao, F. Li, H. Zhan, N. Zhao, F. Xiao, W. Wei, L. Zhong and H. Wang, J. Catal., 298, 51 (2013).
N. D. Hutson and B. C. Attwood, Adsorption, 14, 781 (2008).
Z. Yong and A. E. Rodrigues, Energy Convers. Manag., 43, 1865 (2002).
A. G. Sato, D. P. Volanti, D. M. Meira, S. Damyanova, E. Longo and J.M.C. Bueno, J. Catal., 307, 1 (2013).
F. Frusteri, M. Cordaro, C. Cannilla and G. Bonura, Appl. Catal. B Environ., 162, 57 (2015).
S. Patel and K. K. Pant, Chem. Eng. Sci., 62, 5436 (2007).
L. C. Grabow and M. Mavrikakis, ACS Catal., 1, 365 (2011).
X. Guo, D. Mao, G. Lu, S. Wang and G. Wu, J. Mol. Catal. A Chem., 345, 60 (2011).
X.-M. Liu, G. Q. Lu, Z.-F. Yan and J. Beltramini, Ind. Eng. Chem. Res., 42, 6518 (2003).
T. Witoon, T. Numpilai, T. Phongamwong, W. Donphai, C. Boonyuen, C. Warakulwit, M. Chareonpanich and J. Limtrakul, Chem. Eng. J., 334, 1781 (2018).
K. Nishida, I. Atake, D. Li, T. Shishido, Y. Oumi, T. Sano and K. Takehira, Appl. Catal. A Gen., 337, 48 (2008).
Acknowledgements
The authors gratefully acknowledge the financial support of the China Scholarship Council (No. 201606080053), the University of Melbourne and the Natural Science Foundation of Liaoning Province (No. 2020-BS-053). We acknowledge the Monash X-ray Platform (MXP) for XRD measurements and Monash Centre of Electron Microscopy (MCEM) for SEM-EDX analyses. We also acknowledge the Materials Characterisation and Fabrication Platform (MCFP) at the University of Melbourne and the Victorian Node of the Australian National Fabrication Facility (ANFF) for the HIM characterizations.
Author information
Authors and Affiliations
Corresponding authors
Additional information
Supporting Information
Additional information as noted in the text. This information is available via the Internet at u]http://www.springer.com/chemistry/journal/11814.
Electronic supplementary material
11814_2020_736_MOESM1_ESM.pdf
Highly dispersed Cu-ZnO-ZrO2 nanoparticles on hydrotalcite adsorbent as efficient composite catalysts for CO2 hydrogenation to methanol
Rights and permissions
About this article
Cite this article
Fang, X., Men, Y., Wu, F. et al. Highly dispersed Cu-ZnO-ZrO2 nanoparticles on hydrotalcite adsorbent as efficient composite catalysts for CO2 hydrogenation to methanol. Korean J. Chem. Eng. 38, 747–755 (2021). https://doi.org/10.1007/s11814-020-0736-6
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11814-020-0736-6