Siliceous mesocellular foam supported Cu catalysts for promoting non-thermal plasma activated CO<sub>2</sub> hydrogenation toward methanol synthesis

doi:10.1007/s11705-024-2419-z

2024, Vol. 18

Issue (7) : 77 https://doi.org/10.1007/s11705-024-2419-z

Siliceous mesocellular foam supported Cu catalysts for promoting non-thermal plasma activated CO₂ hydrogenation toward methanol synthesis

Yi Chen¹, Shaowei Chen¹, Yan Shao², Cui Quan³, Ningbo Gao³, Xiaolei Fan^4,^5,⁶(

), Huanhao Chen¹(

)

¹. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
². School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 211816, China
³. School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China
⁴. Department of Chemical Engineering, School of Engineering, The University of Manchester, Manchester M139PL, UK
⁵. Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute, University of Nottingham Ningbo China, Ningbo 315048, China
⁶. Institute of Wenzhou, Zhejiang University, Wenzhou 325006, China

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Abstract

Electrified non-thermal plasma (NTP) catalytic hydrogenation is the promising alternative to the thermal counterparts, being able to be operated under mild conditions and compatible with green electricity/hydrogen. Rational design of the catalysts for such NTP-catalytic systems is one of the keys to improve the process efficiency. Here, we present the development of siliceous mesocellular foam (MCF) supported Cu catalysts for NTP-catalytic CO₂ hydrogenation to methanol. The findings show that the pristine MCF support with high specific surface area and large mesopore of 784 m²·g⁻¹ and ~8.5 nm could promote the plasma discharging and the diffusion of species through its framework, outperforming other control porous materials (viz., silicalite-1, SiO₂, and SBA-15). Compared to the NTP system employing the bare MCF, the inclusion of Cu and Zn in MCF (i.e., Cu₁Zn₁/MCF) promoted the methanol formation of the NTP-catalytic system with a higher space-time yield of methanol at ~275 μmol·g_cat⁻¹·h⁻¹ and a lower energy consumption of 26.4 kJ· $m m o l C H 3 O H$ ⁻¹ (conversely, ~225 μmol·g_cat⁻¹·h⁻¹ and ~71 kJ· $m m o l C H 3 O H$ ⁻¹, respectively, for the bare MCF system at 10.1 kV). The findings suggest that inclusion of active metal sites (especially Zn species) could stabilize the CO₂/CO-related intermediates to facilitate the surface reaction toward methanol formation.

Keywords non-thermal plasma (NTP) catalysis Cu catalyst CO₂ hydrogenation methanol siliceous mesocellular foam (MCF)

Corresponding Author(s): Xiaolei Fan,Huanhao Chen

Just Accepted Date: 07 March 2024 Issue Date: 24 April 2024

Cite this article:

Yi Chen,Shaowei Chen,Yan Shao, et al. Siliceous mesocellular foam supported Cu catalysts for promoting non-thermal plasma activated CO₂ hydrogenation toward methanol synthesis[J]. Front. Chem. Sci. Eng., 2024, 18(7): 77.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2419-z
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I7/77

Fig.1 HAADF images, particle size distribution, and HRTEM micrographs of (a–c) Cu₁/MCF and (d–f) Cu₁Zn₁/MCF.

Fig.2 (a) H₂-TPR, (b) CO₂-TPD, and (c) CO-TPD profiles of Cu₁/MCF and Cu₁Zn₁/MCF.

Tab.1 Textural properties of the materials and catalysts under study

Fig.3 N₂ adsorption/desorption isotherms and pore size distribution curves of different samples: (a, a') MCF, (b, b') Cu₁/MCF, and (c, c') Cu₁Zn₁/MCF.

Fig.4 NTP-assisted CO₂ hydrogenation performance (regarding CO₂ conversion and methanol STY) of the NTP-alone system (noted that the unit of methanol STY for this system is μmol·h^?1), NTP systems with the inert packing and NTP-catalytic systems with the Cu_x/MCF and Cu₁Zn₁/MCF catalysts. (Experimental conditions: feed gas composition = 60 vol % H₂/20 vol % CO₂/20 vol % Ar, total flow rate = 50 mL·min^?1, applied peak voltage = 10.1 ± 0.4 kV, frequency = 7.7 kHz, discharge power = 20.9 ± 1.3 W)

Fig.5 (a) Longevity test of the NTP-catalytic CO₂ hydrogenation systems over the Cu₁/MCF and Cu₁Zn₁/MCF catalysts (regarding CO₂ conversion and methanol STY), (b) energy consumption of methanol formation over MCF, Cu₁/MCF and Cu₁Zn₁/MCF. (Experimental conditions: feed gas composition = 60 vol% H₂/20 vol% CO₂/20 vol% Ar, total flow rate = 50 mL·min^?1, applied peak voltage = 10.1 ± 0.4 kV, frequency = 7.7 kHz, input power = 20.9 ± 1.3 W)

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