Catalytic urea hydrolysis by composite metal oxide catalyst towards efficient urea-based SCR process: performance evaluation and mechanism investigation

doi:10.1007/s11783-023-1658-4

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (5) : 58 https://doi.org/10.1007/s11783-023-1658-4

RESEARCH ARTICLE

Catalytic urea hydrolysis by composite metal oxide catalyst towards efficient urea-based SCR process: performance evaluation and mechanism investigation

Yuchen Li¹, Zhen Chen²(

), Xiangyu Zhang³, Kun Yang², Lidong Wang¹(

), Junhua Li²

¹. MOE Key Laboratory of Resources and Environmental Systems Optimization, Department of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China
². State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
³. Xi’an Thermal Power Research Institute Co., Xi’an 710032, China

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Abstract

● Bimetallic oxide composite catalyst was designed for the urea-based SCR process.

● Surface chemical state and typical microstructure of catalyst was determined.

● Reaction route was improved based on intermediates and active site identification.

● TiO₂@Al₂O₃ presents an obvious promotion for urea hydrolysis.

As a promising option to provide gaseous NH₃ for SCR system, catalytic urea hydrolysis has aroused great attention, and improving surface area and activity of catalysis are the crucial issues to be solved for efficient urea hydrolysis. Therefore, a composite metal oxide (TiO₂@Al₂O₃) catalyst was prepared by a simple hydrothermal method, with mesoporous alumina (γ-Al₂O₃) as substrate. The results verify the mesoporous structure and submicron cluster of TiO₂@Al₂O₃, with exposed crystal faces of (101) and (400) for TiO₂ and γ-Al₂O₃, respectively. The electronegativity difference of Ti⁴⁺ and Al³⁺ changes the charge distribution scheme around the interface, which provides abundant acid/base sites to boost the urea hydrolysis. Consequently, for an optimal proportioning with nano TiO₂ content at 10 wt.%, the hydrolysis efficiency can reach up to 35.2 % at 100 °C in 2 h, increasing by ~7.1 % than that of the blank experiment. ¹³C NMR spectrum measurements provide the impossible intermediate species during urea hydrolysis. Theoretical calculations are performed to clarify the efficient H₂O decomposition at the interface of TiO₂@Al₂O₃. The result offers a favorable technology for energy-efficiency urea hydrolysis.

Keywords SCR Urea hydrolysis Catalytic Water dissociation Electronegativity

Corresponding Author(s): Zhen Chen,Lidong Wang

Issue Date: 12 December 2022

Cite this article:

Yuchen Li,Zhen Chen,Xiangyu Zhang, et al. Catalytic urea hydrolysis by composite metal oxide catalyst towards efficient urea-based SCR process: performance evaluation and mechanism investigation[J]. Front. Environ. Sci. Eng., 2023, 17(5): 58.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1658-4
https://academic.hep.com.cn/fese/EN/Y2023/V17/I5/58

Fig.1 Synthetic route of TiO₂@Al₂O₃ by one-pot hydrothermal method.

Fig.2 Experimental evaluation device for catalytic hydrolysis of urea solution (20 wt.%).

Fig.3 XRD patterns of TiO₂ (a), γ-Al₂O₃ (b) and TiO₂@Al₂O₃ (c and d).

Fig.4 TEM (a) and HADDF-STEM (b–d) images of TiO₂@Al₂O₃.

Fig.5 XPS survey spectra (a), Ti 2p (b), Al 2p (c) and O 1s (d) high resolution XPS spectra of TiO₂@Al₂O₃ sample.

Tab.1 Surface properties of the prepared catalyst

Fig.6 N₂ adsorption-desorption isotherm (a) and incremental pore volume (b) of γ-Al₂O₃ and TiO₂@Al₂O₃.

Fig.7 FT-IR spectra of TiO₂, γ-Al₂O₃ and TiO₂@Al₂O₃.

Tab.2 ICP results of TiO₂@Al₂O₃ with different molar ratio

Fig.8 Standard curve of urea solution with different concentration.

Fig.9 Effect of Ti content in TiO₂@Al₂O₃ on urea hydrolysis efficiency (a); the reusability of TiO₂@Al₂O₃ catalyst for urea hydrolysis at 100 °C for 2 h (b).

Fig.10 Effect of reaction temperature on urea hydrolysis efficiency: 90 °C (a) and 100 °C (b).

Fig.11 ¹H NMR spectra (a) and ¹³C NMR spectra (b) for urea solution before and after heating, with or without TiO₂@Al₂O₃ catalyst.

Fig.12 Structural geometries of TiO₂@Al₂O₃ and TiO₂ (a); atomic position of TiO₂@Al₂O₃ from DFT results (b).

Fig.13 Adsorption energy (E_ads) values of H₂O adsorbed on TiO₂@Al₂O₃ and Al₂O₃ from DFT calculation results (a); the energy diagram related to the equilibrium of de-protonation reaction on Tiⁿ⁺ sites (b).

Fig.14 Proposed catalytic mechanism for urea hydrolysis process under the addition of TiO₂@Al₂O₃.

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