Advances in Catalysts for Urea Electrosynthesis Utilizing CO2 and Nitrogenous Materials: A Mechanistic Perspective
Abstract
:1. Introduction
2. Molecular Catalyst Interaction Mechanism Achieving Reactant Targeted Adsorption
2.1. Bimetallic Catalyst
2.1.1. Double Transition-Metal MXenes
2.1.2. Pd–Cu Bimetallic Catalyst
2.2. Heterogeneous Interface-Rich Catalysts
2.2.1. Perovskite Hybrids BiFeO3/BiVO4
2.2.2. Mott–Schottky Heterostructure Bi-BiVO4
2.3. Frustrated Lewis Pairs (FLPs)
2.3.1. InOOH Nanoparticles
2.3.2. Flower-Like Ni3(BO3)2 Nanocrystals
3. Mechanism for Breaking Chemical Bonds and Directional Coupling: Achieving C–N Bond Coupling
3.1. Theoretical Prediction of Catalysts
3.1.1. Double Transition-Metal MXenes
3.1.2. Conductive MOF Co–PMDA–2-mbIM (PMDA = pyromellitic dianhydride; 2-mbIM = 2-methyl benzimidazole)
3.2. Defective Catalysts
3.2.1. Oxygen Vacancy-Enriched CeO2
3.2.2. PdCu-TiO2
4. Discussion
- (1)
- Compared to CO2, the adsorption and activation of inert and non-polar N2 molecules is significantly problematic when CO2 and N2 are utilized as the feedstock for urea electrosynthesis. Hence, when designing catalysts, priority should be given to enhancing the catalytic activity of N2. The investigation of nitrogen reduction reactions and electrocatalytic urea synthesis should complement each other.
- (2)
- To obtain more insight into the electrocatalytic process, the advanced in situ operational characterization can contribute to analyzing the chemical and electronic structures of the catalytic sites, as well as the essential intermediates and the critical steps in the catalytic reaction. Theoretical calculations can be applied to optimize the electrocatalytic behavior of the catalyst. Furthermore, in situ operational characterization can uncover the exact conformational relationships of the catalyst by monitoring the structural transformation of the active site during the electrocatalytic process.
- (3)
- Multiphase catalytic processes occur at the two- or three-phase interface, and the adsorption, dissolution and diffusion of intermediates as well as the generated products governed by the composition of the electrodes and membranes take place. Simultaneously, diffusion is dramatically impacted by the structure of the electrode and membrane assembly in the catalyst layer. Fluid dynamics can be controlled by optimizing the equipment structure, e.g., by tweaking the batch flow rate. The specificity of the products of the cascade reaction can be adjusted by controlling the fluid dynamics, including the mass velocity and volume pressure of the gas and liquid phases. Meanwhile, the selectivity of cascade reaction can be modulated by evaluating the device structure. A proper electrocatalytic device design can effectively regulate the product selectivity, stability and energy efficiency of electrocatalytic reactions, representing a robust tool for high-performance devices that can achieve superior urea electrosynthesis performance.
- (4)
- Molecular–catalyst interaction mechanisms as well as chemical bond breakage and directional coupling mechanisms have explained the mechanism of electrocatalytic synthesis of urea from different microscopic perspectives, contributing to solving the difficult problems of adsorption, activation and the coupling of reactant molecules in urea synthesis. Meanwhile, this mechanism could be applied in other directions, such as the molecular catalyst interaction mechanisms in electrocatalytic nitrogen reduction, which could enhance the electrophilicity of catalyst surfaces through the carrier effect and inhibit proton reduction. Similarly, the chemical bond breaking and directional coupling mechanisms enhance the efficiency of ammonia synthesis by accelerating the breaking of chemical bonds through electron feeding. Furthermore, this mechanism will be of considerable interest in other areas.
5. Conclusions
Author Contributions
Funding
Informed Consent Statement
Conflicts of Interest
References
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Catalysts | Synthesis Methods | Faraday Efficiency/Yield Rate |
---|---|---|
MXenes [27] | Theoretical calculations | -- |
Pd–Cu [31] | Wet chemistry impregnation + carbonization fixation process | 69.1 ± 3.8% |
BiFeO3/BiVO4 [13] | Hydrothermal method | 17.18% |
Bi-BiVO4 [8] | Hydrothermal method + NaBH4 reduction | 12.55% |
InOOH [53] | Hydrothermal method + annealing treatment | 20.97% |
Ni3(BO3)2 [6] | Wet chemistry + low-temperature annealing | 20.36% |
Co–PMDA–2-mbIM [65] | Hydrothermal method | 48.97% |
CeO2 [58] | Hydrothermal method + annealing treatment | 943.6 mg h−1 g−1 |
PdCu-TiO2 [4] | High temperature reduction | 8.92% |
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Zhang, M.; Feng, T.; Che, X.; Wang, Y.; Wang, P.; Chai, M.; Yuan, M. Advances in Catalysts for Urea Electrosynthesis Utilizing CO2 and Nitrogenous Materials: A Mechanistic Perspective. Materials 2024, 17, 2142. https://doi.org/10.3390/ma17092142
Zhang M, Feng T, Che X, Wang Y, Wang P, Chai M, Yuan M. Advances in Catalysts for Urea Electrosynthesis Utilizing CO2 and Nitrogenous Materials: A Mechanistic Perspective. Materials. 2024; 17(9):2142. https://doi.org/10.3390/ma17092142
Chicago/Turabian StyleZhang, Mengfei, Tianjian Feng, Xuanming Che, Yuhan Wang, Pengxian Wang, Mao Chai, and Menglei Yuan. 2024. "Advances in Catalysts for Urea Electrosynthesis Utilizing CO2 and Nitrogenous Materials: A Mechanistic Perspective" Materials 17, no. 9: 2142. https://doi.org/10.3390/ma17092142