电催化氮集成二氧化碳还原反应合成有机氮化合物

doi:10.3866/PKU.WHXB202307049

Abstract

Abstract:

The social development model relying on coal, oil, natural gas, and other fossil fuels as the primary energy sources has not only hastened the depletion of non-renewable resources but also led to a continuous increase in atmospheric CO₂ concentration. As human society's understanding of energy structures deepens and environmental consciousness grows, the pursuit of effective clean CO₂ capture and catalytic conversion technologies has become a research priority. This is essential for promoting adjustments to the energy mix and achieving global carbon neutrality through artificial carbon cycling. Among the various CO₂ capture and catalytic conversion technologies, electrochemical catalytic CO₂ reduction (CO₂RR) at ambient temperature and pressure holds promise for advancing artificial carbon cycling, carbon storage, and mitigating environmental degradation. This technology can be driven by intermittent renewable energy sources such as solar energy, wind energy, tidal power, geothermal energy, etc. Furthermore, using water as a clean proton source, a wide array of chemicals can be synthesized. While recent studies have made significant progress in CO₂RR within aqueous solutions, there remains untapped potential in generating other important small organic molecules like urea, amides, amines, derivatives, and even amino acids. These compounds are of great interest due to their widespread applications in fertilizers, chemical synthesis, pharmaceuticals, and the aerospace industry. The electrocatalytic synthesis of organonitrogen compounds through N-integrated CO₂RR (NCR) is considered crucial for improving the practical applications and offering a reference for biological small molecules. However, NCR involves multi-step electron and proton transfer processes, leading to current challenges, including slow kinetics and a complex reaction mechanism. In this review, we delve into the detailed reaction pathways and the rational design of catalysts for different NCR products, which are vital for developing highly efficient electrocatalysts. Although some progress has been made through various strategies, there are still challenges to overcome, limiting their large-scale practical applications. The discussion concludes by addressing these existing limitations and outlining potential avenues for future improvements. We hope that this feature article will be instrumental in the development of novel electrocatalysts for NCR.

Key words: CO₂ reduction reaction, Nitrogenous species, Organonitrogen compound, Electrocatalysis, C-N coupling

Yan Kong, Wei Wei, Lekai Xu, Chen Chen. Electrochemical Synthesis of Organonitrogen Compounds from N-integrated CO₂ Reduction Reaction[J]. Acta Phys. -Chim. Sin. 2024, 40(8), 2307049. doi: 10.3866/PKU.WHXB202307049

Figures/Tables 10

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Catalyst	Electrolyte	Product	FE	Formation rate	Ref.
Bi-BiVO₄	0.1 mol∙L⁻¹ KHCO₃	urea	12.55%	5.91 mmol∙h⁻¹∙g⁻¹	34
Cu-Bi	0.1 mol∙L⁻¹ KHCO₃	urea	8.70% ± 1.70%	0.45 ± 0.06 mg∙L⁻¹	39
Cu single atoms/graphene sheets	0.1 mol∙L⁻¹ KHCO₃ + 0.1 mol∙L⁻¹ KNO₃	urea	28.00%	1800 μg∙h⁻¹∙mg⁻¹	56
Fe-Ni single atoms	0.1 mol∙L⁻¹ KHCO₃ + 50 mmol∙L⁻¹ KNO₃	urea	17.80%	20.2 mmol∙h⁻¹∙g⁻¹	57
Fe(amorphous)@C-Fe₃O₄/CNTs	0.1 mol∙L⁻¹ KNO₃	urea	16.50% ± 6.10%	1341.3 ± 112.6 μg∙h⁻¹∙mg⁻¹	61
F-rich CNTs	0.1 mol∙L⁻¹ KNO₃	urea	18%	6.36 mmol∙h⁻¹∙g⁻¹	63
Cu@Zn nanowires	0.1 mol∙L⁻¹ KNO₃ + 0.2 mol∙L⁻¹ KHCO₃	urea	9.28%	7.29 μmol∙cm⁻²∙h⁻¹	65
Co-NiO_x@graphdiyne	0.01 mol∙L⁻¹ NaNO₂	urea	64.30%	913.2 μg∙h⁻¹∙mg⁻¹	67
Co-PMDA-2-mbIM	0.1 mol∙L⁻¹ KHCO₃	urea	48.97%	14.47 mmol∙h⁻¹∙g⁻¹	68
AuCu nanofibers	0.01 mol∙L⁻¹ NaNO₂	urea	24.70%	3.889 μg∙h⁻¹∙mg⁻¹	72
Zn nanobelts	0.2 mol∙L⁻¹ KHCO₃	urea	11.26%	15.13 mmol∙h⁻¹∙g⁻¹	73
In(OH)₃	0.1 mol∙L⁻¹ KNO₃	urea	53.40%	533.1 mg∙h⁻¹∙mg⁻¹	39
InOOH	0.1 mol∙L⁻¹ KHCO₃	urea	51.00%	592.5 μg∙h⁻¹∙mg⁻¹	77
CeO₂	0.1 mol∙L⁻¹ KHCO₃ + 50 mmol∙L⁻¹ KNO₃	urea	–	943.6 μg∙h⁻¹∙mg⁻¹	78
Cu/CuO	1 mol∙L⁻¹ KOH	acetamide + formamide	10% acetamide 0.4% formamide	2.2 mA∙cm⁻² acetamide 0.2 mA∙cm⁻² formamide	25
CoPc-NH₂	0.1 mol∙L⁻¹ KHCO₃	methylamine	13%	3.4 mA∙cm⁻²	35
Oxide-derived Cu	1 mol∙L⁻¹ KHCO₃	Ethylamine	0.30%	–	46

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Electrochemical Synthesis of Organonitrogen Compounds from N-integrated CO₂ Reduction Reaction

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Electrochemical Synthesis of Organonitrogen Compounds from N-integrated CO2 Reduction Reaction

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Electrochemical Synthesis of Organonitrogen Compounds from N-integrated CO₂ Reduction Reaction