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

物理化学学报 >> 2024, Vol. 40 >> Issue (8): 2307049.doi: 10.3866/PKU.WHXB202307049

所属专题：二氧化碳资源化

电催化氮集成二氧化碳还原反应合成有机氮化合物

孔燕†, 危伟†, 徐乐凯, 陈晨*()

清华大学化学系, 先进稀土材料工程研究中心, 北京 100084

收稿日期:2023-07-26 修回日期:2023-09-09 录用日期:2023-09-11 发布日期:2023-09-19
通讯作者: Email: cchen@mail.tsinghua.edu.cn (陈晨)
作者简介:
^†These authors contribute equally to this work.
基金资助:
国家重点研发计划(2021YFF0500503); 国家自然科学基金(21925202); 国家自然科学基金(21872076); 气候变化和碳中和国际联合行动项目

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

Yan Kong, Wei Wei, Lekai Xu, Chen Chen*()

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing 100084, China

Received:2023-07-26 Revised:2023-09-09 Accepted:2023-09-11 Published:2023-09-19
Contact: Email: cchen@mail.tsinghua.edu.cn (Chen Chen)
Supported by:
the National Key R&D Program of China(2021YFF0500503); National Natural Science Foundation of China(21925202); National Natural Science Foundation of China(21872076); International Joint Mission On Climate Change and Carbon Neutrality

摘要/Abstract

摘要：

以化石能源如煤、石油和天然气为主要能源的社会发展模式，不仅导致不可再生资源枯竭，还引发大气中CO₂浓度持续上升的问题。随着人们对能源结构认识的深化和生态环境保护意识的增强，寻求有效的清洁CO₂固定和转化技术已成为研究热点。这些技术可利用太阳能、风能、潮汐能和地热能等可再生能源，促进人工碳循环、碳储存，并缓解环境恶化。在众多CO₂固定和催化转化技术中，常温常压下的CO₂还原技术受到可再生能源的驱动，有助于人工碳循环、碳储存，减轻环境退化。目前，水溶液中的电催化CO₂还原研究已取得显著进展，但在制造其他重要的有机小分子，如尿素、酰胺、胺及其衍生物，甚至氨基酸方面，仍有未开发的潜力。这些产品在肥料、化学品合成、医药化学和航空工业等领域有广泛应用，引起了广泛研究兴趣。通过氮集成的电催化CO₂还原反应制造有机氮化合物，能显著提高CO₂电还原技术的实际应用价值，同时也为生物小分子的起源提供参考，因此具有重要意义。然而，该过程涉及CO₂和含氮无机物的电化学耦合，包含多步电子和质子转移过程，因此面临着缓慢的动力学和复杂的反应机制。在本综述中，我们详细讨论了氮集成电催化CO₂还原生成不同产物的具体反应路径和合理的催化剂设计策略，这对于指导高效电催化剂的设计至关重要。尽管已经通过一系列策略取得了一定的研究进展，但仍然存在一些需要解决的挑战，这限制了它们在大规模实际应用中的发展。最后，我们对该领域的发展限制和改进的可能方向进行了讨论，希望这能有助于氮集成电催化CO₂还原反应催化剂的进一步发展。

关键词: CO₂还原反应, 含氮化合物, 有机氮化合物, 电催化, C-N偶联

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

孔燕, 危伟, 徐乐凯, 陈晨. 电催化氮集成二氧化碳还原反应合成有机氮化合物[J]. 物理化学学报, 2024, 40(8), 2307049. doi: 10.3866/PKU.WHXB202307049

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

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202307049

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I8/2307049

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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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电催化氮集成二氧化碳还原反应合成有机氮化合物

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

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电催化氮集成二氧化碳还原反应合成有机氮化合物

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