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Construction of C–N bonds from small-molecule precursors through heterogeneous electrocatalysis
Nature Reviews Chemistry ( IF 36.3 ) Pub Date : 2022-04-25 , DOI: 10.1038/s41570-022-00379-5
Junnan Li 1 , Yuxuan Zhang 1 , Kiran Kuruvinashetti 1 , Nikolay Kornienko 1
Affiliation  

Energy-intensive thermochemical processes within chemical manufacturing are a major contributor to global CO2 emissions. With the increasing push for sustainability, the scientific community is striving to develop renewable energy-powered electrochemical technologies in lieu of CO2-emitting fossil-fuel-driven methods. However, to fully electrify chemical manufacturing, it is imperative to expand the scope of electrosynthetic technologies, particularly through the innovation of reactions involving nitrogen-based reactants. This Review focuses on a rapidly emerging area, namely the formation of C–N bonds through heterogeneous electrocatalysis. The C–N bond motif is found in many fertilizers (such as urea) as well as commodity and fine chemicals (with functional groups such as amines and amides). The ability to generate C–N bonds from reactants such as CO2, NO3 or N2 would provide sustainable alternatives to the thermochemical routes used at present. We start by examining thermochemical, enzymatic and molecular catalytic systems for C–N bond formation, identifying how concepts from these can be translated to heterogeneous electrocatalysis. Next, we discuss successful heterogeneous electrocatalytic systems and highlight promising research directions. Finally, we discuss the remaining questions and knowledge gaps and thus set the trajectory for future advances in heterogeneous electrocatalytic formation of C–N bonds.



中文翻译:

通过多相电催化从小分子前体构建 C-N 键

化学制造中的能源密集型热化学过程是全球 CO 2排放的主要来源。随着对可持续发展的日益推动,科学界正在努力开发可再生能源驱动的电化学技术来代替 CO 2-排放化石燃料驱动的方法。然而,要使化学制造完全电气化,就必须扩大电合成技术的范围,特别是通过涉及氮基反应物的反应创新。本综述侧重于一个快速兴起的领域,即通过多相电催化形成 C-N 键。C-N 键基序存在于许多肥料(如尿素)以及商品和精细化学品(具有胺和酰胺等官能团)中。从反应物如 CO 2、NO 3 或 N 2生成 C-N 键的能力将为目前使用的热化学路线提供可持续的替代品。我们首先检查 C-N 键形成的热化学、酶促和分子催化系统,确定如何将这些概念转化为多相电催化。接下来,我们讨论成功的多相电催化系统并强调有前途的研究方向。最后,我们讨论了剩余的问题和知识差距,从而为 C-N 键的多相电催化形成的未来发展设定了轨迹。

更新日期:2022-04-26
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