Selective formaldehyde condensation on phosphorus-rich copper catalyst to produce liquid C3+ chemicals in electrocatalytic CO2 reduction

IF 42.8 1区化学 Q1 CHEMISTRY, PHYSICAL

Nature Catalysis Pub Date : 2025-05-22 DOI:10.1038/s41929-025-01341-6

Minjun Choi, Sooan Bae, Yeongin Kim, Youjin Lee, Mokyeon Cho, Sinwoo Kang, Jaeyoung Lee

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Abstract

Recent advancements in the CO₂ reduction reaction (CO₂RR) target multicarbon chemical production and scalable electrode designs for industrial applications. Here we introduce a zero-gap cell utilizing humidified gas-phase CO₂ and circulated alkaline media, achieving a Faradaic efficiency of 66.9% for C₃₊ products and a current density of −1,100 mA cm⁻². In situ spectroscopic analyses revealed formaldehyde as a key intermediate formed on copper oxide/hydroxide interfaces derived from a phosphorus-rich copper catalyst. Unlike conventional pathways based on dimerization of CO intermediates, our study selectively produces liquid-phase multicarbon products because of autonomous local pH variations under a weak alkaline microenvironment, with allyl alcohol as the dominant C₃₊ product. The high selectivity and efficiency for liquid products provide a substantial advantage for storage and transport, highlighting the scalability and practical feasibility of our approach, which offers a potential economically viable solution for CO₂ utilization. This development encourages the adoption of CO₂RR technologies in iron–steel and petrochemical industries to mitigate greenhouse gas emissions.

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选择性甲醛在富磷铜催化剂上缩合生成液态C3+化学物电催化CO2还原

二氧化碳还原反应（CO2RR）的最新进展是针对工业应用的多碳化学生产和可扩展电极设计。在这里，我们介绍了一种利用加湿气相CO2和循环碱性介质的零间隙电池，C3+产品的法拉第效率为66.9%，电流密度为- 1,100 mA cm - 2。原位光谱分析表明，甲醛是富磷铜催化剂衍生的氧化铜/氢氧化物界面上形成的关键中间体。与基于CO中间体二聚化的传统途径不同，我们的研究选择性地产生液相多碳产物，因为在弱碱性微环境下，局部pH值会自主变化，丙烯醇是主要的C3+产物。液体产品的高选择性和高效率为储存和运输提供了巨大的优势，突出了我们方法的可扩展性和实际可行性，为二氧化碳利用提供了潜在的经济可行的解决方案。这一发展鼓励在钢铁和石化行业采用CO2RR技术，以减少温室气体排放。

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.