Pyridinic-N Dominated Carbon Nanotubes With Varying Nitrogen Content for High-Efficient CO2 Electroreduction to CO

IF 3.2 4区化学 Q3 CHEMISTRY, PHYSICAL

Electrocatalysis Pub Date : 2026-01-03 DOI:10.1007/s12678-025-01003-y

Chao Ju, Mingrui Li, Meng Huang, Teng Luo

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Abstract

The rising demand for energy and environmental concerns necessitate sustainable CO₂ utilization. The electrochemical CO₂ reduction reaction (CO₂RR) has emerged as a promising approach for converting CO₂ into fuels and chemicals. The metal-free carbon materials with nitrogen doping have shown great potential in CO₂RR to produce CO, and pyridinic-N is widely believed to be the responsible active sites. The directed preparation of pyridinic-N dominated carbon and the finely regulation of nitrogen content should be vital for regulating the CO₂RR performance and exploring the catalytic mechanism, which are still challenging. This study developed nitrogen-doped carbon nanotubes (N-CNT) with pyridinic-N domination through pyrolysis of oxidized CNT (OCNT) under ammonia. The nitrogen contents of N-CNT were regulated by adjusting the time for acid-oxidizing treatment, ranging from 5 h to 24 h. N-CNT with oxidizing time of 24 h (N-CNT-24 h) demonstrates the highest nitrogen content and the greatest CO₂RR activity among the samples, with a maximum Faradaic efficiency (FE) of 95% for CO production, maintaining FE of 90% over 11 h of electrolysis. This research provides insights into selectively introducing Pyridinic-N into CNT and examines the effects of nitrogen doping on catalytic performance, contributing to the design of efficient metal-free carbon-based electrochemical catalysts for CO₂ reduction.

Graphical Abstract

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变氮含量吡啶- n主导碳纳米管用于高效CO2电还原CO

日益增长的能源需求和环境问题需要可持续地利用二氧化碳。电化学CO2还原反应（CO2RR）已成为将CO2转化为燃料和化学品的一种很有前途的方法。氮掺杂的无金属碳材料在CO2RR中显示出巨大的产CO潜力，而吡啶- n被广泛认为是负责的活性位点。定向制备吡啶- n主导碳和精细调控氮含量是调控CO2RR性能和探索其催化机理的关键，但仍具有挑战性。本研究通过氧化碳纳米管（OCNT）在氨下热解制备吡啶- n为主的氮掺杂碳纳米管（N-CNT）。通过调整酸氧化处理时间（5 ~ 24 h）来调节N-CNT的氮含量。氧化时间为24 h的N-CNT （N-CNT-24 h）样品的氮含量最高，CO2RR活性最高，CO生成的法拉第效率（FE）最高为95%，在电解11 h后FE保持在90%。本研究为选择性地将吡啶- n引入碳纳米管提供了见解，并研究了氮掺杂对催化性能的影响，有助于设计高效的无金属碳基电化学催化剂用于二氧化碳还原。图形抽象

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来源期刊

Electrocatalysis CHEMISTRY, PHYSICAL-ELECTROCHEMISTRY

CiteScore

4.80

自引率

6.50%

发文量

审稿时长

>12 weeks

期刊介绍： Electrocatalysis is cross-disciplinary in nature, and attracts the interest of chemists, physicists, biochemists, surface and materials scientists, and engineers. Electrocatalysis provides the unique international forum solely dedicated to the exchange of novel ideas in electrocatalysis for academic, government, and industrial researchers. Quick publication of new results, concepts, and inventions made involving Electrocatalysis stimulates scientific discoveries and breakthroughs, promotes the scientific and engineering concepts that are critical to the development of novel electrochemical technologies. Electrocatalysis publishes original submissions in the form of letters, research papers, review articles, book reviews, and educational papers. Letters are preliminary reports that communicate new and important findings. Regular research papers are complete reports of new results, and their analysis and discussion. Review articles critically and constructively examine development in areas of electrocatalysis that are of broad interest and importance. Educational papers discuss important concepts whose understanding is vital to advances in theoretical and experimental aspects of electrochemical reactions.