Gram-scale synthesis of single-atom metal–N–CNT catalysts for highly efficient CO2 electroreduction,Chemical Communications

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Gram-scale synthesis of single-atom metal–N–CNT catalysts for highly efficient CO2 electroreduction
Chemical Communications ( IF 4.3 ) Pub Date : 2021-1-7 , DOI: 10.1039/d0cc07263j
Qian Sun _{1,

2,

3,

4} , Wenhao Ren _{1,

2,

3,

4} , Yong Zhao _{1,

2,

3,

4} , Chuan Zhao _{1,

2,

3,

4}

Affiliation

Single-atom catalysts (SACs) have attracted much interest for electrochemical CO₂ reduction because of their high metal utilization and excellent catalytic activity. However, the practical applications of SACs were restricted by the low production yield. Herein, we developed a facile synthetic strategy for fabricating metal–nitrogen–carbon nanotube (M–N–CNT, M = Ni, Co, Cu, Fe, Mn, Zn, Pt, or Ru) SACs at scale (>1 g) by direct pyrolysis of metal cations, phenanthroline and CNTs at high temperature. The pyrolysis leads to forming coordinated Ni–N active sites anchored on CNTs. The prepared Ni–N–CNT catalyst with a remarkable Ni loading of 2 wt% determined by ICP exhibits the highest activity for CO₂-to-CO conversion with a high faradaic efficiency of 94% and excellent stability. Aberration-corrected high-angle annular dark-field transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray absorption spectroscopy confirm the presence of isolated Ni single atoms in Ni–N–CNT, which act as the active centers for CO₂ electroreduction while the CNT support offers fast pathways for electron and mass transports. This work laid foundations for future practical applications in CO₂ electroreduction, oxygen reduction reactions, water splitting and nitrogen reduction and beyond.

中文翻译：

克级合成单原子金属N-CNT催化剂可实现高效CO2电还原

单原子催化剂（SAC）由于其高的金属利用率和出色的催化活性而引起了人们对电化学CO ₂还原的关注。但是，SAC的实际应用受到产量低的限制。在此，我们开发了一种简便的合成策略，用于制备规模（> 1 g）的金属-氮-碳纳米管（M–N–CNT，M = Ni，Co，Cu，Fe，Mn，Zn，Pt或Ru）SAC。通过在高温下直接热解金属阳离子，菲咯啉和CNT。热解导致锚定在CNTs上形成协调的Ni–N活性位点。ICP测定的制备的具有2 wt％的显着Ni含量的Ni–N–CNT催化剂显示出最高的CO ₂活性-CO转化，法拉第效率高达94％，稳定性极佳。像差校正的高角度环形暗场透射电子显微镜，X射线光电子能谱和X射线吸收光谱法证实了在Ni–N–CNT中存在孤立的Ni单原子，这些单原子充当了CO ₂电还原的活性中心而CNT载体为电子和质量传输提供了快速途径。这项工作为将来在CO ₂电还原，氧还原反应，水分解和氮还原等方面的实际应用奠定了基础。

更新日期：2021-01-14

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