Curvature‐induced Zn 3d Electron Return on Zn−N4 Single‐atom Carbon Nanofibers for Boosting Electroreduction of CO2,ChemCatChem

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Curvature‐induced Zn 3d Electron Return on Zn−N4 Single‐atom Carbon Nanofibers for Boosting Electroreduction of CO2
ChemCatChem ( IF 3.8 ) Pub Date : 2020-10-22 , DOI: 10.1002/cctc.202001667
Mingwei Fang ₁ , Xingpu Wang ₁ , Xueyan Li ₁ , Ying Zhu ₁ , Guozheng Xiao ₁ , Jingjing Feng ₁ , Xiaohui Jiang ₁ , Kuilin Lv ₁ , Ying Zhu _{1,

2} , Wen‐Feng Lin ₃

Affiliation

The electrochemical CO₂ reduction to desired chemical feedstocks is of importance, yet it is still challenging to obtain high production selectivity with low overpotential at a current density surpassing the industry benchmark of 100 mA cm⁻². Herein, we constructed a low‐cost Zn single‐atom anchored on curved N‐doped carbon nanofibers (Zn SAs/N−C) by a facile noncovalent self‐assembly approach. At a low overpotential of only 330 mV, the Zn SAs/N−C exhibited simultaneously both a high current density up to 121.5 mA cm⁻² and a CO FE of 94.7 %, superior to the previous reports. Experiments and DFT calculations revealed that the Zn atoms in Zn−N₄ acted as the active sites, while adjacent pyridine‐N coupled with Zn−N₄ could synergistically decrease the free energy barrier for intermediate *COOH formation. Importantly, the curvature of catalyst induced Zn 3d electrons that were bound to the Zn−N bonds to return to Zn atom, thereby leading to an increase in electron density of Zn and accelerating CO₂ electroreduction to CO.

中文翻译：

曲率诱导的Zn-N4单原子碳纳米纤维上的Zn 3d电子返回以促进CO2的电还原

将电化学的CO ₂还原成所需的化学原料非常重要，但是在电流密度超过100 mA cm ^-2的工业密度的情况下，以低过电势获得高生产选择性仍然具有挑战性。本文中，我们通过一种简便的非共价自组装方法，在锚定的N型掺杂碳纳米纤维（Zn SAs / NC）上构建了低成本的Zn单原子。在仅330 mV的低过电势下，Zn SAs / NC同时显示出高达121.5 mA cm ^-2的高电流密度和94.7％的CO FE，优于先前的报道。实验和DFT计算表明，Zn-N ₄中的Zn原子是活性位点，而相邻的N-吡啶基与Zn-N ₄耦合可以协同降低中间* COOH形成的自由能垒。重要的是，催化剂诱导的与Zn-N键结合的Zn 3d电子的曲率返回到Zn原子，从而导致Zn的电子密度增加，并加速了CO ₂电还原为CO。

更新日期：2020-10-22

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