Electrochemical CO2 Reduction with Atomic Iron‐Dispersed on Nitrogen‐Doped Graphene,Advanced Energy Materials

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Electrochemical CO2 Reduction with Atomic Iron‐Dispersed on Nitrogen‐Doped Graphene
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2018-03-25 , DOI: 10.1002/aenm.201703487
Chenhao Zhang ₁ , Shize Yang ₂ , Jingjie Wu ₃ , Mingjie Liu _{3,

4} , Sadegh Yazdi ₃ , Muqing Ren ₁ , Junwei Sha ₁ , Jun Zhong ₅ , Kaiqi Nie ₅ , Almaz S. Jalilov ₁ , Zhenyuan Li ₃ , Huaming Li ₆ , Boris I. Yakobson _{1,

7} , Qin Wu ₄ , Emilie Ringe _{1,

3} , Hui Xu _{3,

6} , Pulickel M. Ajayan _{1,

3,

7} , James M. Tour _{1,

3,

7}

Affiliation

Electrochemical reduction of CO₂ provides an opportunity to reach a carbon‐neutral energy recycling regime, in which CO₂ emissions from fuel use are collected and converted back to fuels. The reduction of CO₂ to CO is the first step toward the synthesis of more complex carbon‐based fuels and chemicals. Therefore, understanding this step is crucial for the development of high‐performance electrocatalyst for CO₂ conversion to higher order products such as hydrocarbons. Here, atomic iron dispersed on nitrogen‐doped graphene (Fe/NG) is synthesized as an efficient electrocatalyst for CO₂ reduction to CO. Fe/NG has a low reduction overpotential with high Faradic efficiency up to 80%. The existence of nitrogen‐confined atomic Fe moieties on the nitrogen‐doped graphene layer is confirmed by aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy and X‐ray absorption fine structure analysis. The Fe/NG catalysts provide an ideal platform for comparative studies of the effect of the catalytic center on the electrocatalytic performance. The CO₂ reduction reaction mechanism on atomic Fe surrounded by four N atoms (Fe–N₄) embedded in nitrogen‐doped graphene is further investigated through density functional theory calculations, revealing a possible promotional effect of nitrogen doping on graphene.

中文翻译：

分散在氮掺杂石墨烯上的原子铁电化学还原二氧化碳

CO _2的电化学还原为实现碳中和的能源循环利用提供了机会，在该机制中，燃料使用产生的CO ₂排放被收集并转化为燃料。将CO ₂还原为CO是合成更复杂的碳基燃料和化学品的第一步。因此，了解这一步骤对于开发将CO ₂转化为碳氢化合物等高级产品的高性能电催化剂至关重要。在此，合成了分散在氮掺杂石墨烯（Fe / NG）上的原子铁，作为CO ₂的有效电催化剂。Fe / NG还原电位低，法拉第效率高达80％。通过像差校正的高角度环形暗场扫描透射电子显微镜和X射线吸收精细结构分析，证实了掺杂氮的石墨烯层上存在含氮原子Fe部分。Fe / NG催化剂为比较研究催化中心对电催化性能的影响提供了理想的平台。通过密度泛函理论计算进一步研究了嵌入氮掺杂石墨烯中被四个N原子（Fe–N ₄）包围的原子Fe的CO ₂还原反应机理，揭示了氮掺杂对石墨烯的促进作用。

更新日期：2018-03-25

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