In Situ Structural Reconstruction to Generate the Active Sites for CO2 Electroreduction on Bismuth Ultrathin Nanosheets,Advanced Energy Materials

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In Situ Structural Reconstruction to Generate the Active Sites for CO2 Electroreduction on Bismuth Ultrathin Nanosheets
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2022-06-16 , DOI: 10.1002/aenm.202200970
Yuliang Yuan ₁ , Qiyou Wang ₂ , Yan Qiao ₁ , Xuli Chen ₁ , Zhilong Yang ₁ , Wenchuan Lai ₁ , Tianwei Chen ₃ , Guanhua Zhang ₃ , Huigao Duan ₃ , Min Liu ₂ , Hongwen Huang _{1,

4}

Affiliation

Electrochemical structural reconstruction of catalysts may generate real active sites that differ from the initial catalyst, but is often ignored. Herein, combining in situ and ex situ techniques, it is identified that the bismuth nanosheets (NS) dotted with large numbers of coordinatively unsaturated pit sites is produced via the in situ structural reconstruction of Bi(OH)₃ NS. Such reconstructed Bi NS shows greatly improved catalytic activity toward CO₂ electroreduction, with a 2.6-fold increase in current density compared with intact Bi NS, high Faradaic efficiency for HCOO⁻ production (>95%), and an extraordinary turnover frequency of 0.35 s⁻¹ at −0.98 V_RHE. In addition, it delivers industrial-relevant current density of 325 mA cm⁻² without compromising selectivity in a flow cell. The mechanistic studies demonstrate that these coordinatively unsaturated sites acting as the real active sites favor the stabilization of key intermediate *OCHO, which thus facilitate the reaction kinetics for HCOO⁻ production. This work not only provides a unique perspective on the construction of efficient catalysts for CO₂ electroreduction, but also implies the importance in recognition of structural reconstruction.

中文翻译：

原位结构重建以在铋超薄纳米片上生成 CO2 电还原活性位点

催化剂的电化学结构重建可能会产生与初始催化剂不同的真实活性位点，但通常被忽略。_{在此，结合原位和非原位技术，确定了通过Bi(OH) 3} NS的原位结构重建产生了点缀着大量配位不饱和凹坑位的铋纳米片（NS）。_{这种重建的Bi NS显示出对CO 2}电还原的催化活性显着提高，与完整的Bi NS相比，电流密度增加了2.6倍，HCOO ^-生产的法拉第效率高（> 95％），以及0.35 s的非凡周转频率^-1在 -0.98 V _RHE. 此外，它可提供 325 mA cm ^-2的工业相关电流密度，而不会影响流通池的选择性。机理研究表明，这些作为真正活性位点的配位不饱和位点有利于关键中间体 *OCHO 的稳定化，从而促进 HCOO ^-生产的反应动力学。这项工作不仅为构建高效的CO ₂电还原催化剂提供了独特的视角，而且暗示了对结构重建的认识的重要性。

更新日期：2022-06-16

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