Supercritical CO2-constructed intralayer [Bi2O2]2+ structural distortion for enhanced CO2 electroreduction,Journal of Materials Chemistry A

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Supercritical CO2-constructed intralayer [Bi2O2]2+ structural distortion for enhanced CO2 electroreduction
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-06-17 , DOI: 10.1039/d0ta04163g
Yannan Zhou _{1,

2,

3,

4} , Pengfei Yan _{1,

2,

3,

4} , Jun Jia _{1,

2,

3,

4} , Suoying Zhang _{4,

5,

6,

7,

8} , Xiaoli Zheng _{1,

2,

3,

4} , Li Zhang _{1,

2,

3,

4} , Bin Zhang _{1,

2,

3,

4} , Jun Chen _{9,

10,

11,

12,

13} , Weichang Hao _{4,

14,

15,

16,

17} , Gongji Chen _{2,

3,

4,

18} , Qun Xu _{1,

2,

3,

4,

19} , Buxing Han _{20,

21,

22,

23,

24}

Affiliation

College of Materials Science and Engineering
Zhengzhou University
Zhengzhou 450052
P. R. China
Key Laboratory of Flexible Electronics (KLOFE)
Institute of Advanced Materials (IAM)
Nanjing Tech University (Nanjing Tech)
Nanjing 211816
Intelligent Polymer Research Institute (IPRI)
ARC Centre of Excellence for Electromaterials Science (ACES)
Australian Institute for Innovative Materials (AIIM)
Innovation Campus
University of Wollongong
Center of Materials Physics and Chemistry
Department of Physics
Beihang University
Beijing 100191
Supercomputing Center
Henan Institute of Advanced Technology
Beijing National Laboratory for Molecular Sciences
Key Laboratory of Colloid and Interface and Thermodynamics
Institute of Chemistry
Chinese Academy of Sciences
Beijing 100190

Inducing crystal distortion in two-dimensional (2D) materials to increase the number of active sites is of great significance in improving the intrinsic activity of electrocatalysts for the CO₂ reduction reaction (CO₂RR). Developing 2D materials as thin as possible is required for this goal. Herein, taking layered BiOCl as a prototype model, we achieved the intralayer [Bi₂O₂]²⁺ structural distortion by using supercritical CO₂ as a solvent to reduce the number of interlayer chlorine atoms involved in the reaction. Contrary to expectations, further CO₂RR experiments indicate that thick nanoplates exhibit a high faradaic efficiency of ∼92% for conversion of CO₂ to formate in a wide potential window, whereas ultrathin nanosheets mainly produce H₂. Density functional theory calculation shows that increased [Bi₂O₂]²⁺ structural distortion in thick nanoplate layers is responsible for the finding. This strategy provides a new route to promoting the intrinsic activity of electrocatalysts, and provides us with a new insight into understanding thickness-dependent activity.

中文翻译：

超临界CO2构造的层内[Bi2O2] 2+结构变形，可增强CO2的电还原

在二维（2D）材料中引起晶体畸变以增加活性位点的数目，对于提高电催化剂的CO ₂还原反应（CO ₂ RR）的固有活性具有重要意义。为此目的，需要开发尽可能薄的2D材料。在此，以层状BiOCl为原型模型，通过使用超临界CO ₂作为溶剂减少反应中涉及的层间氯原子数，实现了层内[Bi ₂ O ₂ ] ^2+的结构变形。与预期相反，进一步的CO ₂ RR实验表明，厚的纳米板对CO的转化显示出高达约92％的法拉第效率。₂在较宽的潜在窗口中形成，而超薄纳米片主要产生H₂。密度泛函理论计算表明，在厚纳米板层中增加的[Bi₂ O₂ ]²⁺结构变形是造成这一发现的原因。该策略为提高电催化剂的固有活性提供了一条新途径，并为我们提供了一个新的洞察力，以了解厚度依赖性活性。

更新日期：2020-07-07

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