Discovery of main group single Sb–N4 active sites for CO2 electroreduction to formate with high efficiency,Energy & Environmental Science

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Discovery of main group single Sb–N4 active sites for CO2 electroreduction to formate with high efficiency
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-07-14 , DOI: 10.1039/d0ee01486a
Zhuoli Jiang _{1,

2,

3,

4,

5} , Tao Wang _{6,

7,

8,

9,

10} , Jiajing Pei _{5,

11,

12,

13} , Huishan Shang _{1,

2,

3,

4,

5} , Danni Zhou _{1,

2,

3,

4,

5} , Haijing Li _{5,

14,

15,

16,

17} , Juncai Dong _{5,

14,

15,

16,

17} , Yu Wang _{5,

18,

19,

20,

21} , Rui Cao _{10,

22,

23,

24} , Zhongbin Zhuang _{5,

11,

12,

13} , Wenxing Chen _{1,

2,

3,

4,

5} , Dingsheng Wang _{5,

25,

26,

27} , Jiatao Zhang _{1,

2,

3,

4,

5} , Yadong Li _{5,

25,

26,

27}

Affiliation

Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications
School of Materials Science and Engineering
Beijing Institute of Technology
Beijing 100081
China
SUNCAT Center for Interface Science and Catalysis
Department of Chemical Engineering
Stanford University
Stanford
USA
College of Chemical Engineering
Beijing University of Chemical Technology
Beijing 100029
Beijing Synchrotron Radiation Facility
Institute of High Energy Physics
Chinese Academy of Sciences
Beijing
Shanghai Synchrotron Radiation Facility
Shanghai Institute of Applied Physics
Chinese Academy of Science
Shanghai 201800
Stanford Synchrotron Radiation Lightsource
SLAC National Accelerator Laboratory
Menlo Park
Department of Chemistry
Tsinghua University
Beijing 100084

Main group antimony (Sb) species are promising electrocatalysts that promote the CO₂ reduction reaction (CO₂RR) to formate, which is an important hydrogen storage material and a key chemical intermediate in many industrial reactions. Herein, we discovered that an Sb single atom (SA) material consisting of Sb–N₄ moieties anchored on N-doped carbon (NC) nanosheets (named Sb SA/NC) could serve as a CO₂RR catalyst to produce formate with high efficiency. Sb SA/NC exhibited a formate faradaic efficiency of 94.0% at −0.8 V vs. RHE. In situ X-ray absorption fine structure (XAFS) investigations and density functional theory (DFT) calculations demonstrated that the excellent CO₂RR activity originated from the positively charged Sb^δ+–N₄ (0 < δ < 3) active sites. Our results present significant guidelines for the rational design and accurate modulation of main group metal (Sb, In, Sn, Bi, etc.) catalysts for the CO₂RR at the atomic scale.

中文翻译：

发现主要的单个Sb–N4活性位点，可高效还原CO2以形成甲酸

主族锑（Sb）是有前途的电催化剂，可促进CO ₂还原反应（CO ₂ RR）形成甲酸盐，该甲酸盐是重要的储氢材料，并且是许多工业反应中的关键化学中间体。在本文中，我们发现由Sb–N ₄部分锚定在N掺杂碳（NC）纳米片上的Sb单原子（SA）材料（称为Sb SA / NC）可以用作CO ₂ RR催化剂以生产高甲酸盐效率。相对于RHE，Sb SA / NC在-0.8 V时的甲酸法拉第效率为94.0％。原位X射线吸收精细结构（XAFS）研究和密度泛函理论（DFT）计算表明，优异的CO ₂RR活性源自带正电的Sb ^{δ +} -N ₄（0 < δ <3）的活性位点。我们的研究结果提出了合理设计和主族金属的准确调制（锑，铟，锡，铋，显著准则等）催化剂的CO ₂在原子尺度RR。

更新日期：2020-09-16

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