Isolated FeN Sites for Efficient Electrocatalytic CO Reduction

Overview

Journal Adv Sci (Weinh)

Specialty Biomedical Engineering

Date 2020 Sep 30

PMID 32995135

Citations 14

Authors

Xiaogang Li

Shibo Xi

Libo Sun

Shuo Dou

Zhenfeng Huang

Tan Su

Xin Wang

Affiliations

Soon will be listed here.

Abstract

The construction of isolated metal sites represents a promising approach for electrocatalyst design toward the efficient electrochemical conversion of carbon dioxide (CO). Herein, Fe-doped graphitic carbon nitride is rationally prepared by a simple adsorption method and is used as template to construct isolated FeN sites through a confined pyrolysis strategy, which avoids the agglomeration of metal atoms to particles during the synthesis process and thus provides abundant active sites for the CO reduction reaction. The isolated FeN sites lower the energy barrier for the key intermediate in the CO reduction process, leading to the enhanced selectivity for CO production with a faradaic efficiency of up to 93%.

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References

Kamiya K, Kamai R, Hashimoto K, Nakanishi S . Platinum-modified covalent triazine frameworks hybridized with carbon nanoparticles as methanol-tolerant oxygen reduction electrocatalysts. Nat Commun. 2014; 5:5040. PMC: 4199112. DOI: 10.1038/ncomms6040. View

Liu S, Xiao J, Lu X, Wang J, Wang X, Lou X . Efficient Electrochemical Reduction of CO to HCOOH over Sub-2 nm SnO Quantum Wires with Exposed Grain Boundaries. Angew Chem Int Ed Engl. 2019; 58(25):8499-8503. DOI: 10.1002/anie.201903613. View

Martin D, Qiu K, Shevlin S, Handoko A, Chen X, Guo Z . Highly efficient photocatalytic H₂ evolution from water using visible light and structure-controlled graphitic carbon nitride. Angew Chem Int Ed Engl. 2014; 53(35):9240-5. PMC: 4257501. DOI: 10.1002/anie.201403375. View

Li X, Bi W, Chen M, Sun Y, Ju H, Yan W . Exclusive Ni-N Sites Realize Near-Unity CO Selectivity for Electrochemical CO Reduction. J Am Chem Soc. 2017; 139(42):14889-14892. DOI: 10.1021/jacs.7b09074. View

Zheng Y, Jiao Y, Zhu Y, Li L, Han Y, Chen Y . High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst. J Am Chem Soc. 2016; 138(49):16174-16181. DOI: 10.1021/jacs.6b11291. View

Wang C, Chen W, Xia K, Xie N, Wang H, Zhang Y . Silk-Derived 2D Porous Carbon Nanosheets with Atomically-Dispersed Fe-N -C Sites for Highly Efficient Oxygen Reaction Catalysts. Small. 2019; 15(7):e1804966. DOI: 10.1002/smll.201804966. View

Qiao B, Wang A, Yang X, Allard L, Jiang Z, Cui Y . Single-atom catalysis of CO oxidation using Pt1/FeOx. Nat Chem. 2011; 3(8):634-41. DOI: 10.1038/nchem.1095. View

Lin Z, Wang X . Nanostructure engineering and doping of conjugated carbon nitride semiconductors for hydrogen photosynthesis. Angew Chem Int Ed Engl. 2013; 52(6):1735-8. DOI: 10.1002/anie.201209017. View

Peng Y, Lu B, Chen S . Carbon-Supported Single Atom Catalysts for Electrochemical Energy Conversion and Storage. Adv Mater. 2018; 30(48):e1801995. DOI: 10.1002/adma.201801995. View

10.

Wang X, Chen Z, Zhao X, Yao T, Chen W, You R . Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO. Angew Chem Int Ed Engl. 2017; 57(7):1944-1948. DOI: 10.1002/anie.201712451. View

11.

Zhang H, Hwang S, Wang M, Feng Z, Karakalos S, Luo L . Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation. J Am Chem Soc. 2017; 139(40):14143-14149. DOI: 10.1021/jacs.7b06514. View

12.

Chen P, Zhou T, Xing L, Xu K, Tong Y, Xie H . Atomically Dispersed Iron-Nitrogen Species as Electrocatalysts for Bifunctional Oxygen Evolution and Reduction Reactions. Angew Chem Int Ed Engl. 2016; 56(2):610-614. DOI: 10.1002/anie.201610119. View

13.

Xie J, Li B, Peng H, Song Y, Li J, Zhang Z . From Supramolecular Species to Self-Templated Porous Carbon and Metal-Doped Carbon for Oxygen Reduction Reaction Catalysts. Angew Chem Int Ed Engl. 2019; 58(15):4963-4967. DOI: 10.1002/anie.201814605. View

14.

Ren W, Tan X, Yang W, Jia C, Xu S, Wang K . Isolated Diatomic Ni-Fe Metal-Nitrogen Sites for Synergistic Electroreduction of CO. Angew Chem Int Ed Engl. 2019; 58(21):6972-6976. DOI: 10.1002/anie.201901575. View

15.

Lei F, Liu W, Sun Y, Xu J, Liu K, Liang L . Metallic tin quantum sheets confined in graphene toward high-efficiency carbon dioxide electroreduction. Nat Commun. 2016; 7:12697. PMC: 5025773. DOI: 10.1038/ncomms12697. View

16.

Ma M, Trzesniewski B, Xie J, Smith W . Selective and Efficient Reduction of Carbon Dioxide to Carbon Monoxide on Oxide-Derived Nanostructured Silver Electrocatalysts. Angew Chem Int Ed Engl. 2016; 55(33):9748-52. DOI: 10.1002/anie.201604654. View

17.

Bi W, Li X, You R, Chen M, Yuan R, Huang W . Surface Immobilization of Transition Metal Ions on Nitrogen-Doped Graphene Realizing High-Efficient and Selective CO Reduction. Adv Mater. 2018; 30(18):e1706617. DOI: 10.1002/adma.201706617. View

18.

Wang J, Li Z, Wu Y, Li Y . Fabrication of Single-Atom Catalysts with Precise Structure and High Metal Loading. Adv Mater. 2018; 30(48):e1801649. DOI: 10.1002/adma.201801649. View

19.

Yu H, Shang L, Bian T, Shi R, Waterhouse G, Zhao Y . Nitrogen-Doped Porous Carbon Nanosheets Templated from g-C3 N4 as Metal-Free Electrocatalysts for Efficient Oxygen Reduction Reaction. Adv Mater. 2016; 28(25):5080-6. DOI: 10.1002/adma.201600398. View

20.

Li X, Bi W, Zhang L, Tao S, Chu W, Zhang Q . Single-Atom Pt as Co-Catalyst for Enhanced Photocatalytic H2 Evolution. Adv Mater. 2016; 28(12):2427-31. DOI: 10.1002/adma.201505281. View