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Potassium-Assisted Fabrication of Intrinsic Defects in Porous Carbons for Electrocatalytic CO2 Reduction

Journal Article


Abstract


  • The fabrication of intrinsic carbon defects is usually tangled with doping effects, and the identification of their unique roles in catalysis remains a tough task. Herein, a K+-assisted synthetic strategy is developed to afford porous carbon (K-defect-C) with abundant intrinsic defects and complete elimination of heteroatom via direct pyrolysis of K+-confined metal���organic frameworks (MOFs). Positron-annihilation lifetime spectroscopy, X-ray absorption fine structure measurement, and scanning transmission electron microscopy jointly illustrate the existence of abundant 12-vacancy-type carbon defects (V12) in K-defect-C. Remarkably, the K-defect-C achieves ultrahigh CO Faradaic efficiency (99%) at ���0.45��V in CO2 electroreduction, far surpassing MOF-derived carbon without K+ etching. Theoretical calculations reveal that the V12 defects in K-defect-C favor CO2 adsorption and significantly accelerate the formation of the rate-determining COOH* intermediate, thereby promoting CO2 reduction. This work develops a novel strategy to generate intrinsic carbon defects and provides new insights into their critical role in catalysis.

Publication Date


  • 2022

Citation


  • Ling, L. L., Jiao, L., Liu, X., Dong, Y., Yang, W., Zhang, H., . . . Jiang, H. L. (2022). Potassium-Assisted Fabrication of Intrinsic Defects in Porous Carbons for Electrocatalytic CO2 Reduction. Advanced Materials, 34(42). doi:10.1002/adma.202205933

Scopus Eid


  • 2-s2.0-85138195386

Volume


  • 34

Issue


  • 42

Place Of Publication


Abstract


  • The fabrication of intrinsic carbon defects is usually tangled with doping effects, and the identification of their unique roles in catalysis remains a tough task. Herein, a K+-assisted synthetic strategy is developed to afford porous carbon (K-defect-C) with abundant intrinsic defects and complete elimination of heteroatom via direct pyrolysis of K+-confined metal���organic frameworks (MOFs). Positron-annihilation lifetime spectroscopy, X-ray absorption fine structure measurement, and scanning transmission electron microscopy jointly illustrate the existence of abundant 12-vacancy-type carbon defects (V12) in K-defect-C. Remarkably, the K-defect-C achieves ultrahigh CO Faradaic efficiency (99%) at ���0.45��V in CO2 electroreduction, far surpassing MOF-derived carbon without K+ etching. Theoretical calculations reveal that the V12 defects in K-defect-C favor CO2 adsorption and significantly accelerate the formation of the rate-determining COOH* intermediate, thereby promoting CO2 reduction. This work develops a novel strategy to generate intrinsic carbon defects and provides new insights into their critical role in catalysis.

Publication Date


  • 2022

Citation


  • Ling, L. L., Jiao, L., Liu, X., Dong, Y., Yang, W., Zhang, H., . . . Jiang, H. L. (2022). Potassium-Assisted Fabrication of Intrinsic Defects in Porous Carbons for Electrocatalytic CO2 Reduction. Advanced Materials, 34(42). doi:10.1002/adma.202205933

Scopus Eid


  • 2-s2.0-85138195386

Volume


  • 34

Issue


  • 42

Place Of Publication