Dynamic (Sub)surface-Oxygen Enables Highly Efficient Carbonyl-Coupling for Electrochemical Carbon Dioxide Reduction.

Autor: Chu YC; Department of Chemistry and Center for Emerging Materials and Advanced Devices, National Taiwan University, Taipei, 10617, Taiwan., Chen KH; Department of Chemistry and Center for Emerging Materials and Advanced Devices, National Taiwan University, Taipei, 10617, Taiwan., Tung CW; Center for Environmental Sustainability and Human Health, Ming Chi University of Technology, New Taipei, 24301, Taiwan., Chen HC; Center for Reliability Science and Technologies, Center for Sustainability and Energy Tecnhologies, Chang Gung University, Taoyuan, 33302, Taiwan., Wang J; Department of Chemistry and Center for Emerging Materials and Advanced Devices, National Taiwan University, Taipei, 10617, Taiwan., Kuo TR; Graduate Institute of Nanomedicine and Medical Engineering, College of Biomedical Engineering, Taipei Medical University, Taipei, 11031, Taiwan.; Precision Medicine and Translational Cancer Research Center, Taipei Medical University Hospital, Taipei, Taiwan., Hsu CS; Department of Chemistry and Center for Emerging Materials and Advanced Devices, National Taiwan University, Taipei, 10617, Taiwan., Lin KH; Material and Chemical Research Laboratories, Industrial Technology Research Institute, Chutung, Hsinchu, 31040, Taiwan., Tsai LD; Material and Chemical Research Laboratories, Industrial Technology Research Institute, Chutung, Hsinchu, 31040, Taiwan., Chen HM; Department of Chemistry and Center for Emerging Materials and Advanced Devices, National Taiwan University, Taipei, 10617, Taiwan.; Graduate Institute of Nanomedicine and Medical Engineering, College of Biomedical Engineering, Taipei Medical University, Taipei, 11031, Taiwan.; National Synchrotron Radiation Research Center, Hsinchu, 30076, Taiwan.
Jazyk: angličtina
Zdroj: Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2024 Jun; Vol. 36 (26), pp. e2400640. Date of Electronic Publication: 2024 Apr 24.
DOI: 10.1002/adma.202400640
Abstrakt: Nowadays, high-valent Cu species (i.e., Cu δ + ) are clarified to enhance multi-carbon production in electrochemical CO 2 reduction reaction (CO 2 RR). Nonetheless, the inconsistent average Cu valence states are reported to significantly govern the product profile of CO 2 RR, which may lead to misunderstanding of the enhanced mechanism for multi-carbon production and results in ambiguous roles of high-valent Cu species. Dynamic Cu δ + during CO 2 RR leads to erratic valence states and challenges of high-valent species determination. Herein, an alternative descriptor of (sub)surface oxygen, the (sub)surface-oxygenated degree (κ), is proposed to quantify the active high-valent Cu species on the (sub)surface, which regulates the multi-carbon production of CO 2 RR. The κ validates a strong correlation to the carbonyl (*CO) coupling efficiency and is the critical factor for the multi-carbon enhancement, in which an optimized Cu 2 O@Pd 2.31 achieves the multi-carbon partial current density of ≈330 mA cm -2 with a faradaic efficiency of 83.5%. This work shows a promising way to unveil the role of high-valent species and further achieve carbon neutralization.
(© 2024 Wiley‐VCH GmbH.)
Databáze: MEDLINE
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