Copper with an atomic-scale spacing for efficient electrocatalytic co-reduction of carbon dioxide and nitrate to urea

Seokmin Shin, Siraj Sultan, Zong Xian Chen, Hojeong Lee, Hansaem Choi, Tae Ung Wi, Changhyun Park, Taewon Kim, Chanhee Lee, Jihong Jeong, Hyeju Shin, Tae Hee Kim, Hyungkuk Ju, Hyung Chul Yoon, Hyun Kon Song, Hyun Wook Lee, Mu Jeng Cheng, Youngkook Kwon

研究成果: Article同行評審

21 引文 斯高帕斯(Scopus)

摘要

The electrochemical co-reduction of carbon dioxide (CO2) and nitrate (NO3) to urea via C-N bond coupling is a promising alternative to traditional industrial processes that are intensive in energy consumption and CO2 emission. However, due to the lack of suitable catalysts, the electrochemical process for urea synthesis suffers from low faradaic efficiency, current density, and product yield, which highlights the importance of developing new catalysts that work efficiently toward the co-reduction of CO2 and nitrate NO3 (CR-CO2/NO3) and the corresponding C-N bond coupling reactions. Here, we report that copper (Cu) with atomic-scale spacings (ds) between copper facets can significantly improve the electrochemical synthesis of urea from CR-CO2/NO3. We used the lithiation approach to create ds between the copper facets. We prepared four Cu samples with different ds values simply by controlling the degree of lithiation on each sample. Among the four samples, Cu with a ds close to 6 Å achieves a remarkably high urea yield rate of 7541.9 μg h−1 mgcat−1 and a partial current density of 115.25 mA cm−2, substantially greater than those of the bare Cu (urea yield rate of only 444.7 μg h−1 mgcat−1 and urea partial current density of 1.96 mA cm−2) counterpart. Our density functional theory calculations suggest that compared with bare Cu, Cu with a ds of 6.0

原文English
期刊Energy and Environmental Science
DOIs
出版狀態Accepted/In press - 2023

All Science Journal Classification (ASJC) codes

  • 環境化學
  • 可再生能源、永續發展與環境
  • 核能與工程
  • 污染

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