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<p>Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) has been regarded as one of the most promising solutions to achieving “zero carbon emission”. In most of the CO<sub>2</sub>RR-related studies, high-purity CO<sub>2</sub> has been employed as the feed gas; however, in practice, CO<sub>2</sub> is generally emitted in low concentrations, so it is of great significance to realize high-selectivity electroreduction of low-concentration CO<sub>2</sub> with large concentration fluctuation. In this work, we constructed a dual-active-site catalyst and successfully achieved CO<sub>2</sub> local enrichment and conversion for low-concentration CO<sub>2</sub>. <i>Operando</i> experiments reveal that the catalyst has one type of site for activating CO<sub>2</sub> and one type of site for binding the reaction intermediates. The dual-active-site catalyst displays a selectivity for formic acid consistently above 97% over a broad potential window (from −0.9 to −1.6 V <i>vs.</i> RHE). Even when fed with a low-concentration CO<sub>2</sub> stream (volume ratio from 50% down to 10%), the dual-active-site catalyst could display high activity and selectivity (&gt;91%). In particular, the selectivity is still above 85% when the CO<sub>2</sub> volume ratio is as low as 5%. This work offers a feasible route for converting low-concentration CO<sub>2</sub> via a synergistic effect for dual-active-site catalysts.</p>

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High-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation

  • 期刊论文

  • 发表日期：

    2025年1月2日

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  • Mengyu Qi,
  • Yanbin Ma,
  • Chao Zhang,
  • Bingwei Li,
  • Xueqing Yang,
  • Zhaolin Shi,
  • Simeng Liu,
  • Changhua An,
  • Jiqing Jiao,
  • Tongbu Lu

摘要

Electrochemical CO2 reduction reaction (CO2RR) has been regarded as one of the most promising solutions to achieving “zero carbon emission”. In most of the CO2RR-related studies, high-purity CO2 has been employed as the feed gas; however, in practice, CO2 is generally emitted in low concentrations, so it is of great significance to realize high-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation. In this work, we constructed a dual-active-site catalyst and successfully achieved CO2 local enrichment and conversion for low-concentration CO2. Operando experiments reveal that the catalyst has one type of site for activating CO2 and one type of site for binding the reaction intermediates. The dual-active-site catalyst displays a selectivity for formic acid consistently above 97% over a broad potential window (from −0.9 to −1.6 V vs. RHE). Even when fed with a low-concentration CO2 stream (volume ratio from 50% down to 10%), the dual-active-site catalyst could display high activity and selectivity (>91%). In particular, the selectivity is still above 85% when the CO2 volume ratio is as low as 5%. This work offers a feasible route for converting low-concentration CO2 via a synergistic effect for dual-active-site catalysts.