Banerjee Anwesha, Jain Siddarth, Dastider Saptarshi Ghosh, Biswas Rathindranath, Das Srewashi, Mondal Krishnakanta, Vishal Vikram, Lahiri Goutam Kumar, Dutta Arnab
Chemistry Department, Indian Institute of Technology Bombay, Powai, Maharashtra, 400076, India.
Department of Chemistry, Central University of Punjab, Bathinda, Punjab, 151401, India.
Small. 2025 Feb;21(7):e2406765. doi: 10.1002/smll.202406765. Epub 2024 Nov 5.
Electrochemical CO reduction reaction (CORR), which is driven by electricity generated from renewable energy sources, is a promising technology for sustainably producing carbon-based chemicals or fuels. Several CORR catalysts have been explored to date, among which copper-based electrocatalysts are the most widely known for electrochemical CORR and are extensively studied for their ability to generate an array of products. Their low selectivity, however, hinders their possibility of being used for practical purposes. In this work, a microwave-assisted one-pot synthesized CuO/N-doped carbon demonstrates the electrochemical conversion of carbon dioxide into multiple C products (mainly formate and methanol), with a maximum Faradaic efficiency of 95% in 0.10 m KHCO aqueous solution at a moderately low applied potential of -0.55 V versus RHE (reversible hydrogen electrode). The in-depth theoretical study reveals the key contribution of pyridinic N-based N-doped carbon sites and CuO clusters in CO adsorption and its subsequent conversion to formate and methanol via an energetically favorable formate pathway. The electrocatalyst continued to demonstrate CO reduction to valuable C products when a simulated flue gas stream containing 15% CO along with 500 ppm SO and 200 ppm NO is used as an inlet feed.
电化学CO还原反应(CORR)由可再生能源产生的电力驱动,是一种可持续生产碳基化学品或燃料的有前景的技术。迄今为止,已经探索了几种CORR催化剂,其中铜基电催化剂因电化学CORR最为人所知,并因其能够生成一系列产物而受到广泛研究。然而,它们的低选择性阻碍了其用于实际目的的可能性。在这项工作中,一种微波辅助一锅法合成的CuO/N掺杂碳在相对于可逆氢电极(RHE)为-0.55 V的适度低施加电位下,在0.10 m KHCO水溶液中展示了将二氧化碳电化学转化为多种C产物(主要是甲酸盐和甲醇),最大法拉第效率为95%。深入的理论研究揭示了吡啶型N基N掺杂碳位点和CuO团簇在CO吸附及其随后通过能量有利的甲酸盐途径转化为甲酸盐和甲醇中的关键作用。当使用含有15% CO以及500 ppm SO和200 ppm NO的模拟烟道气流作为入口进料时,该电催化剂继续展示出将CO还原为有价值的C产物的能力。