Chawdhury Piu, Chansai Sarayute, Conway Matthew, Parker Joseph, Lindley Matthew, Stere Cristina E, Sankar Meenakshisundaram, Haigh Sarah J, Dennis-Smither Ben, Filip Sorin V, Poulston Stephen, Hinde Peter, Hawkins Christopher, Hardacre Christopher
Department of Chemical Engineering, The University of Manchester, Oxford Road, Manchester M13 9PL, U.K.
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Maindy Road, Cardiff CF24 4HQ, United Kingdom.
ACS Catal. 2025 Apr 16;15(9):7053-7065. doi: 10.1021/acscatal.5c00747. eCollection 2025 May 2.
The direct conversion of emitted and captured carbon dioxide into usable fuels remains a significant challenge and is a key element in the transition to net zero. Herein, we examine the reaction of CO and HO over Ni- and Cu-based catalysts combined with nonthermal plasma (NTP) technology. The catalysis under NTP conditions enabled significantly higher CO conversion and product yield, which was almost six times higher than that of the plasma-only system. A maximum H concentration of ∼2500 ppm was achieved for the Cu/ZSM5 catalyst at 17% CO conversion. Comprehensive catalyst characterization together with the reaction performances reveals that Cu in a reduced state promotes both the CO and HO conversion leading to H formation. diffuse reflectance infrared spectroscopy (DRIFTS) coupled with mass spectrometry (MS) analysis of the gas phase products confirms that CO is the major active species to drive the water gas shift reaction to form H in addition to the direct CO and HO interaction. It also explains how the different metal support interactions influence the CO adsorption and its interaction with water. Among the catalysts studied, ZSM5-supported Cu catalysts were found to be the most effective in facilitating the CO and HO reaction to produce H.
将排放和捕获的二氧化碳直接转化为可用燃料仍然是一项重大挑战，也是向净零排放过渡的关键因素。在此，我们研究了CO和H₂O在镍基和铜基催化剂与非热等离子体（NTP）技术相结合的情况下的反应。NTP条件下的催化作用使CO转化率和产物产率显著提高，几乎比仅等离子体系统高出六倍。在CO转化率为17%时，Cu/ZSM5催化剂的最大H₂浓度达到约2500 ppm。综合催化剂表征和反应性能表明，还原态的Cu促进了CO和H₂O的转化，从而导致H₂的形成。漫反射红外光谱（DRIFTS）与气相产物的质谱（MS）分析相结合证实，除了直接的CO和H₂O相互作用外，CO是驱动水煤气变换反应形成H₂的主要活性物种。它还解释了不同的金属-载体相互作用如何影响CO的吸附及其与水的相互作用。在所研究的催化剂中，发现ZSM5负载的Cu催化剂在促进CO和H₂O反应生成H₂方面最为有效。
