CO2 Hydrogenation Using Size-dependent Ru Particles Supported on g-C3N4

Rasmeet Singh, Lizhuo Wang, Haoyue Sun, Jun Huang
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Abstract

Efficient catalysis of CO2 hydrogenation holds significant promise for addressing environmental concerns and advancing sustainable energy solutions. In this study, we report the synthesis of a novel series of Ru-supported on graphitic carbon nitride (g-C3N4) catalysts, with a focus on the impact of ruthenium (Ru) loading on the thermocatalytic performance. Varying Ru concentrations were introduced, including 0.2, 0.5, 1.0, 2.0, and 5.0 wt%, resulting in different Ru particle sizes on g-C3N4 support. Through a multifaceted characterization approach, it was observed that the catalyst containing 1 wt% Ru loading displayed superior performance, with a high density of active sites, indicated by an enhanced CO2 conversion rate of 36.8 % at 450 °C and a CO yield of 25 %. This catalyst also exhibited remarkable CO selectivity of 83 % at 375 °C. Conversely, lower loadings of 0.2 and 0.5 wt % Ru were found to be less effective, yielding minimal CO2 conversion. Loadings above 1 wt% Ru, while achieving high CO2 conversion, demonstrated a preference for CH4 production over CO, indicating lower selectivity for the desired product. This study elucidates the critical role of Ru nanocluster size in the catalytic activity and selectivity, with 1 wt % Ru-supported g-C3N4 emerging as a promising candidate for selective CO generation from CO2 hydrogenation, offering a pathway for the valorization of CO2 as a raw material in the chemical industry.

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利用 g-C3N4 上支持的尺寸依赖性 Ru 粒子进行二氧化碳氢化
二氧化碳加氢的高效催化为解决环境问题和推进可持续能源解决方案带来了巨大希望。在本研究中,我们报告了在氮化石墨碳(g-C3N4)上合成一系列新型 Ru 支持催化剂的情况,重点研究了钌(Ru)负载对热催化性能的影响。引入了不同浓度的 Ru,包括 0.2、0.5、1.0、2.0 和 5.0 wt%,从而在 g-C3N4 载体上形成了不同的 Ru 颗粒大小。通过多方面的表征方法观察发现,Ru 含量为 1 wt% 的催化剂性能优越,活性位点密度高,这表现在 450 °C 时二氧化碳转化率提高了 36.8%,二氧化碳产率提高了 25%。在 375 °C 时,这种催化剂还表现出显著的二氧化碳选择性,达到 83%。相反,较低的 0.2 和 0.5 wt % Ru 负载则效果较差,二氧化碳转化率极低。Ru 的负载量超过 1 wt%,虽然实现了较高的二氧化碳转化率,但却显示出 CH4 的生成优于 CO 的生成,表明对所需产物的选择性较低。这项研究阐明了 Ru 纳米簇尺寸在催化活性和选择性中的关键作用,1 wt % Ru 支持的 g-C3N4 成为从 CO2 加氢中选择性生成 CO 的有前途的候选物质,为化工行业将 CO2 作为原材料进行价值评估提供了一条途径。
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