Study on Catalytic Performance in CO2 Hydrogenation to Methanol over Au–Cu/C3N4 Catalysts

Catalysts Pub Date : 2024-07-23 DOI:10.3390/catal14080470
Chenyang Li, Jian Yang, Chongbin Zhang, Cong Wang, Chen Lyu, Kai Fan
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Abstract

In this paper, Au and Cu nanoparticles were successfully loaded onto porous g-C3N4 material through a hydrothermal synthesis method. By adjusting the proportion of Cu, Au-5%Cu/C3N4, Au-10%Cu/C3N4, and Au-15%Cu/C3N4, catalysts were prepared and used for the catalytic reduction of CO2 to methanol. Characterization analysis using high-resolution XPS spectra showed that with an increase in the doping amount of Cu, the electron cloud density on the Cu surface initially increased and then decreased. Electrons from Au atoms transferred to Cu atoms, leading to the accumulation of a more negative charge on the Cu surface, promoting the adsorption of partially positively charged C in CO2, which is more beneficial for catalyzing CO2. Among them, Au-10%Cu/C3N4 exhibited good reducibility and strong basic sites, as demonstrated by H2-TPR and CO2-TPD, with the conversion rates for CO2, methanol yield, and methanol selectivity being 11.58%, 41.29 g·kg−1·h−1 (0.39 μmol·g−1s−1), and 59.77%, respectively.
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Au-Cu/C3N4 催化剂在二氧化碳加氢制甲醇过程中的催化性能研究
本文通过水热合成法成功地将金和铜纳米粒子负载到多孔 g-C3N4 材料上。通过调整铜的比例,制备了 Au-5%Cu/C3N4、Au-10%Cu/C3N4 和 Au-15%Cu/C3N4 催化剂,并将其用于催化 CO2 还原成甲醇。利用高分辨率 XPS 光谱进行的表征分析表明,随着铜掺杂量的增加,铜表面的电子云密度先增大后减小。金原子的电子转移到铜原子上,导致铜表面积累了更多的负电荷,促进了 CO2 中带部分正电荷的 C 的吸附,更有利于催化 CO2。其中,Au-10%Cu/C3N4 表现出良好的还原性和较强的碱性位点,H2-TPR 和 CO2-TPD 均证明了这一点,其 CO2 转化率、甲醇产率和甲醇选择性分别为 11.58%、41.29 g-kg-1-h-1(0.39 μmol-g-1s-1)和 59.77%。
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