Dual active sites over Cu-ZnO-ZrO2 catalysts for carbon dioxide hydrogenation to methanol

IF 6.9 Q1 Environmental Science Journal of environmental sciences Pub Date : 2023-09-01 DOI:10.1016/j.jes.2022.10.002
Xiucheng Sun, Yifei Jin, Zaizhe Cheng, Guojun Lan, Xiaolong Wang, Yiyang Qiu, Yanjiang Wang, Huazhang Liu, Ying Li
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引用次数: 5

Abstract

CO2 hydrogenation to methanol is a significant approach to tackle the problem of global warming and simultaneously meet the demand for the portable fuel. Cu-ZnO catalysts with various kinds of promoters have received wide attention. However, the role of promoter and the form of active sites in CO2 hydrogenation are still in debate. Here, various molar ratios of ZrO2 were added into the Cu-ZnO catalysts to tune the distributions of Cu0 and Cu+ species. A volcano-like trend between the ratio of Cu+/ (Cu+ + Cu0) and the amount of ZrO2 is presented, among which the CuZn10Zr (the molar ratio of ZrO2 is 10%) catalyst reaches the highest value. Correspondingly, the maximum value of space-time yield to methanol with 0.65 gMeOH/(gcat·hr) is obtained on CuZn10Zr at reaction conditions of 220°C and 3 MPa. Detailed characterizations demonstrate that dual active sites are proposed during CO2 hydrogenation over CuZn10Zr catalyst. The exposed Cu0 takes participate in the activation of H2, while on the Cu+ species, the intermediate of formate from the co-adsorption of CO2 and H2 prefers to be further hydrogenated to CH3OH than decomposing into the by-product of CO, yielding a high selectivity of methanol.

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Cu-ZnO-ZrO2催化剂上二氧化碳加氢制甲醇的双活性位点
CO2加氢制甲醇是解决全球变暖问题同时满足便携式燃料需求的重要途径。具有各种助催化剂的Cu-ZnO催化剂受到了广泛的关注。然而,促进剂的作用和活性位点在CO2加氢中的形式仍存在争议。在此,将不同摩尔比的ZrO2添加到Cu-ZnO催化剂中以调节Cu0和Cu+物种的分布。Cu+/(Cu++Cu0)的比例与ZrO2的量之间呈现火山状的趋势,其中CuZn10Zr(ZrO2的摩尔比为10%)催化剂达到最高值。相应地,在220°C和3MPa的反应条件下,在CuZn10Zr上获得了0.65gMeOH/(gcat·hr)的甲醇时空产率的最大值。详细的表征表明,在CuZn10Zr催化剂上CO2加氢过程中提出了双活性位点。暴露的Cu0参与了H2的活化,而在Cu+物种上,CO2和H2共吸附的甲酸酯中间体更倾向于进一步氢化为CH3OH,而不是分解为co的副产物,从而产生高选择性的甲醇。
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来源期刊
Journal of environmental sciences
Journal of environmental sciences Environmental Science (General)
CiteScore
12.80
自引率
0.00%
发文量
0
审稿时长
17 days
期刊介绍: Journal of Environmental Sciences is an international peer-reviewed journal established in 1989. It is sponsored by the Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, and it is jointly published by Elsevier and Science Press. It aims to foster interdisciplinary communication and promote understanding of significant environmental issues. The journal seeks to publish significant and novel research on the fate and behaviour of emerging contaminants, human impact on the environment, human exposure to environmental contaminants and their health effects, and environmental remediation and management. Original research articles, critical reviews, highlights, and perspectives of high quality are published both in print and online.
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