Abstract
Thermocatalytic conversion of redundant CO2 to useful methanol is an attractive route to address both energy and environmental crises simultaneously. However, existing copper/oxide catalysts widely used in these thermocatalytic processes still suffer from low methanol yield under mild reaction conditions. In this work, we design inverse oxide/Cu catalysts to achieve superior thermal catalytic performance for CO2 hydrogenation. The optimized ZnO/Cu-1.0 catalyst exhibits maximum CH3OH selectivity of 83.4% and space–time yield (STY) of \(170.9\;{\text{g}}_{{{\text{CH}}_{3} {\text{OH}}}} \;{\text{kg}}_{{{\text{cat}}}}^{ - 1} \;{\text{h}}^{ - 1}\) in CO2 hydrogenation at 210 °C, nearly twofold higher STY than the previous optimal inverse ZnO/Cu catalysts (\(89.6\;{\text{g}}_{{{\text{CH}}_{3} {\text{OH}}}} \;{\text{kg}}_{{{\text{cat}}}}^{ - 1} \;{\text{h}}^{ - 1}\)at 250 °C). Importantly, ZnO/Cu-1.0 catalyst displayed not only a satisfactory catalytic stability but also a superior CH3OH STY with a time-on-stream of 24 h. Such inverse configuration of catalysts will pave the way for new strategies to design high-performance thermocatalytic catalysts and promote their commercialization.
Graphical abstract
Typical inverse ZnO/Cu-1.0 catalysts have been demonstrated and achieved to significantly facilitate the activation of inert CO2 molecules to produce methanol, due to its special physicochemical properties and strong ZnO–Cu interaction
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Acknowledgements
The authors gracefully acknowledge the National Natural Science Foundation of China (22002135, 22102001), Natural Science Foundation of the Jiangsu Higher Education Institutions of China (20KJB480004), and Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (No. 2022-K49).
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XL contributed to writing-original, investigation, conceptualization, data curation, formal analysis. YX contributed to conceptualization, data curation, supervision. YX contributed to investigation, experimental assistance. HL contributed to supervision, conceptualization, methodology. JY contributed to methodology, writing-review & editing, data curation. HZ contributed to writing-review & editing, data curation. XG contributed to data curation. JY contributed to validation. LG contributed to resources, validation. JL contributed to methodology, writing-review & editing, data curation, funding acquisition, resources, supervision.
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Li, X., Xia, Y., Xu, Y. et al. Optimizing interfacial interaction between Cu and metal oxides boosts methanol yield in CO2 hydrogenation. Res Chem Intermed 49, 3933–3950 (2023). https://doi.org/10.1007/s11164-023-05063-x
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DOI: https://doi.org/10.1007/s11164-023-05063-x