Enhancing catalytic selectivity and stability for CO2 hydrogenation to methanol using a solid-solution catalyst

Enhancing catalytic selectivity and stability for CO2 hydrogenation to methanol using a... National Science Review 0: 1, 2018 RESEARCH HIGHLIGHTS doi: 10.1093/nsr/nwy014 Advance access publication 23 January 2018 MATERIALS SCIENCE Enhancing catalytic selectivity and stability for CO hydrogenation to methanol using a solid-solution catalyst 1,2 Jingguang G. Chen The catalytic hydrogenation of CO with prevents one from obtaining conclusive catalyst might provide opportunities for renewable H represents a promising information regarding the active sites un- large-scale processes for CO hydrogena- 2 2 pathway for reducing CO emissions. der reaction conditions, therefore mak- tion. Among the various hydrogenation prod- ing it difficult to develop strategies for In summary, the work by Can Li’s ucts, the formation of methanol (CO + significant enhancement of catalytic per- group has identified an alternative, solid- 3H → CH OH + H O) is preferred formance. solution catalyst with promising catalytic 2 3 2 because methanol can be used not only A recent paper by Can Li’s group [5] performance in terms of conversion, se- as a fuel but also as a reactant to produce has demonstrated the possibility of signif- lectivity and stability for CO hydrogena- olefins and other value-added chemicals icantly improving the catalytic selectiv- tion to methanol. These promising results [1]. Due to the chemical inertness of ity and stability at reasonably high CO should provide opportunities for follow- CO , its catalytic conversion to methanol conversions. Using a catalyst consisting up research for solid-solution catalysts, encounters significant challenges, in par- of a ZnO–ZrO solid solution, these au- both for methanol synthesis and poten- ticular in maintaining catalytic selec- thors achieved a methanol selectivity of tially for other applications in hetero- tivity and stability at CO conversion 86%–91% at CO conversions greater geneous catalysis, such as the selective 2 2 levels that are acceptable for industrial than 10%. Equally important, this cata- hydrogenation of molecules containing processes. lyst remains stable after 500 hours on C=Obonds. At present the most commonly used stream. By using a combination of exper- 1,2 catalyst is Cu/ZnO/Al O [2–4]. There imental evaluation, spectroscopic char- 2 3 Jingguang G. Chen are at least two main issues that are poten- acterization and density functional the- Department of Chemical Engineering, Columbia tially hindering the large-scale applica- ory (DFT) calculations, this paper also University, USA tion of this catalyst: (1) the lack of defini- provides convincing evidence regarding Chemistry Department, Brookhaven National tive understanding of the active sites, and the origin of the excellent performance Laboratory, USA (2) the instability of this catalyst at rela- of the ZnO–ZrO solid-solution cata- 2 E-mail: jgchen@columbia.edu tively high CO conversions. For exam- lyst. Furthermore, the ZnO–ZrO cat- 2 2 ple, currently there is debate about the alyst also shows different CO hydro- REFERENCES role of ZnO in this catalyst. One possi- genation mechanisms to those proposed 1. Porosoff MD, Yan BH and Chen JG. Energy Environ bility is that there is an intimate synergy on Cu/ZnO/Al O . There are two po- 2 3 Sci 2016; 9: 62–73. between Cu and ZnO at the interface, tential advantages of this catalyst over 2. Behrens M, Studt F and Kasatkin I et al. Science where ZnO could act as a structural mod- Cu/ZnO/Al O : (1) the relatively more 2 3 2012; 336: 893–7. ifier, hydrogen reservoir or direct pro- homogeneous nature, due to the solid 3. Kuld S, Thorhauge M and Falsig H et al. Science moter for bond activation. The other pos- solution, of ZnO–ZrO makes it easier 2016; 352: 969–74. sibility is that a highly active ZnCu alloy to utilize in situ techniques and compu- 4. Kattel S, Ram´ırez PJ and Chen JG et al. Science forms by partial reduction of ZnO or a tational methods to unravel the active 2017; 355: 1296–9. decoration of Cu with metallic Zn. The sites under reaction conditions to fur- 5. Wang J, Li G and Li Z et al. Sci Adv 2017; 3: inhomogeneous nature of the supported ther improve the catalytic performance, e1701290. Cu/ZnO/Al O catalyst in most cases and (2) the promising stability of this 2 3 The Author(s) 2018. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd. All rights reserved. For permissions, plea se e-mail: journals.permissions@oup.com Downloaded from https://academic.oup.com/nsr/advance-article-abstract/doi/10.1093/nsr/nwy014/4822168 by Ed 'DeepDyve' Gillespie user on 13 July 2018 http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png National Science Review Oxford University Press

Enhancing catalytic selectivity and stability for CO2 hydrogenation to methanol using a solid-solution catalyst

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Oxford University Press
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© The Author(s) 2018. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com
ISSN
2095-5138
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2053-714X
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10.1093/nsr/nwy014
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Abstract

National Science Review 0: 1, 2018 RESEARCH HIGHLIGHTS doi: 10.1093/nsr/nwy014 Advance access publication 23 January 2018 MATERIALS SCIENCE Enhancing catalytic selectivity and stability for CO hydrogenation to methanol using a solid-solution catalyst 1,2 Jingguang G. Chen The catalytic hydrogenation of CO with prevents one from obtaining conclusive catalyst might provide opportunities for renewable H represents a promising information regarding the active sites un- large-scale processes for CO hydrogena- 2 2 pathway for reducing CO emissions. der reaction conditions, therefore mak- tion. Among the various hydrogenation prod- ing it difficult to develop strategies for In summary, the work by Can Li’s ucts, the formation of methanol (CO + significant enhancement of catalytic per- group has identified an alternative, solid- 3H → CH OH + H O) is preferred formance. solution catalyst with promising catalytic 2 3 2 because methanol can be used not only A recent paper by Can Li’s group [5] performance in terms of conversion, se- as a fuel but also as a reactant to produce has demonstrated the possibility of signif- lectivity and stability for CO hydrogena- olefins and other value-added chemicals icantly improving the catalytic selectiv- tion to methanol. These promising results [1]. Due to the chemical inertness of ity and stability at reasonably high CO should provide opportunities for follow- CO , its catalytic conversion to methanol conversions. Using a catalyst consisting up research for solid-solution catalysts, encounters significant challenges, in par- of a ZnO–ZrO solid solution, these au- both for methanol synthesis and poten- ticular in maintaining catalytic selec- thors achieved a methanol selectivity of tially for other applications in hetero- tivity and stability at CO conversion 86%–91% at CO conversions greater geneous catalysis, such as the selective 2 2 levels that are acceptable for industrial than 10%. Equally important, this cata- hydrogenation of molecules containing processes. lyst remains stable after 500 hours on C=Obonds. At present the most commonly used stream. By using a combination of exper- 1,2 catalyst is Cu/ZnO/Al O [2–4]. There imental evaluation, spectroscopic char- 2 3 Jingguang G. Chen are at least two main issues that are poten- acterization and density functional the- Department of Chemical Engineering, Columbia tially hindering the large-scale applica- ory (DFT) calculations, this paper also University, USA tion of this catalyst: (1) the lack of defini- provides convincing evidence regarding Chemistry Department, Brookhaven National tive understanding of the active sites, and the origin of the excellent performance Laboratory, USA (2) the instability of this catalyst at rela- of the ZnO–ZrO solid-solution cata- 2 E-mail: jgchen@columbia.edu tively high CO conversions. For exam- lyst. Furthermore, the ZnO–ZrO cat- 2 2 ple, currently there is debate about the alyst also shows different CO hydro- REFERENCES role of ZnO in this catalyst. One possi- genation mechanisms to those proposed 1. Porosoff MD, Yan BH and Chen JG. Energy Environ bility is that there is an intimate synergy on Cu/ZnO/Al O . There are two po- 2 3 Sci 2016; 9: 62–73. between Cu and ZnO at the interface, tential advantages of this catalyst over 2. Behrens M, Studt F and Kasatkin I et al. Science where ZnO could act as a structural mod- Cu/ZnO/Al O : (1) the relatively more 2 3 2012; 336: 893–7. ifier, hydrogen reservoir or direct pro- homogeneous nature, due to the solid 3. Kuld S, Thorhauge M and Falsig H et al. Science moter for bond activation. The other pos- solution, of ZnO–ZrO makes it easier 2016; 352: 969–74. sibility is that a highly active ZnCu alloy to utilize in situ techniques and compu- 4. Kattel S, Ram´ırez PJ and Chen JG et al. Science forms by partial reduction of ZnO or a tational methods to unravel the active 2017; 355: 1296–9. decoration of Cu with metallic Zn. The sites under reaction conditions to fur- 5. Wang J, Li G and Li Z et al. Sci Adv 2017; 3: inhomogeneous nature of the supported ther improve the catalytic performance, e1701290. Cu/ZnO/Al O catalyst in most cases and (2) the promising stability of this 2 3 The Author(s) 2018. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd. All rights reserved. For permissions, plea se e-mail: journals.permissions@oup.com Downloaded from https://academic.oup.com/nsr/advance-article-abstract/doi/10.1093/nsr/nwy014/4822168 by Ed 'DeepDyve' Gillespie user on 13 July 2018

Journal

National Science ReviewOxford University Press

Published: Jan 23, 2018

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