Journal article
PdIn intermetallic nanoparticles for the hydrogenation of CO2 to methanol
- Abstract:
- Direct hydrogenation of CO2 to methanol could offer significant environmental benefits, if efficient catalysts can be developed. Here, bimetallic Pd-In nanoparticles show good performance as catalysts for this reaction. Unsupported nanoparticles are synthesised by the thermal decomposition of Pd(acetate)2 and In(acetate)3 precursors in a high boiling point solvent (squalane), followed by reduction using dilute H2 gas (210 °C). Adjusting the ratio of the two metallic precursors allow access to 5–10 nm nanoparticles with different phase compositions, including metallic Pd(0), In2O3 and intermetallic PdIn. Liquid phase methanol synthesis experiments (50 bar, 210 °C, H2:CO2 = 3:1) identify the intermetallic PdIn nanoparticles as the most efficient. The catalysts exhibit around 70% higher methanol rates (normalised to the overall molar metal content) compared to the conventional heterogeneous Cu/ZnO/Al2O3 catalyst (900 and 540 μmol mmolPdInorCuZnAl−1.h−1, respectively). In addition, the optimum Pd/In catalyst shows an improved methanol selectivity over the whole temperature range studied (190–270 °C), reaching >80% selectivity at 270 °C, compared to only 45% for the reference Cu/ZnO/Al2O3 catalyst. Experiments showed an improvement in stability; the methanol production rate declined by 20% after 120 h run for the optimum PdIn-based compared with 30% for the Cu/ZnO/Al2O3 catalyst (after 25 h). The optimum catalyst consists of ∼8 nm nanoparticles comprising a surface In-enriched PdIn intermetallic phase as characterised by XRD, HR-TEM, STEM-EDX and XPS. Post-catalysis analysis of the optimum catalyst shows that the same PdIn bimetallic phase is retained with only a slight increase in the nanoparticle size.
- Publication status:
- Published
- Peer review status:
- Peer reviewed
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(Preview, Version of record, pdf, 2.3MB, Terms of use)
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- Publisher copy:
- 10.1016/j.apcatb.2017.07.069
Authors
+ Engineering and Physical Sciences Research Council
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- Grant:
- EP/H046380, EP/K035274/1, EP/M013839/1, EP/M028291/1
- Publisher:
- Elsevier
- Journal:
- Applied Catalysis B: Environmental More from this journal
- Volume:
- 220
- Pages:
- 9-18
- Publication date:
- 2017-07-25
- Acceptance date:
- 2017-07-24
- DOI:
- ISSN:
-
0926-3373
- Keywords:
- Pubs id:
-
pubs:710885
- UUID:
-
uuid:9f74005e-fda0-4445-a4cd-753a3c103554
- Local pid:
-
pubs:710885
- Source identifiers:
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710885
- Deposit date:
-
2017-08-07
- ARK identifier:
Terms of use
- Copyright holder:
- García-Trenco et al
- Copyright date:
- 2017
- Notes:
-
Copyright © 2017 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/4.0/).
- Licence:
- CC Attribution (CC BY)
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