A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface
Mass production of Au–Cu-based catalysts with tailored selectivity is a complex and challenging task. We report a semi-affinity strategy to realize the synthesis of Au–Cu Janus nanocrystals with continuously tuned interfaces (from dimer, Janus, acorn-like Janus, to core-shell) based on Au nanosphere...
| Main Authors: | , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Online Access: | https://hdl.handle.net/10356/179012 |
| _version_ | 1826127407621341184 |
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| author | Zhang, Tao Zhang, Bao Zang, Yipeng Zeng, Pan Li, Yue Fan, Hong Jin |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Zhang, Tao Zhang, Bao Zang, Yipeng Zeng, Pan Li, Yue Fan, Hong Jin |
| author_sort | Zhang, Tao |
| collection | NTU |
| description | Mass production of Au–Cu-based catalysts with tailored selectivity is a complex and challenging task. We report a semi-affinity strategy to realize the synthesis of Au–Cu Janus nanocrystals with continuously tuned interfaces (from dimer, Janus, acorn-like Janus, to core-shell) based on Au nanosphere seeds. We highlight the role of interfacial strain due to a large lattice mismatch in growth control. The systematic electrochemical evaluation shows that the interfacial Cu oxide state, ∗CO coverage, and intermediate adsorption configuration can be well tuned by tailoring the Janus nanostructure. Optimized Au–Cu Janus catalyst reaches an efficiency of up to 80.0% for C2+ product with a partial current density of 466.1 mA cm−2. The reaction products can be selectively switched from methanol (dimer) to ethanol (Janus) and further to ethylene (acorn-like Janus) by increasing the interface area of the Au–Cu heterostructures. The catalytic mechanisms are unraveled by operando surface-enhanced Raman spectroscopy (SERS) analysis and density functional theory calculations. |
| first_indexed | 2024-10-01T07:08:22Z |
| format | Journal Article |
| id | ntu-10356/179012 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T07:08:22Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1790122024-07-22T15:34:28Z A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface Zhang, Tao Zhang, Bao Zang, Yipeng Zeng, Pan Li, Yue Fan, Hong Jin School of Physical and Mathematical Sciences Physics Semi-affinity synthesis Janus heterostructures Mass production of Au–Cu-based catalysts with tailored selectivity is a complex and challenging task. We report a semi-affinity strategy to realize the synthesis of Au–Cu Janus nanocrystals with continuously tuned interfaces (from dimer, Janus, acorn-like Janus, to core-shell) based on Au nanosphere seeds. We highlight the role of interfacial strain due to a large lattice mismatch in growth control. The systematic electrochemical evaluation shows that the interfacial Cu oxide state, ∗CO coverage, and intermediate adsorption configuration can be well tuned by tailoring the Janus nanostructure. Optimized Au–Cu Janus catalyst reaches an efficiency of up to 80.0% for C2+ product with a partial current density of 466.1 mA cm−2. The reaction products can be selectively switched from methanol (dimer) to ethanol (Janus) and further to ethylene (acorn-like Janus) by increasing the interface area of the Au–Cu heterostructures. The catalytic mechanisms are unraveled by operando surface-enhanced Raman spectroscopy (SERS) analysis and density functional theory calculations. Ministry of Education (MOE) Submitted/Accepted version The authors acknowledge financial support from the Singapore Ministry of Education by Tier 1 (RG80/22), the National Science Fund for Distinguished Young Scholars (grant no. 51825103), and the Natural Science Foundation of China (grant nos. 52001306 and 92263209). 2024-07-16T02:35:39Z 2024-07-16T02:35:39Z 2024 Journal Article Zhang, T., Zhang, B., Zang, Y., Zeng, P., Li, Y. & Fan, H. J. (2024). A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface. Chem, 10, 1-16. https://dx.doi.org/10.1016/j.chempr.2024.04.009 2451-9308 https://hdl.handle.net/10356/179012 10.1016/j.chempr.2024.04.009 2-s2.0-85194545120 10 1 16 en RG80/22 Chem © 2024 Elsevier Inc. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1016/j.chempr.2024.04.009. application/pdf |
| spellingShingle | Physics Semi-affinity synthesis Janus heterostructures Zhang, Tao Zhang, Bao Zang, Yipeng Zeng, Pan Li, Yue Fan, Hong Jin A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface |
| title | A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface |
| title_full | A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface |
| title_fullStr | A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface |
| title_full_unstemmed | A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface |
| title_short | A selectivity switch for CO2 electroreduction by continuously tuned semi-coherent interface |
| title_sort | selectivity switch for co2 electroreduction by continuously tuned semi coherent interface |
| topic | Physics Semi-affinity synthesis Janus heterostructures |
| url | https://hdl.handle.net/10356/179012 |
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