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Article: Unraveling the Performance Descriptors for Designing Single‐Atom Catalysts on Defective MXenes for Exclusive Nitrate‐To‐Ammonia Electrocatalytic Upcycling
Title | Unraveling the Performance Descriptors for Designing Single‐Atom Catalysts on Defective MXenes for Exclusive Nitrate‐To‐Ammonia Electrocatalytic Upcycling |
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Authors | |
Keywords | density functional theory (DFT) calculations nitrate reduction reaction oxygen vacancy MXene single-atom catalysts sustainable electrochemical upcycling |
Issue Date | 7-Nov-2023 |
Publisher | Wiley |
Citation | Small, 2023 How to Cite? |
Abstract | Electrocatalytic nitrate reduction reaction (NO3RR) is a promising approach for converting nitrate into environmentally benign or even value-added products such as ammonia (NH3) using renewable electricity. However, the poor understanding of the catalytic mechanism on metal-based surface catalysts hinders the development of high-performance NO3RR catalysts. In this study, the NO3RR mechanism of single-atom catalysts (SACs) is systematically explored by constructing single transition metal atoms supported on MXene with oxygen vacancies (Ov-MXene) using density functional theory (DFT) calculations. The results indicate that Ag/Ov-MXene (for precious metal) and Cu/Ov-MXene (for non-precious metal) are highly efficient SACs for NO3RR toward NH3, with low limiting potentials of −0.24 and −0.34 V, respectively. Furthermore, these catalysts show excellent selectivity toward ammonia due to the high energy barriers associated to the formation of byproducts such as NO2, NO, N2O, and N2 on Ag/Ov-MXene and Cu/Ov-MXene, effectively suppressing the competitive hydrogen evolution reaction (HER). The findings not only offer new strategies for promoting NH3 production by MXene-based SACs electrocatalysts under ambient conditions but also provide insights for the development of next-generation NO3RR electrocatalysts. |
Persistent Identifier | http://hdl.handle.net/10722/339385 |
ISSN | 2021 Impact Factor: 15.153 2020 SCImago Journal Rankings: 3.785 |
DC Field | Value | Language |
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dc.contributor.author | Gao, Xutao | - |
dc.contributor.author | Tse, Edmund CM | - |
dc.date.accessioned | 2024-03-11T10:36:10Z | - |
dc.date.available | 2024-03-11T10:36:10Z | - |
dc.date.issued | 2023-11-07 | - |
dc.identifier.citation | Small, 2023 | - |
dc.identifier.issn | 1613-6810 | - |
dc.identifier.uri | http://hdl.handle.net/10722/339385 | - |
dc.description.abstract | <p>Electrocatalytic nitrate reduction reaction (NO<sub>3</sub>RR) is a promising approach for converting nitrate into environmentally benign or even value-added products such as ammonia (NH<sub>3</sub>) using renewable electricity. However, the poor understanding of the catalytic mechanism on metal-based surface catalysts hinders the development of high-performance NO<sub>3</sub>RR catalysts. In this study, the NO<sub>3</sub>RR mechanism of single-atom catalysts (SACs) is systematically explored by constructing single transition metal atoms supported on MXene with oxygen vacancies (O<sub>v</sub>-MXene) using density functional theory (DFT) calculations. The results indicate that Ag/O<sub>v</sub>-MXene (for precious metal) and Cu/O<sub>v</sub>-MXene (for non-precious metal) are highly efficient SACs for NO<sub>3</sub>RR toward NH<sub>3</sub>, with low limiting potentials of −0.24 and −0.34 V, respectively. Furthermore, these catalysts show excellent selectivity toward ammonia due to the high energy barriers associated to the formation of byproducts such as NO<sub>2</sub>, NO, N<sub>2</sub>O, and N<sub>2</sub> on Ag/O<sub>v</sub>-MXene and Cu/O<sub>v</sub>-MXene, effectively suppressing the competitive hydrogen evolution reaction (HER). The findings not only offer new strategies for promoting NH<sub>3</sub> production by MXene-based SACs electrocatalysts under ambient conditions but also provide insights for the development of next-generation NO<sub>3</sub>RR electrocatalysts.</p> | - |
dc.language | eng | - |
dc.publisher | Wiley | - |
dc.relation.ispartof | Small | - |
dc.rights | This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License. | - |
dc.subject | density functional theory (DFT) calculations | - |
dc.subject | nitrate reduction reaction | - |
dc.subject | oxygen vacancy MXene | - |
dc.subject | single-atom catalysts | - |
dc.subject | sustainable electrochemical upcycling | - |
dc.title | Unraveling the Performance Descriptors for Designing Single‐Atom Catalysts on Defective MXenes for Exclusive Nitrate‐To‐Ammonia Electrocatalytic Upcycling | - |
dc.type | Article | - |
dc.description.nature | published_or_final_version | - |
dc.identifier.doi | 10.1002/smll.202306311 | - |
dc.identifier.scopus | eid_2-s2.0-85176000384 | - |
dc.identifier.eissn | 1613-6829 | - |
dc.identifier.issnl | 1613-6810 | - |