Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction
The electrochemical conversion of carbon dioxide (CO<sub>2</sub>) into high-value-added products under mild conditions is crucial for achieving carbon neutrality. Oxalate (C<sub>2</sub>O<sub>4</sub><sup>2–</sup>) is one of the most important industrial...
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| منشور في: |
2025
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| _version_ | 1852017343233785856 |
|---|---|
| author | Ying Zhou (25031) |
| author2 | Xuan Wu (126953) Ping Zhu (11521) Wenhua Zhang (317886) |
| author2_role | author author author |
| author_facet | Ying Zhou (25031) Xuan Wu (126953) Ping Zhu (11521) Wenhua Zhang (317886) |
| author_role | author |
| dc.creator.none.fl_str_mv | Ying Zhou (25031) Xuan Wu (126953) Ping Zhu (11521) Wenhua Zhang (317886) |
| dc.date.none.fl_str_mv | 2025-08-23T03:16:23Z |
| dc.identifier.none.fl_str_mv | 10.1021/acsami.5c11771.s011 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/dataset/Single-Atom_Catalysts_for_CO_sub_2_sub_Reduction_to_Oxalate_Theoretical_Design_and_Reaction_Condition_Prediction/29972284 |
| dc.rights.none.fl_str_mv | CC BY-NC 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Science Policy Environmental Sciences not elsewhere classified Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified reaction condition prediction 2 –</ sup varying reaction conditions offers theoretical guidance achieving carbon neutrality ti – n cr – n single metal atoms alongside high selectivity 2 </ sub c – c – n x </ theoretical design mild conditions carbon dioxide widely used using single systematically tuning sub >< remarkably low reducing agent promising catalysts operating efficiently mechanistic understanding highly sensitive findings demonstrate energy barrier electrode potential determining step designing high coordination environment catalytic performance catalytic activity atom catalysts also deepens added products 6 v 31 ev |
| dc.title.none.fl_str_mv | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction |
| dc.type.none.fl_str_mv | Dataset info:eu-repo/semantics/publishedVersion dataset |
| description | The electrochemical conversion of carbon dioxide (CO<sub>2</sub>) into high-value-added products under mild conditions is crucial for achieving carbon neutrality. Oxalate (C<sub>2</sub>O<sub>4</sub><sup>2–</sup>) is one of the most important industrial raw materials and is widely used as a reducing agent in the fields of medicine, dyeing, and plastics yet faces challenges in efficient C–C bond formation under mild conditions. In this study, we investigate the reduction of CO<sub>2</sub> to C<sub>2</sub>O<sub>4</sub><sup>2–</sup> using single-atom catalysts (SACs) with M–N<sub><i>x</i></sub>–C configurations, employing density functional theory (DFT) to assess their catalytic performance under varying reaction conditions. Our findings demonstrate that the catalytic activity of Ti–N<sub>3</sub>–C is highly sensitive to the choice of solvent and electrode potential. Lower solvent dielectric constants and more negative electrode potentials promote oxalate formation with Ti–N<sub>3</sub>–C, exhibiting a remarkably low-energy barrier (0.31 eV) for the rate-determining step at −0.7 V in acetonitrile, alongside high selectivity. By systematically tuning the coordination environment of single metal atoms, we identify Ti–N<sub>2</sub>C–C, Cr–N<sub>2</sub>C–C, and Cr–N<sub>3</sub>–C as promising catalysts, operating efficiently at potentials of −0.7, −0.7, and −0.6 V, respectively. This work not only offers theoretical guidance for designing high-performance SACs for CO<sub>2</sub> conversion but also deepens the mechanistic understanding of the electrochemical CO<sub>2</sub> reduction pathways. |
| eu_rights_str_mv | openAccess |
| id | Manara_030e552a030d1eddac4e57b3188d623f |
| identifier_str_mv | 10.1021/acsami.5c11771.s011 |
| network_acronym_str | Manara |
| network_name_str | ManaraRepo |
| oai_identifier_str | oai:figshare.com:article/29972284 |
| publishDate | 2025 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY-NC 4.0 |
| spelling | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition PredictionYing Zhou (25031)Xuan Wu (126953)Ping Zhu (11521)Wenhua Zhang (317886)Science PolicyEnvironmental Sciences not elsewhere classifiedBiological Sciences not elsewhere classifiedChemical Sciences not elsewhere classifiedreaction condition prediction2 –</ supvarying reaction conditionsoffers theoretical guidanceachieving carbon neutralityti – ncr – nsingle metal atomsalongside high selectivity2 </ subc – c– nx </theoretical designmild conditionscarbon dioxidewidely usedusing singlesystematically tuningsub ><remarkably lowreducing agentpromising catalystsoperating efficientlymechanistic understandinghighly sensitivefindings demonstrateenergy barrierelectrode potentialdetermining stepdesigning highcoordination environmentcatalytic performancecatalytic activityatom catalystsalso deepensadded products6 v31 evThe electrochemical conversion of carbon dioxide (CO<sub>2</sub>) into high-value-added products under mild conditions is crucial for achieving carbon neutrality. Oxalate (C<sub>2</sub>O<sub>4</sub><sup>2–</sup>) is one of the most important industrial raw materials and is widely used as a reducing agent in the fields of medicine, dyeing, and plastics yet faces challenges in efficient C–C bond formation under mild conditions. In this study, we investigate the reduction of CO<sub>2</sub> to C<sub>2</sub>O<sub>4</sub><sup>2–</sup> using single-atom catalysts (SACs) with M–N<sub><i>x</i></sub>–C configurations, employing density functional theory (DFT) to assess their catalytic performance under varying reaction conditions. Our findings demonstrate that the catalytic activity of Ti–N<sub>3</sub>–C is highly sensitive to the choice of solvent and electrode potential. Lower solvent dielectric constants and more negative electrode potentials promote oxalate formation with Ti–N<sub>3</sub>–C, exhibiting a remarkably low-energy barrier (0.31 eV) for the rate-determining step at −0.7 V in acetonitrile, alongside high selectivity. By systematically tuning the coordination environment of single metal atoms, we identify Ti–N<sub>2</sub>C–C, Cr–N<sub>2</sub>C–C, and Cr–N<sub>3</sub>–C as promising catalysts, operating efficiently at potentials of −0.7, −0.7, and −0.6 V, respectively. This work not only offers theoretical guidance for designing high-performance SACs for CO<sub>2</sub> conversion but also deepens the mechanistic understanding of the electrochemical CO<sub>2</sub> reduction pathways.2025-08-23T03:16:23ZDatasetinfo:eu-repo/semantics/publishedVersiondataset10.1021/acsami.5c11771.s011https://figshare.com/articles/dataset/Single-Atom_Catalysts_for_CO_sub_2_sub_Reduction_to_Oxalate_Theoretical_Design_and_Reaction_Condition_Prediction/29972284CC BY-NC 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/299722842025-08-23T03:16:23Z |
| spellingShingle | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction Ying Zhou (25031) Science Policy Environmental Sciences not elsewhere classified Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified reaction condition prediction 2 –</ sup varying reaction conditions offers theoretical guidance achieving carbon neutrality ti – n cr – n single metal atoms alongside high selectivity 2 </ sub c – c – n x </ theoretical design mild conditions carbon dioxide widely used using single systematically tuning sub >< remarkably low reducing agent promising catalysts operating efficiently mechanistic understanding highly sensitive findings demonstrate energy barrier electrode potential determining step designing high coordination environment catalytic performance catalytic activity atom catalysts also deepens added products 6 v 31 ev |
| status_str | publishedVersion |
| title | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction |
| title_full | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction |
| title_fullStr | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction |
| title_full_unstemmed | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction |
| title_short | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction |
| title_sort | Single-Atom Catalysts for CO<sub>2</sub> Reduction to Oxalate: Theoretical Design and Reaction Condition Prediction |
| topic | Science Policy Environmental Sciences not elsewhere classified Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified reaction condition prediction 2 –</ sup varying reaction conditions offers theoretical guidance achieving carbon neutrality ti – n cr – n single metal atoms alongside high selectivity 2 </ sub c – c – n x </ theoretical design mild conditions carbon dioxide widely used using single systematically tuning sub >< remarkably low reducing agent promising catalysts operating efficiently mechanistic understanding highly sensitive findings demonstrate energy barrier electrode potential determining step designing high coordination environment catalytic performance catalytic activity atom catalysts also deepens added products 6 v 31 ev |