Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions
Development of high-performance oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalysts is crucial to realizing the electrolytic water cycle. C<sub>60</sub> is an ideal substrate material for single atom catalysts (SACs) due to its unique electron-withdrawing proper...
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2024
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| _version_ | 1852025984148045824 |
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| author | Junkai Xu (19840014) |
| author2 | Yunhao Wang (8914208) Xiaoxue Yu (4682347) Jianjun Fang (783857) Xianfang Yue (2196034) Breno R. L. Galvão (7900016) Jing Li (10611) |
| author2_role | author author author author author author |
| author_facet | Junkai Xu (19840014) Yunhao Wang (8914208) Xiaoxue Yu (4682347) Jianjun Fang (783857) Xianfang Yue (2196034) Breno R. L. Galvão (7900016) Jing Li (10611) |
| author_role | author |
| dc.creator.none.fl_str_mv | Junkai Xu (19840014) Yunhao Wang (8914208) Xiaoxue Yu (4682347) Jianjun Fang (783857) Xianfang Yue (2196034) Breno R. L. Galvão (7900016) Jing Li (10611) |
| dc.date.none.fl_str_mv | 2024-10-12T13:46:41Z |
| dc.identifier.none.fl_str_mv | 10.1021/acs.jpca.4c03413.s001 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/dataset/Single-Atom_Doped_Fullerene_MN_sub_4_sub_C_sub_54_sub_as_Bifunctional_Catalysts_for_the_Oxygen_Reduction_and_Oxygen_Evolution_Reactions/27215754 |
| dc.rights.none.fl_str_mv | CC BY-NC 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Biophysics Biochemistry Medicine Computational Biology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified showing better performance moderate adsorption strength ideal substrate material exhibited low overpotentials established volcano plots electrolytic water cycle atom doped fullerene promising bifunctional catalyst good catalytic performances band centers lead 60 </ sub 54 </ sub oxygen reduction reaction atom catalyst based single atom catalysts oxygen reduction catalytic origin bifunctional catalysts band center withdrawing properties unique electron spherical structure results indicate principles calculations novel single n atoms metal ones linear relationship au ). abundant elements 47 v |
| dc.title.none.fl_str_mv | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions |
| dc.type.none.fl_str_mv | Dataset info:eu-repo/semantics/publishedVersion dataset |
| description | Development of high-performance oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalysts is crucial to realizing the electrolytic water cycle. C<sub>60</sub> is an ideal substrate material for single atom catalysts (SACs) due to its unique electron-withdrawing properties and spherical structure. In this work, we screened for a novel single-atom catalyst based on C<sub>60</sub>, which anchored transition metal atoms in the C<sub>60</sub> molecule by coordination with N atoms. Through first-principles calculations, we evaluated the stability and activity of MN<sub>4</sub>–C<sub>54</sub> (M = Fe, Co, Ni, Cu, Rh, Ru, Pd, Ag, Pt, Ir, Au). The results indicate that CuN<sub>4</sub>–C<sub>54</sub>, which is based only on earth-abundant elements, exhibited low overpotentials of 0.46 and 0.47 V for the OER and ORR, respectively, and was considered a promising bifunctional catalyst, showing better performance than the noble-metal ones. In addition, according to the linear relationship of intermediates, we established volcano plots to describe the activity trends of the OER and ORR on MN<sub>4</sub>–C<sub>54</sub>. Finally, d-band center and crystal orbital Hamiltonian populations methods were used to explain the catalytic origin. Suitable d-band centers lead to moderate adsorption strength, further leading to good catalytic performances. |
| eu_rights_str_mv | openAccess |
| id | Manara_0fede8812455e22fcce8aeeef5ba00a2 |
| identifier_str_mv | 10.1021/acs.jpca.4c03413.s001 |
| network_acronym_str | Manara |
| network_name_str | ManaraRepo |
| oai_identifier_str | oai:figshare.com:article/27215754 |
| publishDate | 2024 |
| 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 Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution ReactionsJunkai Xu (19840014)Yunhao Wang (8914208)Xiaoxue Yu (4682347)Jianjun Fang (783857)Xianfang Yue (2196034)Breno R. L. Galvão (7900016)Jing Li (10611)BiophysicsBiochemistryMedicineComputational BiologyEnvironmental Sciences not elsewhere classifiedChemical Sciences not elsewhere classifiedshowing better performancemoderate adsorption strengthideal substrate materialexhibited low overpotentialsestablished volcano plotselectrolytic water cycleatom doped fullerenepromising bifunctional catalystgood catalytic performancesband centers lead60 </ sub54 </ suboxygen reduction reactionatom catalyst basedsingle atom catalystsoxygen reductioncatalytic originbifunctional catalystsband centerwithdrawing propertiesunique electronspherical structureresults indicateprinciples calculationsnovel singlen atomsmetal oneslinear relationshipau ).abundant elements47 vDevelopment of high-performance oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalysts is crucial to realizing the electrolytic water cycle. C<sub>60</sub> is an ideal substrate material for single atom catalysts (SACs) due to its unique electron-withdrawing properties and spherical structure. In this work, we screened for a novel single-atom catalyst based on C<sub>60</sub>, which anchored transition metal atoms in the C<sub>60</sub> molecule by coordination with N atoms. Through first-principles calculations, we evaluated the stability and activity of MN<sub>4</sub>–C<sub>54</sub> (M = Fe, Co, Ni, Cu, Rh, Ru, Pd, Ag, Pt, Ir, Au). The results indicate that CuN<sub>4</sub>–C<sub>54</sub>, which is based only on earth-abundant elements, exhibited low overpotentials of 0.46 and 0.47 V for the OER and ORR, respectively, and was considered a promising bifunctional catalyst, showing better performance than the noble-metal ones. In addition, according to the linear relationship of intermediates, we established volcano plots to describe the activity trends of the OER and ORR on MN<sub>4</sub>–C<sub>54</sub>. Finally, d-band center and crystal orbital Hamiltonian populations methods were used to explain the catalytic origin. Suitable d-band centers lead to moderate adsorption strength, further leading to good catalytic performances.2024-10-12T13:46:41ZDatasetinfo:eu-repo/semantics/publishedVersiondataset10.1021/acs.jpca.4c03413.s001https://figshare.com/articles/dataset/Single-Atom_Doped_Fullerene_MN_sub_4_sub_C_sub_54_sub_as_Bifunctional_Catalysts_for_the_Oxygen_Reduction_and_Oxygen_Evolution_Reactions/27215754CC BY-NC 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/272157542024-10-12T13:46:41Z |
| spellingShingle | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions Junkai Xu (19840014) Biophysics Biochemistry Medicine Computational Biology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified showing better performance moderate adsorption strength ideal substrate material exhibited low overpotentials established volcano plots electrolytic water cycle atom doped fullerene promising bifunctional catalyst good catalytic performances band centers lead 60 </ sub 54 </ sub oxygen reduction reaction atom catalyst based single atom catalysts oxygen reduction catalytic origin bifunctional catalysts band center withdrawing properties unique electron spherical structure results indicate principles calculations novel single n atoms metal ones linear relationship au ). abundant elements 47 v |
| status_str | publishedVersion |
| title | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions |
| title_full | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions |
| title_fullStr | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions |
| title_full_unstemmed | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions |
| title_short | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions |
| title_sort | Single-Atom Doped Fullerene (MN<sub>4</sub>–C<sub>54</sub>) as Bifunctional Catalysts for the Oxygen Reduction and Oxygen Evolution Reactions |
| topic | Biophysics Biochemistry Medicine Computational Biology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified showing better performance moderate adsorption strength ideal substrate material exhibited low overpotentials established volcano plots electrolytic water cycle atom doped fullerene promising bifunctional catalyst good catalytic performances band centers lead 60 </ sub 54 </ sub oxygen reduction reaction atom catalyst based single atom catalysts oxygen reduction catalytic origin bifunctional catalysts band center withdrawing properties unique electron spherical structure results indicate principles calculations novel single n atoms metal ones linear relationship au ). abundant elements 47 v |