Reinforcing CoO Covalency via Ce(4f)─O(2p)─Co(3d) Gradient Orbital Coupling for High‐Efficiency Oxygen Evolution
Rare‐earth (RE)‐based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesi...
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| Published in | Advanced materials (Weinheim) Vol. 35; no. 30; pp. e2302462 - n/a |
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| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Germany
Wiley Subscription Services, Inc
01.07.2023
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| Subjects | |
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| Abstract | Rare‐earth (RE)‐based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesized by an effective plasma (P)‐assisted strategy as a model (P‐Ce SAs@CoO) to investigate the origin of OER performance in RE–TMO systems. The P‐Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm−2 and robust electrochemical stability, superior to individual CoO. X‐ray absorption spectroscopy and in situ electrochemical Raman spectroscopy reveal that the Ce‐induced electron redistribution inhibits CoO bond breakage in the CoOCe unit site. Theoretical analysis demonstrates that the gradient orbital coupling reinforces the CoO covalency of the Ce(4f)─O(2p)─Co(3d) unit active site with an optimized Co‐3d‐eg occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. It is believed that the establishment of this Ce–CoO model can set a basis for the mechanistic understanding and structural design of high‐performance RE–TMO catalysts.
Atomically dispersed Ce on CoO is prepared as a model to identify the active sites of rare‐earth‐based transition metal oxides toward oxygen evolution reaction (OER) and the corresponding catalytic mechanism is elucidated. The CeOCo unit site is identified as the active center. The enhanced OER performance is ascribed to reinforce CoO covalency through Ce(4f)─O(2p)─Co(3d) gradient orbital coupling. |
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| AbstractList | Rare‐earth (RE)‐based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesized by an effective plasma (P)‐assisted strategy as a model (P‐Ce SAs@CoO) to investigate the origin of OER performance in RE–TMO systems. The P‐Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm−2 and robust electrochemical stability, superior to individual CoO. X‐ray absorption spectroscopy and in situ electrochemical Raman spectroscopy reveal that the Ce‐induced electron redistribution inhibits CoO bond breakage in the CoOCe unit site. Theoretical analysis demonstrates that the gradient orbital coupling reinforces the CoO covalency of the Ce(4f)─O(2p)─Co(3d) unit active site with an optimized Co‐3d‐eg occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. It is believed that the establishment of this Ce–CoO model can set a basis for the mechanistic understanding and structural design of high‐performance RE–TMO catalysts. Rare‐earth (RE)‐based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesized by an effective plasma (P)‐assisted strategy as a model (P‐Ce SAs@CoO) to investigate the origin of OER performance in RE–TMO systems. The P‐Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm −2 and robust electrochemical stability, superior to individual CoO. X‐ray absorption spectroscopy and in situ electrochemical Raman spectroscopy reveal that the Ce‐induced electron redistribution inhibits CoO bond breakage in the CoOCe unit site. Theoretical analysis demonstrates that the gradient orbital coupling reinforces the CoO covalency of the Ce(4f)─O(2p)─Co(3d) unit active site with an optimized Co‐3d‐e g occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. It is believed that the establishment of this Ce–CoO model can set a basis for the mechanistic understanding and structural design of high‐performance RE–TMO catalysts. Rare-earth (RE)-based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesized by an effective plasma (P)-assisted strategy as a model (P-Ce SAs@CoO) to investigate the origin of OER performance in RE-TMO systems. The P-Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm-2 and robust electrochemical stability, superior to individual CoO. X-ray absorption spectroscopy and in situ electrochemical Raman spectroscopy reveal that the Ce-induced electron redistribution inhibits CoO bond breakage in the CoOCe unit site. Theoretical analysis demonstrates that the gradient orbital coupling reinforces the CoO covalency of the Ce(4f)─O(2p)─Co(3d) unit active site with an optimized Co-3d-eg occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. It is believed that the establishment of this Ce-CoO model can set a basis for the mechanistic understanding and structural design of high-performance RE-TMO catalysts.Rare-earth (RE)-based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesized by an effective plasma (P)-assisted strategy as a model (P-Ce SAs@CoO) to investigate the origin of OER performance in RE-TMO systems. The P-Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm-2 and robust electrochemical stability, superior to individual CoO. X-ray absorption spectroscopy and in situ electrochemical Raman spectroscopy reveal that the Ce-induced electron redistribution inhibits CoO bond breakage in the CoOCe unit site. Theoretical analysis demonstrates that the gradient orbital coupling reinforces the CoO covalency of the Ce(4f)─O(2p)─Co(3d) unit active site with an optimized Co-3d-eg occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. It is believed that the establishment of this Ce-CoO model can set a basis for the mechanistic understanding and structural design of high-performance RE-TMO catalysts. Rare‐earth (RE)‐based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesized by an effective plasma (P)‐assisted strategy as a model (P‐Ce SAs@CoO) to investigate the origin of OER performance in RE–TMO systems. The P‐Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm−2 and robust electrochemical stability, superior to individual CoO. X‐ray absorption spectroscopy and in situ electrochemical Raman spectroscopy reveal that the Ce‐induced electron redistribution inhibits CoO bond breakage in the CoOCe unit site. Theoretical analysis demonstrates that the gradient orbital coupling reinforces the CoO covalency of the Ce(4f)─O(2p)─Co(3d) unit active site with an optimized Co‐3d‐eg occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. It is believed that the establishment of this Ce–CoO model can set a basis for the mechanistic understanding and structural design of high‐performance RE–TMO catalysts. Atomically dispersed Ce on CoO is prepared as a model to identify the active sites of rare‐earth‐based transition metal oxides toward oxygen evolution reaction (OER) and the corresponding catalytic mechanism is elucidated. The CeOCo unit site is identified as the active center. The enhanced OER performance is ascribed to reinforce CoO covalency through Ce(4f)─O(2p)─Co(3d) gradient orbital coupling. Rare-earth (RE)-based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO is successfully designed and synthesized by an effective plasma (P)-assisted strategy as a model (P-Ce SAs@CoO) to investigate the origin of OER performance in RE-TMO systems. The P-Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm and robust electrochemical stability, superior to individual CoO. X-ray absorption spectroscopy and in situ electrochemical Raman spectroscopy reveal that the Ce-induced electron redistribution inhibits CoO bond breakage in the CoOCe unit site. Theoretical analysis demonstrates that the gradient orbital coupling reinforces the CoO covalency of the Ce(4f)─O(2p)─Co(3d) unit active site with an optimized Co-3d-e occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. It is believed that the establishment of this Ce-CoO model can set a basis for the mechanistic understanding and structural design of high-performance RE-TMO catalysts. |
| Author | Liu, Kun Xing, Wei Li, Meng Li, Hao Sun, Dongmei Wang, Xuan Sun, Huamei Fu, Gengtao Huang, Kai Tang, Yawen |
| Author_xml | – sequence: 1 givenname: Meng surname: Li fullname: Li, Meng organization: Southeast University – sequence: 2 givenname: Xuan surname: Wang fullname: Wang, Xuan organization: Nanjing Normal University – sequence: 3 givenname: Kun surname: Liu fullname: Liu, Kun organization: Nanjing Normal University – sequence: 4 givenname: Huamei surname: Sun fullname: Sun, Huamei organization: Nanjing Normal University – sequence: 5 givenname: Dongmei surname: Sun fullname: Sun, Dongmei organization: Nanjing Normal University – sequence: 6 givenname: Kai surname: Huang fullname: Huang, Kai organization: Southeast University – sequence: 7 givenname: Yawen surname: Tang fullname: Tang, Yawen organization: Nanjing Normal University – sequence: 8 givenname: Wei surname: Xing fullname: Xing, Wei organization: University of Science and Technology of China – sequence: 9 givenname: Hao surname: Li fullname: Li, Hao email: li.hao.b8@tohoku.ac.jp organization: Tohoku University – sequence: 10 givenname: Gengtao orcidid: 0000-0003-0411-645X surname: Fu fullname: Fu, Gengtao email: gengtaofu@njnu.edu.cn organization: Nanjing Normal University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/37070755$$D View this record in MEDLINE/PubMed |
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| Snippet | Rare‐earth (RE)‐based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their... Rare-earth (RE)-based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet the knowledge regarding their... |
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| SubjectTerms | 4f buffer bands Absorption spectroscopy Ce─O─Co unit site Coupling Co─O covalency gradient orbital coupling oxygen evolution Oxygen evolution reactions Raman spectroscopy Spectrum analysis Structural design Transition metal oxides |
| Title | Reinforcing CoO Covalency via Ce(4f)─O(2p)─Co(3d) Gradient Orbital Coupling for High‐Efficiency Oxygen Evolution |
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