Uncovering Interfacial Oxygen‐Bridged Binuclear Metal Centers of Heterogenized Molecular Catalyst for Water Electrolysis

The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule‐electrode and electrochemical interfaces remains a great challenge....

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Published inAdvanced science Vol. 12; no. 22; pp. e2417607 - n/a
Main Authors Yu, Zhou, Li, Jian‐Ping, Xu, Xian‐Kun, Ding, Zhong‐Chen, Peng, Xiao‐Hui, Gao, Yi‐Jing, Wan, Qiang, Zheng, Ju‐Fang, Zhou, Xiao‐Shun, Wang, Ya‐Hao
Format Journal Article
LanguageEnglish
Published Germany John Wiley & Sons, Inc 01.06.2025
John Wiley and Sons Inc
Wiley
Subjects
Copper
copper‐bipyridine complexes
Electrodes
heterogenized molecular catalyst
in situ Raman spectroscopy
Ligands
Oxidation
oxygen evolution reaction
spectroelectrochemistry
Spectrum analysis
Voltammetry
Water
copper‐bipyridine complexes
in situ Raman spectroscopy
spectroelectrochemistry
oxygen evolution reaction
heterogenized molecular catalyst
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Abstract The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule‐electrode and electrochemical interfaces remains a great challenge. Herein, shell‐isolated nanoparticle‐enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide‐2‐2′ bipyridine on Au electrode ((bpy)Cu(OH)2/Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH)2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O2‐Au with oxygen‐bridged binuclear metal centers of Cu(III)‐O‐Au for the OER. As the potential further increases, Cu(III)‐O‐Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O2. Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)‐O‐Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)‐O‐Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential‐determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized‐molecule catalysts for the development and application of renewable energy conversion devices. In situ Raman monitoring of an electrochemically induced interfacial oxygen‐bridged Cu(III)‐O‐Au binuclear center in heterogenized molecular catalysts, could combine surface hydroxyl groups to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O2. This significantly modifies the elementary reaction steps and lowers the overpotential for oxygen evolution reaction.
AbstractList The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule-electrode and electrochemical interfaces remains a great challenge. Herein, shell-isolated nanoparticle-enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide-2-2' bipyridine on Au electrode ((bpy)Cu(OH) /Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH) oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O -Au with oxygen-bridged binuclear metal centers of Cu(III)-O-Au for the OER. As the potential further increases, Cu(III)-O-Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)-OOH-Au, which then turns into Cu(III)-OO-Au to release O . Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)-O-Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)-O-Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential-determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized-molecule catalysts for the development and application of renewable energy conversion devices.
The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule-electrode and electrochemical interfaces remains a great challenge. Herein, shell-isolated nanoparticle-enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide-2-2' bipyridine on Au electrode ((bpy)Cu(OH)2/Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH)2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O2-Au with oxygen-bridged binuclear metal centers of Cu(III)-O-Au for the OER. As the potential further increases, Cu(III)-O-Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)-OOH-Au, which then turns into Cu(III)-OO-Au to release O2. Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)-O-Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)-O-Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential-determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized-molecule catalysts for the development and application of renewable energy conversion devices.The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule-electrode and electrochemical interfaces remains a great challenge. Herein, shell-isolated nanoparticle-enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide-2-2' bipyridine on Au electrode ((bpy)Cu(OH)2/Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH)2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O2-Au with oxygen-bridged binuclear metal centers of Cu(III)-O-Au for the OER. As the potential further increases, Cu(III)-O-Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)-OOH-Au, which then turns into Cu(III)-OO-Au to release O2. Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)-O-Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)-O-Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential-determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized-molecule catalysts for the development and application of renewable energy conversion devices.
Abstract The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule‐electrode and electrochemical interfaces remains a great challenge. Herein, shell‐isolated nanoparticle‐enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide‐2‐2′ bipyridine on Au electrode ((bpy)Cu(OH)2/Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH)2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O2‐Au with oxygen‐bridged binuclear metal centers of Cu(III)‐O‐Au for the OER. As the potential further increases, Cu(III)‐O‐Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O2. Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)‐O‐Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)‐O‐Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential‐determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized‐molecule catalysts for the development and application of renewable energy conversion devices.
The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule‐electrode and electrochemical interfaces remains a great challenge. Herein, shell‐isolated nanoparticle‐enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide‐2‐2′ bipyridine on Au electrode ((bpy)Cu(OH)2/Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH)2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O2‐Au with oxygen‐bridged binuclear metal centers of Cu(III)‐O‐Au for the OER. As the potential further increases, Cu(III)‐O‐Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O2. Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)‐O‐Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)‐O‐Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential‐determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized‐molecule catalysts for the development and application of renewable energy conversion devices.
The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule‐electrode and electrochemical interfaces remains a great challenge. Herein, shell‐isolated nanoparticle‐enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide‐2‐2′ bipyridine on Au electrode ((bpy)Cu(OH)2/Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH)2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O2‐Au with oxygen‐bridged binuclear metal centers of Cu(III)‐O‐Au for the OER. As the potential further increases, Cu(III)‐O‐Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O2. Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)‐O‐Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)‐O‐Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential‐determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized‐molecule catalysts for the development and application of renewable energy conversion devices. In situ Raman monitoring of an electrochemically induced interfacial oxygen‐bridged Cu(III)‐O‐Au binuclear center in heterogenized molecular catalysts, could combine surface hydroxyl groups to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O2. This significantly modifies the elementary reaction steps and lowers the overpotential for oxygen evolution reaction.
The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule‐electrode and electrochemical interfaces remains a great challenge. Herein, shell‐isolated nanoparticle‐enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide‐2‐2′ bipyridine on Au electrode ((bpy)Cu(OH) 2 /Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH) 2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O 2 ‐Au with oxygen‐bridged binuclear metal centers of Cu(III)‐O‐Au for the OER. As the potential further increases, Cu(III)‐O‐Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O 2 . Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)‐O‐Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)‐O‐Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential‐determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized‐molecule catalysts for the development and application of renewable energy conversion devices. In situ Raman monitoring of an electrochemically induced interfacial oxygen‐bridged Cu(III)‐O‐Au binuclear center in heterogenized molecular catalysts, could combine surface hydroxyl groups to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O 2 . This significantly modifies the elementary reaction steps and lowers the overpotential for oxygen evolution reaction.
The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in photo/electrocatalysis. However, yielding their catalytic mechanisms at complex molecule‐electrode and electrochemical interfaces remains a great challenge. Herein, shell‐isolated nanoparticle‐enhanced Raman spectroscopy is employed to elucidate the dynamic process, interfacial structure, and intermediates of copper hydroxide‐2‐2′ bipyridine on Au electrode ((bpy)Cu(OH) 2 /Au) during the oxygen evolution reaction (OER). Direct Raman molecular evidences reveal that the interfacial (bpy)Cu(OH) 2 oxidizes into Cu(III) and bridges to Au atoms via oxygenated species, forming (bpy)Cu(III)O 2 ‐Au with oxygen‐bridged binuclear metal centers of Cu(III)‐O‐Au for the OER. As the potential further increases, Cu(III)‐O‐Au combines with surface hydroxyl groups (*OH) to form the important intermediate of Cu(III)‐OOH‐Au, which then turns into Cu(III)‐OO‐Au to release O 2 . Furthermore, in situ electrochemical impedance spectroscopy proves that the Cu(III)‐O‐Au has lower resistance and faster mass transport of hydroxy to enhance OER. Theoretical calculations reveal that the formation of Cu(III)‐O‐Au significantly modify the elementary reaction steps of the OER, resulting in a lower potential‐determining step of ≈0.58 V than that of bare Au. This work provides new insights into the OER mechanism of immobilized‐molecule catalysts for the development and application of renewable energy conversion devices.
Author Yu, Zhou
Xu, Xian‐Kun
Ding, Zhong‐Chen
Wan, Qiang
Gao, Yi‐Jing
Wang, Ya‐Hao
Li, Jian‐Ping
Zhou, Xiao‐Shun
Peng, Xiao‐Hui
Zheng, Ju‐Fang
AuthorAffiliation 2 Zhejiang Engineering Laboratory for Green Syntheses and Applications of Fluorine‐Containing Specialty Chemicals Institute of Advanced Fluorine‐Containing Materials Zhejiang Normal University Jinhua 321004 P. R. China
1 Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical Chemistry College of Chemistry and Materials Science Zhejiang Normal University Jinhua 321004 P. R. China
AuthorAffiliation_xml – name: 2 Zhejiang Engineering Laboratory for Green Syntheses and Applications of Fluorine‐Containing Specialty Chemicals Institute of Advanced Fluorine‐Containing Materials Zhejiang Normal University Jinhua 321004 P. R. China
– name: 1 Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical Chemistry College of Chemistry and Materials Science Zhejiang Normal University Jinhua 321004 P. R. China
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BackLink https://www.ncbi.nlm.nih.gov/pubmed/40159461$$D View this record in MEDLINE/PubMed
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Issue 22
Keywords copper‐bipyridine complexes
in situ Raman spectroscopy
spectroelectrochemistry
oxygen evolution reaction
heterogenized molecular catalyst
Language English
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Snippet The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in...
Abstract The success of different heterogeneous strategies of organometallic catalysts has been demonstrated to achieve high selectivity and activity in...
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SubjectTerms Copper
copper‐bipyridine complexes
Electrodes
heterogenized molecular catalyst
in situ Raman spectroscopy
Ligands
Oxidation
oxygen evolution reaction
spectroelectrochemistry
Spectrum analysis
Voltammetry
Water
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Title Uncovering Interfacial Oxygen‐Bridged Binuclear Metal Centers of Heterogenized Molecular Catalyst for Water Electrolysis
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