Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte
A copper complex based on the pentadentate aminopyridine ligand [(9-methyl-1,10-phenanthrolin-2-yl)methyl]bis-(pyridin-2-ylmethyl)amine (Dmphen-DPA), namely [Cu(Dmphen-DPA)](ClO 4 ) 2 ( 1 ), was synthesized and characterized by elemental analysis, HR-MS spectroscopy and X-ray single crystal diffract...
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| Veröffentlicht in: | New journal of chemistry 2019-11, Vol.43 (46), p.18134-1814 |
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| container_issue | 46 |
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| container_title | New journal of chemistry |
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| creator | Gao, Ying-Chun Zhao, Ying-Guo Song, Xiao-Wei Huang, Rong-Yi Meng, Yan Wang, Jun-Wei Wang, Wen-Jing Chen, Chang-Neng |
| description | A copper complex based on the pentadentate aminopyridine ligand [(9-methyl-1,10-phenanthrolin-2-yl)methyl]bis-(pyridin-2-ylmethyl)amine (Dmphen-DPA), namely [Cu(Dmphen-DPA)](ClO
4
)
2
(
1
), was synthesized and characterized by elemental analysis, HR-MS spectroscopy and X-ray single crystal diffraction. The complex has five-coordinated solid-state structures, but has an open coordination site in acetonitrile. The electrochemical studies reveal that complex
1
has an electrocatalytic proton reduction activity in acetonitrile, when using acetic acid as a proton source with
i
cat
/
i
p
∼ 2.5. DFT calculations suggest that the parent copper complex undergoes two successive reductions to generate the radical species [Cu(
i
)(Dmphen-DPA&z.rad;
−
)]
0
, which is protonated at the low-valence copper center to afford a reactive Cu
II
-H intermediate. The Cu
II
-H species combines bimolecularly and generates H
2
via
reductive elimination.
An aminopyridine-based copper complex was synthesized and investigated for its electrocatalytic proton reduction activity and the plausible mechanism. |
| doi_str_mv | 10.1039/c9nj04275j |
| format | Article |
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4
)
2
(
1
), was synthesized and characterized by elemental analysis, HR-MS spectroscopy and X-ray single crystal diffraction. The complex has five-coordinated solid-state structures, but has an open coordination site in acetonitrile. The electrochemical studies reveal that complex
1
has an electrocatalytic proton reduction activity in acetonitrile, when using acetic acid as a proton source with
i
cat
/
i
p
∼ 2.5. DFT calculations suggest that the parent copper complex undergoes two successive reductions to generate the radical species [Cu(
i
)(Dmphen-DPA&z.rad;
−
)]
0
, which is protonated at the low-valence copper center to afford a reactive Cu
II
-H intermediate. The Cu
II
-H species combines bimolecularly and generates H
2
via
reductive elimination.
An aminopyridine-based copper complex was synthesized and investigated for its electrocatalytic proton reduction activity and the plausible mechanism.</description><identifier>ISSN: 1144-0546</identifier><identifier>EISSN: 1369-9261</identifier><identifier>DOI: 10.1039/c9nj04275j</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Acetic acid ; Acetonitrile ; Cartesian coordinates ; Chemical reduction ; Coordination compounds ; Copper ; Copper compounds ; Crystal structure ; Crystallography ; Ligands ; Nonaqueous electrolytes ; Protons ; Single crystals ; Spectrum analysis ; Zinc compounds</subject><ispartof>New journal of chemistry, 2019-11, Vol.43 (46), p.18134-1814</ispartof><rights>Copyright Royal Society of Chemistry 2019</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c281t-23378432bac6f69cbff6c40856578eb429b9ce1778a3b5556375b6b41d10b1803</citedby><cites>FETCH-LOGICAL-c281t-23378432bac6f69cbff6c40856578eb429b9ce1778a3b5556375b6b41d10b1803</cites><orcidid>0000-0003-0130-5394 ; 0000-0003-2139-1242 ; 0000-0001-9250-3147</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Gao, Ying-Chun</creatorcontrib><creatorcontrib>Zhao, Ying-Guo</creatorcontrib><creatorcontrib>Song, Xiao-Wei</creatorcontrib><creatorcontrib>Huang, Rong-Yi</creatorcontrib><creatorcontrib>Meng, Yan</creatorcontrib><creatorcontrib>Wang, Jun-Wei</creatorcontrib><creatorcontrib>Wang, Wen-Jing</creatorcontrib><creatorcontrib>Chen, Chang-Neng</creatorcontrib><title>Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte</title><title>New journal of chemistry</title><description>A copper complex based on the pentadentate aminopyridine ligand [(9-methyl-1,10-phenanthrolin-2-yl)methyl]bis-(pyridin-2-ylmethyl)amine (Dmphen-DPA), namely [Cu(Dmphen-DPA)](ClO
4
)
2
(
1
), was synthesized and characterized by elemental analysis, HR-MS spectroscopy and X-ray single crystal diffraction. The complex has five-coordinated solid-state structures, but has an open coordination site in acetonitrile. The electrochemical studies reveal that complex
1
has an electrocatalytic proton reduction activity in acetonitrile, when using acetic acid as a proton source with
i
cat
/
i
p
∼ 2.5. DFT calculations suggest that the parent copper complex undergoes two successive reductions to generate the radical species [Cu(
i
)(Dmphen-DPA&z.rad;
−
)]
0
, which is protonated at the low-valence copper center to afford a reactive Cu
II
-H intermediate. The Cu
II
-H species combines bimolecularly and generates H
2
via
reductive elimination.
An aminopyridine-based copper complex was synthesized and investigated for its electrocatalytic proton reduction activity and the plausible mechanism.</description><subject>Acetic acid</subject><subject>Acetonitrile</subject><subject>Cartesian coordinates</subject><subject>Chemical reduction</subject><subject>Coordination compounds</subject><subject>Copper</subject><subject>Copper compounds</subject><subject>Crystal structure</subject><subject>Crystallography</subject><subject>Ligands</subject><subject>Nonaqueous electrolytes</subject><subject>Protons</subject><subject>Single crystals</subject><subject>Spectrum analysis</subject><subject>Zinc compounds</subject><issn>1144-0546</issn><issn>1369-9261</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNpFkU1PwzAMhisEEmNw4Y4UiRtSIWmapDlO2_iYJuAA5ypJ061Vl5Qklegv4G_TUgQX24fHfu3XUXSJ4C2CmN8pbmqYJozUR9EMYcpjnlB0PNQoTWNIUnoanXlfQ4gQo2gWfa0brYKzSgTR9KFSwOmiU6GyBtgStM4GazwIFuz7wtmdNkD2QABl21a7IR3aRn-OaNhr0GoTRDGGoEFT7YQpwOrQ7rWJV68LUJmh01gjPjptOw_0pD3o6vPopBSN1xe_eR6936_flo_x9uXhabnYxirJUIgTjFmW4kQKRUvKlSxLqlKYEUpYpmWacMmVRoxlAktCCMWMSCpTVCAoUQbxPLqe5g6XDVv4kNe2c2aQzBOMWEYw5CN1M1HKWe-dLvPWVQfh-hzBfDQ6X_LnzY_RmwG-mmDn1R_3_wj8DacDfAs</recordid><startdate>20191125</startdate><enddate>20191125</enddate><creator>Gao, Ying-Chun</creator><creator>Zhao, Ying-Guo</creator><creator>Song, Xiao-Wei</creator><creator>Huang, Rong-Yi</creator><creator>Meng, Yan</creator><creator>Wang, Jun-Wei</creator><creator>Wang, Wen-Jing</creator><creator>Chen, Chang-Neng</creator><general>Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>H9R</scope><scope>JG9</scope><scope>KA0</scope><orcidid>https://orcid.org/0000-0003-0130-5394</orcidid><orcidid>https://orcid.org/0000-0003-2139-1242</orcidid><orcidid>https://orcid.org/0000-0001-9250-3147</orcidid></search><sort><creationdate>20191125</creationdate><title>Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte</title><author>Gao, Ying-Chun ; Zhao, Ying-Guo ; Song, Xiao-Wei ; Huang, Rong-Yi ; Meng, Yan ; Wang, Jun-Wei ; Wang, Wen-Jing ; Chen, Chang-Neng</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c281t-23378432bac6f69cbff6c40856578eb429b9ce1778a3b5556375b6b41d10b1803</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Acetic acid</topic><topic>Acetonitrile</topic><topic>Cartesian coordinates</topic><topic>Chemical reduction</topic><topic>Coordination compounds</topic><topic>Copper</topic><topic>Copper compounds</topic><topic>Crystal structure</topic><topic>Crystallography</topic><topic>Ligands</topic><topic>Nonaqueous electrolytes</topic><topic>Protons</topic><topic>Single crystals</topic><topic>Spectrum analysis</topic><topic>Zinc compounds</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Gao, Ying-Chun</creatorcontrib><creatorcontrib>Zhao, Ying-Guo</creatorcontrib><creatorcontrib>Song, Xiao-Wei</creatorcontrib><creatorcontrib>Huang, Rong-Yi</creatorcontrib><creatorcontrib>Meng, Yan</creatorcontrib><creatorcontrib>Wang, Jun-Wei</creatorcontrib><creatorcontrib>Wang, Wen-Jing</creatorcontrib><creatorcontrib>Chen, Chang-Neng</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Illustrata: Natural Sciences</collection><collection>Materials Research Database</collection><collection>ProQuest Illustrata: Technology Collection</collection><jtitle>New journal of chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Gao, Ying-Chun</au><au>Zhao, Ying-Guo</au><au>Song, Xiao-Wei</au><au>Huang, Rong-Yi</au><au>Meng, Yan</au><au>Wang, Jun-Wei</au><au>Wang, Wen-Jing</au><au>Chen, Chang-Neng</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte</atitle><jtitle>New journal of chemistry</jtitle><date>2019-11-25</date><risdate>2019</risdate><volume>43</volume><issue>46</issue><spage>18134</spage><epage>1814</epage><pages>18134-1814</pages><issn>1144-0546</issn><eissn>1369-9261</eissn><abstract>A copper complex based on the pentadentate aminopyridine ligand [(9-methyl-1,10-phenanthrolin-2-yl)methyl]bis-(pyridin-2-ylmethyl)amine (Dmphen-DPA), namely [Cu(Dmphen-DPA)](ClO
4
)
2
(
1
), was synthesized and characterized by elemental analysis, HR-MS spectroscopy and X-ray single crystal diffraction. The complex has five-coordinated solid-state structures, but has an open coordination site in acetonitrile. The electrochemical studies reveal that complex
1
has an electrocatalytic proton reduction activity in acetonitrile, when using acetic acid as a proton source with
i
cat
/
i
p
∼ 2.5. DFT calculations suggest that the parent copper complex undergoes two successive reductions to generate the radical species [Cu(
i
)(Dmphen-DPA&z.rad;
−
)]
0
, which is protonated at the low-valence copper center to afford a reactive Cu
II
-H intermediate. The Cu
II
-H species combines bimolecularly and generates H
2
via
reductive elimination.
An aminopyridine-based copper complex was synthesized and investigated for its electrocatalytic proton reduction activity and the plausible mechanism.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/c9nj04275j</doi><tpages>7</tpages><orcidid>https://orcid.org/0000-0003-0130-5394</orcidid><orcidid>https://orcid.org/0000-0003-2139-1242</orcidid><orcidid>https://orcid.org/0000-0001-9250-3147</orcidid></addata></record> |
| fulltext | fulltext |
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| ispartof | New journal of chemistry, 2019-11, Vol.43 (46), p.18134-1814 |
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| language | eng |
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| source | Royal Society Of Chemistry Journals 2008-; Alma/SFX Local Collection |
| subjects | Acetic acid Acetonitrile Cartesian coordinates Chemical reduction Coordination compounds Copper Copper compounds Crystal structure Crystallography Ligands Nonaqueous electrolytes Protons Single crystals Spectrum analysis Zinc compounds |
| title | Electrocatalytic reduction of protons to hydrogen by a copper complex of the pentadentate ligand Dmphen-DPA in a nonaqueous electrolyte |
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