Light-induced hydrogen production from water using nickel() catalysts and N-doped carbon-dot photosensitizers: catalytic efficiency enhancement by increase of catalyst nuclearity
Solar energy conversion to chemical energy via light-induced H 2 O splitting to O 2 and H 2 is considered to be a promising solution to meet the growing global energy demands. To make this transformation economically viable, it is necessary to develop sustainable photocatalytic systems. Herein, we p...
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Veröffentlicht in: | Dalton transactions : an international journal of inorganic chemistry 2023-07, Vol.52 (28), p.989-9822 |
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creator | Gioftsidou, Dimitra K Landrou, Georgios Tzatza, Charikleia Hatzidimitriou, Antonios Orfanos, Emmanouil Charalambidis, Georgios Ladomenou, Kalliopi Coutsolelos, Athanassios G Angaridis, Panagiotis A |
description | Solar energy conversion to chemical energy
via
light-induced H
2
O splitting to O
2
and H
2
is considered to be a promising solution to meet the growing global energy demands. To make this transformation economically viable, it is necessary to develop sustainable photocatalytic systems. Herein, we present an efficient photocatalytic H
2
production system which relies on components comprised of low-cost and high-abundance elements. In particular, a series of mononuclear complexes [Ni(L
N
S)
3
]
−
and [Ni(N
^
N)(L
N
S)
2
] and a hexanuclear complex [Ni(L
N
S)
2
]
6
(N
^
N = diimine and L
N
S
−
= heterocyclic thioamidate with different group-substituents) were synthesized and utilized as catalysts, in combination with N-doped carbon dots as photosensitizer, for efficient H
2
evolution from aqueous protons. Differences in H
2
production efficiency were observed among the studied Ni(
ii
) catalysts, with complexes bearing ligands with stronger electron-donating ability exhibiting higher catalytic activity. A remarkable catalytic efficiency enhancement was observed for the hexanuclear complex, with catalyst loadings lower than those of the mononuclear Ni(
ii
) complexes, affording TONs >1550 (among the highest values reported for photocatalytic systems of similar type operating in H
2
O). These data provide an indication of catalytic cooperativity between the metal centers of the hexanuclear complex, and demonstrate the crucial role of atomically precise polynuclear Ni(
ii
) catalysts in light-induced H
2
production, a result that can guide future catalyst design towards the development of highly efficient, low-cost and environmentally benign photocatalytic systems.
Ni(
ii
) catalysts were synthesized and effectively combined with N-doped carbon dots for light-induced H
2
production in H
2
O; catalyst nuclearity increase and catalytic cooperativity phenomena are key elements for enhanced catalytic activity. |
doi_str_mv | 10.1039/d3dt01052j |
format | Article |
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via
light-induced H
2
O splitting to O
2
and H
2
is considered to be a promising solution to meet the growing global energy demands. To make this transformation economically viable, it is necessary to develop sustainable photocatalytic systems. Herein, we present an efficient photocatalytic H
2
production system which relies on components comprised of low-cost and high-abundance elements. In particular, a series of mononuclear complexes [Ni(L
N
S)
3
]
−
and [Ni(N
^
N)(L
N
S)
2
] and a hexanuclear complex [Ni(L
N
S)
2
]
6
(N
^
N = diimine and L
N
S
−
= heterocyclic thioamidate with different group-substituents) were synthesized and utilized as catalysts, in combination with N-doped carbon dots as photosensitizer, for efficient H
2
evolution from aqueous protons. Differences in H
2
production efficiency were observed among the studied Ni(
ii
) catalysts, with complexes bearing ligands with stronger electron-donating ability exhibiting higher catalytic activity. A remarkable catalytic efficiency enhancement was observed for the hexanuclear complex, with catalyst loadings lower than those of the mononuclear Ni(
ii
) complexes, affording TONs >1550 (among the highest values reported for photocatalytic systems of similar type operating in H
2
O). These data provide an indication of catalytic cooperativity between the metal centers of the hexanuclear complex, and demonstrate the crucial role of atomically precise polynuclear Ni(
ii
) catalysts in light-induced H
2
production, a result that can guide future catalyst design towards the development of highly efficient, low-cost and environmentally benign photocatalytic systems.
Ni(
ii
) catalysts were synthesized and effectively combined with N-doped carbon dots for light-induced H
2
production in H
2
O; catalyst nuclearity increase and catalytic cooperativity phenomena are key elements for enhanced catalytic activity.</description><identifier>ISSN: 1477-9226</identifier><identifier>EISSN: 1477-9234</identifier><identifier>DOI: 10.1039/d3dt01052j</identifier><identifier>PMID: 37401385</identifier><language>eng</language><publisher>England: Royal Society of Chemistry</publisher><subject>Carbon ; Catalysts ; Catalytic activity ; Catalytic converters ; Chemical energy ; Chemical synthesis ; Efficiency ; Hydrogen evolution ; Hydrogen production ; Low cost ; Photocatalysis ; Solar energy conversion</subject><ispartof>Dalton transactions : an international journal of inorganic chemistry, 2023-07, Vol.52 (28), p.989-9822</ispartof><rights>Copyright Royal Society of Chemistry 2023</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c296t-a1e7b29b8020e4fce79a92547fc18b925b6be9fd5187c188ef41a3a092a19e0b3</cites><orcidid>0000-0001-5682-2968 ; 0000-0003-3195-802X ; 0000-0002-1733-9225 ; 0000-0002-8508-1369 ; 0000-0003-1237-9962</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37401385$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Gioftsidou, Dimitra K</creatorcontrib><creatorcontrib>Landrou, Georgios</creatorcontrib><creatorcontrib>Tzatza, Charikleia</creatorcontrib><creatorcontrib>Hatzidimitriou, Antonios</creatorcontrib><creatorcontrib>Orfanos, Emmanouil</creatorcontrib><creatorcontrib>Charalambidis, Georgios</creatorcontrib><creatorcontrib>Ladomenou, Kalliopi</creatorcontrib><creatorcontrib>Coutsolelos, Athanassios G</creatorcontrib><creatorcontrib>Angaridis, Panagiotis A</creatorcontrib><title>Light-induced hydrogen production from water using nickel() catalysts and N-doped carbon-dot photosensitizers: catalytic efficiency enhancement by increase of catalyst nuclearity</title><title>Dalton transactions : an international journal of inorganic chemistry</title><addtitle>Dalton Trans</addtitle><description>Solar energy conversion to chemical energy
via
light-induced H
2
O splitting to O
2
and H
2
is considered to be a promising solution to meet the growing global energy demands. To make this transformation economically viable, it is necessary to develop sustainable photocatalytic systems. Herein, we present an efficient photocatalytic H
2
production system which relies on components comprised of low-cost and high-abundance elements. In particular, a series of mononuclear complexes [Ni(L
N
S)
3
]
−
and [Ni(N
^
N)(L
N
S)
2
] and a hexanuclear complex [Ni(L
N
S)
2
]
6
(N
^
N = diimine and L
N
S
−
= heterocyclic thioamidate with different group-substituents) were synthesized and utilized as catalysts, in combination with N-doped carbon dots as photosensitizer, for efficient H
2
evolution from aqueous protons. Differences in H
2
production efficiency were observed among the studied Ni(
ii
) catalysts, with complexes bearing ligands with stronger electron-donating ability exhibiting higher catalytic activity. A remarkable catalytic efficiency enhancement was observed for the hexanuclear complex, with catalyst loadings lower than those of the mononuclear Ni(
ii
) complexes, affording TONs >1550 (among the highest values reported for photocatalytic systems of similar type operating in H
2
O). These data provide an indication of catalytic cooperativity between the metal centers of the hexanuclear complex, and demonstrate the crucial role of atomically precise polynuclear Ni(
ii
) catalysts in light-induced H
2
production, a result that can guide future catalyst design towards the development of highly efficient, low-cost and environmentally benign photocatalytic systems.
Ni(
ii
) catalysts were synthesized and effectively combined with N-doped carbon dots for light-induced H
2
production in H
2
O; catalyst nuclearity increase and catalytic cooperativity phenomena are key elements for enhanced catalytic activity.</description><subject>Carbon</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Catalytic converters</subject><subject>Chemical energy</subject><subject>Chemical synthesis</subject><subject>Efficiency</subject><subject>Hydrogen evolution</subject><subject>Hydrogen production</subject><subject>Low cost</subject><subject>Photocatalysis</subject><subject>Solar energy conversion</subject><issn>1477-9226</issn><issn>1477-9234</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNpdkstu1DAUhi0EoqWwYQ-y1E1BCviSTGJ2VVsoaASbso58OZ7xkNiD7QiFx-oT4mGGQerq3D7_ts5vhF5S8o4SLt4bbjKhpGGbR-iU1m1bCcbrx8ecLU7Qs5Q2hDBWqKfohLc1obxrTtH90q3WuXLeTBoMXs8mhhV4vI2hdLILHtsYRvxLZoh4Ss6vsHf6BwwXb7CWWQ5zyglLb_DXyoRt0dAyquBLkfF2HXJI4JPL7jfE9OFwJDuNwVqnHXg9Y_Br6TWM4DNWM3ZeR5AJcLDHK7Cf9AAyujw_R0-sHBK8OMQz9P3jzd3VbbX89unz1eWy0kwsciUptIoJ1RFGoLYaWiEFa-rWatqpkqmFAmFNQ7u2dDqwNZVcEsEkFUAUP0MXe92yi58TpNyPLmkYBukhTKlnHedkJ1gX9PwBuglT9OV1O6pr2uITLdTbPaVjSCmC7bfRjTLOPSX9zsn-ml_f_XXyS4FfHyQnNYI5ov-sK8CrPRCTPk7_fwX-BzTYpws</recordid><startdate>20230718</startdate><enddate>20230718</enddate><creator>Gioftsidou, Dimitra K</creator><creator>Landrou, Georgios</creator><creator>Tzatza, Charikleia</creator><creator>Hatzidimitriou, Antonios</creator><creator>Orfanos, Emmanouil</creator><creator>Charalambidis, Georgios</creator><creator>Ladomenou, Kalliopi</creator><creator>Coutsolelos, Athanassios G</creator><creator>Angaridis, Panagiotis A</creator><general>Royal Society of Chemistry</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0001-5682-2968</orcidid><orcidid>https://orcid.org/0000-0003-3195-802X</orcidid><orcidid>https://orcid.org/0000-0002-1733-9225</orcidid><orcidid>https://orcid.org/0000-0002-8508-1369</orcidid><orcidid>https://orcid.org/0000-0003-1237-9962</orcidid></search><sort><creationdate>20230718</creationdate><title>Light-induced hydrogen production from water using nickel() catalysts and N-doped carbon-dot photosensitizers: catalytic efficiency enhancement by increase of catalyst nuclearity</title><author>Gioftsidou, Dimitra K ; Landrou, Georgios ; Tzatza, Charikleia ; Hatzidimitriou, Antonios ; Orfanos, Emmanouil ; Charalambidis, Georgios ; Ladomenou, Kalliopi ; Coutsolelos, Athanassios G ; Angaridis, Panagiotis A</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c296t-a1e7b29b8020e4fce79a92547fc18b925b6be9fd5187c188ef41a3a092a19e0b3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Carbon</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Catalytic converters</topic><topic>Chemical energy</topic><topic>Chemical synthesis</topic><topic>Efficiency</topic><topic>Hydrogen evolution</topic><topic>Hydrogen production</topic><topic>Low cost</topic><topic>Photocatalysis</topic><topic>Solar energy conversion</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Gioftsidou, Dimitra K</creatorcontrib><creatorcontrib>Landrou, Georgios</creatorcontrib><creatorcontrib>Tzatza, Charikleia</creatorcontrib><creatorcontrib>Hatzidimitriou, Antonios</creatorcontrib><creatorcontrib>Orfanos, Emmanouil</creatorcontrib><creatorcontrib>Charalambidis, Georgios</creatorcontrib><creatorcontrib>Ladomenou, Kalliopi</creatorcontrib><creatorcontrib>Coutsolelos, Athanassios G</creatorcontrib><creatorcontrib>Angaridis, Panagiotis A</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Gioftsidou, Dimitra K</au><au>Landrou, Georgios</au><au>Tzatza, Charikleia</au><au>Hatzidimitriou, Antonios</au><au>Orfanos, Emmanouil</au><au>Charalambidis, Georgios</au><au>Ladomenou, Kalliopi</au><au>Coutsolelos, Athanassios G</au><au>Angaridis, Panagiotis A</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Light-induced hydrogen production from water using nickel() catalysts and N-doped carbon-dot photosensitizers: catalytic efficiency enhancement by increase of catalyst nuclearity</atitle><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle><addtitle>Dalton Trans</addtitle><date>2023-07-18</date><risdate>2023</risdate><volume>52</volume><issue>28</issue><spage>989</spage><epage>9822</epage><pages>989-9822</pages><issn>1477-9226</issn><eissn>1477-9234</eissn><abstract>Solar energy conversion to chemical energy
via
light-induced H
2
O splitting to O
2
and H
2
is considered to be a promising solution to meet the growing global energy demands. To make this transformation economically viable, it is necessary to develop sustainable photocatalytic systems. Herein, we present an efficient photocatalytic H
2
production system which relies on components comprised of low-cost and high-abundance elements. In particular, a series of mononuclear complexes [Ni(L
N
S)
3
]
−
and [Ni(N
^
N)(L
N
S)
2
] and a hexanuclear complex [Ni(L
N
S)
2
]
6
(N
^
N = diimine and L
N
S
−
= heterocyclic thioamidate with different group-substituents) were synthesized and utilized as catalysts, in combination with N-doped carbon dots as photosensitizer, for efficient H
2
evolution from aqueous protons. Differences in H
2
production efficiency were observed among the studied Ni(
ii
) catalysts, with complexes bearing ligands with stronger electron-donating ability exhibiting higher catalytic activity. A remarkable catalytic efficiency enhancement was observed for the hexanuclear complex, with catalyst loadings lower than those of the mononuclear Ni(
ii
) complexes, affording TONs >1550 (among the highest values reported for photocatalytic systems of similar type operating in H
2
O). These data provide an indication of catalytic cooperativity between the metal centers of the hexanuclear complex, and demonstrate the crucial role of atomically precise polynuclear Ni(
ii
) catalysts in light-induced H
2
production, a result that can guide future catalyst design towards the development of highly efficient, low-cost and environmentally benign photocatalytic systems.
Ni(
ii
) catalysts were synthesized and effectively combined with N-doped carbon dots for light-induced H
2
production in H
2
O; catalyst nuclearity increase and catalytic cooperativity phenomena are key elements for enhanced catalytic activity.</abstract><cop>England</cop><pub>Royal Society of Chemistry</pub><pmid>37401385</pmid><doi>10.1039/d3dt01052j</doi><tpages>14</tpages><orcidid>https://orcid.org/0000-0001-5682-2968</orcidid><orcidid>https://orcid.org/0000-0003-3195-802X</orcidid><orcidid>https://orcid.org/0000-0002-1733-9225</orcidid><orcidid>https://orcid.org/0000-0002-8508-1369</orcidid><orcidid>https://orcid.org/0000-0003-1237-9962</orcidid></addata></record> |
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issn | 1477-9226 1477-9234 |
language | eng |
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source | Royal Society Of Chemistry Journals; Alma/SFX Local Collection |
subjects | Carbon Catalysts Catalytic activity Catalytic converters Chemical energy Chemical synthesis Efficiency Hydrogen evolution Hydrogen production Low cost Photocatalysis Solar energy conversion |
title | Light-induced hydrogen production from water using nickel() catalysts and N-doped carbon-dot photosensitizers: catalytic efficiency enhancement by increase of catalyst nuclearity |
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