Efficient electrocatalytic nitrogen oxidation to nitrate by the self-assembly of supramolecular cucurbit[6]uril with a heteropolyacid
Developing low-cost and sustainable catalytic systems to realize efficient nitrogen fixation has always been the pursued goal. Here, we report an efficient electrocatalyst synthesized via a simple self-assembly process from supramolecular cucurbit[6]uril (Q[6]) and a heteropolyacid for nitrogen oxid...
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Veröffentlicht in: | Inorganic chemistry frontiers 2024-02, Vol.11 (4), p.1117-1122 |
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creator | Xu, Manli Ao, Xianyan Song, Chengcheng Zeng, Liling Zhang, Chao Zhang, Yunqian Zhao, Wenfeng |
description | Developing low-cost and sustainable catalytic systems to realize efficient nitrogen fixation has always been the pursued goal. Here, we report an efficient electrocatalyst synthesized
via
a simple self-assembly process from supramolecular cucurbit[6]uril (Q[6]) and a heteropolyacid for nitrogen oxidation. The as-prepared self-assembly material Q[6]-PMA with high stability and specific surface area shows a prominent activity in the electrocatalytic nitrogen oxidation reaction (NOR), affording a yield of nitrate (NO
3
−
) of up to 271.5 ± 5.6 μg h
−1
mg
cat
−1
with a Faraday efficiency (FE) of 71.2 ± 3.8%. The
15
N isotope-labeling experiment confirmed that the nitrogen source of nitrate formation is derived from N
2
. The results of the
in situ
XPS technique and
in situ
FITR experiments demonstrate that the molybdenum center of Q[6]-PMA is the main active site of the NOR and the corresponding cucurbit[6]uril unit is conducive to the stability of key intermediates.
A supramolecular self-assembler of cucurbit[6]uril-phosphomolybdic acid with a multi-valence state is constructed to realize an efficient nitrogen oxidation reaction. |
doi_str_mv | 10.1039/d3qi02278a |
format | Article |
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via
a simple self-assembly process from supramolecular cucurbit[6]uril (Q[6]) and a heteropolyacid for nitrogen oxidation. The as-prepared self-assembly material Q[6]-PMA with high stability and specific surface area shows a prominent activity in the electrocatalytic nitrogen oxidation reaction (NOR), affording a yield of nitrate (NO
3
−
) of up to 271.5 ± 5.6 μg h
−1
mg
cat
−1
with a Faraday efficiency (FE) of 71.2 ± 3.8%. The
15
N isotope-labeling experiment confirmed that the nitrogen source of nitrate formation is derived from N
2
. The results of the
in situ
XPS technique and
in situ
FITR experiments demonstrate that the molybdenum center of Q[6]-PMA is the main active site of the NOR and the corresponding cucurbit[6]uril unit is conducive to the stability of key intermediates.
A supramolecular self-assembler of cucurbit[6]uril-phosphomolybdic acid with a multi-valence state is constructed to realize an efficient nitrogen oxidation reaction.</description><identifier>ISSN: 2052-1553</identifier><identifier>ISSN: 2052-1545</identifier><identifier>EISSN: 2052-1553</identifier><identifier>DOI: 10.1039/d3qi02278a</identifier><language>eng</language><publisher>London: Royal Society of Chemistry</publisher><subject>Electrocatalysts ; Nitrogenation ; Oxidation ; Self-assembly ; Surface stability</subject><ispartof>Inorganic chemistry frontiers, 2024-02, Vol.11 (4), p.1117-1122</ispartof><rights>Copyright Royal Society of Chemistry 2024</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c240t-fa9e0b4162ebdc1dff1bbc2baf1ef91c31273e32c4a44e36a9e327c35e1e893e3</cites><orcidid>0000-0003-2638-1457</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids></links><search><creatorcontrib>Xu, Manli</creatorcontrib><creatorcontrib>Ao, Xianyan</creatorcontrib><creatorcontrib>Song, Chengcheng</creatorcontrib><creatorcontrib>Zeng, Liling</creatorcontrib><creatorcontrib>Zhang, Chao</creatorcontrib><creatorcontrib>Zhang, Yunqian</creatorcontrib><creatorcontrib>Zhao, Wenfeng</creatorcontrib><title>Efficient electrocatalytic nitrogen oxidation to nitrate by the self-assembly of supramolecular cucurbit[6]uril with a heteropolyacid</title><title>Inorganic chemistry frontiers</title><description>Developing low-cost and sustainable catalytic systems to realize efficient nitrogen fixation has always been the pursued goal. Here, we report an efficient electrocatalyst synthesized
via
a simple self-assembly process from supramolecular cucurbit[6]uril (Q[6]) and a heteropolyacid for nitrogen oxidation. The as-prepared self-assembly material Q[6]-PMA with high stability and specific surface area shows a prominent activity in the electrocatalytic nitrogen oxidation reaction (NOR), affording a yield of nitrate (NO
3
−
) of up to 271.5 ± 5.6 μg h
−1
mg
cat
−1
with a Faraday efficiency (FE) of 71.2 ± 3.8%. The
15
N isotope-labeling experiment confirmed that the nitrogen source of nitrate formation is derived from N
2
. The results of the
in situ
XPS technique and
in situ
FITR experiments demonstrate that the molybdenum center of Q[6]-PMA is the main active site of the NOR and the corresponding cucurbit[6]uril unit is conducive to the stability of key intermediates.
A supramolecular self-assembler of cucurbit[6]uril-phosphomolybdic acid with a multi-valence state is constructed to realize an efficient nitrogen oxidation reaction.</description><subject>Electrocatalysts</subject><subject>Nitrogenation</subject><subject>Oxidation</subject><subject>Self-assembly</subject><subject>Surface stability</subject><issn>2052-1553</issn><issn>2052-1545</issn><issn>2052-1553</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNpNkV1LwzAUhosoOKY33gsB74Rqvtqul2NOHQxE0CuRkqQnLiNruiRF-wP839ZN1Kvz9fC-8J4kOSP4imBWXtdsazClxUQcJCOKM5qSLGOH__rj5DSENcaYEI5JjkfJ51xroww0EYEFFb1TIgrbR6NQY4bxDRrkPkwtonENim63FRGQ7FFcAQpgdSpCgI20PXIaha71YuMGsc4Kj1SnOi9NfMlfO28sejdxhQRaQQTvWmd7oUx9khxpYQOc_tRx8nw7f5rdp8uHu8VsukwV5TimWpSAJSc5BVkrUmtNpFRUCk1Al0QxQgsGjCouOAeWDzijhWIZEJiUw2WcXOx1W--2HYRYrV3nm8GyoiXNOMl4MRmoyz2lvAvBg65abzbC9xXB1XfS1Q17XOySng7w-R72Qf1yf59gX7N4frw</recordid><startdate>20240213</startdate><enddate>20240213</enddate><creator>Xu, Manli</creator><creator>Ao, Xianyan</creator><creator>Song, Chengcheng</creator><creator>Zeng, Liling</creator><creator>Zhang, Chao</creator><creator>Zhang, Yunqian</creator><creator>Zhao, Wenfeng</creator><general>Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><orcidid>https://orcid.org/0000-0003-2638-1457</orcidid></search><sort><creationdate>20240213</creationdate><title>Efficient electrocatalytic nitrogen oxidation to nitrate by the self-assembly of supramolecular cucurbit[6]uril with a heteropolyacid</title><author>Xu, Manli ; Ao, Xianyan ; Song, Chengcheng ; Zeng, Liling ; Zhang, Chao ; Zhang, Yunqian ; Zhao, Wenfeng</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c240t-fa9e0b4162ebdc1dff1bbc2baf1ef91c31273e32c4a44e36a9e327c35e1e893e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Electrocatalysts</topic><topic>Nitrogenation</topic><topic>Oxidation</topic><topic>Self-assembly</topic><topic>Surface stability</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Xu, Manli</creatorcontrib><creatorcontrib>Ao, Xianyan</creatorcontrib><creatorcontrib>Song, Chengcheng</creatorcontrib><creatorcontrib>Zeng, Liling</creatorcontrib><creatorcontrib>Zhang, Chao</creatorcontrib><creatorcontrib>Zhang, Yunqian</creatorcontrib><creatorcontrib>Zhao, Wenfeng</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><jtitle>Inorganic chemistry frontiers</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Xu, Manli</au><au>Ao, Xianyan</au><au>Song, Chengcheng</au><au>Zeng, Liling</au><au>Zhang, Chao</au><au>Zhang, Yunqian</au><au>Zhao, Wenfeng</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Efficient electrocatalytic nitrogen oxidation to nitrate by the self-assembly of supramolecular cucurbit[6]uril with a heteropolyacid</atitle><jtitle>Inorganic chemistry frontiers</jtitle><date>2024-02-13</date><risdate>2024</risdate><volume>11</volume><issue>4</issue><spage>1117</spage><epage>1122</epage><pages>1117-1122</pages><issn>2052-1553</issn><issn>2052-1545</issn><eissn>2052-1553</eissn><abstract>Developing low-cost and sustainable catalytic systems to realize efficient nitrogen fixation has always been the pursued goal. Here, we report an efficient electrocatalyst synthesized
via
a simple self-assembly process from supramolecular cucurbit[6]uril (Q[6]) and a heteropolyacid for nitrogen oxidation. The as-prepared self-assembly material Q[6]-PMA with high stability and specific surface area shows a prominent activity in the electrocatalytic nitrogen oxidation reaction (NOR), affording a yield of nitrate (NO
3
−
) of up to 271.5 ± 5.6 μg h
−1
mg
cat
−1
with a Faraday efficiency (FE) of 71.2 ± 3.8%. The
15
N isotope-labeling experiment confirmed that the nitrogen source of nitrate formation is derived from N
2
. The results of the
in situ
XPS technique and
in situ
FITR experiments demonstrate that the molybdenum center of Q[6]-PMA is the main active site of the NOR and the corresponding cucurbit[6]uril unit is conducive to the stability of key intermediates.
A supramolecular self-assembler of cucurbit[6]uril-phosphomolybdic acid with a multi-valence state is constructed to realize an efficient nitrogen oxidation reaction.</abstract><cop>London</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d3qi02278a</doi><tpages>6</tpages><orcidid>https://orcid.org/0000-0003-2638-1457</orcidid></addata></record> |
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source | Royal Society Of Chemistry Journals 2008- |
subjects | Electrocatalysts Nitrogenation Oxidation Self-assembly Surface stability |
title | Efficient electrocatalytic nitrogen oxidation to nitrate by the self-assembly of supramolecular cucurbit[6]uril with a heteropolyacid |
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