Modulating the valence electronic structure of Co3O4 to improve catalytic activity of electrochemical nitrate-to-ammonia conversion
Electrochemical conversion of NO 3 − to NH 3 via the nitrate reduction reaction (NO 3 − RR) is a promising approach for ammonia production and storage of “green hydrogen”. Co 3 O 4 has shown satisfactory Faradaic efficiency toward NH 3 ( FE NH 3 ) and stability, making it a potential electrocatalyst...
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| Veröffentlicht in: | Science China materials 2023-10, Vol.66 (10), p.3901-3911 |
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| creator | Chen, Wenda Chen, Zhida Huang, Zhencheng Zheng, Lirong Zhao, Xiaojuan Hu, Jiangtao Cao, Huiqun Li, Yongliang Ren, Xiangzhong Ouyang, Xiaoping Ye, Shenghua Yan, Xueqing Zhang, Qianling Liu, Jianhong |
| description | Electrochemical conversion of NO
3
−
to NH
3
via
the nitrate reduction reaction (NO
3
−
RR) is a promising approach for ammonia production and storage of “green hydrogen”. Co
3
O
4
has shown satisfactory Faradaic efficiency toward
NH
3
(
FE
NH
3
)
and stability, making it a potential electrocatalyst for the NO
3
−
-to-NH
3
conversion. However, the high overpotential required for triggering the NO
3
−
RR on Co
3
O
4
limits its conversion efficiency. In this study, we synthesized Cu-doped Co
3
O
4
porous hollow nanospheres (Cu−Co
3
O
4
PHNSs) for NO
3
−
RR. Cu-doping effectively reduced the required overpotential and improved the NH
3
yield rate on the Co
3
O
4
matrix without reducing
FE
NH
3
and stability. Both experimental and theoretical analyses demonstrated that Cu-doping up-shifted the highest occupied state (HOS) of Co
3
O
4
, narrowed the energy barrier between the HOS of Co
3
O
4
and the lowest unoccupied molecular orbital of NO
3
−
, and thus reduced the overpotential required for triggering the electron transfer from Co
3
O
4
to NO
3
−
, thereby endowing the as-prepared Cu−Co
3
O
4
PHNSs with outstanding electrocatalytic activity and durability for the NO
3
−
-to-NH
3
conversion. This study provides a novel theoretical perspective on the regulation of electrochemical performance. |
| doi_str_mv | 10.1007/s40843-023-2552-1 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_journals_2873978586</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2873978586</sourcerecordid><originalsourceid>FETCH-LOGICAL-c359t-38a22d6e2a657cbf41253120fd4dec1931f1a3fee641d34afcd567e1f984e9d13</originalsourceid><addsrcrecordid>eNp1kE1LxDAQhosoKKs_wFvAczSTj7Y5yuIXrOxFzyGmE420jSbpwp7943bZBU-eZg7P-8zwVtUlsGtgrLnJkrVSUMYF5UpxCkfVGQetqVQMjuedaUVbzuvT6iLnT8YY1ApAt2fVz3Pspt6WML6T8oFkY3scHRLs0ZUUx-BILmlyZUpIoifLKNaSlEjC8JXiBomzxfbbMnPWlbAJZbvDDnH3gUNwtidjKMkWpCVSOwyz1hIXxw2mHOJ4Xp1422e8OMxF9Xp_97J8pKv1w9PydkWdULpQ0VrOuxq5rVXj3rwErgRw5jvZoQMtwIMVHrGW0AlpvetU3SB43UrUHYhFdbX3zp9_T5iL-YxTGueThreN0E2r2nqmYE-5FHNO6M1XCoNNWwPM7Oo2-7rNXLfZ1W12Zr7P5Jkd3zH9mf8P_QLYfoU-</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2873978586</pqid></control><display><type>article</type><title>Modulating the valence electronic structure of Co3O4 to improve catalytic activity of electrochemical nitrate-to-ammonia conversion</title><source>Springer Nature - Complete Springer Journals</source><source>Alma/SFX Local Collection</source><creator>Chen, Wenda ; Chen, Zhida ; Huang, Zhencheng ; Zheng, Lirong ; Zhao, Xiaojuan ; Hu, Jiangtao ; Cao, Huiqun ; Li, Yongliang ; Ren, Xiangzhong ; Ouyang, Xiaoping ; Ye, Shenghua ; Yan, Xueqing ; Zhang, Qianling ; Liu, Jianhong</creator><creatorcontrib>Chen, Wenda ; Chen, Zhida ; Huang, Zhencheng ; Zheng, Lirong ; Zhao, Xiaojuan ; Hu, Jiangtao ; Cao, Huiqun ; Li, Yongliang ; Ren, Xiangzhong ; Ouyang, Xiaoping ; Ye, Shenghua ; Yan, Xueqing ; Zhang, Qianling ; Liu, Jianhong</creatorcontrib><description>Electrochemical conversion of NO
3
−
to NH
3
via
the nitrate reduction reaction (NO
3
−
RR) is a promising approach for ammonia production and storage of “green hydrogen”. Co
3
O
4
has shown satisfactory Faradaic efficiency toward
NH
3
(
FE
NH
3
)
and stability, making it a potential electrocatalyst for the NO
3
−
-to-NH
3
conversion. However, the high overpotential required for triggering the NO
3
−
RR on Co
3
O
4
limits its conversion efficiency. In this study, we synthesized Cu-doped Co
3
O
4
porous hollow nanospheres (Cu−Co
3
O
4
PHNSs) for NO
3
−
RR. Cu-doping effectively reduced the required overpotential and improved the NH
3
yield rate on the Co
3
O
4
matrix without reducing
FE
NH
3
and stability. Both experimental and theoretical analyses demonstrated that Cu-doping up-shifted the highest occupied state (HOS) of Co
3
O
4
, narrowed the energy barrier between the HOS of Co
3
O
4
and the lowest unoccupied molecular orbital of NO
3
−
, and thus reduced the overpotential required for triggering the electron transfer from Co
3
O
4
to NO
3
−
, thereby endowing the as-prepared Cu−Co
3
O
4
PHNSs with outstanding electrocatalytic activity and durability for the NO
3
−
-to-NH
3
conversion. This study provides a novel theoretical perspective on the regulation of electrochemical performance.</description><identifier>ISSN: 2095-8226</identifier><identifier>EISSN: 2199-4501</identifier><identifier>DOI: 10.1007/s40843-023-2552-1</identifier><language>eng</language><publisher>Beijing: Science China Press</publisher><subject>Ammonia ; Catalytic activity ; Catalytic converters ; Chemical reduction ; Chemistry and Materials Science ; Chemistry/Food Science ; Cobalt oxides ; Doping ; Electrocatalysts ; Electrochemical analysis ; Electron transfer ; Electronic structure ; Green hydrogen ; Materials Science ; Molecular orbitals ; Nanospheres ; Stability analysis</subject><ispartof>Science China materials, 2023-10, Vol.66 (10), p.3901-3911</ispartof><rights>Science China Press 2023</rights><rights>Science China Press 2023.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c359t-38a22d6e2a657cbf41253120fd4dec1931f1a3fee641d34afcd567e1f984e9d13</citedby><cites>FETCH-LOGICAL-c359t-38a22d6e2a657cbf41253120fd4dec1931f1a3fee641d34afcd567e1f984e9d13</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1007/s40843-023-2552-1$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s40843-023-2552-1$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>314,776,780,27903,27904,41467,42536,51297</link.rule.ids></links><search><creatorcontrib>Chen, Wenda</creatorcontrib><creatorcontrib>Chen, Zhida</creatorcontrib><creatorcontrib>Huang, Zhencheng</creatorcontrib><creatorcontrib>Zheng, Lirong</creatorcontrib><creatorcontrib>Zhao, Xiaojuan</creatorcontrib><creatorcontrib>Hu, Jiangtao</creatorcontrib><creatorcontrib>Cao, Huiqun</creatorcontrib><creatorcontrib>Li, Yongliang</creatorcontrib><creatorcontrib>Ren, Xiangzhong</creatorcontrib><creatorcontrib>Ouyang, Xiaoping</creatorcontrib><creatorcontrib>Ye, Shenghua</creatorcontrib><creatorcontrib>Yan, Xueqing</creatorcontrib><creatorcontrib>Zhang, Qianling</creatorcontrib><creatorcontrib>Liu, Jianhong</creatorcontrib><title>Modulating the valence electronic structure of Co3O4 to improve catalytic activity of electrochemical nitrate-to-ammonia conversion</title><title>Science China materials</title><addtitle>Sci. China Mater</addtitle><description>Electrochemical conversion of NO
3
−
to NH
3
via
the nitrate reduction reaction (NO
3
−
RR) is a promising approach for ammonia production and storage of “green hydrogen”. Co
3
O
4
has shown satisfactory Faradaic efficiency toward
NH
3
(
FE
NH
3
)
and stability, making it a potential electrocatalyst for the NO
3
−
-to-NH
3
conversion. However, the high overpotential required for triggering the NO
3
−
RR on Co
3
O
4
limits its conversion efficiency. In this study, we synthesized Cu-doped Co
3
O
4
porous hollow nanospheres (Cu−Co
3
O
4
PHNSs) for NO
3
−
RR. Cu-doping effectively reduced the required overpotential and improved the NH
3
yield rate on the Co
3
O
4
matrix without reducing
FE
NH
3
and stability. Both experimental and theoretical analyses demonstrated that Cu-doping up-shifted the highest occupied state (HOS) of Co
3
O
4
, narrowed the energy barrier between the HOS of Co
3
O
4
and the lowest unoccupied molecular orbital of NO
3
−
, and thus reduced the overpotential required for triggering the electron transfer from Co
3
O
4
to NO
3
−
, thereby endowing the as-prepared Cu−Co
3
O
4
PHNSs with outstanding electrocatalytic activity and durability for the NO
3
−
-to-NH
3
conversion. This study provides a novel theoretical perspective on the regulation of electrochemical performance.</description><subject>Ammonia</subject><subject>Catalytic activity</subject><subject>Catalytic converters</subject><subject>Chemical reduction</subject><subject>Chemistry and Materials Science</subject><subject>Chemistry/Food Science</subject><subject>Cobalt oxides</subject><subject>Doping</subject><subject>Electrocatalysts</subject><subject>Electrochemical analysis</subject><subject>Electron transfer</subject><subject>Electronic structure</subject><subject>Green hydrogen</subject><subject>Materials Science</subject><subject>Molecular orbitals</subject><subject>Nanospheres</subject><subject>Stability analysis</subject><issn>2095-8226</issn><issn>2199-4501</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNp1kE1LxDAQhosoKKs_wFvAczSTj7Y5yuIXrOxFzyGmE420jSbpwp7943bZBU-eZg7P-8zwVtUlsGtgrLnJkrVSUMYF5UpxCkfVGQetqVQMjuedaUVbzuvT6iLnT8YY1ApAt2fVz3Pspt6WML6T8oFkY3scHRLs0ZUUx-BILmlyZUpIoifLKNaSlEjC8JXiBomzxfbbMnPWlbAJZbvDDnH3gUNwtidjKMkWpCVSOwyz1hIXxw2mHOJ4Xp1422e8OMxF9Xp_97J8pKv1w9PydkWdULpQ0VrOuxq5rVXj3rwErgRw5jvZoQMtwIMVHrGW0AlpvetU3SB43UrUHYhFdbX3zp9_T5iL-YxTGueThreN0E2r2nqmYE-5FHNO6M1XCoNNWwPM7Oo2-7rNXLfZ1W12Zr7P5Jkd3zH9mf8P_QLYfoU-</recordid><startdate>20231001</startdate><enddate>20231001</enddate><creator>Chen, Wenda</creator><creator>Chen, Zhida</creator><creator>Huang, Zhencheng</creator><creator>Zheng, Lirong</creator><creator>Zhao, Xiaojuan</creator><creator>Hu, Jiangtao</creator><creator>Cao, Huiqun</creator><creator>Li, Yongliang</creator><creator>Ren, Xiangzhong</creator><creator>Ouyang, Xiaoping</creator><creator>Ye, Shenghua</creator><creator>Yan, Xueqing</creator><creator>Zhang, Qianling</creator><creator>Liu, Jianhong</creator><general>Science China Press</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20231001</creationdate><title>Modulating the valence electronic structure of Co3O4 to improve catalytic activity of electrochemical nitrate-to-ammonia conversion</title><author>Chen, Wenda ; Chen, Zhida ; Huang, Zhencheng ; Zheng, Lirong ; Zhao, Xiaojuan ; Hu, Jiangtao ; Cao, Huiqun ; Li, Yongliang ; Ren, Xiangzhong ; Ouyang, Xiaoping ; Ye, Shenghua ; Yan, Xueqing ; Zhang, Qianling ; Liu, Jianhong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c359t-38a22d6e2a657cbf41253120fd4dec1931f1a3fee641d34afcd567e1f984e9d13</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Ammonia</topic><topic>Catalytic activity</topic><topic>Catalytic converters</topic><topic>Chemical reduction</topic><topic>Chemistry and Materials Science</topic><topic>Chemistry/Food Science</topic><topic>Cobalt oxides</topic><topic>Doping</topic><topic>Electrocatalysts</topic><topic>Electrochemical analysis</topic><topic>Electron transfer</topic><topic>Electronic structure</topic><topic>Green hydrogen</topic><topic>Materials Science</topic><topic>Molecular orbitals</topic><topic>Nanospheres</topic><topic>Stability analysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chen, Wenda</creatorcontrib><creatorcontrib>Chen, Zhida</creatorcontrib><creatorcontrib>Huang, Zhencheng</creatorcontrib><creatorcontrib>Zheng, Lirong</creatorcontrib><creatorcontrib>Zhao, Xiaojuan</creatorcontrib><creatorcontrib>Hu, Jiangtao</creatorcontrib><creatorcontrib>Cao, Huiqun</creatorcontrib><creatorcontrib>Li, Yongliang</creatorcontrib><creatorcontrib>Ren, Xiangzhong</creatorcontrib><creatorcontrib>Ouyang, Xiaoping</creatorcontrib><creatorcontrib>Ye, Shenghua</creatorcontrib><creatorcontrib>Yan, Xueqing</creatorcontrib><creatorcontrib>Zhang, Qianling</creatorcontrib><creatorcontrib>Liu, Jianhong</creatorcontrib><collection>CrossRef</collection><jtitle>Science China materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chen, Wenda</au><au>Chen, Zhida</au><au>Huang, Zhencheng</au><au>Zheng, Lirong</au><au>Zhao, Xiaojuan</au><au>Hu, Jiangtao</au><au>Cao, Huiqun</au><au>Li, Yongliang</au><au>Ren, Xiangzhong</au><au>Ouyang, Xiaoping</au><au>Ye, Shenghua</au><au>Yan, Xueqing</au><au>Zhang, Qianling</au><au>Liu, Jianhong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Modulating the valence electronic structure of Co3O4 to improve catalytic activity of electrochemical nitrate-to-ammonia conversion</atitle><jtitle>Science China materials</jtitle><stitle>Sci. China Mater</stitle><date>2023-10-01</date><risdate>2023</risdate><volume>66</volume><issue>10</issue><spage>3901</spage><epage>3911</epage><pages>3901-3911</pages><issn>2095-8226</issn><eissn>2199-4501</eissn><abstract>Electrochemical conversion of NO
3
−
to NH
3
via
the nitrate reduction reaction (NO
3
−
RR) is a promising approach for ammonia production and storage of “green hydrogen”. Co
3
O
4
has shown satisfactory Faradaic efficiency toward
NH
3
(
FE
NH
3
)
and stability, making it a potential electrocatalyst for the NO
3
−
-to-NH
3
conversion. However, the high overpotential required for triggering the NO
3
−
RR on Co
3
O
4
limits its conversion efficiency. In this study, we synthesized Cu-doped Co
3
O
4
porous hollow nanospheres (Cu−Co
3
O
4
PHNSs) for NO
3
−
RR. Cu-doping effectively reduced the required overpotential and improved the NH
3
yield rate on the Co
3
O
4
matrix without reducing
FE
NH
3
and stability. Both experimental and theoretical analyses demonstrated that Cu-doping up-shifted the highest occupied state (HOS) of Co
3
O
4
, narrowed the energy barrier between the HOS of Co
3
O
4
and the lowest unoccupied molecular orbital of NO
3
−
, and thus reduced the overpotential required for triggering the electron transfer from Co
3
O
4
to NO
3
−
, thereby endowing the as-prepared Cu−Co
3
O
4
PHNSs with outstanding electrocatalytic activity and durability for the NO
3
−
-to-NH
3
conversion. This study provides a novel theoretical perspective on the regulation of electrochemical performance.</abstract><cop>Beijing</cop><pub>Science China Press</pub><doi>10.1007/s40843-023-2552-1</doi><tpages>11</tpages><oa>free_for_read</oa></addata></record> |
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| language | eng |
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| source | Springer Nature - Complete Springer Journals; Alma/SFX Local Collection |
| subjects | Ammonia Catalytic activity Catalytic converters Chemical reduction Chemistry and Materials Science Chemistry/Food Science Cobalt oxides Doping Electrocatalysts Electrochemical analysis Electron transfer Electronic structure Green hydrogen Materials Science Molecular orbitals Nanospheres Stability analysis |
| title | Modulating the valence electronic structure of Co3O4 to improve catalytic activity of electrochemical nitrate-to-ammonia conversion |
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