A MoFe nitrogenase-mimicking electrocatalyst for nitrogen fixation with high faradaic efficiency
Electrochemical conversion of N 2 provides an eco-friendly approach for sustainable ammonia (NH 3 ) production, but most electrocatalysts still suffer from low selectivity. Herein, a new three dimensional (3D) graphene aerogel-supported MoO 2 and FeS 2 nanocomposite (MoO 2 /FeS 2 /GA) was developed...
Gespeichert in:
| Veröffentlicht in: | Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2020-10, Vol.8 (37), p.19278-19282 |
|---|---|
| Hauptverfasser: | , , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | 19282 |
|---|---|
| container_issue | 37 |
| container_start_page | 19278 |
| container_title | Journal of materials chemistry. A, Materials for energy and sustainability |
| container_volume | 8 |
| creator | Liu, Jie Kong, Wenhan Jin, Zhaoyong Han, Yaqian Sun, Jie Ma, Liangyu Niu, Yusheng Xu, Yuanhong |
| description | Electrochemical conversion of N
2
provides an eco-friendly approach for sustainable ammonia (NH
3
) production, but most electrocatalysts still suffer from low selectivity. Herein, a new three dimensional (3D) graphene aerogel-supported MoO
2
and FeS
2
nanocomposite (MoO
2
/FeS
2
/GA) was developed through mimicking the elemental composition and proportion of MoFe nitrogenase. Herein, MoO
2
and FeS
2
can both act as active sites for nitrogen fixation, while FeS
2
plays the role of suppressing the competitive hydrogen evolution activity simultaneously. Moreover, the graphene aerogels can promote the charge transfer and increase the specific surface area of the nanocomposites. Based on the synergistic effects of such a ternary architecture, the electrocatalyst exhibits a high NH
3
yield of 40.18 μg h
−1
mg
cat.
−1
and outstanding faradaic efficiency of 37.44% at −0.25 V
versus
the reversible hydrogen electrode (RHE) in 0.1 M HCl. The selectivity of the as-proposed nanocomposite is superior to those of GA, FeS
2
/GA, MoO
2
/GA and most previously reported NRR electrocatalysts. Such a bioinspired strategy provides a new avenue to develop more high-efficiency catalysts with controllable activity for the NRR under ambient conditions.
MoFe nitrogenase-mimic electrocatalyst (MoO
2
/FeS
2
/GA) was proposed for nitrogen fixation, which showed substantially high faradaic efficiency of 37.44%. |
| doi_str_mv | 10.1039/d0ta07757g |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_webof</sourceid><recordid>TN_cdi_proquest_journals_2446975633</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2446975633</sourcerecordid><originalsourceid>FETCH-LOGICAL-c385t-d629d8b98a7dc06d5f7178a1787546d3d715be155fe2620bcd334e897c62af883</originalsourceid><addsrcrecordid>eNqNkUtLAzEURgdRsGg37oWIO2U0M5m8lqXaKlTc1PWY5tGmtpOapNT-e9OO1J0YCAmX891wT7LsooB3BUT8XsEoIKWYTo-yTgkxzGnFyfHhzthp1g1hDtNiEBLOO9l7D7y4gQaNjd5NdSOCzpd2aeWHbaZAL7RMdSmiWGxDBMb5AwmM_RLRugZsbJyBmZ3OgBFeKGEl0MZYaXUjt-fZiRGLoLs_51n2Nngc95_y0evwud8b5RIxHHNFSq7YhDNBlYREYUMLykTaFFdEIUULPNEFxkaXpIQTqRCqNONUklIYxtBZdt32XXn3udYh1nO39k16si6rinCKCUKJumkp6V0IXpt65e1S-G1dwHonsX6A495e4jDBty280RNnwn4efQgkiZgixvhOJ-SJZv-n-zbu3fXduokpetVGfZCHxO9v1itlEnP5F4O-AUCumvs</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2446975633</pqid></control><display><type>article</type><title>A MoFe nitrogenase-mimicking electrocatalyst for nitrogen fixation with high faradaic efficiency</title><source>Royal Society Of Chemistry Journals 2008-</source><creator>Liu, Jie ; Kong, Wenhan ; Jin, Zhaoyong ; Han, Yaqian ; Sun, Jie ; Ma, Liangyu ; Niu, Yusheng ; Xu, Yuanhong</creator><creatorcontrib>Liu, Jie ; Kong, Wenhan ; Jin, Zhaoyong ; Han, Yaqian ; Sun, Jie ; Ma, Liangyu ; Niu, Yusheng ; Xu, Yuanhong</creatorcontrib><description>Electrochemical conversion of N
2
provides an eco-friendly approach for sustainable ammonia (NH
3
) production, but most electrocatalysts still suffer from low selectivity. Herein, a new three dimensional (3D) graphene aerogel-supported MoO
2
and FeS
2
nanocomposite (MoO
2
/FeS
2
/GA) was developed through mimicking the elemental composition and proportion of MoFe nitrogenase. Herein, MoO
2
and FeS
2
can both act as active sites for nitrogen fixation, while FeS
2
plays the role of suppressing the competitive hydrogen evolution activity simultaneously. Moreover, the graphene aerogels can promote the charge transfer and increase the specific surface area of the nanocomposites. Based on the synergistic effects of such a ternary architecture, the electrocatalyst exhibits a high NH
3
yield of 40.18 μg h
−1
mg
cat.
−1
and outstanding faradaic efficiency of 37.44% at −0.25 V
versus
the reversible hydrogen electrode (RHE) in 0.1 M HCl. The selectivity of the as-proposed nanocomposite is superior to those of GA, FeS
2
/GA, MoO
2
/GA and most previously reported NRR electrocatalysts. Such a bioinspired strategy provides a new avenue to develop more high-efficiency catalysts with controllable activity for the NRR under ambient conditions.
MoFe nitrogenase-mimic electrocatalyst (MoO
2
/FeS
2
/GA) was proposed for nitrogen fixation, which showed substantially high faradaic efficiency of 37.44%.</description><identifier>ISSN: 2050-7488</identifier><identifier>EISSN: 2050-7496</identifier><identifier>DOI: 10.1039/d0ta07757g</identifier><language>eng</language><publisher>CAMBRIDGE: Royal Soc Chemistry</publisher><subject>Aerogels ; Ammonia ; Catalysts ; Charge transfer ; Chemical composition ; Chemistry ; Chemistry, Physical ; Efficiency ; Electrocatalysts ; Electrochemistry ; Energy & Fuels ; Graphene ; Hydrogen evolution ; Iron sulfides ; Materials Science ; Materials Science, Multidisciplinary ; Mimicry ; Molybdenum oxides ; Nanocomposites ; Nitrogen fixation ; Nitrogenase ; Nitrogenation ; Physical Sciences ; Pyrite ; Science & Technology ; Selectivity ; Synergistic effect ; Technology</subject><ispartof>Journal of materials chemistry. A, Materials for energy and sustainability, 2020-10, Vol.8 (37), p.19278-19282</ispartof><rights>Copyright Royal Society of Chemistry 2020</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>true</woscitedreferencessubscribed><woscitedreferencescount>22</woscitedreferencescount><woscitedreferencesoriginalsourcerecordid>wos000573889000009</woscitedreferencesoriginalsourcerecordid><citedby>FETCH-LOGICAL-c385t-d629d8b98a7dc06d5f7178a1787546d3d715be155fe2620bcd334e897c62af883</citedby><cites>FETCH-LOGICAL-c385t-d629d8b98a7dc06d5f7178a1787546d3d715be155fe2620bcd334e897c62af883</cites><orcidid>0000-0003-1549-9820</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>315,781,785,27928,27929</link.rule.ids></links><search><creatorcontrib>Liu, Jie</creatorcontrib><creatorcontrib>Kong, Wenhan</creatorcontrib><creatorcontrib>Jin, Zhaoyong</creatorcontrib><creatorcontrib>Han, Yaqian</creatorcontrib><creatorcontrib>Sun, Jie</creatorcontrib><creatorcontrib>Ma, Liangyu</creatorcontrib><creatorcontrib>Niu, Yusheng</creatorcontrib><creatorcontrib>Xu, Yuanhong</creatorcontrib><title>A MoFe nitrogenase-mimicking electrocatalyst for nitrogen fixation with high faradaic efficiency</title><title>Journal of materials chemistry. A, Materials for energy and sustainability</title><addtitle>J MATER CHEM A</addtitle><description>Electrochemical conversion of N
2
provides an eco-friendly approach for sustainable ammonia (NH
3
) production, but most electrocatalysts still suffer from low selectivity. Herein, a new three dimensional (3D) graphene aerogel-supported MoO
2
and FeS
2
nanocomposite (MoO
2
/FeS
2
/GA) was developed through mimicking the elemental composition and proportion of MoFe nitrogenase. Herein, MoO
2
and FeS
2
can both act as active sites for nitrogen fixation, while FeS
2
plays the role of suppressing the competitive hydrogen evolution activity simultaneously. Moreover, the graphene aerogels can promote the charge transfer and increase the specific surface area of the nanocomposites. Based on the synergistic effects of such a ternary architecture, the electrocatalyst exhibits a high NH
3
yield of 40.18 μg h
−1
mg
cat.
−1
and outstanding faradaic efficiency of 37.44% at −0.25 V
versus
the reversible hydrogen electrode (RHE) in 0.1 M HCl. The selectivity of the as-proposed nanocomposite is superior to those of GA, FeS
2
/GA, MoO
2
/GA and most previously reported NRR electrocatalysts. Such a bioinspired strategy provides a new avenue to develop more high-efficiency catalysts with controllable activity for the NRR under ambient conditions.
MoFe nitrogenase-mimic electrocatalyst (MoO
2
/FeS
2
/GA) was proposed for nitrogen fixation, which showed substantially high faradaic efficiency of 37.44%.</description><subject>Aerogels</subject><subject>Ammonia</subject><subject>Catalysts</subject><subject>Charge transfer</subject><subject>Chemical composition</subject><subject>Chemistry</subject><subject>Chemistry, Physical</subject><subject>Efficiency</subject><subject>Electrocatalysts</subject><subject>Electrochemistry</subject><subject>Energy & Fuels</subject><subject>Graphene</subject><subject>Hydrogen evolution</subject><subject>Iron sulfides</subject><subject>Materials Science</subject><subject>Materials Science, Multidisciplinary</subject><subject>Mimicry</subject><subject>Molybdenum oxides</subject><subject>Nanocomposites</subject><subject>Nitrogen fixation</subject><subject>Nitrogenase</subject><subject>Nitrogenation</subject><subject>Physical Sciences</subject><subject>Pyrite</subject><subject>Science & Technology</subject><subject>Selectivity</subject><subject>Synergistic effect</subject><subject>Technology</subject><issn>2050-7488</issn><issn>2050-7496</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><sourceid>AOWDO</sourceid><recordid>eNqNkUtLAzEURgdRsGg37oWIO2U0M5m8lqXaKlTc1PWY5tGmtpOapNT-e9OO1J0YCAmX891wT7LsooB3BUT8XsEoIKWYTo-yTgkxzGnFyfHhzthp1g1hDtNiEBLOO9l7D7y4gQaNjd5NdSOCzpd2aeWHbaZAL7RMdSmiWGxDBMb5AwmM_RLRugZsbJyBmZ3OgBFeKGEl0MZYaXUjt-fZiRGLoLs_51n2Nngc95_y0evwud8b5RIxHHNFSq7YhDNBlYREYUMLykTaFFdEIUULPNEFxkaXpIQTqRCqNONUklIYxtBZdt32XXn3udYh1nO39k16si6rinCKCUKJumkp6V0IXpt65e1S-G1dwHonsX6A495e4jDBty280RNnwn4efQgkiZgixvhOJ-SJZv-n-zbu3fXduokpetVGfZCHxO9v1itlEnP5F4O-AUCumvs</recordid><startdate>20201007</startdate><enddate>20201007</enddate><creator>Liu, Jie</creator><creator>Kong, Wenhan</creator><creator>Jin, Zhaoyong</creator><creator>Han, Yaqian</creator><creator>Sun, Jie</creator><creator>Ma, Liangyu</creator><creator>Niu, Yusheng</creator><creator>Xu, Yuanhong</creator><general>Royal Soc Chemistry</general><general>Royal Society of Chemistry</general><scope>AOWDO</scope><scope>BLEPL</scope><scope>DTL</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SP</scope><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>JG9</scope><scope>L7M</scope><scope>SOI</scope><orcidid>https://orcid.org/0000-0003-1549-9820</orcidid></search><sort><creationdate>20201007</creationdate><title>A MoFe nitrogenase-mimicking electrocatalyst for nitrogen fixation with high faradaic efficiency</title><author>Liu, Jie ; Kong, Wenhan ; Jin, Zhaoyong ; Han, Yaqian ; Sun, Jie ; Ma, Liangyu ; Niu, Yusheng ; Xu, Yuanhong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c385t-d629d8b98a7dc06d5f7178a1787546d3d715be155fe2620bcd334e897c62af883</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Aerogels</topic><topic>Ammonia</topic><topic>Catalysts</topic><topic>Charge transfer</topic><topic>Chemical composition</topic><topic>Chemistry</topic><topic>Chemistry, Physical</topic><topic>Efficiency</topic><topic>Electrocatalysts</topic><topic>Electrochemistry</topic><topic>Energy & Fuels</topic><topic>Graphene</topic><topic>Hydrogen evolution</topic><topic>Iron sulfides</topic><topic>Materials Science</topic><topic>Materials Science, Multidisciplinary</topic><topic>Mimicry</topic><topic>Molybdenum oxides</topic><topic>Nanocomposites</topic><topic>Nitrogen fixation</topic><topic>Nitrogenase</topic><topic>Nitrogenation</topic><topic>Physical Sciences</topic><topic>Pyrite</topic><topic>Science & Technology</topic><topic>Selectivity</topic><topic>Synergistic effect</topic><topic>Technology</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Liu, Jie</creatorcontrib><creatorcontrib>Kong, Wenhan</creatorcontrib><creatorcontrib>Jin, Zhaoyong</creatorcontrib><creatorcontrib>Han, Yaqian</creatorcontrib><creatorcontrib>Sun, Jie</creatorcontrib><creatorcontrib>Ma, Liangyu</creatorcontrib><creatorcontrib>Niu, Yusheng</creatorcontrib><creatorcontrib>Xu, Yuanhong</creatorcontrib><collection>Web of Science - Science Citation Index Expanded - 2020</collection><collection>Web of Science Core Collection</collection><collection>Science Citation Index Expanded</collection><collection>CrossRef</collection><collection>Electronics & Communications Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>Journal of materials chemistry. A, Materials for energy and sustainability</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Liu, Jie</au><au>Kong, Wenhan</au><au>Jin, Zhaoyong</au><au>Han, Yaqian</au><au>Sun, Jie</au><au>Ma, Liangyu</au><au>Niu, Yusheng</au><au>Xu, Yuanhong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>A MoFe nitrogenase-mimicking electrocatalyst for nitrogen fixation with high faradaic efficiency</atitle><jtitle>Journal of materials chemistry. A, Materials for energy and sustainability</jtitle><stitle>J MATER CHEM A</stitle><date>2020-10-07</date><risdate>2020</risdate><volume>8</volume><issue>37</issue><spage>19278</spage><epage>19282</epage><pages>19278-19282</pages><issn>2050-7488</issn><eissn>2050-7496</eissn><abstract>Electrochemical conversion of N
2
provides an eco-friendly approach for sustainable ammonia (NH
3
) production, but most electrocatalysts still suffer from low selectivity. Herein, a new three dimensional (3D) graphene aerogel-supported MoO
2
and FeS
2
nanocomposite (MoO
2
/FeS
2
/GA) was developed through mimicking the elemental composition and proportion of MoFe nitrogenase. Herein, MoO
2
and FeS
2
can both act as active sites for nitrogen fixation, while FeS
2
plays the role of suppressing the competitive hydrogen evolution activity simultaneously. Moreover, the graphene aerogels can promote the charge transfer and increase the specific surface area of the nanocomposites. Based on the synergistic effects of such a ternary architecture, the electrocatalyst exhibits a high NH
3
yield of 40.18 μg h
−1
mg
cat.
−1
and outstanding faradaic efficiency of 37.44% at −0.25 V
versus
the reversible hydrogen electrode (RHE) in 0.1 M HCl. The selectivity of the as-proposed nanocomposite is superior to those of GA, FeS
2
/GA, MoO
2
/GA and most previously reported NRR electrocatalysts. Such a bioinspired strategy provides a new avenue to develop more high-efficiency catalysts with controllable activity for the NRR under ambient conditions.
MoFe nitrogenase-mimic electrocatalyst (MoO
2
/FeS
2
/GA) was proposed for nitrogen fixation, which showed substantially high faradaic efficiency of 37.44%.</abstract><cop>CAMBRIDGE</cop><pub>Royal Soc Chemistry</pub><doi>10.1039/d0ta07757g</doi><tpages>5</tpages><orcidid>https://orcid.org/0000-0003-1549-9820</orcidid></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 2050-7488 |
| ispartof | Journal of materials chemistry. A, Materials for energy and sustainability, 2020-10, Vol.8 (37), p.19278-19282 |
| issn | 2050-7488 2050-7496 |
| language | eng |
| recordid | cdi_proquest_journals_2446975633 |
| source | Royal Society Of Chemistry Journals 2008- |
| subjects | Aerogels Ammonia Catalysts Charge transfer Chemical composition Chemistry Chemistry, Physical Efficiency Electrocatalysts Electrochemistry Energy & Fuels Graphene Hydrogen evolution Iron sulfides Materials Science Materials Science, Multidisciplinary Mimicry Molybdenum oxides Nanocomposites Nitrogen fixation Nitrogenase Nitrogenation Physical Sciences Pyrite Science & Technology Selectivity Synergistic effect Technology |
| title | A MoFe nitrogenase-mimicking electrocatalyst for nitrogen fixation with high faradaic efficiency |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-17T01%3A46%3A54IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_webof&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=A%20MoFe%20nitrogenase-mimicking%20electrocatalyst%20for%20nitrogen%20fixation%20with%20high%20faradaic%20efficiency&rft.jtitle=Journal%20of%20materials%20chemistry.%20A,%20Materials%20for%20energy%20and%20sustainability&rft.au=Liu,%20Jie&rft.date=2020-10-07&rft.volume=8&rft.issue=37&rft.spage=19278&rft.epage=19282&rft.pages=19278-19282&rft.issn=2050-7488&rft.eissn=2050-7496&rft_id=info:doi/10.1039/d0ta07757g&rft_dat=%3Cproquest_webof%3E2446975633%3C/proquest_webof%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=2446975633&rft_id=info:pmid/&rfr_iscdi=true |