Design of a High-Performance Electrocatalyst for N 2 Conversion to NH 3 by Trapping Single Metal Atoms on Stepped CeO 2
Single-atom catalysts (SACs) have recently been shown to have high performance in catalyzing the synthesis of NH from N . Here, we systematically investigated a series of single transition metal atoms anchored on stepped CeO (CeO -S) to screen the potential electrocatalysts for a N reduction reactio...
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| Veröffentlicht in: | ACS applied materials & interfaces 2019-12, Vol.11 (50), p.47525-47534 |
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| container_title | ACS applied materials & interfaces |
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| creator | Qi, Jiamin Gao, Liye Wei, Fenfei Wan, Qiang Lin, Sen |
| description | Single-atom catalysts (SACs) have recently been shown to have high performance in catalyzing the synthesis of NH
from N
. Here, we systematically investigated a series of single transition metal atoms anchored on stepped CeO
(CeO
-S) to screen the potential electrocatalysts for a N
reduction reaction (NRR) via density functional theory computations. We first demonstrated that these SACs are stable via large calculated binding energies. Second, we evaluated the adsorption of *N
over CeO
-S-supported single atoms. Here, those systems that can activate N
molecules were selected as candidates. We then showed that CeO
-S-supported single Mo and Ru atoms have high catalytic activity for NRR via low limiting potentials of -0.52 and -0.35 V, respectively. Meanwhile, the competitive hydrogen evolution reaction is highly suppressed over these two SACs because the adsorption of *N
is prior to *H. Finally, the origin of the NRR activity over these SACs was investigated. This work offers useful insights into designing high-performance CeO
-based electrocatalysts for NRR. |
| doi_str_mv | 10.1021/acsami.9b15570 |
| format | Article |
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from N
. Here, we systematically investigated a series of single transition metal atoms anchored on stepped CeO
(CeO
-S) to screen the potential electrocatalysts for a N
reduction reaction (NRR) via density functional theory computations. We first demonstrated that these SACs are stable via large calculated binding energies. Second, we evaluated the adsorption of *N
over CeO
-S-supported single atoms. Here, those systems that can activate N
molecules were selected as candidates. We then showed that CeO
-S-supported single Mo and Ru atoms have high catalytic activity for NRR via low limiting potentials of -0.52 and -0.35 V, respectively. Meanwhile, the competitive hydrogen evolution reaction is highly suppressed over these two SACs because the adsorption of *N
is prior to *H. Finally, the origin of the NRR activity over these SACs was investigated. This work offers useful insights into designing high-performance CeO
-based electrocatalysts for NRR.</description><identifier>ISSN: 1944-8244</identifier><identifier>EISSN: 1944-8252</identifier><identifier>DOI: 10.1021/acsami.9b15570</identifier><identifier>PMID: 31766839</identifier><language>eng</language><publisher>United States</publisher><ispartof>ACS applied materials & interfaces, 2019-12, Vol.11 (50), p.47525-47534</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c1079-953fa8b814480c5b3d4e08c581ab61665353147754193b0c859d227ebfd6aa23</citedby><cites>FETCH-LOGICAL-c1079-953fa8b814480c5b3d4e08c581ab61665353147754193b0c859d227ebfd6aa23</cites><orcidid>0000-0002-2288-5415</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,2752,27901,27902</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/31766839$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Qi, Jiamin</creatorcontrib><creatorcontrib>Gao, Liye</creatorcontrib><creatorcontrib>Wei, Fenfei</creatorcontrib><creatorcontrib>Wan, Qiang</creatorcontrib><creatorcontrib>Lin, Sen</creatorcontrib><title>Design of a High-Performance Electrocatalyst for N 2 Conversion to NH 3 by Trapping Single Metal Atoms on Stepped CeO 2</title><title>ACS applied materials & interfaces</title><addtitle>ACS Appl Mater Interfaces</addtitle><description>Single-atom catalysts (SACs) have recently been shown to have high performance in catalyzing the synthesis of NH
from N
. Here, we systematically investigated a series of single transition metal atoms anchored on stepped CeO
(CeO
-S) to screen the potential electrocatalysts for a N
reduction reaction (NRR) via density functional theory computations. We first demonstrated that these SACs are stable via large calculated binding energies. Second, we evaluated the adsorption of *N
over CeO
-S-supported single atoms. Here, those systems that can activate N
molecules were selected as candidates. We then showed that CeO
-S-supported single Mo and Ru atoms have high catalytic activity for NRR via low limiting potentials of -0.52 and -0.35 V, respectively. Meanwhile, the competitive hydrogen evolution reaction is highly suppressed over these two SACs because the adsorption of *N
is prior to *H. Finally, the origin of the NRR activity over these SACs was investigated. This work offers useful insights into designing high-performance CeO
-based electrocatalysts for NRR.</description><issn>1944-8244</issn><issn>1944-8252</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNo9kMtOwzAQRS0EoqWwZYnmB1L8TJxlFQpFKi1Su49sxylBSRzZAZS_J6ilm5mR7j2zOAjdEzwnmJJHZYJqqnmqiRAJvkBTknIeSSro5fnmfIJuQvjEOGYUi2s0YSSJY8nSKfp5sqE6tOBKULCqDh_Ru_Wl841qjYVlbU3vnVG9qofQwxjABihkrv22PlSuhd7BZgUM9AB7r7quag-wG0dt4c2OGCx61wQYm7vedp0tILNboLfoqlR1sHenPUP75-U-W0Xr7ctrtlhHhuAkjVLBSiW1JJxLbIRmBbdYGiGJ0jGJY8EEIzxJBCcp09hIkRaUJlaXRawUZTM0P7413oXgbZl3vmqUH3KC8z-B-VFgfhI4Ag9HoPvSjS3O9X9j7BcJ-2t5</recordid><startdate>20191218</startdate><enddate>20191218</enddate><creator>Qi, Jiamin</creator><creator>Gao, Liye</creator><creator>Wei, Fenfei</creator><creator>Wan, Qiang</creator><creator>Lin, Sen</creator><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0002-2288-5415</orcidid></search><sort><creationdate>20191218</creationdate><title>Design of a High-Performance Electrocatalyst for N 2 Conversion to NH 3 by Trapping Single Metal Atoms on Stepped CeO 2</title><author>Qi, Jiamin ; Gao, Liye ; Wei, Fenfei ; Wan, Qiang ; Lin, Sen</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c1079-953fa8b814480c5b3d4e08c581ab61665353147754193b0c859d227ebfd6aa23</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Qi, Jiamin</creatorcontrib><creatorcontrib>Gao, Liye</creatorcontrib><creatorcontrib>Wei, Fenfei</creatorcontrib><creatorcontrib>Wan, Qiang</creatorcontrib><creatorcontrib>Lin, Sen</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><jtitle>ACS applied materials & interfaces</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Qi, Jiamin</au><au>Gao, Liye</au><au>Wei, Fenfei</au><au>Wan, Qiang</au><au>Lin, Sen</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Design of a High-Performance Electrocatalyst for N 2 Conversion to NH 3 by Trapping Single Metal Atoms on Stepped CeO 2</atitle><jtitle>ACS applied materials & interfaces</jtitle><addtitle>ACS Appl Mater Interfaces</addtitle><date>2019-12-18</date><risdate>2019</risdate><volume>11</volume><issue>50</issue><spage>47525</spage><epage>47534</epage><pages>47525-47534</pages><issn>1944-8244</issn><eissn>1944-8252</eissn><abstract>Single-atom catalysts (SACs) have recently been shown to have high performance in catalyzing the synthesis of NH
from N
. Here, we systematically investigated a series of single transition metal atoms anchored on stepped CeO
(CeO
-S) to screen the potential electrocatalysts for a N
reduction reaction (NRR) via density functional theory computations. We first demonstrated that these SACs are stable via large calculated binding energies. Second, we evaluated the adsorption of *N
over CeO
-S-supported single atoms. Here, those systems that can activate N
molecules were selected as candidates. We then showed that CeO
-S-supported single Mo and Ru atoms have high catalytic activity for NRR via low limiting potentials of -0.52 and -0.35 V, respectively. Meanwhile, the competitive hydrogen evolution reaction is highly suppressed over these two SACs because the adsorption of *N
is prior to *H. Finally, the origin of the NRR activity over these SACs was investigated. This work offers useful insights into designing high-performance CeO
-based electrocatalysts for NRR.</abstract><cop>United States</cop><pmid>31766839</pmid><doi>10.1021/acsami.9b15570</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0002-2288-5415</orcidid></addata></record> |
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| source | American Chemical Society Publications |
| title | Design of a High-Performance Electrocatalyst for N 2 Conversion to NH 3 by Trapping Single Metal Atoms on Stepped CeO 2 |
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