Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation
The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of...
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| Veröffentlicht in: | Angewandte Chemie 2019-12, Vol.131 (51), p.18777-18782 |
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| container_title | Angewandte Chemie |
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| creator | Zheng, Jianyun Lyu, Yanhong Qiao, Man Veder, Jean P. Marco, Roland D. Bradley, John Wang, Ruilun Li, Yafei Huang, Aibin Jiang, San Ping Wang, Shuangyin |
| description | The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N2 to NH3. The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 yield rate of 15.1 μg cm−2 h−1 and a good faradic efficiency of 19 % at −0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH3.
Unter Kontrolle: Das Abstimmen der lokalen elektronischen Struktur von Au‐Nanopartikeln mit positiven Valenzpositionen kann den Umsatz von N2 zu NH3 durch Kontrollieren der N2‐Adsorption und der damit einhergehenden Energiebarriere für die Stickstoffreduktion (NRR) drastisch erhöhen. Die Einführung eines Metalls mit lokaler elektronischer Struktur kann einen neuen Weg zur Herstellung hocheffizienter Katalysatoren für die NRR ebnen. |
| doi_str_mv | 10.1002/ange.201909477 |
| format | Article |
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Unter Kontrolle: Das Abstimmen der lokalen elektronischen Struktur von Au‐Nanopartikeln mit positiven Valenzpositionen kann den Umsatz von N2 zu NH3 durch Kontrollieren der N2‐Adsorption und der damit einhergehenden Energiebarriere für die Stickstoffreduktion (NRR) drastisch erhöhen. Die Einführung eines Metalls mit lokaler elektronischer Struktur kann einen neuen Weg zur Herstellung hocheffizienter Katalysatoren für die NRR ebnen.</description><identifier>ISSN: 0044-8249</identifier><identifier>EISSN: 1521-3757</identifier><identifier>DOI: 10.1002/ange.201909477</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Ammonia ; Catalysts ; Chemical reduction ; Chemistry ; Cobalt oxides ; Developmental stages ; Electrochemistry ; Electronic structure ; Elektrokatalyse ; Gold ; Localization ; Nanoparticles ; Nanopartikel ; Oxidation ; Photoelektrochemie ; Renewable energy ; Selectivity ; Stickstoffreduktion ; Valence</subject><ispartof>Angewandte Chemie, 2019-12, Vol.131 (51), p.18777-18782</ispartof><rights>2019 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c2027-9ac30e988c55f7bb2d6bba7939ca7c0f39b6305669848f11de3f7d031ca52453</citedby><cites>FETCH-LOGICAL-c2027-9ac30e988c55f7bb2d6bba7939ca7c0f39b6305669848f11de3f7d031ca52453</cites><orcidid>0000-0002-6136-863X ; 0000-0002-2262-7694</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fange.201909477$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fange.201909477$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27924,27925,45574,45575</link.rule.ids></links><search><creatorcontrib>Zheng, Jianyun</creatorcontrib><creatorcontrib>Lyu, Yanhong</creatorcontrib><creatorcontrib>Qiao, Man</creatorcontrib><creatorcontrib>Veder, Jean P.</creatorcontrib><creatorcontrib>Marco, Roland D.</creatorcontrib><creatorcontrib>Bradley, John</creatorcontrib><creatorcontrib>Wang, Ruilun</creatorcontrib><creatorcontrib>Li, Yafei</creatorcontrib><creatorcontrib>Huang, Aibin</creatorcontrib><creatorcontrib>Jiang, San Ping</creatorcontrib><creatorcontrib>Wang, Shuangyin</creatorcontrib><title>Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation</title><title>Angewandte Chemie</title><description>The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N2 to NH3. The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 yield rate of 15.1 μg cm−2 h−1 and a good faradic efficiency of 19 % at −0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH3.
Unter Kontrolle: Das Abstimmen der lokalen elektronischen Struktur von Au‐Nanopartikeln mit positiven Valenzpositionen kann den Umsatz von N2 zu NH3 durch Kontrollieren der N2‐Adsorption und der damit einhergehenden Energiebarriere für die Stickstoffreduktion (NRR) drastisch erhöhen. Die Einführung eines Metalls mit lokaler elektronischer Struktur kann einen neuen Weg zur Herstellung hocheffizienter Katalysatoren für die NRR ebnen.</description><subject>Ammonia</subject><subject>Catalysts</subject><subject>Chemical reduction</subject><subject>Chemistry</subject><subject>Cobalt oxides</subject><subject>Developmental stages</subject><subject>Electrochemistry</subject><subject>Electronic structure</subject><subject>Elektrokatalyse</subject><subject>Gold</subject><subject>Localization</subject><subject>Nanoparticles</subject><subject>Nanopartikel</subject><subject>Oxidation</subject><subject>Photoelektrochemie</subject><subject>Renewable energy</subject><subject>Selectivity</subject><subject>Stickstoffreduktion</subject><subject>Valence</subject><issn>0044-8249</issn><issn>1521-3757</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNqFkL9OwzAQhy0EEqWwMkdiTjnbcRyPVZUWpKos3Y3jOMVVahcnFX8mHoFn5ElwWwQjy91Z_r476YfQNYYRBiC3yq3MiAAWIDLOT9AAM4JTyhk_RQOALEsLkolzdNF1awDICRcD9LjcOetWSf9kkrI1ug_eJXOvVWvfVW_jwzfJzLd1UjpVtaY7kBPvItju_xY2Tivjvj4-ex_LeLPxzqpkal8P_iU6a1TbmaufPkTLabmc3KXzh9n9ZDxPNQHCU6E0BSOKQjPW8KoidV5VigsqtOIaGiqqnALLc1FkRYNxbWjDa6BYK0YyRofo5rh2G_zzznS9XPtdcPGiJJQQnuWC0UiNjpQOvuuCaeQ22I0KbxKD3Ico9yHK3xCjII7Ci23N2z-0HC9m5Z_7DTnNeBY</recordid><startdate>20191216</startdate><enddate>20191216</enddate><creator>Zheng, Jianyun</creator><creator>Lyu, Yanhong</creator><creator>Qiao, Man</creator><creator>Veder, Jean P.</creator><creator>Marco, Roland D.</creator><creator>Bradley, John</creator><creator>Wang, Ruilun</creator><creator>Li, Yafei</creator><creator>Huang, Aibin</creator><creator>Jiang, San Ping</creator><creator>Wang, Shuangyin</creator><general>Wiley Subscription Services, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><orcidid>https://orcid.org/0000-0002-6136-863X</orcidid><orcidid>https://orcid.org/0000-0002-2262-7694</orcidid></search><sort><creationdate>20191216</creationdate><title>Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation</title><author>Zheng, Jianyun ; Lyu, Yanhong ; Qiao, Man ; Veder, Jean P. ; Marco, Roland D. ; Bradley, John ; Wang, Ruilun ; Li, Yafei ; Huang, Aibin ; Jiang, San Ping ; Wang, Shuangyin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c2027-9ac30e988c55f7bb2d6bba7939ca7c0f39b6305669848f11de3f7d031ca52453</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Ammonia</topic><topic>Catalysts</topic><topic>Chemical reduction</topic><topic>Chemistry</topic><topic>Cobalt oxides</topic><topic>Developmental stages</topic><topic>Electrochemistry</topic><topic>Electronic structure</topic><topic>Elektrokatalyse</topic><topic>Gold</topic><topic>Localization</topic><topic>Nanoparticles</topic><topic>Nanopartikel</topic><topic>Oxidation</topic><topic>Photoelektrochemie</topic><topic>Renewable energy</topic><topic>Selectivity</topic><topic>Stickstoffreduktion</topic><topic>Valence</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zheng, Jianyun</creatorcontrib><creatorcontrib>Lyu, Yanhong</creatorcontrib><creatorcontrib>Qiao, Man</creatorcontrib><creatorcontrib>Veder, Jean P.</creatorcontrib><creatorcontrib>Marco, Roland D.</creatorcontrib><creatorcontrib>Bradley, John</creatorcontrib><creatorcontrib>Wang, Ruilun</creatorcontrib><creatorcontrib>Li, Yafei</creatorcontrib><creatorcontrib>Huang, Aibin</creatorcontrib><creatorcontrib>Jiang, San Ping</creatorcontrib><creatorcontrib>Wang, Shuangyin</creatorcontrib><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><jtitle>Angewandte Chemie</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zheng, Jianyun</au><au>Lyu, Yanhong</au><au>Qiao, Man</au><au>Veder, Jean P.</au><au>Marco, Roland D.</au><au>Bradley, John</au><au>Wang, Ruilun</au><au>Li, Yafei</au><au>Huang, Aibin</au><au>Jiang, San Ping</au><au>Wang, Shuangyin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation</atitle><jtitle>Angewandte Chemie</jtitle><date>2019-12-16</date><risdate>2019</risdate><volume>131</volume><issue>51</issue><spage>18777</spage><epage>18782</epage><pages>18777-18782</pages><issn>0044-8249</issn><eissn>1521-3757</eissn><abstract>The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N2 to NH3. The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 yield rate of 15.1 μg cm−2 h−1 and a good faradic efficiency of 19 % at −0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH3.
Unter Kontrolle: Das Abstimmen der lokalen elektronischen Struktur von Au‐Nanopartikeln mit positiven Valenzpositionen kann den Umsatz von N2 zu NH3 durch Kontrollieren der N2‐Adsorption und der damit einhergehenden Energiebarriere für die Stickstoffreduktion (NRR) drastisch erhöhen. Die Einführung eines Metalls mit lokaler elektronischer Struktur kann einen neuen Weg zur Herstellung hocheffizienter Katalysatoren für die NRR ebnen.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/ange.201909477</doi><tpages>6</tpages><orcidid>https://orcid.org/0000-0002-6136-863X</orcidid><orcidid>https://orcid.org/0000-0002-2262-7694</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | Ammonia Catalysts Chemical reduction Chemistry Cobalt oxides Developmental stages Electrochemistry Electronic structure Elektrokatalyse Gold Localization Nanoparticles Nanopartikel Oxidation Photoelektrochemie Renewable energy Selectivity Stickstoffreduktion Valence |
| title | Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation |
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