The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon‐Based Catalysts for Electrocatalytic Nitrogen Reduction
Cost‐effective carbon‐based catalysts are promising for catalyzing the electrochemical N2 reduction reaction (NRR). However, the activity origin of carbon‐based catalysts towards NRR remains unclear, and regularities and rules for the rational design of carbon‐based NRR electrocatalysts are still la...
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| Veröffentlicht in: | Angewandte Chemie International Edition 2020-03, Vol.59 (11), p.4525-4531 |
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| container_title | Angewandte Chemie International Edition |
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| creator | Yang, Yuanyuan Zhang, Lifu Hu, Zhenpeng Zheng, Yao Tang, Cheng Chen, Ping Wang, Ruguang Qiu, Kangwen Mao, Jing Ling, Tao Qiao, Shi‐Zhang |
| description | Cost‐effective carbon‐based catalysts are promising for catalyzing the electrochemical N2 reduction reaction (NRR). However, the activity origin of carbon‐based catalysts towards NRR remains unclear, and regularities and rules for the rational design of carbon‐based NRR electrocatalysts are still lacking. Based on a combination of theoretical calculations and experimental observations, chalcogen/oxygen group element (O, S, Se, Te) doped carbon materials were systematically evaluated as potential NRR catalysts. Heteroatom‐doping‐induced charge accumulation facilitates N2 adsorption on carbon atoms and spin polarization boosts the potential‐determining step of the first protonation to form *NNH. Te‐doped and Se‐doped C catalysts exhibited high intrinsic NRR activity that is superior to most metal‐based catalysts. Establishing the correlation between the electronic structure and NRR performance for carbon‐based materials paves the pathway for their NRR application.
Unearthing the NRR: This systematically combined computational and experimental work uncovers the catalytic nature of carbon‐based materials towards the electrocatalytic nitrogen reduction reaction (NRR). |
| doi_str_mv | 10.1002/anie.201915001 |
| format | Article |
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Unearthing the NRR: This systematically combined computational and experimental work uncovers the catalytic nature of carbon‐based materials towards the electrocatalytic nitrogen reduction reaction (NRR).</description><subject>Accumulation</subject><subject>Carbon</subject><subject>carbon materials</subject><subject>Catalysts</subject><subject>chalcogens</subject><subject>Chemical reduction</subject><subject>electrocatalysis</subject><subject>Electrocatalysts</subject><subject>Electrochemistry</subject><subject>Electronic structure</subject><subject>nitrogen reduction reaction</subject><subject>Polarization</subject><subject>Polarization (spin alignment)</subject><subject>Protonation</subject><subject>Tellurium</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNqFkU9P2zAYhy00BIXtynGytMsuKXYcJ86xi8ofCcHUsXPkOG9aI9fu7GSonPgAO-wz8klwKRRpl53s36vnfWTrh9AJJWNKSHoqrYZxSmhJOSF0D40oT2nCioJ9iPeMsaQQnB6ioxDuIi8EyQ_QIaMlJ5yTEfpzuwBc-UFpafDMGcCuw9VC-jngiVLDcjCy185iaVv8Y6Ut_u6M9PphO415onr9OyY7x5X0jbNPj3-_yQBtjL0069AH3DmPpwZU7516GfZa4Wsd4xwsnkE7qI3uI9rvpAnw6fU8Rj_PprfVRXJ1c35ZTa4SlRU5TUAwVXacNUUuQbSMd41MWUYZT7loGwEMyqyl8a8kp7xJRZ6TDFogPG4VJbBj9HXrXXn3a4DQ10sdFBgjLbgh1BtZnhKR8Yh--Qe9c4O38XWRysuUZEVWRGq8pZR3IXjo6pXXS-nXNSX1pqd601O96ykufH7VDs0S2h3-VkwEyi1wrw2s_6OrJ9eX03f5MzfyoH8</recordid><startdate>20200309</startdate><enddate>20200309</enddate><creator>Yang, Yuanyuan</creator><creator>Zhang, Lifu</creator><creator>Hu, Zhenpeng</creator><creator>Zheng, Yao</creator><creator>Tang, Cheng</creator><creator>Chen, Ping</creator><creator>Wang, Ruguang</creator><creator>Qiu, Kangwen</creator><creator>Mao, Jing</creator><creator>Ling, Tao</creator><creator>Qiao, Shi‐Zhang</creator><general>Wiley Subscription Services, Inc</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-8830-4492</orcidid></search><sort><creationdate>20200309</creationdate><title>The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon‐Based Catalysts for Electrocatalytic Nitrogen Reduction</title><author>Yang, Yuanyuan ; Zhang, Lifu ; Hu, Zhenpeng ; Zheng, Yao ; Tang, Cheng ; Chen, Ping ; Wang, Ruguang ; Qiu, Kangwen ; Mao, Jing ; Ling, Tao ; Qiao, Shi‐Zhang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c4761-e83c9f53b76ae8d35fba234135258db8e3e94d18800615b286604ede059f579e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Accumulation</topic><topic>Carbon</topic><topic>carbon materials</topic><topic>Catalysts</topic><topic>chalcogens</topic><topic>Chemical reduction</topic><topic>electrocatalysis</topic><topic>Electrocatalysts</topic><topic>Electrochemistry</topic><topic>Electronic structure</topic><topic>nitrogen reduction reaction</topic><topic>Polarization</topic><topic>Polarization (spin alignment)</topic><topic>Protonation</topic><topic>Tellurium</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Yang, Yuanyuan</creatorcontrib><creatorcontrib>Zhang, Lifu</creatorcontrib><creatorcontrib>Hu, Zhenpeng</creatorcontrib><creatorcontrib>Zheng, Yao</creatorcontrib><creatorcontrib>Tang, Cheng</creatorcontrib><creatorcontrib>Chen, Ping</creatorcontrib><creatorcontrib>Wang, Ruguang</creatorcontrib><creatorcontrib>Qiu, Kangwen</creatorcontrib><creatorcontrib>Mao, Jing</creatorcontrib><creatorcontrib>Ling, Tao</creatorcontrib><creatorcontrib>Qiao, Shi‐Zhang</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Yang, Yuanyuan</au><au>Zhang, Lifu</au><au>Hu, Zhenpeng</au><au>Zheng, Yao</au><au>Tang, Cheng</au><au>Chen, Ping</au><au>Wang, Ruguang</au><au>Qiu, Kangwen</au><au>Mao, Jing</au><au>Ling, Tao</au><au>Qiao, Shi‐Zhang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon‐Based Catalysts for Electrocatalytic Nitrogen Reduction</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2020-03-09</date><risdate>2020</risdate><volume>59</volume><issue>11</issue><spage>4525</spage><epage>4531</epage><pages>4525-4531</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Cost‐effective carbon‐based catalysts are promising for catalyzing the electrochemical N2 reduction reaction (NRR). However, the activity origin of carbon‐based catalysts towards NRR remains unclear, and regularities and rules for the rational design of carbon‐based NRR electrocatalysts are still lacking. Based on a combination of theoretical calculations and experimental observations, chalcogen/oxygen group element (O, S, Se, Te) doped carbon materials were systematically evaluated as potential NRR catalysts. Heteroatom‐doping‐induced charge accumulation facilitates N2 adsorption on carbon atoms and spin polarization boosts the potential‐determining step of the first protonation to form *NNH. Te‐doped and Se‐doped C catalysts exhibited high intrinsic NRR activity that is superior to most metal‐based catalysts. Establishing the correlation between the electronic structure and NRR performance for carbon‐based materials paves the pathway for their NRR application.
Unearthing the NRR: This systematically combined computational and experimental work uncovers the catalytic nature of carbon‐based materials towards the electrocatalytic nitrogen reduction reaction (NRR).</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>31950550</pmid><doi>10.1002/anie.201915001</doi><tpages>7</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-8830-4492</orcidid></addata></record> |
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| subjects | Accumulation Carbon carbon materials Catalysts chalcogens Chemical reduction electrocatalysis Electrocatalysts Electrochemistry Electronic structure nitrogen reduction reaction Polarization Polarization (spin alignment) Protonation Tellurium |
| title | The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon‐Based Catalysts for Electrocatalytic Nitrogen Reduction |
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