Unveiling the high-activity origin of single-atom iron catalysts for oxygen reduction reaction
It is still a grand challenge to develop a highly efficient nonprecious-metal electrocatalyst to replace the Pt-based catalysts for oxygen reduction reaction (ORR). Here, we propose a surfactant-assisted method to synthesize single-atom iron catalysts (SA-Fe/NG). The halfwave potential of SA-Fe/NG i...
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| Veröffentlicht in: | Proceedings of the National Academy of Sciences - PNAS 2018-06, Vol.115 (26), p.6626-6631 |
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| container_title | Proceedings of the National Academy of Sciences - PNAS |
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| creator | Yang, Liu Cheng, Daojian Xu, Haoxiang Zeng, Xiaofei Wan, Xin Shui, Jianglan Xiang, Zhonghua Cao, Dapeng |
| description | It is still a grand challenge to develop a highly efficient nonprecious-metal electrocatalyst to replace the Pt-based catalysts for oxygen reduction reaction (ORR). Here, we propose a surfactant-assisted method to synthesize single-atom iron catalysts (SA-Fe/NG). The halfwave potential of SA-Fe/NG is only 30 mV less than 20% Pt/C in acidic medium, while it is 30 mV superior to 20% Pt/C in alkaline medium. Moreover, SA-Fe/NG shows extremely high stability with only 12 mV and 15 mV negative shifts after 5,000 cycles in acidic and alkaline media, respectively. Impressively, the SA-Fe/NG-based acidic proton exchange membrane fuel cell (PEMFC) exhibits a high power density of 823 mW cm−2. Combining experimental results and density-functional theory (DFT) calculations, we further reveal that the origin of high-ORR activity of SA-Fe/NG is from the Fe-pyrrolic-N species, because such molecular incorporation is the key, leading to the active site increase in an order of magnitude which successfully clarifies the bottleneck puzzle of why a small amount of iron in the SA-Fe catalysts can exhibit extremely superior ORR activity. |
| doi_str_mv | 10.1073/pnas.1800771115 |
| format | Article |
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Here, we propose a surfactant-assisted method to synthesize single-atom iron catalysts (SA-Fe/NG). The halfwave potential of SA-Fe/NG is only 30 mV less than 20% Pt/C in acidic medium, while it is 30 mV superior to 20% Pt/C in alkaline medium. Moreover, SA-Fe/NG shows extremely high stability with only 12 mV and 15 mV negative shifts after 5,000 cycles in acidic and alkaline media, respectively. Impressively, the SA-Fe/NG-based acidic proton exchange membrane fuel cell (PEMFC) exhibits a high power density of 823 mW cm−2. Combining experimental results and density-functional theory (DFT) calculations, we further reveal that the origin of high-ORR activity of SA-Fe/NG is from the Fe-pyrrolic-N species, because such molecular incorporation is the key, leading to the active site increase in an order of magnitude which successfully clarifies the bottleneck puzzle of why a small amount of iron in the SA-Fe catalysts can exhibit extremely superior ORR activity.</description><identifier>ISSN: 0027-8424</identifier><identifier>EISSN: 1091-6490</identifier><identifier>DOI: 10.1073/pnas.1800771115</identifier><identifier>PMID: 29891686</identifier><language>eng</language><publisher>United States: National Academy of Sciences</publisher><subject>Atoms & subatomic particles ; Carbon ; Catalysis ; Catalysts ; Chemical reduction ; Chemical synthesis ; Density functional theory ; Fuel technology ; Iron ; Oxygen ; Oxygen reduction reactions ; Physical Sciences ; Platinum ; Proton exchange membrane fuel cells</subject><ispartof>Proceedings of the National Academy of Sciences - PNAS, 2018-06, Vol.115 (26), p.6626-6631</ispartof><rights>Volumes 1–89 and 106–114, copyright as a collective work only; author(s) retains copyright to individual articles</rights><rights>Copyright National Academy of Sciences Jun 26, 2018</rights><rights>2018</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c509t-bf0477c6b05c6cb75d26caaef24b0bde1a40ceef7bb36eeae677f9f4831aa2533</citedby><cites>FETCH-LOGICAL-c509t-bf0477c6b05c6cb75d26caaef24b0bde1a40ceef7bb36eeae677f9f4831aa2533</cites><orcidid>0000-0002-6981-7794</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.jstor.org/stable/pdf/26510788$$EPDF$$P50$$Gjstor$$H</linktopdf><linktohtml>$$Uhttps://www.jstor.org/stable/26510788$$EHTML$$P50$$Gjstor$$H</linktohtml><link.rule.ids>230,314,723,776,780,799,881,27901,27902,53766,53768,57992,58225</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/29891686$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Yang, Liu</creatorcontrib><creatorcontrib>Cheng, Daojian</creatorcontrib><creatorcontrib>Xu, Haoxiang</creatorcontrib><creatorcontrib>Zeng, Xiaofei</creatorcontrib><creatorcontrib>Wan, Xin</creatorcontrib><creatorcontrib>Shui, Jianglan</creatorcontrib><creatorcontrib>Xiang, Zhonghua</creatorcontrib><creatorcontrib>Cao, Dapeng</creatorcontrib><title>Unveiling the high-activity origin of single-atom iron catalysts for oxygen reduction reaction</title><title>Proceedings of the National Academy of Sciences - PNAS</title><addtitle>Proc Natl Acad Sci U S A</addtitle><description>It is still a grand challenge to develop a highly efficient nonprecious-metal electrocatalyst to replace the Pt-based catalysts for oxygen reduction reaction (ORR). Here, we propose a surfactant-assisted method to synthesize single-atom iron catalysts (SA-Fe/NG). The halfwave potential of SA-Fe/NG is only 30 mV less than 20% Pt/C in acidic medium, while it is 30 mV superior to 20% Pt/C in alkaline medium. Moreover, SA-Fe/NG shows extremely high stability with only 12 mV and 15 mV negative shifts after 5,000 cycles in acidic and alkaline media, respectively. Impressively, the SA-Fe/NG-based acidic proton exchange membrane fuel cell (PEMFC) exhibits a high power density of 823 mW cm−2. Combining experimental results and density-functional theory (DFT) calculations, we further reveal that the origin of high-ORR activity of SA-Fe/NG is from the Fe-pyrrolic-N species, because such molecular incorporation is the key, leading to the active site increase in an order of magnitude which successfully clarifies the bottleneck puzzle of why a small amount of iron in the SA-Fe catalysts can exhibit extremely superior ORR activity.</description><subject>Atoms & subatomic particles</subject><subject>Carbon</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemical reduction</subject><subject>Chemical synthesis</subject><subject>Density functional theory</subject><subject>Fuel technology</subject><subject>Iron</subject><subject>Oxygen</subject><subject>Oxygen reduction reactions</subject><subject>Physical Sciences</subject><subject>Platinum</subject><subject>Proton exchange membrane fuel cells</subject><issn>0027-8424</issn><issn>1091-6490</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNpdkUFv1DAQhS0EokvhzAlkiQuXtGPHsZ0LEqpaQKrUS3vFcryTrFdZe7GdFfvvyXZLSznNk943TzN6hLxncMZA1efbYPMZ0wBKMcaaF2TBoGWVFC28JAsAriotuDghb3JeA0DbaHhNTnirWya1XJCfd2GHfvRhoGWFdOWHVWVd8Ttf9jQmP_hAY0_zDIxY2RI31KcYqLPFjvtcMu1jovH3fsBAEy6neTcelL0Xb8mr3o4Z3z3MU3J3dXl78b26vvn24-LrdeUaaEvV9SCUcrKDxknXqWbJpbMWey466JbIrACH2KuuqyWiRalU3_ZC18xa3tT1KflyzN1O3QaXDkNJdjTb5Dc27U203jx3gl-ZIe6MBMFBqjng80NAir8mzMVsfHY4jjZgnLLh0IhWSKH4jH76D13HKYX5PcMZgNZcMJip8yPlUsw5Yf94DANz6M4cujNP3c0bH__94ZH_W9YMfDgC61xievJlM-dpXf8B9cmiVQ</recordid><startdate>20180626</startdate><enddate>20180626</enddate><creator>Yang, Liu</creator><creator>Cheng, Daojian</creator><creator>Xu, Haoxiang</creator><creator>Zeng, Xiaofei</creator><creator>Wan, Xin</creator><creator>Shui, Jianglan</creator><creator>Xiang, Zhonghua</creator><creator>Cao, Dapeng</creator><general>National Academy of Sciences</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QG</scope><scope>7QL</scope><scope>7QP</scope><scope>7QR</scope><scope>7SN</scope><scope>7SS</scope><scope>7T5</scope><scope>7TK</scope><scope>7TM</scope><scope>7TO</scope><scope>7U9</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>H94</scope><scope>M7N</scope><scope>P64</scope><scope>RC3</scope><scope>7X8</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0002-6981-7794</orcidid></search><sort><creationdate>20180626</creationdate><title>Unveiling the high-activity origin of single-atom iron catalysts for oxygen reduction reaction</title><author>Yang, Liu ; 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Here, we propose a surfactant-assisted method to synthesize single-atom iron catalysts (SA-Fe/NG). The halfwave potential of SA-Fe/NG is only 30 mV less than 20% Pt/C in acidic medium, while it is 30 mV superior to 20% Pt/C in alkaline medium. Moreover, SA-Fe/NG shows extremely high stability with only 12 mV and 15 mV negative shifts after 5,000 cycles in acidic and alkaline media, respectively. Impressively, the SA-Fe/NG-based acidic proton exchange membrane fuel cell (PEMFC) exhibits a high power density of 823 mW cm−2. Combining experimental results and density-functional theory (DFT) calculations, we further reveal that the origin of high-ORR activity of SA-Fe/NG is from the Fe-pyrrolic-N species, because such molecular incorporation is the key, leading to the active site increase in an order of magnitude which successfully clarifies the bottleneck puzzle of why a small amount of iron in the SA-Fe catalysts can exhibit extremely superior ORR activity.</abstract><cop>United States</cop><pub>National Academy of Sciences</pub><pmid>29891686</pmid><doi>10.1073/pnas.1800771115</doi><tpages>6</tpages><orcidid>https://orcid.org/0000-0002-6981-7794</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | Atoms & subatomic particles Carbon Catalysis Catalysts Chemical reduction Chemical synthesis Density functional theory Fuel technology Iron Oxygen Oxygen reduction reactions Physical Sciences Platinum Proton exchange membrane fuel cells |
| title | Unveiling the high-activity origin of single-atom iron catalysts for oxygen reduction reaction |
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