Unconventional Interconnected High-Entropy Alloy Nanodendrites for Remarkably Efficient C-C Bond Cleavage toward Complete Ethanol Oxidation
Developing ethanol oxidation electrocatalysts with high catalytic activity, durability, and resistance to CO poisoning remains a major challenge. High-entropy alloys (HEAs) with unique physical and chemical properties have garnered substantial attention. Herein, a class of HEA nanodendrites are desi...
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description | Developing ethanol oxidation electrocatalysts with high catalytic activity, durability, and resistance to CO poisoning remains a major challenge. High-entropy alloys (HEAs) with unique physical and chemical properties have garnered substantial attention. Herein, a class of HEA nanodendrites are designed by a simple wet-chemical method. The mass activity and specific activity of the septenary PtIrRhCoFeNiCu high-entropy alloy catalyst are 2.13 A mgPt-1/1.05 A mgPt+Ir+Rh-1 and 2.95 mA cm-2, which reach 5.76-/2.84-fold and 5.57-fold improvements relative to commercial Pt/C (0.37 A mgPt-1 and 0.53 mA cm-2), respectively. Remarkably, after the i-t test of up to 100,000s and the accelerated durability test of 1500 cycles, 81.22% and 68.54% of the initial mass activity are well retained, respectively. The lattice distortion-associated local tensile strain as demonstrated by increased Pt-Pt bond length enhances ethanol adsorption and reduces reaction barriers. The upshift d-band center promotes ethanol oxidation and anti-CO capability of the catalysts. Moreover, hysteresis diffusion effect induced by lattice distortion in the HEA nanodendrites contributes to their superb ethanol oxidation stability. In-situ infrared absorption spectroscopy reveals that the three HEA nanodendrites mainly follow C1 pathway with C-C bond breaking to form CO followed by CO oxidation especially at a wide range of high potentials. |
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High-entropy alloys (HEAs) with unique physical and chemical properties have garnered substantial attention. Herein, a class of HEA nanodendrites are designed by a simple wet-chemical method. The mass activity and specific activity of the septenary PtIrRhCoFeNiCu high-entropy alloy catalyst are 2.13 A mgPt-1/1.05 A mgPt+Ir+Rh-1 and 2.95 mA cm-2, which reach 5.76-/2.84-fold and 5.57-fold improvements relative to commercial Pt/C (0.37 A mgPt-1 and 0.53 mA cm-2), respectively. Remarkably, after the i-t test of up to 100,000s and the accelerated durability test of 1500 cycles, 81.22% and 68.54% of the initial mass activity are well retained, respectively. The lattice distortion-associated local tensile strain as demonstrated by increased Pt-Pt bond length enhances ethanol adsorption and reduces reaction barriers. The upshift d-band center promotes ethanol oxidation and anti-CO capability of the catalysts. Moreover, hysteresis diffusion effect induced by lattice distortion in the HEA nanodendrites contributes to their superb ethanol oxidation stability. In-situ infrared absorption spectroscopy reveals that the three HEA nanodendrites mainly follow C1 pathway with C-C bond breaking to form CO followed by CO oxidation especially at a wide range of high potentials.</description><identifier>ISSN: 1433-7851</identifier><identifier>ISSN: 1521-3773</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202420752</identifier><identifier>PMID: 39714408</identifier><language>eng</language><publisher>Germany</publisher><ispartof>Angewandte Chemie International Edition, 2024-12, p.e202420752</ispartof><rights>2024 Wiley‐VCH GmbH.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,778,782,27907,27908</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/39714408$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Wang, Yan</creatorcontrib><creatorcontrib>Meng, Huiying</creatorcontrib><creatorcontrib>Yu, Renqin</creatorcontrib><creatorcontrib>Hong, Jie</creatorcontrib><creatorcontrib>Zhang, Yifan</creatorcontrib><creatorcontrib>Xia, Zhonghong</creatorcontrib><creatorcontrib>Wang, Yong</creatorcontrib><title>Unconventional Interconnected High-Entropy Alloy Nanodendrites for Remarkably Efficient C-C Bond Cleavage toward Complete Ethanol Oxidation</title><title>Angewandte Chemie International Edition</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>Developing ethanol oxidation electrocatalysts with high catalytic activity, durability, and resistance to CO poisoning remains a major challenge. High-entropy alloys (HEAs) with unique physical and chemical properties have garnered substantial attention. Herein, a class of HEA nanodendrites are designed by a simple wet-chemical method. The mass activity and specific activity of the septenary PtIrRhCoFeNiCu high-entropy alloy catalyst are 2.13 A mgPt-1/1.05 A mgPt+Ir+Rh-1 and 2.95 mA cm-2, which reach 5.76-/2.84-fold and 5.57-fold improvements relative to commercial Pt/C (0.37 A mgPt-1 and 0.53 mA cm-2), respectively. Remarkably, after the i-t test of up to 100,000s and the accelerated durability test of 1500 cycles, 81.22% and 68.54% of the initial mass activity are well retained, respectively. The lattice distortion-associated local tensile strain as demonstrated by increased Pt-Pt bond length enhances ethanol adsorption and reduces reaction barriers. The upshift d-band center promotes ethanol oxidation and anti-CO capability of the catalysts. Moreover, hysteresis diffusion effect induced by lattice distortion in the HEA nanodendrites contributes to their superb ethanol oxidation stability. In-situ infrared absorption spectroscopy reveals that the three HEA nanodendrites mainly follow C1 pathway with C-C bond breaking to form CO followed by CO oxidation especially at a wide range of high potentials.</description><issn>1433-7851</issn><issn>1521-3773</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNo9kEtPGzEUha2KqlDabZfISzaT2mM79ixhFAoSKlJF1yM_7oCLYwfbAfIb-qfrCMrqPnTuuTofQt8oWVBC-u86elj0pOc9kaL_gI6o6GnHpGQHreeMdVIJeog-l_Kn6ZUiy0_okA2Sck7UEfr7O9oUnyBWn6IO-CpWyG0TwVZw-NLf3XerWHPa7PBZCGmHf-qYHESXfYWC55TxL1jr_KBN2OHVPHvrmxseuxGfp-jwGEA_6TvANT3r3Oa03gSogFf1vlkFfPPind6__4I-zjoU-PpWj9Htxep2vOyub35cjWfXnR2E6gQFbZZaOsa1GowdnFaGGy4YtERWKsN6RgfBlRTCampmxgif7dIQsnTcsGN0-mq7yelxC6VOa18shKAjpG2ZGOVKECJ62aSLV6nNqZQM87TJvoXdTZRMe_7Tnv_0zr8dnLx5b80a3Lv8P3D2D7zPgyY</recordid><startdate>20241223</startdate><enddate>20241223</enddate><creator>Wang, Yan</creator><creator>Meng, Huiying</creator><creator>Yu, Renqin</creator><creator>Hong, Jie</creator><creator>Zhang, Yifan</creator><creator>Xia, Zhonghong</creator><creator>Wang, Yong</creator><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20241223</creationdate><title>Unconventional Interconnected High-Entropy Alloy Nanodendrites for Remarkably Efficient C-C Bond Cleavage toward Complete Ethanol Oxidation</title><author>Wang, Yan ; Meng, Huiying ; Yu, Renqin ; Hong, Jie ; Zhang, Yifan ; Xia, Zhonghong ; Wang, Yong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c958-51eab6a7d34a89bc9da8b4b453e408c78b32319548755ca1bf3304fc6b006d4b3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wang, Yan</creatorcontrib><creatorcontrib>Meng, Huiying</creatorcontrib><creatorcontrib>Yu, Renqin</creatorcontrib><creatorcontrib>Hong, Jie</creatorcontrib><creatorcontrib>Zhang, Yifan</creatorcontrib><creatorcontrib>Xia, Zhonghong</creatorcontrib><creatorcontrib>Wang, Yong</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Wang, Yan</au><au>Meng, Huiying</au><au>Yu, Renqin</au><au>Hong, Jie</au><au>Zhang, Yifan</au><au>Xia, Zhonghong</au><au>Wang, Yong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Unconventional Interconnected High-Entropy Alloy Nanodendrites for Remarkably Efficient C-C Bond Cleavage toward Complete Ethanol Oxidation</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2024-12-23</date><risdate>2024</risdate><spage>e202420752</spage><pages>e202420752-</pages><issn>1433-7851</issn><issn>1521-3773</issn><eissn>1521-3773</eissn><abstract>Developing ethanol oxidation electrocatalysts with high catalytic activity, durability, and resistance to CO poisoning remains a major challenge. High-entropy alloys (HEAs) with unique physical and chemical properties have garnered substantial attention. Herein, a class of HEA nanodendrites are designed by a simple wet-chemical method. The mass activity and specific activity of the septenary PtIrRhCoFeNiCu high-entropy alloy catalyst are 2.13 A mgPt-1/1.05 A mgPt+Ir+Rh-1 and 2.95 mA cm-2, which reach 5.76-/2.84-fold and 5.57-fold improvements relative to commercial Pt/C (0.37 A mgPt-1 and 0.53 mA cm-2), respectively. Remarkably, after the i-t test of up to 100,000s and the accelerated durability test of 1500 cycles, 81.22% and 68.54% of the initial mass activity are well retained, respectively. The lattice distortion-associated local tensile strain as demonstrated by increased Pt-Pt bond length enhances ethanol adsorption and reduces reaction barriers. The upshift d-band center promotes ethanol oxidation and anti-CO capability of the catalysts. Moreover, hysteresis diffusion effect induced by lattice distortion in the HEA nanodendrites contributes to their superb ethanol oxidation stability. In-situ infrared absorption spectroscopy reveals that the three HEA nanodendrites mainly follow C1 pathway with C-C bond breaking to form CO followed by CO oxidation especially at a wide range of high potentials.</abstract><cop>Germany</cop><pmid>39714408</pmid><doi>10.1002/anie.202420752</doi></addata></record> |
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title | Unconventional Interconnected High-Entropy Alloy Nanodendrites for Remarkably Efficient C-C Bond Cleavage toward Complete Ethanol Oxidation |
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