Tailoring the spin state of active sites in amorphous transition metal sulfides to promote oxygen electrocatalysis
Spin regulation of active sites is sparking much interest in boosting oxygen electrocatalytic performance. However, in amorphous electrocatalysts, the design principle of spin regulation to promote catalytic activity remains unclear. Herein, we synthesized a series of heteroatom-doped amorphous tran...
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| Veröffentlicht in: | Science China materials 2022-12, Vol.65 (12), p.3479-3489 |
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| container_title | Science China materials |
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| creator | Li, Xiaopeng Zhang, Hong Wang, Yang Wang, Haozhi Wang, Jiajun Zhang, Jinfeng Qiu, Liuzhe Deng, Yida Han, Xiaopeng Hu, Wenbin |
| description | Spin regulation of active sites is sparking much interest in boosting oxygen electrocatalytic performance. However, in amorphous electrocatalysts, the design principle of spin regulation to promote catalytic activity remains unclear. Herein, we synthesized a series of heteroatom-doped amorphous transition metal sulfides with regulated spin states using a one-step hydrothermal process. Especially in Mo-doped CoS, the spin state of Co
2+
was successfully modulated to the low-spin state, which could optimize the adsorption free energy of various intermediates, improving the oxygen reduction reaction kinetics. The fabricated Zn-air batteries (ZABs) delivered good cycle stability (over 100 h). The large ZAB (100 cm
2
) exhibited a high discharge voltage (1.25 V under 0.5 A) and a superior overall mass-energy density (93 W h kg
−1
), which illuminated a 2.5-m light-emitting-diode ribbon for over seven days. This work provides new insight into the mechanism of engineering spin states in amorphous materials for oxygen electrocatalysis. |
| doi_str_mv | 10.1007/s40843-022-2048-2 |
| format | Article |
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2+
was successfully modulated to the low-spin state, which could optimize the adsorption free energy of various intermediates, improving the oxygen reduction reaction kinetics. The fabricated Zn-air batteries (ZABs) delivered good cycle stability (over 100 h). The large ZAB (100 cm
2
) exhibited a high discharge voltage (1.25 V under 0.5 A) and a superior overall mass-energy density (93 W h kg
−1
), which illuminated a 2.5-m light-emitting-diode ribbon for over seven days. This work provides new insight into the mechanism of engineering spin states in amorphous materials for oxygen electrocatalysis.</description><identifier>ISSN: 2095-8226</identifier><identifier>EISSN: 2199-4501</identifier><identifier>DOI: 10.1007/s40843-022-2048-2</identifier><language>eng</language><publisher>Beijing: Science China Press</publisher><subject>Amorphous materials ; Catalytic activity ; Chemical reduction ; Chemistry and Materials Science ; Chemistry/Food Science ; Cobalt ; Electrocatalysis ; Electrocatalysts ; Free energy ; Light emitting diodes ; Materials Science ; Metal air batteries ; Metal sulfides ; Oxygen reduction reactions ; Reaction kinetics ; Transition metals ; Zinc-oxygen batteries</subject><ispartof>Science China materials, 2022-12, Vol.65 (12), p.3479-3489</ispartof><rights>Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2022</rights><rights>Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2022.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c359t-f6bc2b5d57e844d5b6bd29df6b08a239f5b0d1f68f4d8b866c184dd87dbd412b3</citedby><cites>FETCH-LOGICAL-c359t-f6bc2b5d57e844d5b6bd29df6b08a239f5b0d1f68f4d8b866c184dd87dbd412b3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1007/s40843-022-2048-2$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s40843-022-2048-2$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>314,777,781,27905,27906,41469,42538,51300</link.rule.ids></links><search><creatorcontrib>Li, Xiaopeng</creatorcontrib><creatorcontrib>Zhang, Hong</creatorcontrib><creatorcontrib>Wang, Yang</creatorcontrib><creatorcontrib>Wang, Haozhi</creatorcontrib><creatorcontrib>Wang, Jiajun</creatorcontrib><creatorcontrib>Zhang, Jinfeng</creatorcontrib><creatorcontrib>Qiu, Liuzhe</creatorcontrib><creatorcontrib>Deng, Yida</creatorcontrib><creatorcontrib>Han, Xiaopeng</creatorcontrib><creatorcontrib>Hu, Wenbin</creatorcontrib><title>Tailoring the spin state of active sites in amorphous transition metal sulfides to promote oxygen electrocatalysis</title><title>Science China materials</title><addtitle>Sci. China Mater</addtitle><description>Spin regulation of active sites is sparking much interest in boosting oxygen electrocatalytic performance. However, in amorphous electrocatalysts, the design principle of spin regulation to promote catalytic activity remains unclear. Herein, we synthesized a series of heteroatom-doped amorphous transition metal sulfides with regulated spin states using a one-step hydrothermal process. Especially in Mo-doped CoS, the spin state of Co
2+
was successfully modulated to the low-spin state, which could optimize the adsorption free energy of various intermediates, improving the oxygen reduction reaction kinetics. The fabricated Zn-air batteries (ZABs) delivered good cycle stability (over 100 h). The large ZAB (100 cm
2
) exhibited a high discharge voltage (1.25 V under 0.5 A) and a superior overall mass-energy density (93 W h kg
−1
), which illuminated a 2.5-m light-emitting-diode ribbon for over seven days. This work provides new insight into the mechanism of engineering spin states in amorphous materials for oxygen electrocatalysis.</description><subject>Amorphous materials</subject><subject>Catalytic activity</subject><subject>Chemical reduction</subject><subject>Chemistry and Materials Science</subject><subject>Chemistry/Food Science</subject><subject>Cobalt</subject><subject>Electrocatalysis</subject><subject>Electrocatalysts</subject><subject>Free energy</subject><subject>Light emitting diodes</subject><subject>Materials Science</subject><subject>Metal air batteries</subject><subject>Metal sulfides</subject><subject>Oxygen reduction reactions</subject><subject>Reaction kinetics</subject><subject>Transition metals</subject><subject>Zinc-oxygen batteries</subject><issn>2095-8226</issn><issn>2199-4501</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNp1kM1qxCAUhUNpocN0HqA7oWtbNZqYZRn6BwPdTNeiUWcckpiqKZ23ryGFrrq6l-M558pXFLcY3WOE6odIEaclRIRAgiiH5KJYEdw0kDKEL_OOGgY5IdV1sYnxhBDCFcO44asi7KXrfHDDAaSjAXF0A4hJJgO8BbJN7iuLLpkI8oPsfRiPfoogBTlk2fkB9CbJDsSps05nW_JgDL73c8P3-WAGYDrTpuBbmX3n6OJNcWVlF83md66Lj-en_fYV7t5f3raPO9iWrEnQVqolimlWG06pZqpSmjQ6y4hLUjaWKaSxrbilmiteVS3mVGtea6UpJqpcF3dLb_7P52RiEic_hSGfFKSmNWOYcJJdeHG1wccYjBVjcL0MZ4GRmOmKha7IdMVMV8wZsmTiOJMz4a_5_9APj1Z_sQ</recordid><startdate>20221201</startdate><enddate>20221201</enddate><creator>Li, Xiaopeng</creator><creator>Zhang, Hong</creator><creator>Wang, Yang</creator><creator>Wang, Haozhi</creator><creator>Wang, Jiajun</creator><creator>Zhang, Jinfeng</creator><creator>Qiu, Liuzhe</creator><creator>Deng, Yida</creator><creator>Han, Xiaopeng</creator><creator>Hu, Wenbin</creator><general>Science China Press</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20221201</creationdate><title>Tailoring the spin state of active sites in amorphous transition metal sulfides to promote oxygen electrocatalysis</title><author>Li, Xiaopeng ; Zhang, Hong ; Wang, Yang ; Wang, Haozhi ; Wang, Jiajun ; Zhang, Jinfeng ; Qiu, Liuzhe ; Deng, Yida ; Han, Xiaopeng ; Hu, Wenbin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c359t-f6bc2b5d57e844d5b6bd29df6b08a239f5b0d1f68f4d8b866c184dd87dbd412b3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Amorphous materials</topic><topic>Catalytic activity</topic><topic>Chemical reduction</topic><topic>Chemistry and Materials Science</topic><topic>Chemistry/Food Science</topic><topic>Cobalt</topic><topic>Electrocatalysis</topic><topic>Electrocatalysts</topic><topic>Free energy</topic><topic>Light emitting diodes</topic><topic>Materials Science</topic><topic>Metal air batteries</topic><topic>Metal sulfides</topic><topic>Oxygen reduction reactions</topic><topic>Reaction kinetics</topic><topic>Transition metals</topic><topic>Zinc-oxygen batteries</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Li, Xiaopeng</creatorcontrib><creatorcontrib>Zhang, Hong</creatorcontrib><creatorcontrib>Wang, Yang</creatorcontrib><creatorcontrib>Wang, Haozhi</creatorcontrib><creatorcontrib>Wang, Jiajun</creatorcontrib><creatorcontrib>Zhang, Jinfeng</creatorcontrib><creatorcontrib>Qiu, Liuzhe</creatorcontrib><creatorcontrib>Deng, Yida</creatorcontrib><creatorcontrib>Han, Xiaopeng</creatorcontrib><creatorcontrib>Hu, Wenbin</creatorcontrib><collection>CrossRef</collection><jtitle>Science China materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Li, Xiaopeng</au><au>Zhang, Hong</au><au>Wang, Yang</au><au>Wang, Haozhi</au><au>Wang, Jiajun</au><au>Zhang, Jinfeng</au><au>Qiu, Liuzhe</au><au>Deng, Yida</au><au>Han, Xiaopeng</au><au>Hu, Wenbin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Tailoring the spin state of active sites in amorphous transition metal sulfides to promote oxygen electrocatalysis</atitle><jtitle>Science China materials</jtitle><stitle>Sci. China Mater</stitle><date>2022-12-01</date><risdate>2022</risdate><volume>65</volume><issue>12</issue><spage>3479</spage><epage>3489</epage><pages>3479-3489</pages><issn>2095-8226</issn><eissn>2199-4501</eissn><abstract>Spin regulation of active sites is sparking much interest in boosting oxygen electrocatalytic performance. However, in amorphous electrocatalysts, the design principle of spin regulation to promote catalytic activity remains unclear. Herein, we synthesized a series of heteroatom-doped amorphous transition metal sulfides with regulated spin states using a one-step hydrothermal process. Especially in Mo-doped CoS, the spin state of Co
2+
was successfully modulated to the low-spin state, which could optimize the adsorption free energy of various intermediates, improving the oxygen reduction reaction kinetics. The fabricated Zn-air batteries (ZABs) delivered good cycle stability (over 100 h). The large ZAB (100 cm
2
) exhibited a high discharge voltage (1.25 V under 0.5 A) and a superior overall mass-energy density (93 W h kg
−1
), which illuminated a 2.5-m light-emitting-diode ribbon for over seven days. This work provides new insight into the mechanism of engineering spin states in amorphous materials for oxygen electrocatalysis.</abstract><cop>Beijing</cop><pub>Science China Press</pub><doi>10.1007/s40843-022-2048-2</doi><tpages>11</tpages><oa>free_for_read</oa></addata></record> |
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| subjects | Amorphous materials Catalytic activity Chemical reduction Chemistry and Materials Science Chemistry/Food Science Cobalt Electrocatalysis Electrocatalysts Free energy Light emitting diodes Materials Science Metal air batteries Metal sulfides Oxygen reduction reactions Reaction kinetics Transition metals Zinc-oxygen batteries |
| title | Tailoring the spin state of active sites in amorphous transition metal sulfides to promote oxygen electrocatalysis |
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