Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production
The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solution to the energy crisis, but its low efficiency hinders its scale-up feasibility. In this work, a hollow core-shell structure OCN@In 2 S 3 composite photocatalyst was constructed by growing In 2 S...
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Veröffentlicht in: | Science China materials 2024, Vol.67 (1), p.153-161 |
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description | The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solution to the energy crisis, but its low efficiency hinders its scale-up feasibility. In this work, a hollow core-shell structure OCN@In
2
S
3
composite photocatalyst was constructed by growing In
2
S
3
ultrathin nanosheets on the surface of O-doped hollow g-C
3
N
4
nanospheres using a two-step hydrothermal method. The hollow structure provided a high specific surface area and enhanced light absorption. O doping increased the number of active sites, and the heterojunction promoted the rapid separation and transfer of photogenerated carriers. Under visible light irradiation, the H
2
O
2
yield of OCN@In
2
S
3
reached 632.5 µmol h
−1
g
−1
, which was 5.7 times higher than that of g-C
3
N
4
and 12.3 times that of In
2
S
3
, as well as higher than most g-C
3
N
4
-based photocatalysts. Quenching experiments and electron paramagnetic resonance spectroscopy showed that ·O
2
−
was an intermediate product formed during photocatalytic H
2
O
2
generation. The reaction primarily followed a two-step single-electron pathway. The Koutecky-Levich diagram confirmed that the synthesized OCN@In
2
S
3
maintained a high two-electron ORR selectivity during the catalytic reaction (
n
= 1.67). The photocatalytic mechanism was elucidated by photoluminescence, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectro-scopy, which confirmed that OCN@In
2
S
3
inhibited the recombination of photogenerated carriers. This work provides a simple and attractive strategy for developing highly active energy-conversion photocatalysts. |
doi_str_mv | 10.1007/s40843-023-2659-9 |
format | Article |
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2
S
3
composite photocatalyst was constructed by growing In
2
S
3
ultrathin nanosheets on the surface of O-doped hollow g-C
3
N
4
nanospheres using a two-step hydrothermal method. The hollow structure provided a high specific surface area and enhanced light absorption. O doping increased the number of active sites, and the heterojunction promoted the rapid separation and transfer of photogenerated carriers. Under visible light irradiation, the H
2
O
2
yield of OCN@In
2
S
3
reached 632.5 µmol h
−1
g
−1
, which was 5.7 times higher than that of g-C
3
N
4
and 12.3 times that of In
2
S
3
, as well as higher than most g-C
3
N
4
-based photocatalysts. Quenching experiments and electron paramagnetic resonance spectroscopy showed that ·O
2
−
was an intermediate product formed during photocatalytic H
2
O
2
generation. The reaction primarily followed a two-step single-electron pathway. The Koutecky-Levich diagram confirmed that the synthesized OCN@In
2
S
3
maintained a high two-electron ORR selectivity during the catalytic reaction (
n
= 1.67). The photocatalytic mechanism was elucidated by photoluminescence, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectro-scopy, which confirmed that OCN@In
2
S
3
inhibited the recombination of photogenerated carriers. This work provides a simple and attractive strategy for developing highly active energy-conversion photocatalysts.</description><identifier>ISSN: 2095-8226</identifier><identifier>EISSN: 2199-4501</identifier><identifier>DOI: 10.1007/s40843-023-2659-9</identifier><language>eng</language><publisher>Beijing: Science China Press</publisher><subject>Carbon nitride ; Chemistry and Materials Science ; Chemistry/Food Science ; Core-shell structure ; Doping ; Electrochemical impedance spectroscopy ; Electromagnetic absorption ; Electron paramagnetic resonance ; Electron transfer ; Energy conversion ; Heterojunctions ; Hydrogen peroxide ; Hydrogen production ; Light irradiation ; Materials Science ; Nanospheres ; Photocatalysis ; Photocatalysts ; Photoelectrons ; Photoluminescence ; Single electrons ; Solar energy ; Spectrum analysis</subject><ispartof>Science China materials, 2024, Vol.67 (1), p.153-161</ispartof><rights>Science China Press 2023</rights><rights>Science China Press 2023.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c359t-53f97367597325dd6057d8e889c179ffa26032d0ac90f128f575f68fce759dae3</citedby><cites>FETCH-LOGICAL-c359t-53f97367597325dd6057d8e889c179ffa26032d0ac90f128f575f68fce759dae3</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/s40843-023-2659-9$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s40843-023-2659-9$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>314,776,780,27901,27902,41464,42533,51294</link.rule.ids></links><search><creatorcontrib>Xu, Yandong</creatorcontrib><creatorcontrib>Tai, Wanyu</creatorcontrib><creatorcontrib>Wang, Zhirui</creatorcontrib><creatorcontrib>Zhang, Linlin</creatorcontrib><creatorcontrib>Wang, Dexin</creatorcontrib><creatorcontrib>Liao, Jianjun</creatorcontrib><title>Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production</title><title>Science China materials</title><addtitle>Sci. China Mater</addtitle><description>The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solution to the energy crisis, but its low efficiency hinders its scale-up feasibility. In this work, a hollow core-shell structure OCN@In
2
S
3
composite photocatalyst was constructed by growing In
2
S
3
ultrathin nanosheets on the surface of O-doped hollow g-C
3
N
4
nanospheres using a two-step hydrothermal method. The hollow structure provided a high specific surface area and enhanced light absorption. O doping increased the number of active sites, and the heterojunction promoted the rapid separation and transfer of photogenerated carriers. Under visible light irradiation, the H
2
O
2
yield of OCN@In
2
S
3
reached 632.5 µmol h
−1
g
−1
, which was 5.7 times higher than that of g-C
3
N
4
and 12.3 times that of In
2
S
3
, as well as higher than most g-C
3
N
4
-based photocatalysts. Quenching experiments and electron paramagnetic resonance spectroscopy showed that ·O
2
−
was an intermediate product formed during photocatalytic H
2
O
2
generation. The reaction primarily followed a two-step single-electron pathway. The Koutecky-Levich diagram confirmed that the synthesized OCN@In
2
S
3
maintained a high two-electron ORR selectivity during the catalytic reaction (
n
= 1.67). The photocatalytic mechanism was elucidated by photoluminescence, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectro-scopy, which confirmed that OCN@In
2
S
3
inhibited the recombination of photogenerated carriers. This work provides a simple and attractive strategy for developing highly active energy-conversion photocatalysts.</description><subject>Carbon nitride</subject><subject>Chemistry and Materials Science</subject><subject>Chemistry/Food Science</subject><subject>Core-shell structure</subject><subject>Doping</subject><subject>Electrochemical impedance spectroscopy</subject><subject>Electromagnetic absorption</subject><subject>Electron paramagnetic resonance</subject><subject>Electron transfer</subject><subject>Energy conversion</subject><subject>Heterojunctions</subject><subject>Hydrogen peroxide</subject><subject>Hydrogen production</subject><subject>Light irradiation</subject><subject>Materials Science</subject><subject>Nanospheres</subject><subject>Photocatalysis</subject><subject>Photocatalysts</subject><subject>Photoelectrons</subject><subject>Photoluminescence</subject><subject>Single electrons</subject><subject>Solar energy</subject><subject>Spectrum analysis</subject><issn>2095-8226</issn><issn>2199-4501</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNp1UMtKAzEUHUTBUvsB7gKuo0mmySRLKb5A6EbXISY37ZTpZEwy2P6Bn22GCq7c3Hs5nAf3VNU1JbeUkOYuLYlc1piwGjPBFVZn1YxRpfCSE3pebqI4loyJy2qR0o4QQgWnVMlZ9b0-HDfQIxeGtt8g0zu0DV0XvlDKcbR5jID34FqTwSHwHmxOKAcEvfnoAEUztAXvChxDj3I0ffIQkRvjZDdsQw7WZNMdc2vR9uhimNIGiOHQOkBDDK6ktKG_qi686RIsfve8en98eFs949f108vq_hXbmquMee1VU4uGl8m4c4LwxkmQUlnaKO8NE6RmjhiriKdMet5wL6S3UCTOQD2vbk6-JfpzhJT1LoyxL5GaKSqEFA1dFhY9sWwMKUXweojt3sSjpkRPnetT57p0rqfOtSoadtKkYXoe4p_z_6Ifgw-HdA</recordid><startdate>2024</startdate><enddate>2024</enddate><creator>Xu, Yandong</creator><creator>Tai, Wanyu</creator><creator>Wang, Zhirui</creator><creator>Zhang, Linlin</creator><creator>Wang, Dexin</creator><creator>Liao, Jianjun</creator><general>Science China Press</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>2024</creationdate><title>Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production</title><author>Xu, Yandong ; Tai, Wanyu ; Wang, Zhirui ; Zhang, Linlin ; Wang, Dexin ; Liao, Jianjun</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c359t-53f97367597325dd6057d8e889c179ffa26032d0ac90f128f575f68fce759dae3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Carbon nitride</topic><topic>Chemistry and Materials Science</topic><topic>Chemistry/Food Science</topic><topic>Core-shell structure</topic><topic>Doping</topic><topic>Electrochemical impedance spectroscopy</topic><topic>Electromagnetic absorption</topic><topic>Electron paramagnetic resonance</topic><topic>Electron transfer</topic><topic>Energy conversion</topic><topic>Heterojunctions</topic><topic>Hydrogen peroxide</topic><topic>Hydrogen production</topic><topic>Light irradiation</topic><topic>Materials Science</topic><topic>Nanospheres</topic><topic>Photocatalysis</topic><topic>Photocatalysts</topic><topic>Photoelectrons</topic><topic>Photoluminescence</topic><topic>Single electrons</topic><topic>Solar energy</topic><topic>Spectrum analysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Xu, Yandong</creatorcontrib><creatorcontrib>Tai, Wanyu</creatorcontrib><creatorcontrib>Wang, Zhirui</creatorcontrib><creatorcontrib>Zhang, Linlin</creatorcontrib><creatorcontrib>Wang, Dexin</creatorcontrib><creatorcontrib>Liao, Jianjun</creatorcontrib><collection>CrossRef</collection><jtitle>Science China materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Xu, Yandong</au><au>Tai, Wanyu</au><au>Wang, Zhirui</au><au>Zhang, Linlin</au><au>Wang, Dexin</au><au>Liao, Jianjun</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production</atitle><jtitle>Science China materials</jtitle><stitle>Sci. China Mater</stitle><date>2024</date><risdate>2024</risdate><volume>67</volume><issue>1</issue><spage>153</spage><epage>161</epage><pages>153-161</pages><issn>2095-8226</issn><eissn>2199-4501</eissn><abstract>The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solution to the energy crisis, but its low efficiency hinders its scale-up feasibility. In this work, a hollow core-shell structure OCN@In
2
S
3
composite photocatalyst was constructed by growing In
2
S
3
ultrathin nanosheets on the surface of O-doped hollow g-C
3
N
4
nanospheres using a two-step hydrothermal method. The hollow structure provided a high specific surface area and enhanced light absorption. O doping increased the number of active sites, and the heterojunction promoted the rapid separation and transfer of photogenerated carriers. Under visible light irradiation, the H
2
O
2
yield of OCN@In
2
S
3
reached 632.5 µmol h
−1
g
−1
, which was 5.7 times higher than that of g-C
3
N
4
and 12.3 times that of In
2
S
3
, as well as higher than most g-C
3
N
4
-based photocatalysts. Quenching experiments and electron paramagnetic resonance spectroscopy showed that ·O
2
−
was an intermediate product formed during photocatalytic H
2
O
2
generation. The reaction primarily followed a two-step single-electron pathway. The Koutecky-Levich diagram confirmed that the synthesized OCN@In
2
S
3
maintained a high two-electron ORR selectivity during the catalytic reaction (
n
= 1.67). The photocatalytic mechanism was elucidated by photoluminescence, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectro-scopy, which confirmed that OCN@In
2
S
3
inhibited the recombination of photogenerated carriers. This work provides a simple and attractive strategy for developing highly active energy-conversion photocatalysts.</abstract><cop>Beijing</cop><pub>Science China Press</pub><doi>10.1007/s40843-023-2659-9</doi><tpages>9</tpages><oa>free_for_read</oa></addata></record> |
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subjects | Carbon nitride Chemistry and Materials Science Chemistry/Food Science Core-shell structure Doping Electrochemical impedance spectroscopy Electromagnetic absorption Electron paramagnetic resonance Electron transfer Energy conversion Heterojunctions Hydrogen peroxide Hydrogen production Light irradiation Materials Science Nanospheres Photocatalysis Photocatalysts Photoelectrons Photoluminescence Single electrons Solar energy Spectrum analysis |
title | Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production |
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