Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction

Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mecha...
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Autor*in:	Yimin Zhang [verfasserIn] Lei Yan [verfasserIn] Mengxue Guan [verfasserIn] Daqiang Chen [verfasserIn] Zhe Xu [verfasserIn] Haizhong Guo [verfasserIn] Shiqi Hu [verfasserIn] Shengjie Zhang [verfasserIn] Xinbao Liu [verfasserIn] Zhengxiao Guo [verfasserIn] Shunfang Li [verfasserIn] Sheng Meng [verfasserIn]

Format:	E-Artikel
Sprache:	Englisch

Erschienen:	2022

Schlagwörter:	CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory

Übergeordnetes Werk:	In: Advanced Science - Wiley, 2015, 9(2022), 2, Seite n/a-n/a
Übergeordnetes Werk:	volume:9 ; year:2022 ; number:2 ; pages:n/a-n/a

Links:	Link aufrufen Link aufrufen Link aufrufen Journal toc

DOI / URN:	10.1002/advs.202102978

Katalog-ID:	DOAJ063286343

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245	1	0	\|a Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction
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520			\|a Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis.
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allfields	10.1002/advs.202102978 doi (DE-627)DOAJ063286343 (DE-599)DOAJ676e1ec0632347c59fa6f8be75a178bc DE-627 ger DE-627 rakwb eng Yimin Zhang verfasserin aut Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis. CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory Science Q Lei Yan verfasserin aut Mengxue Guan verfasserin aut Daqiang Chen verfasserin aut Zhe Xu verfasserin aut Haizhong Guo verfasserin aut Shiqi Hu verfasserin aut Shengjie Zhang verfasserin aut Xinbao Liu verfasserin aut Zhengxiao Guo verfasserin aut Shunfang Li verfasserin aut Sheng Meng verfasserin aut In Advanced Science Wiley, 2015 9(2022), 2, Seite n/a-n/a (DE-627)817357777 (DE-600)2808093-2 21983844 nnns volume:9 year:2022 number:2 pages:n/a-n/a https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/article/676e1ec0632347c59fa6f8be75a178bc kostenfrei https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/toc/2198-3844 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2022 2 n/a-n/a
spelling	10.1002/advs.202102978 doi (DE-627)DOAJ063286343 (DE-599)DOAJ676e1ec0632347c59fa6f8be75a178bc DE-627 ger DE-627 rakwb eng Yimin Zhang verfasserin aut Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis. CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory Science Q Lei Yan verfasserin aut Mengxue Guan verfasserin aut Daqiang Chen verfasserin aut Zhe Xu verfasserin aut Haizhong Guo verfasserin aut Shiqi Hu verfasserin aut Shengjie Zhang verfasserin aut Xinbao Liu verfasserin aut Zhengxiao Guo verfasserin aut Shunfang Li verfasserin aut Sheng Meng verfasserin aut In Advanced Science Wiley, 2015 9(2022), 2, Seite n/a-n/a (DE-627)817357777 (DE-600)2808093-2 21983844 nnns volume:9 year:2022 number:2 pages:n/a-n/a https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/article/676e1ec0632347c59fa6f8be75a178bc kostenfrei https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/toc/2198-3844 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2022 2 n/a-n/a
allfields_unstemmed	10.1002/advs.202102978 doi (DE-627)DOAJ063286343 (DE-599)DOAJ676e1ec0632347c59fa6f8be75a178bc DE-627 ger DE-627 rakwb eng Yimin Zhang verfasserin aut Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis. CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory Science Q Lei Yan verfasserin aut Mengxue Guan verfasserin aut Daqiang Chen verfasserin aut Zhe Xu verfasserin aut Haizhong Guo verfasserin aut Shiqi Hu verfasserin aut Shengjie Zhang verfasserin aut Xinbao Liu verfasserin aut Zhengxiao Guo verfasserin aut Shunfang Li verfasserin aut Sheng Meng verfasserin aut In Advanced Science Wiley, 2015 9(2022), 2, Seite n/a-n/a (DE-627)817357777 (DE-600)2808093-2 21983844 nnns volume:9 year:2022 number:2 pages:n/a-n/a https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/article/676e1ec0632347c59fa6f8be75a178bc kostenfrei https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/toc/2198-3844 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2022 2 n/a-n/a
allfieldsGer	10.1002/advs.202102978 doi (DE-627)DOAJ063286343 (DE-599)DOAJ676e1ec0632347c59fa6f8be75a178bc DE-627 ger DE-627 rakwb eng Yimin Zhang verfasserin aut Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis. CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory Science Q Lei Yan verfasserin aut Mengxue Guan verfasserin aut Daqiang Chen verfasserin aut Zhe Xu verfasserin aut Haizhong Guo verfasserin aut Shiqi Hu verfasserin aut Shengjie Zhang verfasserin aut Xinbao Liu verfasserin aut Zhengxiao Guo verfasserin aut Shunfang Li verfasserin aut Sheng Meng verfasserin aut In Advanced Science Wiley, 2015 9(2022), 2, Seite n/a-n/a (DE-627)817357777 (DE-600)2808093-2 21983844 nnns volume:9 year:2022 number:2 pages:n/a-n/a https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/article/676e1ec0632347c59fa6f8be75a178bc kostenfrei https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/toc/2198-3844 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2022 2 n/a-n/a
allfieldsSound	10.1002/advs.202102978 doi (DE-627)DOAJ063286343 (DE-599)DOAJ676e1ec0632347c59fa6f8be75a178bc DE-627 ger DE-627 rakwb eng Yimin Zhang verfasserin aut Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis. CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory Science Q Lei Yan verfasserin aut Mengxue Guan verfasserin aut Daqiang Chen verfasserin aut Zhe Xu verfasserin aut Haizhong Guo verfasserin aut Shiqi Hu verfasserin aut Shengjie Zhang verfasserin aut Xinbao Liu verfasserin aut Zhengxiao Guo verfasserin aut Shunfang Li verfasserin aut Sheng Meng verfasserin aut In Advanced Science Wiley, 2015 9(2022), 2, Seite n/a-n/a (DE-627)817357777 (DE-600)2808093-2 21983844 nnns volume:9 year:2022 number:2 pages:n/a-n/a https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/article/676e1ec0632347c59fa6f8be75a178bc kostenfrei https://doi.org/10.1002/advs.202102978 kostenfrei https://doaj.org/toc/2198-3844 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2022 2 n/a-n/a
language	English
source	In Advanced Science 9(2022), 2, Seite n/a-n/a volume:9 year:2022 number:2 pages:n/a-n/a
sourceStr	In Advanced Science 9(2022), 2, Seite n/a-n/a volume:9 year:2022 number:2 pages:n/a-n/a
format_phy_str_mv	Article
institution	findex.gbv.de
topic_facet	CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory Science Q
isfreeaccess_bool	true
container_title	Advanced Science
authorswithroles_txt_mv	Yimin Zhang @@aut@@ Lei Yan @@aut@@ Mengxue Guan @@aut@@ Daqiang Chen @@aut@@ Zhe Xu @@aut@@ Haizhong Guo @@aut@@ Shiqi Hu @@aut@@ Shengjie Zhang @@aut@@ Xinbao Liu @@aut@@ Zhengxiao Guo @@aut@@ Shunfang Li @@aut@@ Sheng Meng @@aut@@
publishDateDaySort_date	2022-01-01T00:00:00Z
hierarchy_top_id	817357777
id	DOAJ063286343
language_de	englisch
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author	Yimin Zhang
spellingShingle	Yimin Zhang misc CO2 photoreduction misc direct charge transfer misc indirect hot electron transfer misc plasmon‐enabled photocatalysis misc time‐dependent density functional theory misc Science misc Q Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction
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topic_title	Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction CO2 photoreduction direct charge transfer indirect hot electron transfer plasmon‐enabled photocatalysis time‐dependent density functional theory
topic	misc CO2 photoreduction misc direct charge transfer misc indirect hot electron transfer misc plasmon‐enabled photocatalysis misc time‐dependent density functional theory misc Science misc Q
topic_unstemmed	misc CO2 photoreduction misc direct charge transfer misc indirect hot electron transfer misc plasmon‐enabled photocatalysis misc time‐dependent density functional theory misc Science misc Q
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title	Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction
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title_full	Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction
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title_sort	indirect to direct charge transfer transition in plasmon‐enabled co2 photoreduction
title_auth	Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction
abstract	Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis.
abstractGer	Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis.
abstract_unstemmed	Abstract Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon‐enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO2 reduction as an example, the underlying mechanisms of plasmon‐driven catalysis at the single‐molecule level using time‐dependent density functional theory calculations is clearly probed. The CO2 molecule adsorbed on two typical nanoclusters, Ag20 and Ag147, is photoreduced by optically excited plasmon, accompanied by the excitation of asymmetric stretching and bending modes of CO2. A nonlinear relationship has been identified between laser intensity and reaction rate, demonstrating a synergic interplay and transition from indirect hot‐electron transfer to direct charge transfer, enacted by strong localized surface plasmons. These findings offer new insights for CO2 photoreduction and for the design of effective pathways toward highly efficient plasmon‐mediated photocatalysis.
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title_short	Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction
url	https://doi.org/10.1002/advs.202102978 https://doaj.org/article/676e1ec0632347c59fa6f8be75a178bc https://doaj.org/toc/2198-3844
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up_date	2024-07-03T16:51:44.808Z
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Indirect to Direct Charge Transfer Transition in Plasmon‐Enabled CO2 Photoreduction

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