Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis

Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skel...
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Autor*in:	Gao, Yang [verfasserIn] Xu, Xiaohui Niu, Yue Hu, Xinran Li, Zeyu Yang, Longkun Zhi, Linjie Wang, Bin

Format:	E-Artikel
Sprache:	Englisch

Erschienen:	2023

Schlagwörter:	viologens electrocatalysis hydrogen peroxide redox mediator oxygen reduction

Anmerkung:	© Tsinghua University Press 2023

Übergeordnetes Werk:	Enthalten in: Nano research - [S.l.] : Tsinghua Press, 2008, 16(2023), 12 vom: 03. Juli, Seite 12936-12941
Übergeordnetes Werk:	volume:16 ; year:2023 ; number:12 ; day:03 ; month:07 ; pages:12936-12941

Links:	Volltext

DOI / URN:	10.1007/s12274-023-5887-4

Katalog-ID:	SPR054227143

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520			\|a Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts.
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650		4	\|a electrocatalysis \|7 (dpeaa)DE-He213
650		4	\|a hydrogen peroxide \|7 (dpeaa)DE-He213
650		4	\|a redox mediator \|7 (dpeaa)DE-He213
650		4	\|a oxygen reduction \|7 (dpeaa)DE-He213
700	1		\|a Xu, Xiaohui \|4 aut
700	1		\|a Niu, Yue \|4 aut
700	1		\|a Hu, Xinran \|4 aut
700	1		\|a Li, Zeyu \|4 aut
700	1		\|a Yang, Longkun \|4 aut
700	1		\|a Zhi, Linjie \|4 aut
700	1		\|a Wang, Bin \|4 aut
773	0	8	\|i Enthalten in \|t Nano research \|d [S.l.] : Tsinghua Press, 2008 \|g 16(2023), 12 vom: 03. Juli, Seite 12936-12941 \|w (DE-627)57375361X \|w (DE-600)2442216-2 \|x 1998-0000 \|7 nnns
773	1	8	\|g volume:16 \|g year:2023 \|g number:12 \|g day:03 \|g month:07 \|g pages:12936-12941
856	4	0	\|u https://dx.doi.org/10.1007/s12274-023-5887-4 \|z lizenzpflichtig \|3 Volltext
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912			\|a GBV_ILN_105
912			\|a GBV_ILN_110
912			\|a GBV_ILN_120
912			\|a GBV_ILN_138
912			\|a GBV_ILN_150
912			\|a GBV_ILN_151
912			\|a GBV_ILN_152
912			\|a GBV_ILN_161
912			\|a GBV_ILN_170
912			\|a GBV_ILN_171
912			\|a GBV_ILN_187
912			\|a GBV_ILN_213
912			\|a GBV_ILN_224
912			\|a GBV_ILN_230
912			\|a GBV_ILN_250
912			\|a GBV_ILN_281
912			\|a GBV_ILN_285
912			\|a GBV_ILN_293
912			\|a GBV_ILN_370
912			\|a GBV_ILN_602
912			\|a GBV_ILN_636
912			\|a GBV_ILN_702
912			\|a GBV_ILN_2001
912			\|a GBV_ILN_2003
912			\|a GBV_ILN_2004
912			\|a GBV_ILN_2005
912			\|a GBV_ILN_2006
912			\|a GBV_ILN_2007
912			\|a GBV_ILN_2008
912			\|a GBV_ILN_2009
912			\|a GBV_ILN_2010
912			\|a GBV_ILN_2011
912			\|a GBV_ILN_2014
912			\|a GBV_ILN_2015
912			\|a GBV_ILN_2020
912			\|a GBV_ILN_2021
912			\|a GBV_ILN_2025
912			\|a GBV_ILN_2026
912			\|a GBV_ILN_2027
912			\|a GBV_ILN_2031
912			\|a GBV_ILN_2034
912			\|a GBV_ILN_2037
912			\|a GBV_ILN_2038
912			\|a GBV_ILN_2039
912			\|a GBV_ILN_2044
912			\|a GBV_ILN_2048
912			\|a GBV_ILN_2049
912			\|a GBV_ILN_2050
912			\|a GBV_ILN_2055
912			\|a GBV_ILN_2056
912			\|a GBV_ILN_2057
912			\|a GBV_ILN_2059
912			\|a GBV_ILN_2061
912			\|a GBV_ILN_2064
912			\|a GBV_ILN_2065
912			\|a GBV_ILN_2068
912			\|a GBV_ILN_2088
912			\|a GBV_ILN_2093
912			\|a GBV_ILN_2106
912			\|a GBV_ILN_2107
912			\|a GBV_ILN_2108
912			\|a GBV_ILN_2110
912			\|a GBV_ILN_2111
912			\|a GBV_ILN_2112
912			\|a GBV_ILN_2113
912			\|a GBV_ILN_2118
912			\|a GBV_ILN_2122
912			\|a GBV_ILN_2129
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912			\|a GBV_ILN_2548
912			\|a GBV_ILN_4035
912			\|a GBV_ILN_4037
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912			\|a GBV_ILN_4249
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912			\|a GBV_ILN_4307
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912			\|a GBV_ILN_4323
912			\|a GBV_ILN_4324
912			\|a GBV_ILN_4325
912			\|a GBV_ILN_4326
912			\|a GBV_ILN_4328
912			\|a GBV_ILN_4333
912			\|a GBV_ILN_4334
912			\|a GBV_ILN_4335
912			\|a GBV_ILN_4336
912			\|a GBV_ILN_4338
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Indexfelder

author_variant	y g yg x x xx y n yn x h xh z l zl l y ly l z lz b w bw
matchkey_str	article:19980000:2023----::ilgnbsdeomdaosihualhmlmeeggpohglefcieyr
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allfields	10.1007/s12274-023-5887-4 doi (DE-627)SPR054227143 (SPR)s12274-023-5887-4-e DE-627 ger DE-627 rakwb eng Gao, Yang verfasserin aut Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis 2023 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press 2023 Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. viologens (dpeaa)DE-He213 electrocatalysis (dpeaa)DE-He213 hydrogen peroxide (dpeaa)DE-He213 redox mediator (dpeaa)DE-He213 oxygen reduction (dpeaa)DE-He213 Xu, Xiaohui aut Niu, Yue aut Hu, Xinran aut Li, Zeyu aut Yang, Longkun aut Zhi, Linjie aut Wang, Bin aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 16(2023), 12 vom: 03. Juli, Seite 12936-12941 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:16 year:2023 number:12 day:03 month:07 pages:12936-12941 https://dx.doi.org/10.1007/s12274-023-5887-4 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 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_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 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_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 16 2023 12 03 07 12936-12941
spelling	10.1007/s12274-023-5887-4 doi (DE-627)SPR054227143 (SPR)s12274-023-5887-4-e DE-627 ger DE-627 rakwb eng Gao, Yang verfasserin aut Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis 2023 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press 2023 Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. viologens (dpeaa)DE-He213 electrocatalysis (dpeaa)DE-He213 hydrogen peroxide (dpeaa)DE-He213 redox mediator (dpeaa)DE-He213 oxygen reduction (dpeaa)DE-He213 Xu, Xiaohui aut Niu, Yue aut Hu, Xinran aut Li, Zeyu aut Yang, Longkun aut Zhi, Linjie aut Wang, Bin aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 16(2023), 12 vom: 03. Juli, Seite 12936-12941 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:16 year:2023 number:12 day:03 month:07 pages:12936-12941 https://dx.doi.org/10.1007/s12274-023-5887-4 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 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_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 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_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 16 2023 12 03 07 12936-12941
allfields_unstemmed	10.1007/s12274-023-5887-4 doi (DE-627)SPR054227143 (SPR)s12274-023-5887-4-e DE-627 ger DE-627 rakwb eng Gao, Yang verfasserin aut Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis 2023 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press 2023 Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. viologens (dpeaa)DE-He213 electrocatalysis (dpeaa)DE-He213 hydrogen peroxide (dpeaa)DE-He213 redox mediator (dpeaa)DE-He213 oxygen reduction (dpeaa)DE-He213 Xu, Xiaohui aut Niu, Yue aut Hu, Xinran aut Li, Zeyu aut Yang, Longkun aut Zhi, Linjie aut Wang, Bin aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 16(2023), 12 vom: 03. Juli, Seite 12936-12941 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:16 year:2023 number:12 day:03 month:07 pages:12936-12941 https://dx.doi.org/10.1007/s12274-023-5887-4 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 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_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 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_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 16 2023 12 03 07 12936-12941
allfieldsGer	10.1007/s12274-023-5887-4 doi (DE-627)SPR054227143 (SPR)s12274-023-5887-4-e DE-627 ger DE-627 rakwb eng Gao, Yang verfasserin aut Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis 2023 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press 2023 Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. viologens (dpeaa)DE-He213 electrocatalysis (dpeaa)DE-He213 hydrogen peroxide (dpeaa)DE-He213 redox mediator (dpeaa)DE-He213 oxygen reduction (dpeaa)DE-He213 Xu, Xiaohui aut Niu, Yue aut Hu, Xinran aut Li, Zeyu aut Yang, Longkun aut Zhi, Linjie aut Wang, Bin aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 16(2023), 12 vom: 03. Juli, Seite 12936-12941 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:16 year:2023 number:12 day:03 month:07 pages:12936-12941 https://dx.doi.org/10.1007/s12274-023-5887-4 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 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_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 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_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 16 2023 12 03 07 12936-12941
allfieldsSound	10.1007/s12274-023-5887-4 doi (DE-627)SPR054227143 (SPR)s12274-023-5887-4-e DE-627 ger DE-627 rakwb eng Gao, Yang verfasserin aut Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis 2023 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press 2023 Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. viologens (dpeaa)DE-He213 electrocatalysis (dpeaa)DE-He213 hydrogen peroxide (dpeaa)DE-He213 redox mediator (dpeaa)DE-He213 oxygen reduction (dpeaa)DE-He213 Xu, Xiaohui aut Niu, Yue aut Hu, Xinran aut Li, Zeyu aut Yang, Longkun aut Zhi, Linjie aut Wang, Bin aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 16(2023), 12 vom: 03. Juli, Seite 12936-12941 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:16 year:2023 number:12 day:03 month:07 pages:12936-12941 https://dx.doi.org/10.1007/s12274-023-5887-4 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 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_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 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_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 16 2023 12 03 07 12936-12941
language	English
source	Enthalten in Nano research 16(2023), 12 vom: 03. Juli, Seite 12936-12941 volume:16 year:2023 number:12 day:03 month:07 pages:12936-12941
sourceStr	Enthalten in Nano research 16(2023), 12 vom: 03. Juli, Seite 12936-12941 volume:16 year:2023 number:12 day:03 month:07 pages:12936-12941
format_phy_str_mv	Article
institution	findex.gbv.de
topic_facet	viologens electrocatalysis hydrogen peroxide redox mediator oxygen reduction
isfreeaccess_bool	false
container_title	Nano research
authorswithroles_txt_mv	Gao, Yang @@aut@@ Xu, Xiaohui @@aut@@ Niu, Yue @@aut@@ Hu, Xinran @@aut@@ Li, Zeyu @@aut@@ Yang, Longkun @@aut@@ Zhi, Linjie @@aut@@ Wang, Bin @@aut@@
publishDateDaySort_date	2023-07-03T00:00:00Z
hierarchy_top_id	57375361X
id	SPR054227143
language_de	englisch
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Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. 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author	Gao, Yang
spellingShingle	Gao, Yang misc viologens misc electrocatalysis misc hydrogen peroxide misc redox mediator misc oxygen reduction Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis
authorStr	Gao, Yang
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topic_title	Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis viologens (dpeaa)DE-He213 electrocatalysis (dpeaa)DE-He213 hydrogen peroxide (dpeaa)DE-He213 redox mediator (dpeaa)DE-He213 oxygen reduction (dpeaa)DE-He213
topic	misc viologens misc electrocatalysis misc hydrogen peroxide misc redox mediator misc oxygen reduction
topic_unstemmed	misc viologens misc electrocatalysis misc hydrogen peroxide misc redox mediator misc oxygen reduction
topic_browse	misc viologens misc electrocatalysis misc hydrogen peroxide misc redox mediator misc oxygen reduction
format_facet	Elektronische Aufsätze Aufsätze Elektronische Ressource
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title	Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis
ctrlnum	(DE-627)SPR054227143 (SPR)s12274-023-5887-4-e
title_full	Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis
author_sort	Gao, Yang
journal	Nano research
journalStr	Nano research
lang_code	eng
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container_start_page	12936
author_browse	Gao, Yang Xu, Xiaohui Niu, Yue Hu, Xinran Li, Zeyu Yang, Longkun Zhi, Linjie Wang, Bin
container_volume	16
format_se	Elektronische Aufsätze
author-letter	Gao, Yang
doi_str_mv	10.1007/s12274-023-5887-4
title_sort	viologens-based redox mediators with tunable homo–lumo energy gap for highly effective hydrogen peroxide electrosynthesis
title_auth	Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis
abstract	Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. © Tsinghua University Press 2023
abstractGer	Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. © Tsinghua University Press 2023
abstract_unstemmed	Abstract In comparison with the developing nano-carbon catalysts, some small organic molecules are also emerging as catalysts with typical features, however, their working mechanism is still unclear. Here, we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering. These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based $ H_{2} %$ O_{2} $ electrosynthesis. Differing from the commonly reported carbon-based electrocatalysts, viologens can produce $ H_{2} %$ O_{2} $ in a synergistic manner, which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator. We found that the ring current and $ H_{2} %$ O_{2} $ selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group. As a result, a benzyl-substituted viologen (BV) delivers the best electrocatalytic performance among the samples, including the highest $ H_{2} %$ O_{2} $ selectivity of 96.9% at 0.6 V and the largest ring current density of about 13.6 mA·$ mmol^{−1} $. Furthermore, density functional theory (DFT) calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gap of BV is beneficial to the synergistic mechanism for $ H_{2} %$ O_{2} $ production. This work sheds new insight into the efficient $ H_{2} %$ O_{2} $ production in a synergistic manner for small molecules-based electrocatalysts. © Tsinghua University Press 2023
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container_issue	12
title_short	Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis
url	https://dx.doi.org/10.1007/s12274-023-5887-4
remote_bool	true
author2	Xu, Xiaohui Niu, Yue Hu, Xinran Li, Zeyu Yang, Longkun Zhi, Linjie Wang, Bin
author2Str	Xu, Xiaohui Niu, Yue Hu, Xinran Li, Zeyu Yang, Longkun Zhi, Linjie Wang, Bin
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hochschulschrift_bool	false
doi_str	10.1007/s12274-023-5887-4
up_date	2024-07-04T00:34:25.666Z
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Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis

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