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Inorganic ligands-mediated hole attraction and surface structuralreorganization in InP/ZnS QD photocatalysts studied via ultrafast visibleand midinfrared spectroscopies
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- Liu, Yang (författare)
- Lund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Chengdu University of Technology,Southwest Petroleum University,Southwest Petr Univ, State Key Lab Oil & Gas Reservoir Geol & Exploita, Chengdu 610500, Peoples R China.;Chengdu Univ Informat Technol, Coll Optoelect Technol, Chengdu 610225, Peoples R China.;Southwest Petr Univ, Sch New Energy & Mat, Chengdu 610500, Peoples R China.;Lund Univ, Div Chem Phys & Nanolund, S-22100 Lund, Sweden.
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- Zhou, Ying (författare)
- Southwest Petroleum University,Southwest Petr Univ, State Key Lab Oil & Gas Reservoir Geol & Exploita, Chengdu 610500, Peoples R China.;Southwest Petr Univ, Sch New Energy & Mat, Chengdu 610500, Peoples R China.
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- Abdellah, Mohamed (författare)
- Uppsala universitet,Uppsala University,Institutionen för kemi - Ångström
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- 2022-03-30
- 2022
- Engelska.
- Ingår i: SCIENCE CHINA Materials. - : Springer Science and Business Media LLC. - 2095-8226 .- 2199-4501. ; 65:9, s. 2529-2539
- Tidskriftsartikel (refereegranskat)
Abstract
Ämnesord
Stäng
- Photoinduced carrier dynamical processes dominate the optical excitation properties of photocatalysts and further determine the photocatalytic performance. In addition, as the electrons generally possess a faster transfer rate than holes, hole transfer and accumulation are critical, and they play the key efficiency-limiting step during the photocatalytic process. Therefore, a comprehensive understanding of the dynamics of photogenerated holes and their determining factors in the photocatalytic system is highly essential to rationalize the full catalytic mechanism and develop highly efficient photocatalysts, which have not yet been revealed. In this work, the photoinduced charge carrier dynamics in InP/ZnS quantum dots (QDs) capped with long-chain L-typed ligands (oleylamine) and inorganic ligands (sulfide ion (S2−)) were explored. Time-resolved photoluminescence and femtosecond transient-absorption spectroscopy unambiguously confirmed the ultrafast hole transfer from the InP core to S2− ligands. Moreover, by probing the bleach of vibrational stretching of the ligands with transient midinfrared absorption spectroscopy, the hole transfer time was determined to be 4.2 ps. The injected holes are long-lived at the S2− ligands (>4.5 ns), and they can remove electrostatically attached surfactants to compensate for the spatial charge redistribution. Finally, compared with other inorganic ligands such as Cl− and PO43−, S2− balances the ionic radii and net charge to ensure the optimal condition for charge transfer. Such observation rationalizes the excellent photocatalytic H2 evolution (213.6 µmol mg−1 within 10 h) in InP/ZnS QDs capped with S2− compared with those capped with other ligands and elucidates the role of surface ligands in the photocatalytic activity of colloidal QDs.
Ämnesord
- NATURVETENSKAP -- Fysik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences (hsv//eng)
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Nyckelord
- hole transfer
- InP/ZnS QD photocatalysts
- midinfrared spectroscopies
- surface ligands
- ultrafast visible spectroscopies
- InP/ZnS QD photocatalysts
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- Lin, Weihua
- Meng, Jie
- Zhao, Qian
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- Yu, Shan
- Xie, Zhanghui
- Pan, Qinying
- Zhang, Fengying
- Pullerits, Tonu
- Zheng, Kaibo
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