Title: Vectorial Electron Transfer for Improved Hydrogen Evolution by Mercaptopropionic‐Acid‐Regulated CdSe Quantum‐Dots–TiO<sub>2</sub>–Ni(OH)<sub>2</sub> Assembly
Abstract: ChemSusChemVolume 8, Issue 4 p. 642-649 Full Paper Vectorial Electron Transfer for Improved Hydrogen Evolution by Mercaptopropionic-Acid-Regulated CdSe Quantum-Dots–TiO2–Ni(OH)2 Assembly Dr. Shan Yu, Dr. Shan Yu These authors contributed equally to this work. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorDr. Zhi-Jun Li, Dr. Zhi-Jun Li These authors contributed equally to this work. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorXiang-Bing Fan, Xiang-Bing Fan Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorJia-Xin Li, Jia-Xin Li Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorFei Zhan, Fei Zhan Beijing Synchrotron Radiation Facility, Institute of High Energy Physics the Chinese Academy of Sciences, Beijing 100049 (P.R. China)Search for more papers by this authorXu-Bing Li, Xu-Bing Li Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorProf. Ye Tao, Prof. Ye Tao Beijing Synchrotron Radiation Facility, Institute of High Energy Physics the Chinese Academy of Sciences, Beijing 100049 (P.R. China)Search for more papers by this authorProf. Chen-Ho Tung, Prof. Chen-Ho Tung Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorProf. Li-Zhu Wu, Corresponding Author Prof. Li-Zhu Wu [email protected] Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this author Dr. Shan Yu, Dr. Shan Yu These authors contributed equally to this work. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorDr. Zhi-Jun Li, Dr. Zhi-Jun Li These authors contributed equally to this work. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorXiang-Bing Fan, Xiang-Bing Fan Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorJia-Xin Li, Jia-Xin Li Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorFei Zhan, Fei Zhan Beijing Synchrotron Radiation Facility, Institute of High Energy Physics the Chinese Academy of Sciences, Beijing 100049 (P.R. China)Search for more papers by this authorXu-Bing Li, Xu-Bing Li Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorProf. Ye Tao, Prof. Ye Tao Beijing Synchrotron Radiation Facility, Institute of High Energy Physics the Chinese Academy of Sciences, Beijing 100049 (P.R. China)Search for more papers by this authorProf. Chen-Ho Tung, Prof. Chen-Ho Tung Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this authorProf. Li-Zhu Wu, Corresponding Author Prof. Li-Zhu Wu [email protected] Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry the Chinese Academy of Sciences, Beijing 100190 (P.R. China), Fax: (+86) 10-8254-3580Search for more papers by this author First published: 03 December 2014 https://doi.org/10.1002/cssc.201402885Citations: 37Read the full textAboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onFacebookTwitterLinkedInRedditWechat Graphical Abstract Dotty about hydrogen: If mercaptopropionic acid is used as the linker, a turnover frequency of 5140 h−1 based on CdSe quantum dots (QDs) for photocatalytic hydrogen evolution is achieved by a CdSe QDs–TiO2–Ni(OH)2 ternary assembly at pH 11. Vectorial electron transfer from CdSe QDs to TiO2 and then to Ni(OH)2 is crucial for this high efficiency. Abstract A visible-light-induced hydrogen evolution system based on a CdSe quantum dots (QDs)–TiO2–Ni(OH)2 ternary assembly has been constructed under an ambient environment, and a bifunctional molecular linker, mercaptopropionic acid, is used to facilitate the interaction between CdSe QDs and TiO2. This hydrogen evolution system works effectively in a basic aqueous solution (pH 11.0) to achieve a hydrogen evolution rate of 10.1 mmol g−1 h−1 for the assembly and a turnover frequency of 5140 h−1 with respect to CdSe QDs (10 h); the latter is comparable with the highest value reported for QD systems in an acidic environment. X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and control experiments demonstrate that Ni(OH)2 is an efficient hydrogen evolution catalyst. In addition, inductively coupled plasma optical emission spectroscopy and the emission decay of the assembly combined with the hydrogen evolution experiments show that TiO2 functions mainly as the electron mediator; the vectorial electron transfer from CdSe QDs to TiO2 and then from TiO2 to Ni(OH)2 enhances the efficiency for hydrogen evolution. The assembly comprises light antenna CdSe QDs, electron mediator TiO2, and catalytic Ni(OH)2, which mimics the strategy of photosynthesis exploited in nature and takes us a step further towards artificial photosynthesis. Citing Literature Supporting Information As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Filename Description cssc_201402885_sm_miscellaneous_information.pdf511.1 KB miscellaneous_information Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article. Volume8, Issue4February 2015Pages 642-649 RelatedInformation
Publication Year: 2014
Publication Date: 2014-12-03
Language: en
Type: article
Indexed In: ['crossref', 'pubmed']
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Cited By Count: 39
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