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Title: Synergies between Unsaturated Zn/Cu Doping Sites in Carbon Dots Provide New Pathways for Photocatalytic Oxidation

Unsaturated metal species (UMS) confined in nanomaterials play important roles for electron transfer in a wide range of catalytic reactions. However, the limited fabrication methods of UMS restrict their wider catalytic applications. Here in this paper, we report on the synergy of unsaturated Zn and Cu dopants confined in carbon dots (ZnCu-CDs) to produce enhanced electron transfer and photooxidation processes in the doped CDs. The Zn/Cu species chelate with the carbon matrix mainly through Cu-O(N)-Zn-O(N)-Cu complexes. Within this structure, Cu 2+ acts as a mild oxidizer that facilely increases the unsaturated Zn content and also precisely tunes the unsaturated Zn valence state to Zn d+, where d is between 1 and 2, instead of Zn. With the help of UMS, electron-transfer pathways are produced, enhancing both the electron donating (7.0 times) and-accepting (5.3 times) abilities relative to conventional CDs. Because of these synergistic effects, the photocatalytic efficiency of CDs in photooxidation reactions is shown to improve more than 5-fold.
Authors:
ORCiD logo [1] ;  [2] ;  [2] ;  [3] ;  [2] ;  [2] ;  [2] ;  [4] ; ORCiD logo [5] ; ORCiD logo [2]
  1. China Univ. of Petroleum, Qingdao (China). State Key Lab. of Heavy Oil Processing, College of Chemical Engineering; Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  2. China Univ. of Petroleum, Qingdao (China). State Key Lab. of Heavy Oil Processing, College of Chemical Engineering
  3. Chinese Academy of Sciences, Beijing (China). Key Lab. of Photochemical Conversion and Optoelectronic Materials, Technical Inst. of Physics and Chemistry
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  5. Dalian Univ. of Technology, Dalian (China). State Key Lab. of Fine Chemicals, School of Chemical Engineering
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal Issue: 2; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC); China Scholarship Council; China Postdoctoral Science Foundation; Shandong Provincial Natural Science Foundation
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; carbon dots; electron transfer; photooxidation; superoxide radical anion; unsaturated Zn/Cu species
OSTI Identifier:
1426233

Wu, Wenting, Zhang, Qinggang, Wang, Ruiqin, Zhao, Yufei, Li, Zhongtao, Ning, Hui, Zhao, Qingshan, Wiederrecht, Gary P., Qiu, Jieshan, and Wu, Mingbo. Synergies between Unsaturated Zn/Cu Doping Sites in Carbon Dots Provide New Pathways for Photocatalytic Oxidation. United States: N. p., Web. doi:10.1021/acscatal.7b03423.
Wu, Wenting, Zhang, Qinggang, Wang, Ruiqin, Zhao, Yufei, Li, Zhongtao, Ning, Hui, Zhao, Qingshan, Wiederrecht, Gary P., Qiu, Jieshan, & Wu, Mingbo. Synergies between Unsaturated Zn/Cu Doping Sites in Carbon Dots Provide New Pathways for Photocatalytic Oxidation. United States. doi:10.1021/acscatal.7b03423.
Wu, Wenting, Zhang, Qinggang, Wang, Ruiqin, Zhao, Yufei, Li, Zhongtao, Ning, Hui, Zhao, Qingshan, Wiederrecht, Gary P., Qiu, Jieshan, and Wu, Mingbo. 2017. "Synergies between Unsaturated Zn/Cu Doping Sites in Carbon Dots Provide New Pathways for Photocatalytic Oxidation". United States. doi:10.1021/acscatal.7b03423. https://www.osti.gov/servlets/purl/1426233.
@article{osti_1426233,
title = {Synergies between Unsaturated Zn/Cu Doping Sites in Carbon Dots Provide New Pathways for Photocatalytic Oxidation},
author = {Wu, Wenting and Zhang, Qinggang and Wang, Ruiqin and Zhao, Yufei and Li, Zhongtao and Ning, Hui and Zhao, Qingshan and Wiederrecht, Gary P. and Qiu, Jieshan and Wu, Mingbo},
abstractNote = {Unsaturated metal species (UMS) confined in nanomaterials play important roles for electron transfer in a wide range of catalytic reactions. However, the limited fabrication methods of UMS restrict their wider catalytic applications. Here in this paper, we report on the synergy of unsaturated Zn and Cu dopants confined in carbon dots (ZnCu-CDs) to produce enhanced electron transfer and photooxidation processes in the doped CDs. The Zn/Cu species chelate with the carbon matrix mainly through Cu-O(N)-Zn-O(N)-Cu complexes. Within this structure, Cu2+ acts as a mild oxidizer that facilely increases the unsaturated Zn content and also precisely tunes the unsaturated Zn valence state to Znd+, where d is between 1 and 2, instead of Zn. With the help of UMS, electron-transfer pathways are produced, enhancing both the electron donating (7.0 times) and-accepting (5.3 times) abilities relative to conventional CDs. Because of these synergistic effects, the photocatalytic efficiency of CDs in photooxidation reactions is shown to improve more than 5-fold.},
doi = {10.1021/acscatal.7b03423},
journal = {ACS Catalysis},
number = 2,
volume = 8,
place = {United States},
year = {2017},
month = {12}
}