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Title: Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C 3N 4 for boosting photocatalytic H 2 production

Abstract

Tuning reactive metal-support interaction (RMSI) is a promising approach to optimizing catalytic active sites via the electronic, geometric and compositional effects. In general, the RMSI is conducted on the reducible oxides via a high-temperature reaction (>550 °C). We report a strong RMSI between Pt single atom (PtSA) and non-oxide-based g-C 3N 4 built by an in-situ photocatalytic reduction method at a sub-zero temperature. The experimental observation confirms that the rich N vacancies in g-C 3N 4 produce an obvious electron-deficient effect, which greatly enhances the RMSI. This strong RMSI contributes to the highest PtSA coverage density of 0.35 mg m -2 reported to date in carbon-based materials and outstanding H 2-evolution activity of 174.5 mmol g -1 h -1per PtSA relative to those on the electron-rich g-C 3N 4. The structure simulation reveals that the RMSI can not only stabilize the PtSA on the electron-deficient g-C 3N 4via the strong chemical bond between PtSA and the two-coordinated C (C 2C) sites caused by the N vacancies, but also promises the PtSA with an optimized electronic and geometric structures for capturing photogenerated electrons and producing H 2. This finding opens a new channel for designing and manipulating single atom-loaded photocatalyst viamore » the RMSI at a sub-zero low temperature.« less

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [3]
  1. Peking Univ., Beijing (China). Dept. of Materials Science and Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  3. Peking Univ., Beijing (China). Dept. of Materials Science and Engineering. The Beijing Innovation Center for Engineering Science and Advanced Technology. Dept. of Energy and Resources Engineering. Key Lab. of Theory and Technology of Advanced Batteries Materials. College of Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Peking Univ., Beijing (China)
Sponsoring Org.:
USDOE; National Natural Science Foundation of China (NNSFC); National Basic Research Program of China
OSTI Identifier:
1498858
Report Number(s):
BNL-211350-2019-JAAM
Journal ID: ISSN 2211-2855
Grant/Contract Number:  
SC0012704; 51671003; 2016YFB0100201
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 56; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; RMSI; PtSA; g-C3N4; N vacancy; H2 production

Citation Formats

Zhou, Peng, Lv, Fan, Li, Na, Zhang, Yelong, Mu, Zijie, Tang, Yonghua, Lai, Jianping, Chao, Yuguang, Luo, Mingchuan, Lin, Fei, Zhou, Jinhui, Su, Dong, and Guo, Shaojun. Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C3N4 for boosting photocatalytic H2 production. United States: N. p., 2018. Web. doi:10.1016/j.nanoen.2018.11.033.
Zhou, Peng, Lv, Fan, Li, Na, Zhang, Yelong, Mu, Zijie, Tang, Yonghua, Lai, Jianping, Chao, Yuguang, Luo, Mingchuan, Lin, Fei, Zhou, Jinhui, Su, Dong, & Guo, Shaojun. Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C3N4 for boosting photocatalytic H2 production. United States. doi:10.1016/j.nanoen.2018.11.033.
Zhou, Peng, Lv, Fan, Li, Na, Zhang, Yelong, Mu, Zijie, Tang, Yonghua, Lai, Jianping, Chao, Yuguang, Luo, Mingchuan, Lin, Fei, Zhou, Jinhui, Su, Dong, and Guo, Shaojun. Thu . "Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C3N4 for boosting photocatalytic H2 production". United States. doi:10.1016/j.nanoen.2018.11.033.
@article{osti_1498858,
title = {Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C3N4 for boosting photocatalytic H2 production},
author = {Zhou, Peng and Lv, Fan and Li, Na and Zhang, Yelong and Mu, Zijie and Tang, Yonghua and Lai, Jianping and Chao, Yuguang and Luo, Mingchuan and Lin, Fei and Zhou, Jinhui and Su, Dong and Guo, Shaojun},
abstractNote = {Tuning reactive metal-support interaction (RMSI) is a promising approach to optimizing catalytic active sites via the electronic, geometric and compositional effects. In general, the RMSI is conducted on the reducible oxides via a high-temperature reaction (>550 °C). We report a strong RMSI between Pt single atom (PtSA) and non-oxide-based g-C3N4 built by an in-situ photocatalytic reduction method at a sub-zero temperature. The experimental observation confirms that the rich N vacancies in g-C3N4 produce an obvious electron-deficient effect, which greatly enhances the RMSI. This strong RMSI contributes to the highest PtSA coverage density of 0.35 mg m-2 reported to date in carbon-based materials and outstanding H2-evolution activity of 174.5 mmol g-1 h-1per PtSA relative to those on the electron-rich g-C3N4. The structure simulation reveals that the RMSI can not only stabilize the PtSA on the electron-deficient g-C3N4via the strong chemical bond between PtSA and the two-coordinated C (C2C) sites caused by the N vacancies, but also promises the PtSA with an optimized electronic and geometric structures for capturing photogenerated electrons and producing H2. This finding opens a new channel for designing and manipulating single atom-loaded photocatalyst via the RMSI at a sub-zero low temperature.},
doi = {10.1016/j.nanoen.2018.11.033},
journal = {Nano Energy},
issn = {2211-2855},
number = ,
volume = 56,
place = {United States},
year = {2018},
month = {11}
}

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