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Title: Tuning the electrocatalytic activity of Pt by structurally ordered PdFe/C for the hydrogen oxidation reaction in alkaline media

Abstract

Tuning the hydrogen adsorption energy (E H) by controlling the surface electronic structure of Pt is essential for enhancing the hydrogen oxidation reaction (HOR) performance in alkaline media. This could be achieved by forming a Pt skin on PdFe/C nanoparticles with structurally ordered intermetallic (O-PdFe@Pt/C) or disordered alloy (D-PdFe@Pt/C). The HOR activity on O-PdFe@Pt/C exhibits an exchange current density of 1.49 A mg Pt -1, which is 3.87 and 7.56 times higher than that on D-PdFe@Pt/C (0.385 A mg Pt -1) and Pt/C (0.197 A mg Pt -1), respectively. The excellent electrocatalytic HOR performance on O-PdFe@Pt/C can be ascribed to the attenuation of E H on the Pt shell induced by the structurally ordered PdFe core, where the E H on O-PdFe@Pt surface is 0.18 eV smaller than that on Pt according to DFT calculations.

Authors:
 [1];  [1];  [2]; ORCiD logo [3];  [1];  [4];  [4];  [1]; ORCiD logo [2];  [5];  [4];  [2]; ORCiD logo [1]
  1. Huazhong Univ. of Science and Technology, Wuhan (China). Key Lab. of Material Chemistry for Energy Conversion and Storage, Hubei Key Lab. of Material Chemistry and Service Failure and School of Chemistry and Chemical Engineering
  2. Hong Kong Polytechnic Univ., Hong Kong (China). Dept. of Applied Physics
  3. Huazhong Univ. of Science and Technology, Wuhan (China). School of Physics
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; National Natural Science Foundation of China (NNSFC); 1000 Talents Program (China)
OSTI Identifier:
1464106
Report Number(s):
BNL-207956-2018-JAAM
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:  
SC0012704; 21573083; 2017KFYXJJ164; 25301617; 1-ZE6G; AC02-98CH10886
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 24; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Xiao, Weiping, Lei, Wen, Wang, Jie, Gao, Guoying, Zhao, Tonghui, Cordeiro, Macro A.  L., Lin, Ruoqian, Gong, Mingxing, Guo, Xuyun, Stavitski, Eli, Xin, Huolin L., Zhu, Ye, and Wang, Deli. Tuning the electrocatalytic activity of Pt by structurally ordered PdFe/C for the hydrogen oxidation reaction in alkaline media. United States: N. p., 2018. Web. doi:10.1039/C8TA03250E.
Xiao, Weiping, Lei, Wen, Wang, Jie, Gao, Guoying, Zhao, Tonghui, Cordeiro, Macro A.  L., Lin, Ruoqian, Gong, Mingxing, Guo, Xuyun, Stavitski, Eli, Xin, Huolin L., Zhu, Ye, & Wang, Deli. Tuning the electrocatalytic activity of Pt by structurally ordered PdFe/C for the hydrogen oxidation reaction in alkaline media. United States. doi:10.1039/C8TA03250E.
Xiao, Weiping, Lei, Wen, Wang, Jie, Gao, Guoying, Zhao, Tonghui, Cordeiro, Macro A.  L., Lin, Ruoqian, Gong, Mingxing, Guo, Xuyun, Stavitski, Eli, Xin, Huolin L., Zhu, Ye, and Wang, Deli. Fri . "Tuning the electrocatalytic activity of Pt by structurally ordered PdFe/C for the hydrogen oxidation reaction in alkaline media". United States. doi:10.1039/C8TA03250E. https://www.osti.gov/servlets/purl/1464106.
@article{osti_1464106,
title = {Tuning the electrocatalytic activity of Pt by structurally ordered PdFe/C for the hydrogen oxidation reaction in alkaline media},
author = {Xiao, Weiping and Lei, Wen and Wang, Jie and Gao, Guoying and Zhao, Tonghui and Cordeiro, Macro A.  L. and Lin, Ruoqian and Gong, Mingxing and Guo, Xuyun and Stavitski, Eli and Xin, Huolin L. and Zhu, Ye and Wang, Deli},
abstractNote = {Tuning the hydrogen adsorption energy (EH) by controlling the surface electronic structure of Pt is essential for enhancing the hydrogen oxidation reaction (HOR) performance in alkaline media. This could be achieved by forming a Pt skin on PdFe/C nanoparticles with structurally ordered intermetallic (O-PdFe@Pt/C) or disordered alloy (D-PdFe@Pt/C). The HOR activity on O-PdFe@Pt/C exhibits an exchange current density of 1.49 A mgPt-1, which is 3.87 and 7.56 times higher than that on D-PdFe@Pt/C (0.385 A mgPt-1) and Pt/C (0.197 A mgPt-1), respectively. The excellent electrocatalytic HOR performance on O-PdFe@Pt/C can be ascribed to the attenuation of EH on the Pt shell induced by the structurally ordered PdFe core, where the EH on O-PdFe@Pt surface is 0.18 eV smaller than that on Pt according to DFT calculations.},
doi = {10.1039/C8TA03250E},
journal = {Journal of Materials Chemistry. A},
number = 24,
volume = 6,
place = {United States},
year = {2018},
month = {5}
}

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Figures / Tables:

Fig. 1 Fig. 1: (a) XRD patterns of D-PdFe/C, O-PdFe/C and O-PdFe@Pt/C nanoparticles. The vertical red and black lines correspond to L10-ordered PdFe (PDF card # 00-002-1440) and fcc-Pd (PDF card # 01- 089-4897), respectively. (b) k2-weighted extended X-ray absorption fine structure (EXAFS) region (green dots) together with the best-fit simulation ofmore » the data (red line) with parameters given in Table S2.† (c) The fine spectra of Pt 4f on Pt/C, D-PdFe@Pt/C and O-PdFe@Pt/C catalysts.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.