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Title: Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption

Abstract

The efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. Here, we took the view that generating transition metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Using density functional theory, we find that the formation energy of desired Ni4+ sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal phosphorus. Here we synthesized NiCoFeP oxyhydroxides and probed their oxidation kinetics by employing in situ soft X-ray absorption (sXAS). In situ sXAS studies of neutral-pH OER catalysts indicate ready promotion of Ni4+ under low overpotential conditions. NiCoFeP catalyst outperforms IrO2 and retains its performance following 100 hours of operation. We showcase NiCoFeP in a membrane-free CO2 electroreduction system that achieves a 1.99 V cell voltage at 10 mA cm-2, reducing CO2 into CO and oxidizing H2O to O2 with a 64% electricity-to-chemical-fuel efficiency.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo;  [3];  [4]; ORCiD logo [4];  [5];  [4];  [4];  [4];  [6];  [6];  [7]; ORCiD logo [8];  [7];  [3];  [9]; ORCiD logo [4]
  1. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; Tianjin Univ. (China). Inst. of New-Energy Materials and School of Materials Science and Engineering
  2. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; Fudan Univ., Shanghai (China). State Key Lab. of Molecular Engineering of Polymers, Dept. of Macromolecular Science and Lab. of Advanced Materials
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
  4. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering
  5. Tianjin Univ. (China). Inst. of New-Energy Materials and School of Materials Science and Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  6. Canadian Light Sources, Inc., Saskatoon, SK (Canada)
  7. Fudan Univ., Shanghai (China). State Key Lab. of Molecular Engineering of Polymers, Dept. of Macromolecular Science and Lab. of Advanced Materials
  8. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  9. Tianjin Univ. (China). Inst. of New-Energy Materials and School of Materials Science and Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Ontario Research Fund; Natural Sciences and Engineering Research Council of Canada (NSERC); Canadian Inst. for Advanced Research (CIFAR); China Scholarship Council (CSC); National Basic Research Program of China; Shanghai Science and Technology Committee (STCSM); National Natural Science Foundation of China (NSFC); Univ. of Toronto (Canada); Canadian Light Sources, Inc., Saskatoon, SK (Canada); Beijing Synchrotron Radiation Facility; Southern Ontario Smart Computing Innovation Platform (SOSCIP)
OSTI Identifier:
1431449
Report Number(s):
BNL-203448-2018-JAAM
Journal ID: ISSN 1755-4330; TRN: US1802778
Grant/Contract Number:  
SC0012704; AC02-05CH11231; 20140625004; 2014CB931703; 16JC1400702; 14ZR14110200; 21503079; 201406745001
Resource Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Volume: 10; Journal Issue: 2; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 30 DIRECT ENERGY CONVERSION; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; in situ soft X-ray absorption; electrocatalysis; energy; fluorescence spectroscopy

Citation Formats

Zheng, Xueli, Zhang, Bo, De Luna, Phil, Liang, Yufeng, Comin, Riccardo, Voznyy, Oleksandr, Han, Lili, Garcia de Arquer, F. Pelayo, Liu, Min, Dinh, Cao Thang, Regier, Tom, Dynes, James J., He, Sisi, Xin, Huolin L., Peng, Huisheng, Prendergast, David, Du, Xiwen, and Sargent, Edward H. Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption. United States: N. p., 2017. Web. https://doi.org/10.1038/nchem.2886.
Zheng, Xueli, Zhang, Bo, De Luna, Phil, Liang, Yufeng, Comin, Riccardo, Voznyy, Oleksandr, Han, Lili, Garcia de Arquer, F. Pelayo, Liu, Min, Dinh, Cao Thang, Regier, Tom, Dynes, James J., He, Sisi, Xin, Huolin L., Peng, Huisheng, Prendergast, David, Du, Xiwen, & Sargent, Edward H. Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption. United States. https://doi.org/10.1038/nchem.2886
Zheng, Xueli, Zhang, Bo, De Luna, Phil, Liang, Yufeng, Comin, Riccardo, Voznyy, Oleksandr, Han, Lili, Garcia de Arquer, F. Pelayo, Liu, Min, Dinh, Cao Thang, Regier, Tom, Dynes, James J., He, Sisi, Xin, Huolin L., Peng, Huisheng, Prendergast, David, Du, Xiwen, and Sargent, Edward H. Mon . "Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption". United States. https://doi.org/10.1038/nchem.2886. https://www.osti.gov/servlets/purl/1431449.
@article{osti_1431449,
title = {Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption},
author = {Zheng, Xueli and Zhang, Bo and De Luna, Phil and Liang, Yufeng and Comin, Riccardo and Voznyy, Oleksandr and Han, Lili and Garcia de Arquer, F. Pelayo and Liu, Min and Dinh, Cao Thang and Regier, Tom and Dynes, James J. and He, Sisi and Xin, Huolin L. and Peng, Huisheng and Prendergast, David and Du, Xiwen and Sargent, Edward H.},
abstractNote = {The efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. Here, we took the view that generating transition metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Using density functional theory, we find that the formation energy of desired Ni4+ sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal phosphorus. Here we synthesized NiCoFeP oxyhydroxides and probed their oxidation kinetics by employing in situ soft X-ray absorption (sXAS). In situ sXAS studies of neutral-pH OER catalysts indicate ready promotion of Ni4+ under low overpotential conditions. NiCoFeP catalyst outperforms IrO2 and retains its performance following 100 hours of operation. We showcase NiCoFeP in a membrane-free CO2 electroreduction system that achieves a 1.99 V cell voltage at 10 mA cm-2, reducing CO2 into CO and oxidizing H2O to O2 with a 64% electricity-to-chemical-fuel efficiency.},
doi = {10.1038/nchem.2886},
journal = {Nature Chemistry},
number = 2,
volume = 10,
place = {United States},
year = {2017},
month = {11}
}

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