CoCrFeNi High-Entropy Alloy as an Enhanced Hydrogen Evolution Catalyst in an Acidic Solution

被引:44
作者
McKay, Frank [1 ]
Fang, Yuxin [2 ]
Kizilkaya, Orhan [3 ]
Singh, Prashant [4 ]
Johnson, Duane D. [4 ,5 ]
Roy, Amitava [3 ]
Young, David P. [1 ]
Sprunger, Phillip T. [1 ]
Flake, John C. [2 ]
Shelton, William A. [2 ]
Xu, Ye [2 ]
机构
[1] Louisiana State Univ, Dept Phys & Astron, Baton Rouge, LA 70803 USA
[2] Louisiana State Univ, Cain Dept Chem Engn, Baton Rouge, LA 70803 USA
[3] Louisiana State Univ, Ctr Adv Microstruct & Devices, Baton Rouge, LA 70803 USA
[4] US DOE, Ames Lab, Ames, IA 50011 USA
[5] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA
基金
美国国家科学基金会;
关键词
OXYGEN REDUCTION; STABLE ELECTROCATALYST; ELECTROLYTIC HYDROGEN; MOLECULAR ADSORPTION; H-2; EVOLUTION; TOTAL-ENERGY; EFFICIENT; NICKEL; CO; NANOPARTICLES;
D O I
10.1021/acs.jpcc.1c03646
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
High-entropy alloys (HEAs) have intriguing material properties, but their potential as catalysts has not been widely explored. Based on a concise theoretical model, we predict that the surface of a quaternary HEA of base metals, CoCrFeNi, should go from being nearly fully oxidized except for pure Ni sites when exposed to O-2 to being partially oxidized in an acidic solution under cathodic bias, and that such a partially oxidized surface should be more active for the electrochemical hydrogen evolution reaction (HER) in acidic solutions than all the component metals. These predictions are confirmed by electrochemical and surface science experiments: the Ni in the HEA is found to be most resistant to oxidation, and when deployed in 0.5 M H2SO4, the HEA exhibits an overpotential of only 60 mV relative to Pt for the HER at a current density of 1 mA/cm(2).
引用
收藏
页码:17008 / 17018
页数:11
相关论文
共 78 条
[1]   Optimal site-centered electronic structure basis set from a displaced-center expansion: Improved results via a priori estimates of saddle points in the density [J].
Alam, Aftab ;
Johnson, D. D. .
PHYSICAL REVIEW B, 2009, 80 (12)
[2]   LINEAR METHODS IN BAND THEORY [J].
ANDERSEN, OK .
PHYSICAL REVIEW B, 1975, 12 (08) :3060-3083
[3]  
[Anonymous], 2020, ANN ONCOL, DOI DOI 10.1093/annonc/mdy517
[4]   Cathodic hydrogen evolution in acidic solutions using electrodeposited nano-crystalline Ni-Co cathodes [J].
Badawy, W. A. ;
Nady, H. ;
Negem, M. .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2014, 39 (21) :10824-10832
[5]   Efficient and stable electrocatalyst for hydrogen evolution reaction prepared by hybrid technique in surface engineering: Electrochemical and magnetron sputtering methods [J].
Bagheri, Robabeh ;
Wattoo, Abdul Ghafar ;
Yao, Yan ;
Liu, Jikang ;
Xu, Cheng ;
Moradi-Haghighi, Masoumeh ;
Song, Zhenlun .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2018, 43 (02) :757-771
[6]   Atomic and molecular adsorption on Ni(111) [J].
Bai, Yunhai ;
Kirvassilis, Demetrios ;
Xu, Lang ;
Mavrikakis, Manos .
SURFACE SCIENCE, 2019, 679 :240-253
[7]   Complex-Solid-Solution Electrocatalyst Discovery by Computational Prediction and High-Throughput Experimentation** [J].
Batchelor, Thomas A. A. ;
Loeffler, Tobias ;
Xiao, Bin ;
Krysiak, Olga A. ;
Strotkoetter, Valerie ;
Pedersen, Jack K. ;
Clausen, Christian M. ;
Savan, Alan ;
Li, Yujiao ;
Schuhmann, Wolfgang ;
Rossmeisl, Jan ;
Ludwig, Alfred .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2021, 60 (13) :6932-6937
[8]   High-Entropy Alloys as a Discovery Platform for Electrocatalysis [J].
Batchelor, Thomas A. A. ;
Pedersen, Jack K. ;
Winther, Simon H. ;
Castelli, Ivano E. ;
Jacobsen, Karsten W. ;
Rossmeisl, Jan .
JOULE, 2019, 3 (03) :834-845
[9]   Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Cr, Mn, Fe, Co and Ni [J].
Biesinger, Mark C. ;
Payne, Brad P. ;
Grosvenor, Andrew P. ;
Lau, Leo W. M. ;
Gerson, Andrea R. ;
Smart, Roger St. C. .
APPLIED SURFACE SCIENCE, 2011, 257 (07) :2717-2730
[10]   Dissociative adsorption of O2 molecules on o-precovered fe(110) and fe(100):: Density-functional calculations [J].
Blonski, Piotr ;
Kiejna, Adam ;
Hafner, Juergen .
PHYSICAL REVIEW B, 2008, 77 (15)