TY - JOUR
T1 - A General Synthetic Method for High-Entropy Alloy Subnanometer Ribbons
AU - Tao, Lu
AU - Sun, Mingzi
AU - Zhou, Yin
AU - Luo, Mingchuan
AU - Lv, Fan
AU - Li, Menggang
AU - Zhang, Qinghua
AU - Gu, Lin
AU - Huang, Bolong
AU - Guo, Shaojun
N1 - Funding Information:
This work was financially supported by National Key R&D Program of China (2021YFA1501000), the National Science Fund for Distinguished Young Scholars (52025133), the Tencent Foundation through the XPLORER PRIZE, National Natural Science Foundation of China (NSFC) (21771156 and 51671003), the China Postdoctoral Science Foundation (No. 2019M660290), the Natural Science Foundation of China/RGC Joint Research Scheme (N_PolyU502/21), and the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University (Project Code: 1-ZE2 V).
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/6/15
Y1 - 2022/6/15
N2 - High-entropy alloys (HEAs) are attracting intensive attention due to their broad compositional tunability and interesting catalytic properties. However, precisely shaping the HEAs into suprathin low-dimensional nanostructures for achieving diverse applications remains an enormous challenge owing to their intrinsic thermodynamic instability. Herein we propose a new and general low-temperature method for incorporating up to eight metallic elements into one single-phase subnanometer ribbon to achieve the thinnest HEA metal materials in the world. We experimentally demonstrate that synthetic processes for suprathin HEA subnanometer ribbons (SNRs) include (1) different metal atom nucleation via galvanic exchange reaction between different metal precursors and Ag nanowire template, (2) co-reduction of different metal precursors on nanowire template, and (3) the removal of the inner Ag core. Density functional theory (DFT) calculations reveal that the crystallization and stabilization of HEA SNRs strongly depend on the "highly dynamic"Ag from the template, and the crystallization levels of HEA subnanometer ribbons are closely correlated with the concentration of Pt and Pd. We demonstrate that the present synthetic method enables the flexible control of components and concentrations in HEAs SNRs for achieving a library of HEA SNRs and also superior electrocatalytic properties. The well-designed HEA SNRs show great improvement in catalyzing the oxygen reduction reaction of fuel cells and also high discharge capacity, low charge overpotential, and excellent durability for Li-O2 batteries. DFT calculations reveal the superior electrochemical performances are attributed to the strong reduction capability from high-concentration reductive elements in HEAs, while the other elements guarantee the site-to-site efficient electron transfer.
AB - High-entropy alloys (HEAs) are attracting intensive attention due to their broad compositional tunability and interesting catalytic properties. However, precisely shaping the HEAs into suprathin low-dimensional nanostructures for achieving diverse applications remains an enormous challenge owing to their intrinsic thermodynamic instability. Herein we propose a new and general low-temperature method for incorporating up to eight metallic elements into one single-phase subnanometer ribbon to achieve the thinnest HEA metal materials in the world. We experimentally demonstrate that synthetic processes for suprathin HEA subnanometer ribbons (SNRs) include (1) different metal atom nucleation via galvanic exchange reaction between different metal precursors and Ag nanowire template, (2) co-reduction of different metal precursors on nanowire template, and (3) the removal of the inner Ag core. Density functional theory (DFT) calculations reveal that the crystallization and stabilization of HEA SNRs strongly depend on the "highly dynamic"Ag from the template, and the crystallization levels of HEA subnanometer ribbons are closely correlated with the concentration of Pt and Pd. We demonstrate that the present synthetic method enables the flexible control of components and concentrations in HEAs SNRs for achieving a library of HEA SNRs and also superior electrocatalytic properties. The well-designed HEA SNRs show great improvement in catalyzing the oxygen reduction reaction of fuel cells and also high discharge capacity, low charge overpotential, and excellent durability for Li-O2 batteries. DFT calculations reveal the superior electrochemical performances are attributed to the strong reduction capability from high-concentration reductive elements in HEAs, while the other elements guarantee the site-to-site efficient electron transfer.
UR - http://www.scopus.com/inward/record.url?scp=85132007900&partnerID=8YFLogxK
U2 - 10.1021/jacs.2c03544
DO - 10.1021/jacs.2c03544
M3 - Journal article
C2 - 35652187
AN - SCOPUS:85132007900
SN - 0002-7863
VL - 144
SP - 10582
EP - 10590
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 23
ER -