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Title: Ligand-Exchange-Induced Amorphization of Pd Nanomaterials for Highly Efficient Electrocatalytic Hydrogen Evolution Reaction

Abstract

Various kinds of amorphous materials, such as transition metal dichalcogenides, metal oxides, and metal phosphates, have demonstrated superior electrocatalytic performance compared with their crystalline counterparts. Compared to other materials for electrocatalysis, noble metals exhibit intrinsically high activity and excellent durability. However, it is still very challenging to prepare amorphous noble-metal nanomaterials due to the strong interatomic metallic bonding. Herein, the discovery of a unique thiol molecule is reported, namely bismuthiol I, which can induce the transformation of Pd nanomaterials from face-centered-cubic (fcc) phase into amorphous phase without destroying their integrity. This ligand-induced amorphization is realized by post-synthetic ligand exchange under ambient conditions, and is applicable to fcc Pd nanomaterials with different capping ligands. Importantly, the obtained amorphous Pd nanoparticles exhibit remarkably enhanced activity and excellent stability toward electrocatalytic hydrogen evolution in acidic solution. This work provides a facile and effective method for preparing amorphous Pd nanomaterials, and demonstrates their promising electrocatalytic application.

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [4];  [5];  [1];  [1]; ORCiD logo [6]
+ Show Author Affiliations
  1. Nanyang Technological Univ. (Singapore)
  2. Nanyang Technological Univ. (Singapore); Chinese Academy of Sciences (CAS), Beijing (China)
  3. Center for Programmable MaterialsSchool of Materials Science and EngineeringNanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore
  4. Inst. of Chemical and Engineering Sciences (Singapore). A*STAR (Agency for Science, Technology and Research); Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  5. Advanced Photon SourceArgonne National Laboratory 9700 South Cass Avenue Argonne IL 60439 USA
  6. Nanyang Technological Univ. (Singapore); City Univ. of Hong Kong (Hong Kong)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Nanyang Technological University (NTU); City University of Hong Kong
OSTI Identifier:
1603282
Alternate Identifier(s):
OSTI ID: 1598058; OSTI ID: 1630068
Report Number(s):
BNL-213658-2020-JAAM
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
SC0012704; AC02‐06CH11357; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 32; Journal Issue: 11; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; amorphization; electrocatalysis; ligand exchange; Pd nanomaterials

Citation Formats

Cheng, Hongfei, Yang, Nailiang, Liu, Guigao, Ge, Yiyao, Huang, Jingtao, Yun, Qinbai, Du, Yonghua, Sun, Cheng‐Jun, Chen, Bo, Liu, Jiawei, and Zhang, Hua. Ligand-Exchange-Induced Amorphization of Pd Nanomaterials for Highly Efficient Electrocatalytic Hydrogen Evolution Reaction. United States: N. p., 2020. Web. https://doi.org/10.1002/adma.201902964.
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Cheng, Hongfei, Yang, Nailiang, Liu, Guigao, Ge, Yiyao, Huang, Jingtao, Yun, Qinbai, Du, Yonghua, Sun, Cheng‐Jun, Chen, Bo, Liu, Jiawei, & Zhang, Hua. Ligand-Exchange-Induced Amorphization of Pd Nanomaterials for Highly Efficient Electrocatalytic Hydrogen Evolution Reaction. United States. https://doi.org/10.1002/adma.201902964
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Cheng, Hongfei, Yang, Nailiang, Liu, Guigao, Ge, Yiyao, Huang, Jingtao, Yun, Qinbai, Du, Yonghua, Sun, Cheng‐Jun, Chen, Bo, Liu, Jiawei, and Zhang, Hua. Thu . "Ligand-Exchange-Induced Amorphization of Pd Nanomaterials for Highly Efficient Electrocatalytic Hydrogen Evolution Reaction". United States. https://doi.org/10.1002/adma.201902964. https://www.osti.gov/servlets/purl/1603282.
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@article{osti_1603282,
title = {Ligand-Exchange-Induced Amorphization of Pd Nanomaterials for Highly Efficient Electrocatalytic Hydrogen Evolution Reaction},
author = {Cheng, Hongfei and Yang, Nailiang and Liu, Guigao and Ge, Yiyao and Huang, Jingtao and Yun, Qinbai and Du, Yonghua and Sun, Cheng‐Jun and Chen, Bo and Liu, Jiawei and Zhang, Hua},
abstractNote = {Various kinds of amorphous materials, such as transition metal dichalcogenides, metal oxides, and metal phosphates, have demonstrated superior electrocatalytic performance compared with their crystalline counterparts. Compared to other materials for electrocatalysis, noble metals exhibit intrinsically high activity and excellent durability. However, it is still very challenging to prepare amorphous noble-metal nanomaterials due to the strong interatomic metallic bonding. Herein, the discovery of a unique thiol molecule is reported, namely bismuthiol I, which can induce the transformation of Pd nanomaterials from face-centered-cubic (fcc) phase into amorphous phase without destroying their integrity. This ligand-induced amorphization is realized by post-synthetic ligand exchange under ambient conditions, and is applicable to fcc Pd nanomaterials with different capping ligands. Importantly, the obtained amorphous Pd nanoparticles exhibit remarkably enhanced activity and excellent stability toward electrocatalytic hydrogen evolution in acidic solution. This work provides a facile and effective method for preparing amorphous Pd nanomaterials, and demonstrates their promising electrocatalytic application.},
doi = {10.1002/adma.201902964},
journal = {Advanced Materials},
number = 11,
volume = 32,
place = {United States},
year = {2020},
month = {2}
}
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https://doi.org/10.1002/adma.201902964
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