Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/161743
Title: Strong metal-support interaction boosts activity, selectivity, and stability in electrosynthesis of H₂O₂
Authors: Zhang, Junming
Ma, Jun
Choksi, Tej S.
Zhou, Daojin
Han, Shaobo
Liao, Yen-Fa
Yang, Hong Bin
Liu, Dong
Zeng, Zhiping
Liu, Wei
Sun, Xiaoming
Zhang, Tianyu
Liu, Bin
Keywords: Engineering::Chemical engineering
Issue Date: 2022
Source: Zhang, J., Ma, J., Choksi, T. S., Zhou, D., Han, S., Liao, Y., Yang, H. B., Liu, D., Zeng, Z., Liu, W., Sun, X., Zhang, T. & Liu, B. (2022). Strong metal-support interaction boosts activity, selectivity, and stability in electrosynthesis of H₂O₂. Journal of the American Chemical Society, 144(5), 2255-2263. https://dx.doi.org/10.1021/jacs.1c12157
Project: RG4/20
RG2/21
RS04/19
MOET2EP10120-0002 
A20E5c0080
Journal: Journal of the American Chemical Society
Abstract: Noble metals have an irreplaceable role in catalyzing electrochemical reactions. However, large overpotential and poor long-term stability still prohibit their usage in many reactions (e.g., oxygen evolution/reduction). With regard to the low natural abundance, the improvement of their overall electrocatalytic performance (activity, selectivity, and stability) was urgently necessary. Herein, strong metal-support interaction (SMSI) was modulated through an unprecedented time-dependent mechanical milling method on Pd-loaded oxygenated TiC electrocatalysts. The encapsulation of Pd surfaces with reduced TiO2-x overlayers is precisely controlled by the mechanical milling time. This encapsulation induced a valence band restructuring and lowered the d-band center of surface Pd atoms. For hydrogen peroxide electrosynthesis through the two-electron oxygen reduction reaction (ORR), these electronic and geometric modifications resulted in optimal adsorption energies of reaction intermediates. Thus, SMSI phenomena not only enhanced electrocatalytic activity and selectivity but also created an encapsulating oxide overlayer that protected the Pd species, increasing its long-term stability. This SMSI induced by mechanical milling was also extended to other noble metal systems, showing great promise for the large-scale production of highly stable and tunable electrocatalysts.
URI: https://hdl.handle.net/10356/161743
ISSN: 0002-7863
DOI: 10.1021/jacs.1c12157
Schools: School of Chemical and Biomedical Engineering 
Interdisciplinary Graduate School (IGS) 
School of Physical and Mathematical Sciences 
Research Centres: Nanyang Environment and Water Research Institute 
Rights: © 2022 American Chemical Society. All rights reserved.
Fulltext Permission: none
Fulltext Availability: No Fulltext
Appears in Collections:IGS Journal Articles
NEWRI Journal Articles
SCBE Journal Articles
SPMS Journal Articles

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