April 7 - 11, 2025
Seattle, Washington
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2025 MRS Spring Meeting & Exhibit
MT04.04.02

Nanometer-Resolved Observation of Electrochemical Microenvironment Formation at the Nanoparticle–Ligand Interface

When and Where

Apr 8, 2025
2:00pm - 2:15pm
Summit, Level 4, Room 422

Presenter(s)

Co-Author(s)

Yu Shan1,Xiao Zhao2,Maria Fonseca Guzman1,Asmita Jana2,Shouping Chen1,Sunmoon Yu1,Ka Chon Ng2,Inwhan Roh1,Hao Chen2,Virginia Altoe2,Stephanie Corder2,Hans Bechtel2,Jin Qian2,Miquel Salmeron2,Peidong Yang1

University of California, Berkeley1,Lawrence Berkeley National Laboratory2

Abstract

Yu Shan1,Xiao Zhao2,Maria Fonseca Guzman1,Asmita Jana2,Shouping Chen1,Sunmoon Yu1,Ka Chon Ng2,Inwhan Roh1,Hao Chen2,Virginia Altoe2,Stephanie Corder2,Hans Bechtel2,Jin Qian2,Miquel Salmeron2,Peidong Yang1

University of California, Berkeley1,Lawrence Berkeley National Laboratory2
The electrocatalytic microenvironment surrounding nanocatalysts plays a pivotal role in dictating catalytic reactivity and selectivity by influencing solvent orientation, counterion solvation, reactant transportation, and the stabilization of intermediates near active sites. Despite its importance, the rational design of nanocatalysts with optimized microenvironments remains underdeveloped, primarily due to a limited molecular-level understanding of microenvironment formation and evolution at the electrolyte–nanocatalyst interface. In situ and operando techniques with nanometer-scale spatial resolution and chemical sensitivity are therefore essential for revealing the real-time molecular dynamics of this interface. In our recent work, we utilized in situ Fourier transform infrared nanospectroscopy (nano-FTIR) to successfully capture the formation of an electrochemical microenvironment that promotes CO2 electroreduction at the nanoparticle–ligand interface. Complemented by Surface Enhanced Raman Spectroscopy (SERS), we uncovered a bias-induced consecutive ligand dissociation mechanism in aggregating silver nanoparticles. These findings provide critical insights for guiding the rational design of electrocatalysts by tracking the structural evolution of nanoparticle-ligand systems. Moreover, the methodology we present is broadly applicable to studying the dynamic response of interfacial species—such as capping ligands, reaction intermediates, and solvent molecules—to various external stimuli at nanometer resolution, thereby substantially facilitating the mechanistic understanding of how the molecular-level events ultimately lead to specific NP functionalities.

Keywords

in situ | infrared (IR) spectroscopy | nanoscale

Symposium Organizers

Shoji Hall, Johns Hopkins University
Megan Jackson, University of North Carolina at Chapel Hill
Yao Yang, Cornell University
Emil Hernandez-Pagan, University of Delaware

Session Chairs

Shoji Hall
Emil Hernandez-Pagan
Megan Jackson

In this Session