Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Operando methods: A new era of electrochemistry

Journal Article · · Current Opinion in Electrochemistry
 [1];  [2];  [3];  [4];  [4];  [5];  [5];  [6];  [7];  [7];  [8];  [9];  [10];  [4];  [4];  [11]
  1. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Cornell Univ., Ithaca, NY (United States)
  2. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  3. Forschungszentrum Juelich, Erlangen (Germany). Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IEK-11)
  4. Cornell Univ., Ithaca, NY (United States)
  5. CIC NanoGUNE BRTA, Donostia (Spain). Electron Microscopy Laboratory
  6. CIC NanoGUNE BRTA, Donostia (Spain). Electron Microscopy Laboratory; Basque Foundation for Science, Bilbao (Spain). IKERBASQUE
  7. University of California, Berkeley, CA (United States)
  8. Cornell Univ., Ithaca, NY (United States). Cornell High Energy Synchrotron Source (CHESS)
  9. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)
  10. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  11. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Cornell Univ., Ithaca, NY (United States). Cornell High Energy Synchrotron Source (CHESS); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
One of the grand challenges facing electrochemistry is to directly resolve the complex nature of (electro)catalyst active sites and capture real-time “movies” of reaction dynamics, i.e. “watching chemistry in action”. The need for such fundamental understanding has stimulated the development of operando/in situ methods, which have greatly enhanced our ability to identify activity descriptors of electrocatalysts and establish structure–property relationships of energy materials. Here, this review summarizes the frontiers of operando electrochemical liquid-cell scanning transmission electron microscopy and correlative synchrotron X-ray methods, which are complementary tools to comprehensively investigate reaction dynamics across multiple spatiotemporal scales. In an effort to encourage greater adoption of advanced operando methods by the general electrochemistry community, this review points out the need to benchmark electrochemistry in confined and heterogenous liquid environment with minimal beam-induced damage. We anticipate that multimodal operando methods will become indispensable for understanding interfacial reaction mechanisms for the broad chemistry and energy materials communities.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231; SC0019445
OSTI ID:
2467424
Journal Information:
Current Opinion in Electrochemistry, Journal Name: Current Opinion in Electrochemistry Vol. 42; ISSN 2451-9103
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (68)

Real‐time Monitoring Reveals Dissolution/Redeposition Mechanism in Copper Nanocatalysts during the Initial Stages of the CO 2 Reduction Reaction journal November 2020
Anodic and Cathodic Platinum Dissolution Processes Involve Different Oxide Species journal July 2023
In Situ Liquid Electrochemical TEM Investigation of LiMn1.5Ni0.5O4 Thin Film Cathode for Micro‐Battery Applications journal December 2021
Operando methodology: combination of in situ spectroscopy and simultaneous activity measurements under catalytic reaction conditions journal February 2005
A materials driven approach for understanding single entity nano impact electrochemistry journal December 2017
Using soft x-ray absorption spectroscopy to characterize electrode/electrolyte interfaces in-situ and operando journal November 2017
Differential electrochemical mass spectrometry journal December 2004
The exit-wave power-cepstrum transform for scanning nanobeam electron diffraction: robust strain mapping at subnanometer resolution and subpicometer precision journal July 2020
Quantification of reagent mixing in liquid flow cells for Liquid Phase-TEM journal March 2023
In Situ Electron Energy-Loss Spectroscopy in Liquids journal May 2013
Quantitative Electrochemical Measurements Using In Situ ec-S/TEM Devices journal March 2014
High Dynamic Range Pixel Array Detector for Scanning Transmission Electron Microscopy journal January 2016
Very-High Dynamic Range, 10,000 Frames/Second Pixel Array Detector for Electron Microscopy journal March 2022
Leakless, Bipolar Reference Electrodes: Fabrication, Performance, and Miniaturization journal July 2021
The Necessity for Multiscale In Situ Characterization of Tailored Electrocatalyst Nanoparticle Stability journal January 2023
Electrocatalysis in Alkaline Media and Alkaline Membrane-Based Energy Technologies journal February 2022
Operando Scanning Electrochemical Probe Microscopy during Electrocatalysis journal March 2023
Environment-Dependent Radiation Damage in Atmospheric Pressure X-ray Spectroscopy journal September 2017
In Situ Study of Lithiation and Delithiation of MoS 2 Nanosheets Using Electrochemical Liquid Cell Transmission Electron Microscopy journal July 2015
Selective Electrochemical CO 2 Reduction during Pulsed Potential Stems from Dynamic Interface journal June 2020
Operando Methods in Electrocatalysis journal January 2021
Metal Monolayers on Command: Underpotential Deposition at Nanocrystal Surfaces: A Quantitative Operando Electrochemical Transmission Electron Microscopy Study journal March 2022
Nanoscale Chemical and Structural Analysis during In Situ Scanning/Transmission Electron Microscopy in Liquids journal May 2021
Morphological and Structural Evolution of Co 3 O 4 Nanoparticles Revealed by in Situ Electrochemical Transmission Electron Microscopy during Electrocatalytic Water Oxidation journal September 2019
Understanding the Dynamics of Molecular Water Oxidation Catalysts with Liquid-Phase Transmission Electron Microscopy: The Case of Vitamin B12 journal July 2021
Operando Electrochemical Liquid-Cell Scanning Transmission Electron Microscopy (EC-STEM) Studies of Evolving Cu Nanocatalysts for CO2 Electroreduction journal February 2023
Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting journal January 2015
Dynamic Reoxidation/Reduction-Driven Atomic Interdiffusion for Highly Selective CO 2 Reduction toward Methane journal June 2020
Revealing the Dynamics and Roles of Iron Incorporation in Nickel Hydroxide Water Oxidation Catalysts journal October 2021
Operando Resonant Soft X-ray Scattering Studies of Chemical Environment and Interparticle Dynamics of Cu Nanocatalysts for CO2 Electroreduction journal May 2022
Elucidating Cathodic Corrosion Mechanisms with Operando Electrochemical Transmission Electron Microscopy journal August 2022
Structure of the Photo-catalytically Active Surface of SrTiO 3 journal June 2016
Nanoscale Surface Structure–Activity in Electrochemistry and Electrocatalysis journal November 2018
Identification of Stabilizing High-Valent Active Sites by Operando High-Energy Resolution Fluorescence-Detected X-ray Absorption Spectroscopy for High-Efficiency Water Oxidation journal November 2018
In Situ X-ray Absorption Spectroscopy of a Synergistic Co–Mn Oxide Catalyst for the Oxygen Reduction Reaction journal December 2018
A Strategy for Increasing the Efficiency of the Oxygen Reduction Reaction in Mn-Doped Cobalt Ferrites journal February 2019
Regulating Key Variables and Visualizing Lithium Dendrite Growth: An Operando X-ray Study journal May 2019
Electron–Water Interactions and Implications for Liquid Cell Electron Microscopy journal September 2014
Nanoscale Imaging of Lithium Ion Distribution During In Situ Operation of Battery Electrode and Electrolyte journal February 2014
Nanoscale Imaging of Fundamental Li Battery Chemistry: Solid-Electrolyte Interphase Formation and Preferential Growth of Lithium Metal Nanoclusters journal February 2015
Unravelling the electrochemical double layer by direct probing of the solid/liquid interface journal August 2016
Structure and bonding at the atomic scale by scanning transmission electron microscopy journal April 2009
Dynamic microscopy of nanoscale cluster growth at the solid–liquid interface journal July 2003
Copper adparticle enabled selective electrosynthesis of n-propanol journal November 2018
Morphology and mechanism of highly selective Cu(II) oxide nanosheet catalysts for carbon dioxide electroreduction journal February 2021
Dynamic transformation of cubic copper catalysts during CO2 electroreduction and its impact on catalytic selectivity journal November 2021
Uncovering material deformations via machine learning combined with four-dimensional scanning transmission electron microscopy journal May 2022
Resolution and aberration correction in liquid cell transmission electron microscopy journal December 2018
Correlative operando microscopy of oxygen evolution electrocatalysts journal May 2021
Operando studies reveal active Cu nanograins for CO2 electroreduction journal February 2023
Designing materials for electrochemical carbon dioxide recycling journal July 2019
Real-time imaging and local elemental analysis of nanostructures in liquids journal January 2014
Direct visualization of sulfur cathodes: new insights into Li–S batteries via operando X-ray based methods journal January 2018
Real-time imaging of activation and degradation of carbon supported octahedral Pt–Ni alloy fuel cell catalysts at the nanoscale using in situ electrochemical liquid cell STEM journal January 2019
In situ electrochemistry inside a TEM with controlled mass transport journal January 2020
Snapshots of a working catalyst: possibilities and limitations of in situ spectroscopy in the field of heterogeneous catalysis journal January 2002
An in situ cell for characterization of solids by soft x-ray absorption journal September 2004
Electrochemically scrambled nanocrystals are catalytically active for CO 2 -to-multicarbons journal April 2020
The effect of flow on radiolysis in liquid phase-TEM flow cells journal December 2022
Aberration-corrected ADF-STEM depth sectioning and prospects for reliable 3D imaging in S/TEM journal January 2009
Elimination of the inner-shell lifetime broadening in x-ray-absorption spectroscopy journal November 1991
A soft XAS transmission cell for operando studies journal October 2016
Transmission electron microscopy with a liquid flow cell journal January 2011
Nonprecious transition metal nitrides as efficient oxygen reduction electrocatalysts for alkaline fuel cells journal February 2022
The structure of interfacial water on gold electrodes studied by x-ray absorption spectroscopy journal October 2014
The Study of Solid/Liquid Interfaces with X-ray Standing Waves journal October 1990
Selective increase in CO 2 electroreduction activity at grain-boundary surface terminations journal November 2017
Electron ptychography achieves atomic-resolution limits set by lattice vibrations journal May 2021