Research
We are involved in the three following research themes:
• Operando X-ray spectroscopy of electrocatalytic reactions
• Electronic structure of biomimetic and bioinspired molecular systems
• Microfluidic and electochemical instrumentation
Operando X-ray spectroscopy of electrocatalytic reactions
Since more than a decade, we have been interested in the study of electrocatalytic systems based on transition metal oxides or sulfides, as well as molecular complexes. These systems are active for the oxygen (OER) and hydrogen (HER) evolving reactions, as well as the CO2 reduction reaction (CO2RR). X-ray absorption spectroscopy is our main tool to understand the local and electronic structure of these catalysts and follow their evolution under operating conditions.
Collaborations
Dr. Marion Giraud, Dr. Jennifer Peron, Université Paris Cité, Paris, France
Dr. Cédric Tard, Institut Polytechnique de Paris, Palaiseau, France
Dr. Sophie Carenco, Dr. David Portehault, Sorbonne Université, Paris, France
Pr. Ovidiu Ersen, Université de Strasbourg, Strasbourg, France
Pr. Marc Robert, Dr. Elodie Anxolabéhère-Mallart, Université Paris Cité, Paris, France
Selected publications
Multiple C–C bond formation upon electrocatalytic reduction of CO2 by an iron-based molecular macrocycle
Si-Thanh Dong, Chen Xu and Benedikt Lassalle-Kaiser.*
Chemical Science, 2023, 14, 550-556.
https://doi.org/10.1039/D2SC04729B
Experimental Evidence of the Role of Short-Range Order on the Electrochemical Activity of Iridium Oxides
M. Elmaalouf, M. Odziomek, S. Duran, M. Gayrard, M. Bari, C. Tard, C. Boissière, A. Zitolo, B. Lassalle-Kaiser, J-Y. Piquemal, O. Ersen, C. Sanchez, M. Giraud, M. Faustini* and J. Peron.*
Nature Communications, 2021, 12, 1, 3935.
https://doi.org/10.1038/s41467-021-24181-x
Morphological and Structural Evolution of Co3O4 Nanoparticles Revealed by in Situ Electrochemical Transmission Electron Microscopy during Electrocatalytic Water Oxidation
N. Pena, D. Ihiawakrim, M. Han, B. Lassalle-Kaiser, S. Carenco, C. Sanchez, C. Laberty, D. Portehault,* O. Ersen.*
ACS Nano, 2019, 13, 10, 11372-11381.
https://doi.org/10.1021/acsnano.9b04745
In Situ Observation of the Formation and Structure of Hydrogen-Evolving Amorphous Cobalt Electrocatalysts
B. Lassalle-Kaiser,* A. Zitolo, E. Fonda, M. Robert, E. Anxolabéhère-Mallart.*
ACS Energy Letters, 2017, 2, 2545-2551.
https://doi.org/10.1021/acsenergylett.7b00789
Structure–Activity Correlations in a Nickel–Borate Oxygen Evolution Catalyst
D. K. Bediako, B. Lassalle-Kaiser, Y. Surendranath, J. Yano, V. K. Yachandra, and D. G. Nocera.*
Journal of the American Chemical Society, 2012, 134, 15, 6801-6809.
https://doi.org/10.1021/ja301018q
Electronic structure of biomimetic and bioinspired molecular systems
We have been interested in synthesizing and characterizing biomimetic molecular complexes that model the Oxygen Evolving Center of Photosystem II for more than a decade, using both electrochemistry and spectroscopy. We are particularly interested in understanding their electronic structure and the distribution of the electronic density between the metal and its ligands. To this end, we use a combination of electrochemistry, UV-Visible, EPR and mostly X-ray spectroscopies. These techniques allow determining the oxidation and spin state, as well as the geometry of the metal of interest. We have studied mononuclear and polynuclear manganese complexes, and more recently Rhodium, Ruthenium and Iron complexes, all relevent to energy-related reactions such as the OER, HER or CO2RR.
Collaborations
Dr. Zakaria Halime, Pr. Ally Aukauloo, Université Paris-Saclay, Orsay, France
Pr. Gary Moore, Arizona State University, Tempe, USA
Pr. Julio Lloret-Fillol, ICIQ, Tarragona, Spain
Pr. James Blakemore, University of Kansas, Lawrence, USA
Selected publications
In situ X-ray absorption spectroscopy in homogeneous conditions reveals interactions between CO2 and a doubly and triply reduced iron(III) porphyrin, then leading to catalysis
Daniela Mendoza, Si-Thanh Dong, Nikolaos Kostopoulos, Victor Pinty, Orestes Rivada-Wheelaghan, Elodie Anxolabéhère-Mallart,* Marc Robert* and Benedikt Lassalle-Kaiser.*
ChemCatChem, 2022, accepted
https://doi.org/10.1002/cctc.202201298
Synthesis and Structural and Electronic Characterization of an Iron Fused Porphyrin
E. A. Reyes Cruz, D. Khusnutdinova, D. Nishiori, B. Lassalle-Kaiser* and Gary F. Moore.*
ChemElectroChem, 2021, 8, 19, 3614-3620.
https://doi.org/10.1002/celc.202100550
Isolation of a missing link in the water oxidation reaction
B. Casadevall, V. Martin-Diaconescu, W. R. Browne, S. Fernandez, F. Franco, N. Cabello, J. Benet-Buchholz, B. Lassalle-Kaiser, J. lloret-Fillol.*
Nature Chemistry, 2021, 13, 8, 800+.
https://doi.org/10.1038/s41557-021-00702-5
High-spin Mn-oxo complexes and their relevance to the oxygen-evolving complex within PS II
R. Gupta, T. Taguchi, B. Lassalle-Kaiser, E. L. Bominaar, J. Yano, M. P. Hendrich and A. S. Borovik.*
Proceedings of the National Academy of Science of the USA, 2015, 112, 17, 5319-5324.
https://doi.org/10.1073/pnas.1422800112
Activation of a water molecule using a mononuclear Mn complex: from Mn-aquo, to Mn-hydroxo, to Mn-oxyl via charge compensation
B. Lassalle-Kaiser, C. Hureau, D. A. Pantazis, Y. Pushkar, R. Guillot, V. K. Yachandra, J. Yano, F. Neese*, E. Anxolabéhère-Mallart.*
Energy and Environmental Science, 2010, 3, 7, 924-938.
Instrumentation
Electrochemical cell design
We develop specific electrochemical cells that allow probing electroactive or catalytic species with X-ray spectroscopy under in situ/operando conditions. These cells can feature heterogeneous or homogeneous systems under static or flowing conditions.
Microfluidics: mixing, sorting, trapping, freezing
We develop microfluidic systems that allow mixing, sorting or trapping (bio)chemical species or biological objects (cells, crystals). Theses systems are combined with synchrotron-base techniques, which are used to probe the structure of these objects under in situ conditions and with time-resolution.
Collaborations
Pr. Yves Méchulam, Dr. Emmanuelle Schmitt, Dr. Pierre-Damien Coureux, Institut Polytechnique de Paris, Palaiseau, France
Dr. Jean-Blaise Brubach, Synchrotron SOLEIL, Gif-sur-Yvette, France
Selected publications
A millisecond passive micromixer with low flow rate, low sample consumption and easy fabrication
Y. Liao, Y. Mechulam and B. Lassalle-Kaiser.*
Scientific Reports, 2021, 11, 1, 201119.
https://doi.org/10.1038/s41598-021-99471-x
The microfluidic laboratory at Synchrotron SOLEIL
I. Chaussavoine, A. Beauvois, T. Mateo, R. Vasireddi, N. Douri, J. Priam, Y. Liatimi, S. Lefrançois, H. Tabuteau, M. Davranche, D. Vantelon,* T. Bizien,* L. M. G. Chavas,* B. Lassalle-Kaiser.*
Journal of Synchrotron Radiation, 2020, 27, 1, 230-237.
https://doi.org/10.1107/S1600577519015042
Time-resolved X-ray absorption spectroelectrochemistry of redox active species in solution
K. Cheaib, B. Maurice, T. Mateo, Z. Halime,* B. Lassalle-Kaiser.*
Journal of Synchrotron Radiation, 2019, 26, 6, 1980-1985.
https://doi.org/10.1107/S1600577519013614
In Situ/Operando Studies of Electrocatalysts Using Hard X-ray Spectroscopies
B. Lassalle-Kaiser, S. Gul, J. Kern, V. K. Yachandra and J. Yano.*
Journal of electron spectroscopy and related Phenomena, 2017, 221, 18-27