Shining light on electrochemistry: a synchrotron-based X-ray spectroscopic interrogation

Abstract

Over the last few decades, synchrotron radiation has experienced a flourishing growth, fueled by cutting-edge spectroscopic techniques that have empowered its remarkable ability to probe down to the atomic level. Indeed, this advancement has been inspiring, unlocking powerful insights and capabilities in the realm of electrochemistry community. This perspective showcases recent ground-breaking efforts and remaining challenges with respect to X-ray spectroscopy, as well as their implications for ongoing research.

Keywords

Synchrotron radiation / electrochemistry / X-ray absorption/emission spectroscopy / interface

References

[1] Elder FR,Langmuir RV.Radiation from electrons in a synchrotron.Phys Rev1947;71:829

[2] The circles of light.Nat Rev Mater2018;3:281-2

[3] Ice GE,Pang JWL.The race to X-ray microbeam and nanobeam science.Science2011;334:1234-9

[4] Zhang XW,Zhou ZR.Arsenic trioxide controls the fate of the PML-RARα oncoprotein by directly binding PML.Science2010;328:240-3

[5] Kern J,Tran R.Simultaneous femtosecond X-ray spectroscopy and diffraction of photosystem II at room temperature.Science2013;340:491-5 PMCID:PMC3732582

[6] Wu J.Understanding the electric double-layer structure, capacitance, and charging dynamics.Chem Rev2022;122:10821-59

[7] Velasco-Velez JJ,Pascal TA.Interfacial water. The structure of interfacial water on gold electrodes studied by x-ray absorption spectroscopy.Science2014;346:831-4

[8] Ledezma-Yanez I,Sebastián-Pascual P,Feliu JM.Interfacial water reorganization as a pH-dependent descriptor of the hydrogen evolution rate on platinum electrodes.Nat Energy2017;2:17031

[9] Kolb DM.Electrochemical surface science this manuscript is based on the Bonhoeffer-Eucken-Scheibe lectures of the Deutsche Bunsengesellschaft, given by the author at Erlangen, Berlin, and Leipzig in 1999/2000.Angew Chem Int Ed2001;40:1162-81

[10] Brown MA,Abbas Z.Effect of electrolyte concentration on the stern layer thickness at a charged interface.Angew Chem Int Ed Engl2016;55:3790-4

[11] Axnanda S,Mao B.Using “Tender” X-ray ambient pressure X-ray photoelectron spectroscopy as a direct probe of solid-liquid interface.Sci Rep2015;5:9788 PMCID:PMC4650780

[12] Favaro M,Ross PN.Unravelling the electrochemical double layer by direct probing of the solid/liquid interface.Nat Commun2016;7:12695 PMCID:PMC5013669

[13] Strmcnik D,van der Vliet D,Stamenkovic VR.The role of non-covalent interactions in electrocatalytic fuel-cell reactions on platinum.Nat Chem2009;1:466-72

[14] Subbaraman R,Strmcnik D.Enhancing hydrogen evolution activity in water splitting by tailoring Li⁺-Ni(OH)₂-Pt interfaces.Science2011;334:1256-60

[15] Goyal A.The interrelated effect of cations and electrolyte pH on the hydrogen evolution reaction on gold electrodes in alkaline media.Angew Chem Int Ed Engl2021;60:13452-62 PMCID:PMC8252582

[16] Shah AH,Huang Z.The role of alkali metal cations and platinum-surface hydroxyl in the alkaline hydrogen evolution reaction.Nat Catal2022;5:923-33

[17] Li P,Hu Y.Hydrogen bond network connectivity in the electric double layer dominates the kinetic pH effect in hydrogen electrocatalysis on Pt.Nat Catal2022;5:900-11

[18] Lucas CA,Gründer Y.The structure of the electrochemical double layer: Ag(111) in alkaline electrolyte.Electrochem Commun2011;13:1205-8

[19] Sun Z,Yao T,Xie Y.XAFS in dilute magnetic semiconductors.Dalton Trans2013;42:13779-801

[20] Huang J,Liu Z.Experimental Sabatier plot for predictive design of active and stable Pt-alloy oxygen reduction reaction catalysts.Nat Catal2022;5:513-23

[21] Kang J,Hu Q.Valence oscillation and dynamic active sites in monolayer NiCo hydroxides for water oxidation.Nat Catal2021;4:1050-8

[22] Bergmann A,Martinez Moreno E.Unified structural motifs of the catalytically active state of Co(oxyhydr)oxides during the electrochemical oxygen evolution reaction.Nat Catal2018;1:711-9

[23] Jia Q,Hafiz H.Experimental observation of redox-induced Fe-N switching behavior as a determinant role for oxygen reduction activity.ACS Nano2015;9:12496-505

[24] Velasco-Vélez JJ,Bernsmeier D.A comparative study of electrochemical cells for in situ x-ray spectroscopies in the soft and tender x-ray range.J Phys D Appl Phys2021;54:124003

[25] Diercks JS,Ebner K.Spectroscopy vs. electrochemistry: catalyst layer thickness effects on operando/in situ measurements.Angew Chem Int Ed Engl2023;62:e202216633

[26] Zitolo A,Mineva T.Identification of catalytic sites in cobalt-nitrogen-carbon materials for the oxygen reduction reaction.Nat Commun2017;8:957 PMCID:PMC5715157

[27] Hu J,Xin C.Uncovering dynamic edge-sites in atomic Co-N-C electrocatalyst for selective hydrogen peroxide production.Angew Chem Int Ed Engl2023;62:e202304754

[28] Zhang M,Frei H.Time-resolved observations of water oxidation intermediates on a cobalt oxide nanoparticle catalyst.Nat Chem2014;6:362-7

[29] Dong JC,Briega-Martos V.In situ Raman spectroscopic evidence for oxygen reduction reaction intermediates at platinum single-crystal surfaces.Nat Energy2019;4:60-7

[30] Mefford JT,Kang M.Correlative operando microscopy of oxygen evolution electrocatalysts.Nature2021;593:67-73

[31] Saveleva VA,Ni L.Potential-induced spin changes in Fe/N/C electrocatalysts assessed by in situ X-ray emission spectroscopy.Angew Chem Int Ed Engl2021;60:11707-12

[32] Gallo E.Valence to core X-ray emission spectroscopy.Adv Mater2014;26:7730-46

[33] Cutsail GE III.Challenges and opportunities for applications of advanced X-ray spectroscopy in catalysis research.ACS Catal2022;12:5864-86

[34] Chen J,Wang Z.Strain and ligand effects in Pt-Ni alloys studied by valence-to-core X-ray emission spectroscopy.Sci Rep2021;11:13698 PMCID:PMC8249455

[35] Lancaster KM,Ettenhuber P.X-ray emission spectroscopy evidences a central carbon in the nitrogenase iron-molybdenum cofactor.Science2011;334:974-7 PMCID:PMC3800678

[36] Pollock CJ.Valence-to-core X-ray emission spectroscopy: a sensitive probe of the nature of a bound ligand.J Am Chem Soc2011;133:5594-601