Photoactivated Nanoscale Temperature Gradient Detection Using X-ray Absorption Spectroscopy as a Direct Nanothermometry Method

Abstract

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Emerging high-prospect applications in photothermal catalysis

“…It 5 is important to analyze the interaction between reactants and catalysts, to discriminate between spectator species and species actively involved in the catalytic reaction, and to understand the catalytic mechanism, especially photochemical pathways, behind photothermal activation. Particularly crucial albeit highly challenging is the development of direct or indirect methods allowing for sensitive and accurate (local) surface temperature measurements and the elaboration of thermal mapping, spatiallyresolved and with a good thermal definition at the nanoscale [14][15][16][17]. Cortés et al recently reviewed the specific experimental techniques used to characterize optical near fields, temperature and hot carriers with spatial, energetic and/or temporal resolution, and to attempt to disentangle their roles.…”

Transient Temperature Response of Supported Rh Nanoparticles in Photothermal Dry Reforming of Methane─An Operando Dispersive X-ray Absorption Spectroscopy Study

“…Thus, it is highly desirable to perform an operando analysis to simultaneously reveal the key information of the chemical states, morphological structures, and local temperatures of the NPs. Among the temperature measurement methods that use spectroscopic techniques, − X-ray absorption spectroscopy (XAS) is a powerful and suitable tool for the above objectives, to clarify the chemical states, structural information, − and local temperatures − of the target materials at the nanoscale. Van de Broek et al determined the local temperatures of plasmonic Au NPs under irradiation by analyzing the Debye–Waller (DW) factor (σ 2 ), which is the sum of the thermal (σ t 2 ) and static disorder (σ s 2 ) components (eq ).…”

“…Van de Broek et al determined the local temperatures of plasmonic Au NPs under irradiation by analyzing the Debye–Waller (DW) factor (σ 2 ), which is the sum of the thermal (σ t 2 ) and static disorder (σ s 2 ) components (eq ). Several researchers successfully measured the local temperatures of metal NPs using the σ 2 values obtained via curve-fitting analysis (DW method). − However, the DW factor inevitably contains relatively large errors derived from the curve-fitting analysis. Moreover, at elevated temperatures, the simple extended X-ray absorption fine structure (EXAFS) theory is not applicable in analyzing the metal NPs due to the non-Gaussian distribution of the metal–metal bond lengths .…”

Precise Regulation of Enzyme–Nanozyme Cascade Reaction Kinetics by Magnetic Actuation toward Efficient Tumor Therapy

“…Recently, a growing body of data, either via direct or indirect temperature mapping, ,, have pointed out the existence of a nanoscale temperature gradient at the surface of nanoparticles upon external stimuli actuation. Therefore, we anticipated that with precise spatial distance control to place a MNP nanozyme in close proximity to an enzyme, the magneto-heat gradient around the MNPs could be effectively harnessed to stimulate the individual kinetics of the enzyme and the MNP nanozyme, leading to a tuned kinetic match between them and thus modulated cascade activity.…”