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Reuse of sodium–doped iridium oxide nanoparticles as a bio–stimulating electrode by a chemical and electrochemical recovery process

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Ceramics International 2024年第4期50卷 6220-6228页

作者： Tso, Kuang-Chih Chen, Chieh-Hsuan Chen, Po-Chun Li, Shao-Sian Chen, Jeng-Lung Ohta, Jun Wu, Pu-Wei Division of Materials Science Graduate School of Science and Technology Nara Institute of Science and Technology Nara630-0192 Japan Graduate Degree Program of Science and Technology of Accelerator Light Source National Yang Ming Chiao Tung University Hsinchu300 Taiwan Department of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu300 Taiwan Institute of Materials Science and Engineering National Taipei University of Technology Taipei106 Taiwan National Synchrotron Radiation Research Center Hsinchu300 Taiwan

A sequential chlorination and electrochemical reduction process is demonstrated to convert Na–doped iridium oxide nanoparticles into useful IrIIICl63−(aq) serving as the precursor for the fabrication of bio–stimulating electrode. The Na–doped iridium oxide nanoparticles are treated in 35 wt% hydrochloric acid at 70 °C for 18 h to form IrIVCl62−(aq) with pH of 0.3, so the latter could be readily reduced to IrIIICl63−(aq) at a potentiostatic mode of 0.6 V (vs. SCE). The oxidation state and the nature of complexing ligands for the regenerated IrIIICl63− and IrIVCl62−, as well as commercially available IrIIICl63− are validated by X–ray Absorption Spectroscopy. UV–Vis profiles of regenerated IrIVCl62−(aq) are recorded and the absorbance at 487 nm signal is benchmarked against that of standard IrIVCl62−(aq) to obtain the effective regeneration ratio of 68.6%. X–ray diffraction patterns of Na–doped iridium oxide nanoparticles before and after the annealing treatment indicate the amorphous structure facilitates the chlorination step. The regenerated IrIIICl63− is reused to synthesize Na–doped iridium oxide thin film serving as a bio–stimulating electrode for implantable bio–electronics. The regenerated Na–doped iridium oxide thin film reveals a charge-storage capacity of 0.32 mC/cm2-nm and impressive stability that are comparable to those of fresh Na–doped iridium oxide thin film derived from commercially available IrIIICl63−. © 2023 Elsevier Ltd and Techna Group S.r.l.

关键词： Transition metal oxides

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Influence of Ru-substitution on the performance of pyrochlore catalysts in oxidative steam reforming of ethanol

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Sustainable Energy and Fuels 2024年第9期8卷 2104-2114页

作者： Huang, Yu-Hsuan Hsieh, Ho-Chen Wang, Yun-Hsin Weng, Sheng-Feng Lee, Chi-Shen Department of Applied Chemistry National Yang Ming Chiao Tung University 1001 University Rd Hsinchu 30010 Taiwan Graduate Degree Program of Science and Technology of Accelerator Light Source National Yang Ming Chiao Tung University Hsinchu 30010 Taiwan Center for Emergent Functional Matter Science National Chiao-Tung University Hsinchu 30010 Taiwan

This study introduces a series of Ru-substituted pyrochlore catalysts, achieved by using La2Zr2−xRuxO7−δ (LZRO-00-04, x = 0.0-0.4) during the oxidative steam reforming of ethanol reaction (OSRE). The samples were cha...

This study introduces a series of Ru-substituted pyrochlore catalysts, achieved by using La₂Zr_2−xRu_xO_7−δ (LZRO-00-04, x = 0.0-0.4) during the oxidative steam reforming of ethanol reaction (OSRE). The samples were characterized using X-ray diffraction (XRD), temperature programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS). The reduction behavior and catalytic performance correlate directly with the Ru content. The 5 wt% LZRO02 catalytic system outperforms the supported Ru-based catalyst (5 wt% RuO₂/LZO), boasting lower Ru concentrations (2.66 wt%). The enhancement is attributed to the uniform dispersion of Ru ≥ 4+ ions embedded within the pyrochlore structure, as convincingly supported by the XPS result. This underscores notable distinctions between the internal and external structures of the two systems. On the other hand, our extensive long-term testing of LZRO02 across γ-Al₂O₃ and lab-made LZO carriers, coupled with meticulous mapping and Raman analysis, revealed a significant observation: the catalyst exhibits notably reduced aggregation tendencies and enhanced activity when utilized on the LZO carrier. The La₂Zr_1.8Ru_0.2O_7−δ catalyst supported on LZO demonstrated selectivity of hydrogen S_H = 86.4(1)%;Y_H = 2.55(3) (mol/mol EtOH) for long-term stability tests at T = 400 °C, C/O = 0.6, and O₂/C₂H₅OH = 1.5. This discovery underscores the catalyst's remarkable stability and activity, making it a promising candidate for catalytic applications. © 2024 The Royal Society of Chemistry.

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Unravelling the strong interplay for interfacial magnetic switching in metal-organic-based spintronics

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Journal of Materials Chemistry C 2024年第11期12卷 3931-3942页

作者： Chen, Wan-Ting Yu, Li-Chung Lin, Jiu-Hua Cheng, Su Ling Shiu, Hung Wei Lai, Yu-Ling Chu, Ying-Hao Chin, Yi-Ying Wang, Jeng-Han Hsu, Yao-Jane National Synchrotron Radiation Research Center Hsinchu30076 Taiwan Graduate Program for Science and Technology of Accelerator Light Sources National Yang Ming Chiao Tung University Hsinchu30076 Taiwan Department of Materials Science and Engineering National Tsing Hua University Hsinchu30013 Taiwan Department of Chemistry National Taiwan Normal University Taipei11677 Taiwan Department of Photonics National Cheng Kung University Tainan70101 Taiwan Department of Physics National Chung Cheng University Chiayi62102 Taiwan

Organic semiconductors are promising building blocks for multifunctional spintronics. The spinterface plays a key role in affecting the magnetic properties of the performance of spin-based devices. Herein, we reveal the strong interfacial interplay affecting the magnetic switching at the interface of the synthetic paramagnetic tris(8-hydroxyquinoline)iron(iii) (Feq3) layer on the ferromagnetic surface. In combination with synchrotron-based analysis and density functional theory (DFT) calculations, we observed that the robust magnetic interactions of the Co/Feq3 system were strongly influenced by the interfacial reaction between Co and Feq3. As the charge transferred from the contacted Co to Feq3, the central iron was reduced from Fe(iii) to Fe(ii) and hybridized with the 8-hydroxyquinoline, causing spin polarization at the interface. The reduced central Fe(ii) exhibited apparent ferromagnetic ordering after contact with the ferromagnetic Co substrate. With increasing the Feq3 layer thickness, the central Fe reverted to its original Fe(iii) state, resulting in the disappearance of ferromagnetic ordering. The thickness dependence of the Feq3 layer on the magnetic response could be used to tune the spinterface properties and thus the interfacial magnetic interplay. These findings reveal the effect of the strong interfacial redox on the spinterface and open up a promising approach for the use of metal-organic materials in oragnic spintronic devices. © 2024 The Royal Society of Chemistry.

关键词： Organometallics

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A robust bendable IrO_x thin film via mild alkaline solution process for neuron stimulating electrodes

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Surfaces and Interfaces 2024年 44卷

作者： Tso, Kuang-Chih Chan, Tzu-Ying Yu, Tsung-Chun Tao, Yu-Jen Chu, Chao-Yi Chen, San-Yuan Lee, Jyh-Fu Ohta, Jun Chen, Po-Chun Wu, Pu-Wei Graduate Program of Accelerator Light Source National Yang Ming Chiao Tung University Hsinchu 300 Taiwan Division of Materials Science Graduate School of Science and Technology Nara Institute of Science Technology Nara Ikoma Takayama 8916-5 Japan Department of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 300 Taiwan Institute of Materials Science and Engineering National Taipei University of Technology Taipei 106 Taiwan National Synchrotron Radiation Research Center Hsinchu 300 Taiwan

We demonstrate a unique chemical formula to deposit hydrous iridium oxide thin film on a platinum-coated polyimide substrate. In a mild alkaline solution, the iridium (III) precursor undergoes the ligand exchange and hydrolysis reaction to become the iridium (III) dimers that are physically adsorbed on the substrate for subsequent heterogeneous condensation and growth of amorphous hydrous iridium oxide thin film. Both UV–Vis and X-ray absorption spectroscopy (XAS) are employed to determine the reaction steps involved. The chemical nature and crystallinity of the hydrous iridium oxide thin film are investigated by XAS, X-ray photon spectroscopy, and X-ray diffraction. The hydrous iridium oxide thin film reveals an impressive normalized charge storage capacity (CSC) of 0.3 mC/cm²-nm and a low impedance (80.5 Ω) at 1k Hz. In addition, in bending test of 3,000 cycles, the hydrous iridium oxide thin film retains 91.2 % of its initial normalized CSC without any physical crack and delamination. The cell viability test suggests negligible bio-toxicity. Our results provide a solid evidence of fabricating a robust flexible electrode for neural interfaces for potential use in implantable electronic devices. © 2023 Elsevier B.V.

关键词： Bio-electrode Flexible substrate Implantable electronic devices Iridium dimers Iridium oxide Polyimide

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A Robust Bendable Irox Thin Film Via Mild Alkaline Solution Process for Neuron Stimulating Electrodes

SSRN

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SSRN 2023年

作者： Tso, Kuang-Chih Chan, Tzu-Ying Yu, Tsung-Chun Pan, Shih-Chin Chu, Chao-Yi Chen, San-Yuan Lee, Jyh-Fu Ohta, Jun Wu, Pu-Wei Chen, Po-Chun Graduate Program of Accelerator Light Source National Yang Ming Chiao Tung University Hsinchu300 Taiwan Division of Materials Science Graduate School of Science and Technology Nara Institute of Science Technology Takayama Ikoma Nara8916-5 Japan Department of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu300 Taiwan Institute of Materials Science and Engineering National Taipei University of Technology Taipei106 Taiwan National Synchrotron Radiation Research Center Hsinchu300 Taiwan

We demonstrate a unique chemical formula to deposit hydrous iridium oxide thin film on a platinum-coated polyimide substrate. In a mild alkaline solution, the iridium (III) precursor undergoes the ligand exchange and hydrolysis reaction to become the iridium (III) dimers that are physically adsorbed on the substrate for subsequent heterogeneous condensation and growth of amorphous hydrous iridium oxide thin film. Both UV-Vis and X-ray absorption spectroscopy (XAS) are employed to determine the reaction steps involved. The chemical nature and crystallinity of the hydrous iridium oxide thin film are investigated by XAS, X-ray photon spectroscopy, and X-ray diffraction. The hydrous iridium oxide thin film reveals an impressive normalized charge storage capacity (CSC) of 0.3 mC/cm2-nm and a low impedance (80.5 Ω) at 1k Hz. In addition, in bending test of 3,000 cycles, the hydrous iridium oxide thin film retains 91.2% of its initial normalized CSC without any physical crack and delamination. The cell viability test suggests negligible bio-toxicity. Our results provide a solid evidence of fabricating a robust flexible electrode for neural interfaces for potential use in implantable electronic devices. © 2023, The Authors. All rights reserved.

关键词： Iridium compounds

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Spontaneous spin chirality reversal and competing phases in the topological magnet EuAl4

arXiv

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arXiv 2024年

作者： Vibhakar, A.M. Khalyavin, D.D. Orlandi, F. Moya, J.M. Lei, S. Morosan, E. Bombardi, A. Diamond Light Source Ltd Harwell Science and Innovation Campus Didcot OxfordshireOX11 0DE United Kingdom ISIS facility Rutherford Appleton Laboratory-STFC Chilton DidcotOX11 0QX United Kingdom Applied Physics Graduate Program Smalley-Curl Institute Rice University HoustonTX77005 United States Department of Physics and Astronomy Rice University HoustonTX77005 United States Hong Kong University of Science and Technology Clear Water Bay Hong Kong

We demonstrate the spontaneous reversal of spin chirality in a single crystal sample of the inter-metallic magnet EuAl4. We solve the nanoscopic nature of each of the four magnetically phases of EuAl4 using resonant magnetic x-ray scattering, and demonstrate all four phases order with single-k incommensurate magnetic modulation vectors. Below 15.4 K the system forms a spin density modulated spin structure where the spins are orientated in the ab plane perpendicular to the orientation of the magnetic propagation vector. Below 13.2 K a second spin density wave orders with moments aligned parallel to the c-axis, such that the two spin density wave orders coexist. Below 12.2 K a magnetic helix of a single chirality is stabilised across the entire sample. Below 10 K the chirality of the magnetic helix reverses, and the sample remains a single chiral domain. Concomitant with the establishment of the helical magnetic ordering is the lowering of the crystal symmetry to monoclinic, as evidenced the formation of uniaxial charge and spin strip domains. A group theoretical analysis demonstrates that below 12.2 K the symmetry lowers to polar monoclinic, which is necessary to explain the observed asymmetry in the chiral states of the magnetic helix and the spin chiral reversal. We find that in every magnetically ordered phase of EuAl4 the in-plane moment is perpendicular to the orientation of the magnetic propagation vector, which we demonstrate is favoured by magnetic dipolar interactions. Copyright © 2024, The Authors. All rights reserved.

关键词： Aluminum alloys

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Manipulation of the nanoscale heliconical structure of a twist-bend nematic material with polarized light

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Physical Review Research 2020年第3期2卷 032004(R)-032004(R)页

作者： C. Feng J. Feng R. Saha Y. Arakawa J. Gleeson S. Sprunt C. Zhu A. Jákli Chemical Physics Interdisciplinary Program Advanced Materials and Liquid Crystal Institute Kent State University Kent Ohio 44242 USA Advanced Light Source Lawrence Berkeley National Lab Berkeley California 94720 USA Department of Physics Kent State University Kent Ohio 44242 USA Department of Applied Chemistry and Life Science Graduate School of Engineering Toyohashi University of Technology Toyohashi 441-8580 Japan

The effect of polarized violet light on the alignment and the heliconical pitch of a liquid crystal dimer containing both sulfur atoms and an azo linkage has been studied by tender resonant x-ray scattering. The results provide evidence of the manipulation of the nanoscale heliconical structure by polarized light. In addition to the bulk alignment of the heliconical nanostructure, the value of the heliconical pitch can be varied as well. After turning the light on, an increase of the pitch is observed in two steps. The increase with a subsecond timescale is attributed to the reduced heliconical order related to trans-cis photoisomerization. This is followed by a smaller increase over a 10-s timescale, which is likely related to the annihilation of defects. After turning the light off, the pitch first decreases within a few seconds to a value larger than the original (before illumination), and then relaxes further on a much longer (hours) timescale.

关键词： Chiral symmetry Dynamical phase transitions Twist deformation

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Ubiquitous Flat Bands in a Cr-based Kagome Superconductor

arXiv

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arXiv 2024年

作者： Guo, Yucheng Wang, Zehao Xie, Fang Huang, Yuefei Gao, Bin Oh, Ji Seop Wu, Han Liu, Zhaoyu Ren, Zheng Fang, Yuan Biswas, Ananya Zhang, Yichen Yue, Ziqin Hu, Cheng Jozwiak, Chris Bostwick, Aaron Rotenberg, Eli Hashimoto, Makoto Lu, Donghui Kono, Junichiro Chu, Jiun-Haw Yakobson, Boris I. Birgeneau, Robert J. Si, Qimiao Dai, Pengcheng Yi, Ming Department of Physics and Astronomy Rice University HoustonTX77005 United States Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Department of Materials Science and NanoEngineering Rice University HoustonTX77005 United States Department of Physics University of California BerkeleyCA94720 United States Department of Physics University of Washington Washington98105 United States Applied Physics Graduate Program Smalley-Curl Institute Rice University HoustonTX77005 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Smalley-Curl Institute Rice University HoustonTX77005 United States Department of Materials Science and NanoEngineering Rice University HoustonTX77005 United States

In the quest for novel quantum states driven by topology and correlation, kagome lattice materials have garnered significant interest due to their distinctive electronic band structures, featuring flat bands (FBs) arising from the quantum destructive interference of the electronic wave function. The tuning of the FBs to the chemical potential would lead to the possibility of liberating electronic instabilities that lead to emergent electronic orders. Despite extensive studies, direct evidence of FBs tuned to the chemical potential and their participation in emergent electronic orders have been lacking in bulk quantum materials. Here using a combination of Angle-Resolved Photoemission Spectroscopy (ARPES) and Density Functional Theory (DFT), we reveal that the low-energy electronic structure of the recently discovered Cr-based kagome metal superconductor CsCr3Sb5 is dominated by a pervasive FB in close proximity to, and below the Fermi level. A comparative analysis with orbital-projected DFT and polarization dependence measurement uncovers that an orbital-selective renormalization mechanism is needed to reconcile the discrepancy with the DFT calculations, which predict the FB to appear 200 meV above the Fermi level. Furthermore, we observe the FB to shift away from the Fermi level by 20 meV in the low-temperature density wave-ordered phase, highlighting the role of the FB in the emergent electronic order. Our results reveal CsCr3Sb5 to stand out as a promising platform for further exploration into the effects of FBs near the Fermi level on kagome lattices, and their role in emergent orders in bulk quantum materials. © 2024, CC BY.

关键词： Density functional theory

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Two-step electronic response to magnetic ordering in a van der Waals ferromagnet

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Physical Review B 2024年第4期109卷 045416-045416页

作者： Han Wu Jian-Xin Zhu Lebing Chen Matthew W. Butcher Ziqin Yue Dongsheng Yuan Yu He Ji Seop Oh Bin Gao Jianwei Huang Shan Wu Cheng Gong Yucheng Guo Sung-Kwan Mo Jonathan Denlinger Donghui Lu Makoto Hashimoto Matthew B. Stone Alexander I. Kolesnikov Songxue Chi Junichiro Kono Andriy H. Nevidomskyy Robert J. Birgeneau Pengcheng Dai Ming Yi Department of Physics and Astronomy and Rice Center for Quantum Materials Rice University Houston Texas 77005 USA Theoretical Division Los Alamos National Laboratory Los Alamos New Mexico 87545 USA Center for Integrated Nanotechnologies Los Alamos National Laboratory Los Alamos New Mexico 87545 USA Department of Physics University of California at Berkeley Berkeley California 94720 USA Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston Texas 77005 USA Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley California 94720 USA National Institute for Materials Science 1-1 Namiki Tsukuba Ibaraki 305-0044 Japan Department of Applied Physics Yale University New Haven Connecticut 06511 USA Department of Electrical and Computer Engineering and Quantum Technology Center University of Maryland College Park Maryland 20742 USA Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California 94720 USA Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park California 94025 USA Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA Department of Electrical and Computer Engineering Rice University Houston Texas 77005 USA Smalley-Curl Institute Rice University Houston Texas 77005 USA Department of Material Science and Nanoengineering Rice University Houston Texas 77005 USA Department of Materials Science and Engineering University of California Berkeley California 94720 USA

The two-dimensional material Cr2Ge2Te6 is a member of the class of insulating van der Waals (vdW) magnets. Here, using high resolution angle-resolved photoemission spectroscopy in a detailed temperature dependence study, we identify a clear response of the electronic structure to a dimensional crossover in the form of two distinct temperature scales marking onsets of modifications in the electronic structure. Specifically, we observe Te p-orbital-dominated bands to undergo changes at the Curie transition temperature TC while the Cr d-orbital-dominated bands begin evolving at a higher temperature scale. Combined with neutron scattering, density functional theory calculations, and Monte Carlo simulations, we find that the electronic system can be consistently understood to respond sequentially to the distinct temperatures at which in-plane and out-of-plane spin correlations exceed a characteristic length scale. Our findings reveal the sensitivity of the orbital-selective electronic structure for probing the dynamical evolution of local moment correlations in vdW insulating magnets.

关键词： Electronic structure Magnetic order Magnetic phase transitions Van der Waals systems Angle-resolved photoemission spectroscopy

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Spectral evidence for unidirectional charge density wave in detwinned BaNi2As2

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Physical Review B 2023年第8期108卷 L081104-L081104页

作者： Yucheng Guo Mason Klemm Ji Seop Oh Yaofeng Xie Bing-Hua Lei Luca Moreschini Cheng Chen Ziqin Yue Sergey Gorovikov Tor Pedersen Matteo Michiardi Sergey Zhdanovich Andrea Damascelli Jonathan Denlinger Makoto Hashimoto Donghui Lu Chris Jozwiak Aaron Bostwick Eli Rotenberg Sung-Kwan Mo Rob G. Moore Junichiro Kono Robert J. Birgeneau David J. Singh Pengcheng Dai Ming Yi Department of Physics and Astronomy Rice University Houston Texas 77005 USA Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California 94720 USA Department of Physics University of California Berkeley California 94720 USA Department of Physics and Astronomy University of Missouri Columbia Missouri 65211 USA Materials Science Division Lawrence Berkeley National Laboratory Berkeley California 94720 USA Department of Physics University of Oxford Oxford OX1 3PU United Kingdom Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston Texas 77005 USA Canadian Light Source Inc. 44 Innovation Boulevard Saskatoon SK S7N 2V3 Canada Department of Physics and Astronomy University of British Columbia Vancouver British Columbia V6T 1Z1 Canada Quantum Matter Institute University of British Columbia Vancouver British Columbia V6T 1Z4 Canada Max Planck Institute for Chemical Physics of Solids Nöthnitzer Straße 40 01187 Dresden Germany Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park California 94025 USA Materials Science and Technology Division Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA Department of Electrical and Computer Engineering Rice University Houston Texas 77005 USA Smalley-Curl Institute Rice University Houston Texas 77005 USA Department of Materials Science and NanoEngineering Rice University Houston Texas 77005 USA Department of Chemistry University of Missouri Columbia Missouri 65211 USA

In the iron-based superconductors, unconventional superconductivity emerges in proximity to intertwined electronic orders consisting of an electronic nematic order and a spin density wave (SDW). Recently, BaNi2As2, like its well-known iron-based analog BaFe2As2, has been discovered to host a symmetry-breaking structural transition but coupled to a unidirectional charge density wave (CDW) instead of SDW, providing a novel platform to study intertwined orders. Here, through a systematic angle-resolved photoemission spectroscopy study combined with a detwinning B1g uniaxial strain, we identify distinct spectral evidence of band evolution due to the structural transition as well as CDW-induced band folding. In contrast to the nematicity and spin density wave in BaFe2As2, the structural and CDW order parameters in BaNi2As2 are observed to be strongly coupled and do not separate in the presence of uniaxial strain. Furthermore, no nematic band splitting is resolved above the structural transition. Our measurements point to a likely lattice origin of the CDW order in BaNi2As2.

关键词： Charge density waves Nematic phase transition Iron-based superconductors Angle-resolved photoemission spectroscopy

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