The Journal of Physical Chemistry C最新文献

Assessment of the Reproducibility of Experimental Results in Aqueous Alkaline Media Using Pt Electrodes

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-11 DOI: 10.1021/acs.jpcc.6c06513

Niusha Mouchani,Derek Esau,Gregory Jerkiewicz

{"title":"Assessment of the Reproducibility of Experimental Results in Aqueous Alkaline Media Using Pt Electrodes","authors":"Niusha Mouchani,Derek Esau,Gregory Jerkiewicz","doi":"10.1021/acs.jpcc.6c06513","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c06513","url":null,"abstract":"Research in interfacial electrochemistry and electrocatalysis requires establishing standard experimental procedures and conditions that ensure reproducibility and reliability of results. While standard procedures for experimental research employing Pt electrodes in aqueous acidic solutions were established ca. 50 years ago, similar benchmarks for aqueous alkaline media do not exist. In this contribution, cyclic voltammetry (CV) experiments are performed in the 0.05–1.40 V range using polycrystalline and monocrystalline platinum electrodes (Pt(poly) and Pt(POSSC)) in 0.50 M aqueous H2SO4 (a reference electrolyte solution) and 0.10 M aqueous NaOH (a studied electrolyte solution) to verify the systems’ cleanliness and to determine the electrodes’ electrochemically active surface area (Aecsa). Afterward, chronoamperometry (CA) measurements are conducted by holding the applied potential at 0.50 V for various holding times in the 30–1,800 s range, and then Aecsa is re-evaluated by CV experiments. The results demonstrate that unavoidable contamination, present even in the highest purity chemicals and water, adsorbs on the surface of the Pt electrodes and reduces their Aecsa. The reduction in Aecsa increases with increasing the holding time in CA measurements. Energy-dispersive X-ray (EDS) spectroscopy and X-ray photoelectron spectroscopy (XPS) analyses of the Pt(poly) and Pt(POSSC) electrodes reveal the presence of C and O-containing compounds in the case of aqueous H2SO4 solution and C, O, and Pb compounds in the case of aqueous NaOH solution. The results demonstrate the complementarity of electrochemical and surface science methods in assessing the cleanliness of electrode materials and highlight the need for rigorous experimental protocols that ensure reproducibility and reliability of experimental results.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"19 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374900","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Experimental and Theoretical Charge Density Study of Isonicotinamide Polymorphs

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-10 DOI: 10.1021/acs.jpcc.6c05509

Shagun Gogna,Debra J. Iskandar,Jonathan J. Du,Paul W. Groundwater,Jan-Willem C. Alffenaar,Jonathan C. Arnold,David E. Hibbs

{"title":"Experimental and Theoretical Charge Density Study of Isonicotinamide Polymorphs","authors":"Shagun Gogna,Debra J. Iskandar,Jonathan J. Du,Paul W. Groundwater,Jan-Willem C. Alffenaar,Jonathan C. Arnold,David E. Hibbs","doi":"10.1021/acs.jpcc.6c05509","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05509","url":null,"abstract":"Isonicotinamide is widely studied for its strong and directional hydrogen bonds, which play a critical role in crystal engineering and polymorphism. To address the absence of a quantitative charge density comparison for the two most studied isonicotinamide polymorphs (denoted 1a and 1b), this study maps the electron density distribution and topological properties of 1a and 1b, which differ in intermolecular connectivity, linking their respective H-bonding networks, intermolecular interaction strengths and lattice energetics within a single experimental and theoretical framework. High-resolution X-ray diffraction data were analyzed using the Hansen–Coppens multipole model. Topological parameters at bond critical points were evaluated to quantify hydrogen bonding, weak interactions, and electron density redistribution across the molecule. Both polymorphs exhibit well-defined hydrogen bonding networks dominated by N–H···N interactions, with bond strengths ranging from 6.48 to 35.5 kJ mol–1. Topological analysis revealed high electron densities and negative Laplacian values for covalent bonds, whereas the hydrogen-bond critical points exhibited positive Laplacian values consistent with closed-shell interactions. Notably, 1a shows stronger lattice stabilization (−114 kJ mol–1) compared to 1b (−82 kJ mol–1), indicating more efficient packing. By mapping the electron density topology and energy framework partitioning that distinguish the more stable P21/c form 1a from its less efficiently packed polymorph 1b (also P21/c), at the atomic level, this study provides a quantitative reference framework that can be used to predict and rationalize stability and solubility differences among the growing family of isonicotinamide-based pharmaceutical cocrystals.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"75 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Solid Solution Engineering via Zr Doping in the Pd/ZrInOx Catalyst Switches Reaction Pathways for Enhanced Methanol Production from CO2

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-10 DOI: 10.1021/acs.jpcc.6c05338

Zhefeng Li,Hao Li,Zhuo Chen,Yongbin Zhong,Wentao Du,Tongyun Zhang,Jingwen Xu,Shengxuan Luo,Yuxiang Mao,Rongxin Xia,Jun Cheng

{"title":"Solid Solution Engineering via Zr Doping in the Pd/ZrInOx Catalyst Switches Reaction Pathways for Enhanced Methanol Production from CO2","authors":"Zhefeng Li,Hao Li,Zhuo Chen,Yongbin Zhong,Wentao Du,Tongyun Zhang,Jingwen Xu,Shengxuan Luo,Yuxiang Mao,Rongxin Xia,Jun Cheng","doi":"10.1021/acs.jpcc.6c05338","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05338","url":null,"abstract":"The Pd/In2O3 catalyst is promising for CO2-to-methanol conversion, yet it is limited by poor stability and sluggish conversion of formate intermediates. Replacing the In2O3 support in Pd/In2O3 with an In2O3-based solid solution, such as ZrInOx, is an effective strategy to balance activity and stability. However, how the Zr species regulates the Pd/In2O3 catalyst, especially its effect on the reaction pathway, remains unclear. Herein, by introducing atomically dispersed Zr on the Pd/In2O3 catalyst, we demonstrate an electronic disparity strategy to tune the reaction pathway for efficient CO2-to-methanol production. Characterizations confirm that Zr promotes oxygen vacancy formation and enhances the dispersion of Pd nanoparticles. These enhance the electronic metal–support interaction between Pd and the support to accelerate the electron transfer from Pd to the support, thereby making the In sites more electron-rich and Pd more electron-deficient, as well as enhancing CO2 adsorption and H2 dissociation. Theoretical studies show that during the reaction, the In sites at the oxygen vacancy and Pd species work in synergy to induce cleavage of the C═O bond in CO2 and switch the formate pathway to the RWGS+CO* hydrogenation pathway. Consequently, the Pd/ZrInOx catalyst achieved an 18% CO2 conversion with 710 gMeOH kgcat–1 h–1 methanol space-time yield at 300 °C and 5 MPa. This work highlights the influence of the solid solution structure on the CO2 hydrogenation process.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"41 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374872","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Elucidation of Mg-Ion Diffusion Factors in Mg–O-Based Materials Using Machine-Learning Interatomic Potentials and Causal Analysis

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-10 DOI: 10.1021/acs.jpcc.6c04722

Keisuke Makino,Koichi Gocho,Haruka Okada,Naoto Tanibata,Hayami Takeda,Ryo Kobayashi,Masayuki Karasuyama,Masanobu Nakayama

{"title":"Elucidation of Mg-Ion Diffusion Factors in Mg–O-Based Materials Using Machine-Learning Interatomic Potentials and Causal Analysis","authors":"Keisuke Makino,Koichi Gocho,Haruka Okada,Naoto Tanibata,Hayami Takeda,Ryo Kobayashi,Masayuki Karasuyama,Masanobu Nakayama","doi":"10.1021/acs.jpcc.6c04722","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04722","url":null,"abstract":"Mg-ion batteries are promising next-generation energy-storage systems because Mg metal offers high volumetric capacity, abundant resources, and intrinsic safety. However, Mg2+ usually diffuses slowly in solids because of its strong interaction with surrounding anion frameworks and cation environments. Here, Mg–O-based candidate materials extracted from The Materials Project were investigated to clarify the compositional and structural factors governing Mg-ion diffusion. Representative materials were selected by clustering composition descriptors and structural descriptors derived from radial distribution functions (RDFs) and angular distribution functions (ADFs). High-throughput molecular dynamics simulations using an M3GNet-based machine-learning interatomic potential were then performed to construct a Mg-ion diffusion-coefficient data set. LightGBM regression, SHAP-based feature importance analysis, and nonlinear NOTEARS causal discovery were integrated to analyze the hierarchical relationships among descriptors and log D. The inferred causal structure indicates that Mg-ion diffusion is not governed by a single compositional factor. Instead, composition affects the short- and medium-range order of the oxygen framework, which regulates the local Mg environment and migration-pathway connectivity. Excessively close-packed and ordered oxygen frameworks restrict Mg-ion migration, whereas moderately disordered oxygen frameworks can promote continuous migration-accessible sites around Mg ions. These results suggest that Mg-ion-conducting oxides should be designed by controlling the oxygen framework and Mg local environment through host-cation selection, particularly using lightweight host materials containing d-block cations with sizes similar to that of Mg.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"9 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Thermal Activation under Electrochemical Conditions: CO and N2 Bond Dissociation on Co(B5)

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-10 DOI: 10.1021/acs.jpcc.6c06722

Mohd Riyaz,Alexander Bagger

{"title":"Thermal Activation under Electrochemical Conditions: CO and N2 Bond Dissociation on Co(B5)","authors":"Mohd Riyaz,Alexander Bagger","doi":"10.1021/acs.jpcc.6c06722","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c06722","url":null,"abstract":"In aqueous electrocatalytic environments, the protonation of stable *CO and *N2 to *COH/*CHO and *NNH is fundamentally challenged by the competing hydrogen evolution reaction (HER). In this context, direct dissociation of these molecules offers an alternative pathway, forming reactive *C or *N fragments that can be reduced further if surface bonding is not too strong. However, the strong C≡O and N≡N bonds make dissociation challenging under ambient electrochemical conditions, and the extent to which solvent, local field, and electrolyte ions can promote bond dissociation remains unclear. In this work, we quantify these dissociation pathways at a Co(B5) step site using density functional theory, implicit-solvent calculations, and explicit-solvent calculations using enhanced sampling with machine-learned interatomic potential (MLIP). Implicit-solvent calculations reveal only weak sensitivity to dielectric constant, dipole moment, and solvent radius, with barrier variations typically ≤0.1 eV. In contrast, the local H-bonding network in explicit-solvent simulations lowers the dissociation barrier by ∼0.3 eV relative to vacuum by stabilizing the dissociating atoms. Across different solvents and aqueous solutes, the barrier correlates qualitatively with hydrogen-bond donor strength, pKa, and the local H-coordination number near the transition-state region. Interfacial cations (Li+ and Cs+) modify the work function but do not significantly change the dissociation barrier compared with pure water, suggesting that solvent-mediated interactions dominate under the studied conditions.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"151 1 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Decoding Configurational Populations and Temperature of Flexible Chiral Molecules from Chiral Optical Spectra with Machine Learning

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-10 DOI: 10.1021/acs.jpcc.6c07271

Ruifang Gao,Zhiyuan Chen,Bingsuo Zou,Wenyong Su,Yongyou Zhang

{"title":"Decoding Configurational Populations and Temperature of Flexible Chiral Molecules from Chiral Optical Spectra with Machine Learning","authors":"Ruifang Gao,Zhiyuan Chen,Bingsuo Zou,Wenyong Su,Yongyou Zhang","doi":"10.1021/acs.jpcc.6c07271","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c07271","url":null,"abstract":"Quantitative determination of configurational populations in flexible chiral molecules is challenging due to spectral overlap, conformational averaging, and random noise. Here, we present a multitask residual network that integrates quantum chemical calculations, spectral simulation, and deep learning to achieve configurational inversion from spectroscopic data. As a proof-of-concept study, the neural network uses DFT-computed ultraviolet–visible absorption and electronic circular dichroism spectra as input to simultaneously predict the populations of configurational isomers and the thermodynamic temperature of the system. Demonstrated on the flexible chiral drug molecule labetalol, the method achieves high accuracy: under 10% spectral noise, the root-mean-square error for configurational populations is about 8.2%, and the temperature error is below 3.4 °C. The successful inversion demonstrates that machine learning can effectively bridge spectroscopic observables and statistical thermodynamics, providing a rapid, data-driven paradigm for resolving structural distributions in complex flexible chiral systems.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"20 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374870","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Evolution of Surface Intermediate Species in the Direct N2O-Mediated Conversion of Methane to Methanol over H+-Ferrierite nh2o直接介导甲烷在H+-铁素体上转化为甲醇过程中表面中间体的演化

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-09 DOI: 10.1021/acs.jpcc.6c04890

Miaomiao Wen,Alyssa McNarney,Bradley F. Chmelka,Magnus Skoglundh

{"title":"Evolution of Surface Intermediate Species in the Direct N2O-Mediated Conversion of Methane to Methanol over H+-Ferrierite","authors":"Miaomiao Wen,Alyssa McNarney,Bradley F. Chmelka,Magnus Skoglundh","doi":"10.1021/acs.jpcc.6c04890","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04890","url":null,"abstract":"The direct conversion of methane to methanol under mild conditions remains a central challenge in catalysis. In this study, we employ a series of ferrierite (FER) zeolite catalysts to investigate the surface species and acid-site characteristics associated with methane activation in the presence of N2O. In situ DRIFTS measurements reveal the formation of surface methoxy-related species on protonic ferrierite (H+-FER) at temperatures above 200 °C, with their spectral intensity increasing with reaction temperature. Variation of the parent NH4+-FER calcination temperature (450, 550 °C) and alkali-ion exchange (Na+, K+) demonstrates a correlation between methoxy formation and the presence and density of Brønsted acid sites. Importantly, H+-FER maintains methoxy stabilization up to 300 °C, exhibiting enhanced persistence of methoxy-related species at elevated temperatures, consistent with the influence of the confined FER pore environment on the stability of surface intermediates. Complementary solid-state NMR, NH3-TPD, XPS, and pyridine-desorption IR spectroscopy provide consistent evidence for the structural and acidic properties of the FER catalysts. Additional DRIFTS-MS experiments show that H2O exposure leads to the attenuation of surface methoxy-related bands and a transient methanol-related mass-spectrometric response, supporting the formation of methanol-related products from surface species generated during CH4 + N2O exposure. Overall, this study provides spectroscopic evidence linking the acid environment of H+-FER to the formation of surface methoxy-related species and highlights the potential role of zeolite confinement in stabilizing reactive surface intermediates during methane oxidation.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"14 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368356","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Understanding the Contrasting Effects of V vs Mn Doping on the OER Activity of Co3O4(001): A DFT+U Study V和Mn掺杂对Co3O4 OER活性影响的对比研究（001）：DFT+U研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-09 DOI: 10.1021/acs.jpcc.6c06330

Palani Muthu Kumar,Rossitza Pentcheva

{"title":"Understanding the Contrasting Effects of V vs Mn Doping on the OER Activity of Co3O4(001): A DFT+U Study","authors":"Palani Muthu Kumar,Rossitza Pentcheva","doi":"10.1021/acs.jpcc.6c06330","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c06330","url":null,"abstract":"Designing efficient electrocatalysts for clean energy conversion requires atomic-scale insight into the relationship between targeted surface modifications and catalytic performance. Using density functional calculations with an on-site Hubbard U term (DFT+U), we investigate the effect of Mn and V doping on the performance of Co3O4(001) as an anode material for the oxygen evolution reaction (OER). Our results show that Mn, which is preferentially incorporated at a surface octahedral site at both the B- and A-terminated Co3O4(001) surfaces, has a detrimental effect on the OER efficiency. In contrast, V, which also prefers a surface octahedral site at the B-layer termination, acquires a 5+ oxidation state and reduces the overpotential (η) of a Cooct reaction site from 0.48 to 0.43 V. Remarkably, at the A-termination, V is incorporated as V4+ in the subsurface layer, which reduces the overpotential at the tetrahedral Co site from 0.74 to 0.18 V. This enhancement in catalytic activity is attributed to the modification of the surface Cooct oxidation state from Co3+ (IS) to Co2+ prior to OER and its further variation during OER. This substantially reduces the binding energy of *OH and thereby the potential-determining step height by 0.56 eV. Taking into account implicit solvation increases the overpotential for both undoped and Mn-doped surfaces, whereas it marginally decreases the overpotential for the V-doped A-layer termination. The deprotonation of *OH to *O constitutes the potential-determining step for all investigated surface reaction sites, thereby positioning them on the right leg of the volcano plot, while η of the Cotet reaction site at the V-doped A-layer lies beyond the top of the volcano. These insights demonstrate how selective doping can be used as a promising strategy to tailor catalyst’s performance.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"6 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368359","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Building Metal–Oxygen Connectivity in Amorphous Iridium Oxide through Electrochemical Cycling in Acid 通过酸中电化学循环建立非晶态氧化铱金属-氧连通性

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-09 DOI: 10.1021/acs.jpcc.6c05130

Dongyoon Shin,Damith D. Lekamge,Boqiang Chen,Mikael Maraschin,Tianying Liu,James R. Wilkes,Andrew B. Maurer,Wei Li,Tyler J. Murray,Jinghua Guo,Joseph A. Gauthier,Dunwei Wang,Matthias M. Waegele

{"title":"Building Metal–Oxygen Connectivity in Amorphous Iridium Oxide through Electrochemical Cycling in Acid","authors":"Dongyoon Shin,Damith D. Lekamge,Boqiang Chen,Mikael Maraschin,Tianying Liu,James R. Wilkes,Andrew B. Maurer,Wei Li,Tyler J. Murray,Jinghua Guo,Joseph A. Gauthier,Dunwei Wang,Matthias M. Waegele","doi":"10.1021/acs.jpcc.6c05130","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05130","url":null,"abstract":"The development of oxygen evolution reaction (OER) catalysts has been hindered by the high overpotential requirements, challenges in catalyst stability, and the complexity of OER mechanisms. Under water oxidation conditions, multiple concurrent processes, such as catalyst dissolution and surface reconstruction, further complicate mechanistic understandings. One factor that makes studies of water oxidation mechanisms especially difficult is the dynamic nature of the catalytic structure under reaction conditions. Herein, we report the observation of a stabilization effect of an amorphous iridium oxide (IrOx) catalyst under water oxidation conditions. The effect was revealed to be caused by improved connectivity between neighboring Ir and O atoms on the surface. The reaction was found to proceed in parallel to the oxidation of H2O and was only observed under potentials above the onset of water oxidation. X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and density functional theory calculations further confirmed this understanding. The results shed light on the competing reaction pathways once an active metal center is activated and highlight the favorable outcomes by improved connectivity for water oxidation catalysis.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"4 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368358","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Near-Infrared Spectroscopic Identification of Ethylene Adsorption States on Ag+-Exchanged ZSM-5 Zeolites Ag+交换ZSM-5沸石上乙烯吸附态的近红外光谱鉴定

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-11-09 DOI: 10.1021/acs.jpcc.6c05527

Masato Takeuchi,Yutaku Yamao,Akihiro Mikuni,Masaya Matsuoka

{"title":"Near-Infrared Spectroscopic Identification of Ethylene Adsorption States on Ag+-Exchanged ZSM-5 Zeolites","authors":"Masato Takeuchi,Yutaku Yamao,Akihiro Mikuni,Masaya Matsuoka","doi":"10.1021/acs.jpcc.6c05527","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05527","url":null,"abstract":"Near-infrared (NIR) spectroscopy was applied to investigate the adsorption behavior of ethylene on ZSM-5 zeolites containing Na+, Ag+, and H+ sites. Ethylene adsorbed on Na+ and Ag+ sites could be distinguished by its characteristic NIR absorption band. Further, ethylene adsorbed on Brønsted acid sites was identified by the formation of protonated ethyl species. Temperature-dependent measurements also revealed distinct desorption behaviors associated with different cation sites. The applicability of NIR spectroscopy was further demonstrated by in situ monitoring of ethanol dehydration over Ag+0.5/H+0.5/ZSM-5. Upon ethanol adsorption, ethoxy species were first formed on Brønsted acid sites. At reaction temperatures above 200 °C, ethylene was generated and subsequently adsorbed on Ag+ sites, while water was simultaneously produced. In contrast, the characteristic C–H stretching bands of ethylene were not detected in the mid-IR region under the same reaction conditions. This may lead to the misleading conclusion that ethylene produced during ethanol dehydration is not adsorbed on the catalyst surface. These results demonstrate that NIR spectroscopy provides complementary information to conventional FT-IR measurements for investigating adsorption phenomena and catalytic reactions.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"6 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368355","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0