The Journal of Physical Chemistry C最新文献_第9页

Formation and Coexistence of Metastable Phases during Solidification of Single AuGe Nanoparticles: An In Situ TEM Study

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-11 DOI: 10.1021/acs.jpcc.4c06444

O. Khshanovska, W. Salamon, A. Kryshtal

{"title":"Formation and Coexistence of Metastable Phases during Solidification of Single AuGe Nanoparticles: An In Situ TEM Study","authors":"O. Khshanovska, W. Salamon, A. Kryshtal","doi":"10.1021/acs.jpcc.4c06444","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06444","url":null,"abstract":"Understanding phase transformations in binary alloy nanoparticles is an important scientific and technological problem. We tackled the challenge by experimentally studying the solidification pathways of single AuGe nanoparticles on Si3N4 substrate using in situ TEM techniques. The nanoparticles with sizes of 100–160 nm were slowly cooled from temperatures below and above the liquidus, enabling visualization of solidification pathways of liquid and partly molten alloy on the same AuGe nanoparticle in a TEM. Consequently, the crystalline structure, size, and composition of equilibrium and metastable phases formed in solidifying nanoparticles of near-eutectic (28 at. % Ge), hypo-eutectic (25 at. % Ge), and hyper-eutectic (38 at. % Ge) compositions were determined. We found a nonclassical solidification pathway of near-eutectic and hypo-eutectic composition AuGe nanoparticles. Solidification of highly undercooled nanoparticles occurred over a temperature range rather than at a single temperature. The heterogeneous nucleation process governed the onset solidification temperature, while the thermodynamic stability of the undercooled liquid defined the terminal temperature. It was shown that the number of phases coexisting in a single nanoparticle during the solidification depended on its composition and initial phase state, reaching a maximum of four phases. Thus, the liquid phase, fcc Au, hcp Au, and Ge coexisted in nanoparticles of hypo-eutectic composition in the temperature range of 260–210 °C. For the first time, a single-crystalline hexagonal Au phase was observed in liquid AuGe nanoparticles. Thermodynamic analysis showed that hcp Au is the equilibrium phase of the nucleus during the solidification of undercooled AuGe nanoparticles.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"15 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805105","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

Application of Advanced Characterization Techniques for Lithium Iron Phosphate: Paving the Way for an In-Depth Understanding of Operation and Fading Mechanisms

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-11 DOI: 10.1021/acs.jpcc.4c05992

Chao Wang, Wenjie Wu, Jinxia Wang, Hanbing Liu, Junyuan Xu, Limin Guo, Zhangquan Peng

{"title":"Application of Advanced Characterization Techniques for Lithium Iron Phosphate: Paving the Way for an In-Depth Understanding of Operation and Fading Mechanisms","authors":"Chao Wang, Wenjie Wu, Jinxia Wang, Hanbing Liu, Junyuan Xu, Limin Guo, Zhangquan Peng","doi":"10.1021/acs.jpcc.4c05992","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c05992","url":null,"abstract":"The exploitation and application of advanced characterization techniques play a significant role in understanding the operation and fading mechanisms as well as the development of high-performance energy storage devices. Taking lithium iron phosphate (LFP) as an example, the advancement of sophisticated characterization techniques, particularly operando/in situ ones, has led to a clearer understanding of the underlying reaction mechanisms of LFP, driving continuous improvements in its performance. This Review provides a systematic summary of recent progress in studying LFP by using a wide range of advanced characterization techniques. Based on the principles and functions, two types of characterization techniques, bulk and surface/interface studies, and the corresponding application in understanding the bulk phase transition and the surface/interface reaction mechanisms of LFP are introduced. Additionally, the limitations of current research methods, the controversial viewpoints, as well as the suggestions for the future research directions are also addressed for inspiring further developments in related systems.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"10 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805099","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

High-Performance Self-Powered Photodetectors Based on the MnS/MoS2 Heterojunction with Smooth Interfacial Band Bending

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-11 DOI: 10.1021/acs.jpcc.4c05548

Kunle Li, Chaojie Xie, Tong Chen, Weijie Li, Shaoxiong Du, Yibin Yang, Lili Tao, Zhaoqiang Zheng, Xing Feng, Yu Zhao

{"title":"High-Performance Self-Powered Photodetectors Based on the MnS/MoS2 Heterojunction with Smooth Interfacial Band Bending","authors":"Kunle Li, Chaojie Xie, Tong Chen, Weijie Li, Shaoxiong Du, Yibin Yang, Lili Tao, Zhaoqiang Zheng, Xing Feng, Yu Zhao","doi":"10.1021/acs.jpcc.4c05548","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c05548","url":null,"abstract":"Self-powered photodetectors operate without external power sources, offering potential as critical components in next-generation smart systems that function independently, wirelessly, and sustainably. Enhancing the photoresponse of self-driven devices to light is crucial. In this work, a type-II heterojunction of MnS/MoS2 is rationally designed and fabricated without interfacial abrupt band bending using nonlayered MnS and layered MoS2. The discrepancy in the Fermi level between MnS and MoS2 flakes, revealed by Kelvin probe force microscope and first-principles calculations, is as small as 30 and 60.6 meV, respectively, forming smooth band bending at the heterojunction interface and facilitating the separation of photoinduced electron–hole pairs. As a result, the MnS/MoS2 heterojunction exhibits exceptional performance as a self-powered photodetector, with a photoresponsivity of 1.31 A W–1 and an external quantum efficiency of 316% at zero bias under 532 nm laser irradiation. Additionally, the photodetectors demonstrate broadband detection in the visible range with a maximal photoresponsivity of 11.58 A W–1 and a response time of 20/30 ms, outperforming the component materials MoS2 and MnS. The strategy of band engineering demonstrated in this work may provide a useful guideline for designing high-performance self-powered photodetectors.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"21 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809482","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

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-11 DOI: 10.1021/acs.jpcc.4c06882

Pavel Malakhovsky, Mikhail Erofeev, Mikhail Artemyev

{"title":"Charge-Related Spectral Shift of Localized Surface Plasmon Resonance in Silver Nanoplates Induced by Deprotonation and Complexation of Surface Carboxyl Groups with Metal Cations","authors":"Pavel Malakhovsky, Mikhail Erofeev, Mikhail Artemyev","doi":"10.1021/acs.jpcc.4c06882","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06882","url":null,"abstract":"We investigated the spectral shift of localized surface plasmon resonance (LSPR) in a monolayer of mercaptopropionic-acid-stabilized silver nanoplates induced by deprotonation or complexation of surface carboxyl groups with metal cations in an aqueous solution. The deprotonation-induced LSPR red shift of about 10 nm in magnitude linearly depends on the degree of protonation of the carboxyl groups, while complexation with divalent or trivalent cations induces an additional red shift. We apply a simple model to establish a correlation between LSPR spectral shifts and pH, the stability constants of metal–carboxylate complexes, and the type and concentration of metal cations in the solution. Unlike complexation with metal cations, electrostatic adsorption of cationic macromolecules (polyethylenimine and trypsin) induces only a minor spectral shift due to incomplete compensation of the surface negative charges. Our results pave the way for the development of new optical chemical sensors based on the charge-related spectral shift of the LSPR in colloidal plasmonic nanoparticles.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"117 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809543","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

First-Principles Investigation of Surface pKa and the Behavior of Acids at Aqueous–Metal Interfaces

IF 3.3 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-10 DOI: 10.1021/acs.jpcc.4c0655410.1021/acs.jpcc.4c06554

Basil Raju Karimadom, Dan Meyerstein*, Amir Mizrahi and Haya Kornweitz*,

{"title":"First-Principles Investigation of Surface pKa and the Behavior of Acids at Aqueous–Metal Interfaces","authors":"Basil Raju Karimadom, Dan Meyerstein*, Amir Mizrahi and Haya Kornweitz*, ","doi":"10.1021/acs.jpcc.4c0655410.1021/acs.jpcc.4c06554","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06554https://doi.org/10.1021/acs.jpcc.4c06554","url":null,"abstract":"Several computational methods were reported for the accurate determination of pKa values in a solvent medium, but the research on surfaces and interfaces is limited. This study reports a new method for accurately determining the surface pKa (*pKa) of acids on surfaces. The *pKa is defined as the function of the adsorption energies of neutral acids and their deprotonated form. In the suggested method, the estimated proton solvation-free energy value is not required, a fact that increases the accuracy of the results. The *pKa values of various organic and inorganic acids on the (111) surfaces of Ag, Au, and Pt were evaluated. The results are validated with available experimental results on various surface coverage ratios. The results point out that weak acids adsorbed on the metal-aqueous interface are orders of magnitude stronger acids than those in homogeneous solutions. The shift of the pKas is largest on platinum. These results are of major importance in electrochemistry and heterogeneous catalysis.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"128 50","pages":"21572–21580 21572–21580"},"PeriodicalIF":3.3,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpcc.4c06554","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850308","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Extracting Residence Times of Nitric Oxide on Graphene through Combination of Time-of-Flight and Velocity Map Imaging

IF 3.3 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-10 DOI: 10.1021/acs.jpcc.4c0634210.1021/acs.jpcc.4c06342

Thomas Greenwood, and , Sven P. K. Koehler*,

引用次数: 0

Novel Heterostructure as a H2-Evolving Photocatalyst Boosting the Z-Scheme Overall Water Splitting Performance under Visible Light Irradiation

IF 3.3 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-10 DOI: 10.1021/acs.jpcc.4c0660710.1021/acs.jpcc.4c06607

Yu Qi, Yuanfeng Zhu, Tengfeng Xie and Fuxiang Zhang*,

{"title":"Novel Heterostructure as a H2-Evolving Photocatalyst Boosting the Z-Scheme Overall Water Splitting Performance under Visible Light Irradiation","authors":"Yu Qi, Yuanfeng Zhu, Tengfeng Xie and Fuxiang Zhang*, ","doi":"10.1021/acs.jpcc.4c0660710.1021/acs.jpcc.4c06607","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06607https://doi.org/10.1021/acs.jpcc.4c06607","url":null,"abstract":"Tantalum nitride (Ta3N5) has been widely investigated as an extremely promising photocatalyst or photoanode for solar water splitting, but its performance is blocked by inefficient charge separation regardless of using a one-step or two-step excitation method. Here, we demonstrate significantly enhanced proton reduction on the particulate Ta3N5 photocatalyst with an effort for the promotion of charge separation via forming a solid solution-based heterostructure composite. One-pot nitridation was adopted to synthesize this novel heterostructure, which is composed of Ta3N5 and BaZrO3–BaTaO2N solid solution. The as-obtained composite (BaZrO3–BaTaO2N/Ta3N5) is found to exhibit superior charge separation and transfer ability compared with Ta3N5 and BaZrO3–BaTaO2N. As a result, the visible-light-driven Z-scheme overall water splitting (OWS) activity using the optimal BaZrO3–BaTaO2N/Ta3N5 composite as the H2-evolving photocatalyst can be promoted by about 20 times. This work not only gives the first example to fabricate heterostructures based on solid solution for enhanced charge separation but also offers a new avenue to improve the photocatalytic OWS performance of Ta3N5.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"128 50","pages":"21302–21309 21302–21309"},"PeriodicalIF":3.3,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842132","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

Extracting Residence Times of Nitric Oxide on Graphene through Combination of Time-of-Flight and Velocity Map Imaging 通过飞行时间和速度图成像相结合提取一氧化氮在石墨烯上的停留时间

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-10 DOI: 10.1021/acs.jpcc.4c06342

Thomas Greenwood, Sven P. K. Koehler

引用次数: 0

CO2 Desorption Dynamics Reveal Structure Insensitivity in Formate Decomposition on Copper Surfaces

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-10 DOI: 10.1021/acs.jpcc.4c06596

Jiamei Quan, Takahiro Kondo, Junji Nakamura

{"title":"CO2 Desorption Dynamics Reveal Structure Insensitivity in Formate Decomposition on Copper Surfaces","authors":"Jiamei Quan, Takahiro Kondo, Junji Nakamura","doi":"10.1021/acs.jpcc.4c06596","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06596","url":null,"abstract":"The formation of formate (HCOOa) adsorbate from CO2 and H2 on Cu catalysts, one of the most important elementary steps in methanol synthesis, is known to exhibit structure-insensitive kinetics and thermally nonequilibrium dynamics. In contrast, the kinetics of formate decomposition, the reverse reaction of formate formation, differs significantly across various Cu surfaces in terms of activation energy. The decomposition mechanism and its structure sensitivity remain unclear. In this study, we investigated the structure-dependent dynamics of formate decomposition by analyzing the angular distributions of CO2 and H2 desorbed from Cu(111), Cu(110), and Cu(100) surfaces under ultrahigh vacuum conditions. All CO2 angular distributions, measured between 400 and 500 K, were sharply collimated along the surface normal, following an identical function of cos8 θ, regardless of surface structure, formate coverage, or the presence of adsorbed oxygen. This lack of structure sensitivity can be attributed to the nearly identical local structure of the transition state (TS) on all Cu surfaces and the presence of monodentate, rather than bidentate, formate just before the TS. The results of this study align with previous molecular beam experiments in which structure-insensitive dynamics were observed during formate formation. In those experiments, hot CO2 gas molecules directly reacted with H adatoms via an Eley–Rideal-type mechanism, leading to the formation of monodentate formate. Our findings underscore the critical role of monodentate formate in CO2 hydrogenation over Cu-based catalysts, particularly in methanol synthesis.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"28 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797853","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

CO2 Desorption Dynamics Reveal Structure Insensitivity in Formate Decomposition on Copper Surfaces

IF 3.3 3区化学

The Journal of Physical Chemistry C Pub Date : 2024-12-10 DOI: 10.1021/acs.jpcc.4c0659610.1021/acs.jpcc.4c06596

Jiamei Quan, Takahiro Kondo and Junji Nakamura*,

{"title":"CO2 Desorption Dynamics Reveal Structure Insensitivity in Formate Decomposition on Copper Surfaces","authors":"Jiamei Quan, Takahiro Kondo and Junji Nakamura*, ","doi":"10.1021/acs.jpcc.4c0659610.1021/acs.jpcc.4c06596","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06596https://doi.org/10.1021/acs.jpcc.4c06596","url":null,"abstract":"The formation of formate (HCOOa) adsorbate from CO2 and H2 on Cu catalysts, one of the most important elementary steps in methanol synthesis, is known to exhibit structure-insensitive kinetics and thermally nonequilibrium dynamics. In contrast, the kinetics of formate decomposition, the reverse reaction of formate formation, differs significantly across various Cu surfaces in terms of activation energy. The decomposition mechanism and its structure sensitivity remain unclear. In this study, we investigated the structure-dependent dynamics of formate decomposition by analyzing the angular distributions of CO2 and H2 desorbed from Cu(111), Cu(110), and Cu(100) surfaces under ultrahigh vacuum conditions. All CO2 angular distributions, measured between 400 and 500 K, were sharply collimated along the surface normal, following an identical function of cos8 θ, regardless of surface structure, formate coverage, or the presence of adsorbed oxygen. This lack of structure sensitivity can be attributed to the nearly identical local structure of the transition state (TS) on all Cu surfaces and the presence of monodentate, rather than bidentate, formate just before the TS. The results of this study align with previous molecular beam experiments in which structure-insensitive dynamics were observed during formate formation. In those experiments, hot CO2 gas molecules directly reacted with H adatoms via an Eley–Rideal-type mechanism, leading to the formation of monodentate formate. Our findings underscore the critical role of monodentate formate in CO2 hydrogenation over Cu-based catalysts, particularly in methanol synthesis.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"128 50","pages":"21438–21446 21438–21446"},"PeriodicalIF":3.3,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842134","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