The Journal of Physical Chemistry C最新文献

{"title":"Computational Study on the Lifting of Aluminum Particles from a Hydroxyl-Terminated Polybutadiene Burning Surface","authors":"Yuxin Zhou, Michael R Zachariah","doi":"10.1021/acs.jpcc.4c08542","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c08542","url":null,"abstract":"The addition of aluminum particulates to polymer fuels is desired as a means to increase energy density. While nanosized aluminum has some attractive features with respect to its micrometer counterpart in terms of the burn rate, when incorporated into a fuel such as hydroxyl-terminated polybutadiene (HTPB), its release is often retarded, leading to crust formation on the fuel grain surface. Here, we undertake a molecular dynamics study to understand the size dependence of the polymer–particle interaction and how this impacts the size dependence of particle ejection. Comparing the interaction energy with the kinetic energy imparted to particles from the lifting force during polymer pyrolysis, we find that indeed, nanosized aluminum, due to its increased particle–polymer interaction binding energy, does not eject from the surface, while micrometer aluminum will. This is consistent with the experimental observation in a stagnation-flow burner. Further theoretical analysis indicated that replacing Al nanoparticles by nanosized Al/nitrocellulose (NC) mesoparticles may enhance the lifting of particles since the gas expansion from NC decomposition can generate sufficient kinetic energy to overcome the binding energy with the polymer.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"113 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561237","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}

{"title":"Effects of Structural Phase Transformation-Induced 2H/1T′ Interfaces in Group VI Transition-Metal Dichalcogenide Monolayers","authors":"Lei Yang, Yang Xia","doi":"10.1021/acs.jpcc.4c08391","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c08391","url":null,"abstract":"Transition-metal dichalcogenide monolayers have garnered significant attention due to their structural phase transformation properties. Phase engineering enables their application in the design and fabrication of advanced two-dimensional electronic devices. However, the existence of phase interfaces is inevitable in this situation, which may negatively impact the system performance. In this study, we employ geometrical analysis to systematically classify the 2H/1T′ interfaces formed during the 2H to 1T′ transition. We then derive a predictive equation for interfacial buckling based on elasticity theory, which is validated using density functional theory calculations. Additionally, we apply semiclassical Boltzmann transport theory to evaluate the electronic conductivity of different interfaces. By integrating these approaches, we assess the probability of the 2H/1T′ interface exhibiting varying electronic conductivities and interfacial buckling. Our results indicate that the 2H/1T′ interface is highly susceptible to interfacial buckling and typically demonstrates relatively poor electronic conductivity.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"57 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570120","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}

{"title":"Celebrating 10 Years of the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)","authors":"Zhihua Wu, Jian-Feng Li, Zhong-Qun Tian","doi":"10.1021/acs.jpcc.5c00704","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c00704","url":null,"abstract":"Published as part of <i>The Journal of Physical Chemistry C</i> special issue “Celebrating 10 Years of the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)”. The Collaborative Innovation Center of Chemistry for Energy Materials (<i>i</i>ChEM) was approved in October 2014, jointly by Xiamen University (XMU), Fudan University (FDU), the University of Science and Technology of China (USTC), and the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS). The mission of the consortium is to integrate key innovative elements from universities, research institutes, and enterprises both in China and abroad. In addition, <i>i</i>ChEM leverages the strengths in chemistry and materials sciences of the four member-institutions to further advance cutting-edge energy-related research while also training younger generations for research excellence by strengthening collaboration between the research community and industry. Over the past decade, <i>i</i>ChEM has focused on common scientific issues in energy chemistry by jointly tackling energy chemistry and energy material systems and introducing a number of core key technologies. Researchers at <i>i</i>ChEM focus on three main areas: the optimal utilization of carbon resources, chemical energy storage and conversion, and solar energy conversion chemistry. Investigations in these energy-oriented areas use a number of approaches: basic research in synthesis and fabrication, theory and simulation, and instrumentation and methodology. As a result, we are able to make advances in the approaches themselves, as well as in the aforementioned three research areas. To realize the new energy strategic objectives, <i>i</i>ChEM has adhered to the principle of “chemistry as the foundation, materials as the carrier, and energy as the goal”, addressing critical scientific issues in the development of petroleum alternatives. This approach has led to a series of original results that are both urgently needed by the country and recognized as world-class. In order to celebrate the 10th anniversary of the <i>i</i>ChEM, The Journal of Physical Chemistry C (JPC C), The Journal of Physical Chemistry Letters (JPCL), and ACS Energy Letters are publishing a joint Special Issue (SI). This SI, organized by the center’s directors, Zhong-Qun Tian (Xiamen Univ.), Dongyuan Zhao (Fudan Univ.), Can Li (DICP, CAS), and Jinlong Yang (USTC), brings together 37 articles on energy materials and chemistry. It is with great pride and reflection that we look back on a decade of groundbreaking research, collaboration, and innovation. <i>i</i>ChEM has grown into a world-class hub for scientific exploration, fostering multidisciplinary partnerships and pioneering advancements in energy materials chemistry. Since its inception, <i>i</i>ChEM has been driven by a vision to address the critical challenges facing our world’s energy future. Our researchers, drawn from diverse backgrounds and expertise, have w","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"8 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561240","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}

{"title":"Luminescent Erbium-Based Nanoparticles Synthesized by Pulsed Laser Ablation in Liquid","authors":"B. Almohammed, D. Barba, E. Haddad, R. Nechache, F. Rosei, F. Vetrone","doi":"10.1021/acs.jpcc.4c07101","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07101","url":null,"abstract":"Erbium and erbium oxide nanoparticles (Er-NPs) have been synthesized in deionized (DI) water using the green and environmentally friendly technique of pulsed laser ablation in liquid (PLAL), with laser fluence ranging from 2.5 to 20.9 J/cm². Owing to the careful examination of the nanoparticle morphology, crystal structure, and chemical composition, the occurrence of various growth regimes is evidenced. The size of the Er-NPs is found to increase with the laser fluence, and the formed nanoparticles are surrounded by a thin hydroxide layer of a few nanometers thickness, originating from water and chemical residues. The activation of 4f–4f optical transitions associated with trivalent Er³⁺ ions is promoted by the formation of erbium oxide. The Er-NPs having diameters lower than 100 nm are made of Er₂O₃, whereas Er-NPs of larger dimensions are made of an oxidized erbium oxide matrix containing a large amount of excess Er, the concentration of which increases gradually inside the Er-NPs. The formation of this graded Er/Er₂O₃ core–shell structure gives rise to a decrease in the Er visible photoluminescence emission. These findings shed light on the influence of the PLAL laser fluence on both the geometry and the composition of Er-NPs, as well as its consequence on their photoemission capacity, making them relevant for easy implementation with tunable properties in advanced photonics devices.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"11 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560907","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}

{"title":"Machine Learning-Guided Prediction of Activation Energies for Catalyst Design in the Water Gas Shift Reaction","authors":"José L. C. Fajín, Amit Kumar Halder, M. Natália D. S. Cordeiro","doi":"10.1021/acs.jpcc.4c08108","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c08108","url":null,"abstract":"The water gas shift (WGS) reaction is a critical process in various industrial applications, with its rate often governed by the activation energy of water dissociation on metal-based catalysts. In this work, we develop a machine learning model to predict the activation energy for water dissociation across diverse catalytic surfaces, including monometallic, bimetallic, and trimetallic surfaces, metallic nanotubes, and platinum nanoparticles. The model links activation energy to easily computable descriptors, such as adsorption energies or distances of the involved reaction species, derived from density functional theory (DFT) calculations. Our multilayer perceptron-based regression model demonstrates exceptional predictive accuracy. A Shapley additive explanation (SHAP) analysis discloses that all input variables contribute positively to the activation energy, with the adsorption energy of reaction products identified as the most influential feature. Remarkably, our model enables the prediction of activation energy for water dissociation and WGS on metal-based catalysts not included in the training set by simply DFT computing adsorption energies and distances, significantly reducing computational effort. This approach thus provides a powerful tool for the rapid screening and optimization of catalysts for the WGS reaction, paving the way for more efficient industrial processes.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"32 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561234","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}

{"title":"Revealing the Influence of Binding Motifs on Electron Transfer and Recombination Kinetics for CdSe Quantum Dots Functionalized with a Modified Viologen","authors":"Olivia F. Bird, Kenneth M. Drbohlav, Evan K. Gowdy, Faith A. Flinkingshelt, Lauren M. Pellows, Benjamin F. Hammel, Bradley W. Layne, Shane Ardo, Jenny Y. Yang, Kenneth A. Miller, Gordana Dukovic","doi":"10.1021/acs.jpcc.5c00740","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c00740","url":null,"abstract":"Anchoring of molecules to the surfaces of semiconductor nanocrystals (NCs) presents an opportunity to leverage the precise synthetic tunability of molecular function and the remarkable light harvesting properties of NCs to drive photochemical reactions. However, charge transfer between the two species depends not only on the energy level alignments but also on the details of their binding interactions, which are difficult to probe. Here, we characterize the binding between CdSe quantum dots (QDs) and a new phosphonated derivative of the electron acceptor methyl viologen, designed to attach to the QD surface via the phosphonate group. We use isothermal titration calorimetry to probe the thermodynamics of the QD–molecule interaction and use the parameters determined therein to analyze transient absorption spectroscopy measurements of forward and back electron transfer from QDs to the viologen. We find that the ligand-like phosphonate binding leads to an electron-transfer rate constant that is 3 orders of magnitude smaller than that for the face-on binding of the bipyridine ring of methyl viologen. Back electron transfer is also significantly slower in the derivative. Interestingly, a minor fraction of the phosphonated derivative also binds in the face-on configuration, with similar forward and back electron transfer kinetics as methyl viologen. Numerical simulations show that the ligand-like binding will lead to significantly improved quantum yields of photocatalysis over a wide range of reaction rates. By independently characterizing binding thermodynamics and charge transfer kinetics, this work reveals how the complexities underlying electron transfer at the NC<b>–</b>molecule interface determine photocatalytic outcomes. This work also represents a step toward controlling forward and back electron transfer kinetics via rational molecular design.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"13 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570122","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}

{"title":"Vibration Promotes Mass Transfer of Products in Photoelectrochemical Water Splitting by Enhancing Forced Convection","authors":"Tengfei Nie, Qiang Xu, Yonglu She, Xinyi Luo, Mengsha Wang, Liejin Guo","doi":"10.1021/acs.jpcc.4c08219","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c08219","url":null,"abstract":"Improving the productivity of photoelectrochemical water splitting hinges on discovering a viable method to facilitate bubble release from the surface of the photoelectrode, which, in turn, enhances the mass transfer of the resulting products. In this study, an experimental platform for photoelectrochemical water splitting to produce hydrogen by a coupled vibration system was built to realize the visualization of bubble behavior. By applying vibration to the electrode through a vibration exciter, this work explored how amplitude and frequency affect the photocurrent and geometric parameters during the bubble evolution process on the photoelectrode surface. Based on the expression of bubble coverage and gas evolution efficiency, mass transfer coefficients of gas products were deduced and calculated. The results showed that the increase in amplitude will increase the onset potential of nucleation, reducing the possibility of nucleation. Increasing the amplitude and frequency helps to release the bubbles from the electrode surface. For stationary electrodes, the mass transfer of gas products mainly depends on single-phase natural microconvection. For the vibrating electrode, macroscopic forced convection plays a dominant role. In this experiment, the average total mass transfer coefficient after applying vibration to the electrode can reach 11.16 × 10^–5 m/s, which is about 7.6 times the mass transfer coefficient under static conditions. Therefore, vibration can significantly improve the reaction efficiency and mass transfer during the water splitting process for hydrogen generation.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"131 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561235","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}

{"title":"Li-Salt of Adipic Acid Incorporated Flexible Poly(vinylidene fluoride) Composite for Piezoelectric Energy Harvester with Superior Energy Density Toward Self-Powered Traffic Monitoring System","authors":"Ananya Aishwarya, Suvankar Mondal, Akanksha Adaval, Titas Dasgupta, Arup R. Bhattacharyya","doi":"10.1021/acs.jpcc.4c07023","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07023","url":null,"abstract":"The development of the composite material based on poly(vinylidene fluoride) (PVDF) incorporating lithium salt of adipic acid (Li-AA) presents a promising avenue for sustainable and renewable energy generation via piezoelectric nanogenerators. In this study, PVDF/Li-AA composites were prepared through melt-mixing, followed by the fabrication of thin films using compression molding and solution casting techniques, with Li-AA concentration ranging from 1% to 10% by weight. Analysis via Fourier transform infrared spectroscopy (FTIR) confirmed hydrogen bonding interactions between −CF₂ moieties of PVDF and the acid functional groups of Li-AA. Additionally, FTIR analysis revealed that the solution-cast PVDF/Li-AA composite containing 10 wt % Li-AA exhibited the highest polar phase amount (∼ 65%) among all the composites, with remnant polarization of ∼4.2 × 10^–3 μC/cm² (50 Hz and 500 V). Furthermore, the solution cast PVDF/Li-AA composite film containing 10 wt % Li-AA achieved the highest piezoelectric coefficient (<i>d</i>₃₃ value ∼ 42 pm/V), indicating superior piezoelectric response. Energy harvesting devices fabricated using compression molded and solution-cast films demonstrated an output voltage of ∼80 and ∼100 V, respectively, obtained from PVDF/Li-AA composite containing 10 wt % Li-AA. Furthermore, devices fabricated with compression molded and solution-cast composite films containing 10 wt % Li-AA exhibited higher power densities of ∼80 and ∼100 μW/cm², respectively. Finally, PVDF/Li-AA composite film based self-powered speed sensor was fabricated for speed detection of the vehicles.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"36 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560905","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}

{"title":"77Se Solid-State NMR Investigation of Selenium Chemical Shift Tensors of Chalcogen Bonds in Selenadiazole Cocrystals","authors":"Tristan Georges, Jacynthe Beaudoin, Mubassira Rahman, Alireza Nari, Jeffrey S. Ovens, David L. Bryce","doi":"10.1021/acs.jpcc.4c07712","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07712","url":null,"abstract":"This study focuses on 3,4-dicyano-1,2,5-selenadiazole and substituted 2,1,3-benzoselenadiazole-based cocrystals synthesized via mechanochemical methods and characterized by a combination of X-ray diffraction and solid-state NMR spectroscopy. Eight new single-crystal structures are reported, revealing a variety of chalcogen bond (ChB) geometries and binding motifs that are found to promote low-dimensional molecular architectures. We find that ⁷⁷Se isotropic chemical shifts follow exponential decay or growth trends along with the ChB length, while also depending on the electrostatic contribution of the ChB donor. These trends are shown to be governed by changes to the intermediate selenium chemical shift tensor component, δ₂₂. Such behavior is further exploited to estimate ChB lengths in compounds unsuitable for single-crystal structure determination. This methodology highlights the utility of solid-state NMR as a powerful alternative for probing ChB interactions, particularly in systems where traditional crystallographic techniques are not applicable. The results offer critical physical insights into the origins of the selenium chemical shift tensors of ChB-based materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"47 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560908","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}

{"title":"Celebrating 10 Years of the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)","authors":"Zhihua Wu,&nbsp;Jian-Feng Li* and Zhong-Qun Tian*,&nbsp;","doi":"10.1021/acs.jpcc.5c0070410.1021/acs.jpcc.5c00704","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c00704https://doi.org/10.1021/acs.jpcc.5c00704","url":null,"abstract":"","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"129 9","pages":"4321–4322 4321–4322"},"PeriodicalIF":3.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143547776","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}