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Carbon Monoxide Promotes the Catalytic Hydrogenation on Metal Cluster Catalysts

研究（英文） 2021年第1期 235-243页

作者： Ruixuan Qin Pei Wang Pengxin Liu Shiguang Mo Yue Gong Liting Ren Chaofa Xu Kunlong Liu Lin Gu Gang Fu Nanfeng Zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand National (&) Local Joint Engineering Research Center for Preparation Technology of Nanomaterials College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand National (&) Local Joint Engineering Research Center for Preparation Technology of Nanomaterials College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China College of Science Huazhong Agricultural University Wuhan 430070 China Institute of Physics Chinese Academy of Sciences Beijing 100190 China

Size effect plays a crucial role in catalytic *** highly dispersed ultrasmall clusters with a limited number of metal atoms are one candidate of the next generation catalysts that bridge the single-atom metal catalysts and metal ***,for the unfavorable electronic property and their interaction with the substrates,they usually exhibit sluggish *** advantage of the small size,their catalytic property would be mediated by surface binding *** combination of metal cluster coordination chemistry brings new *** poisoning is notorious for Pt group metal catalysts as the strong adsorption of CO would block the active *** this work,we will demonstrate that CO could serve as a promoter for the catalytic hydrogenation when ultrasmall Pd clusters are *** means of DFT calculations,we show that Pd?(n = 2-147)clusters display sluggish activity for hydrogenation due to the too strong binding of hydrogen atom and reaction intermediates thereon,whereas introducing CO would reduce the binding energies of vicinal sites,thus enhancing the hydrogenation ***,supported Pd2CO catalysts are fabricated by depositing preestablished[Pd2(μ-CO)2Cl4]2-clusters on oxides and demonstrated as an outstanding catalyst for the hydrogenation of *** promoting effect of CO is further verified experimentally by removing and reintroducing a proper amount of CO on the Pd cluster catalysts.

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Modeling Fluid Polyamorphism Through a Maximum-Valence Approach

arXiv

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arXiv 2021年

作者： Shumovskyi, Nikolay A. Longo, Thomas J. Buldyrev, Sergey V. Anisimov, Mikhail A. Department of Physics Boston University BostonMA02215 United States Institute for Physical Science and Technology University of Maryland College ParkMD20742 United States Department of Physics Yeshiva University New YorkNY10033 United States Department of Physics Boston University MA02215 United States Department of Chemical and Biomolecular Engineering Institute for Physical Science and Technology University of Maryland College ParkMD20742 United States

We suggest a simple model to describe polyamorphism in single-component uids using a maximum-valence approach. The model contains three types of interactions: i) atoms attract each other by van der Waals forces that generate a liquid-gas transition at low pressures, ii) atoms may form covalent bonds that induce association, and iii) bonded atoms attract or repel each other stronger than non-bonded atoms, thus generating liquid-liquid separation. As an example, we qualitatively compare this model with the behavior of liquid sulfur and show that condition (iii) generates a liquid-liquid phase transition in addition to the liquid-gas phase transition. © 2021, CC BY-NC-ND.

关键词： Van der Waals forces

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Diamine Surface Passivation and Post-Annealing Enhance Performance of Silicon-Perovskite Tandem Solar Cells

arXiv

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arXiv 2024年

作者： Taddei, Margherita Contreras, Hannah Doan, Hai-Nam McCarthy, Declan P. Seo, Seongrok Westbrook, Robert J.E. Graham, Daniel J. Datta, Kunal Carroy, Perrine Muñoz, Delfina Correa-Baena, Juan-Pablo Barlow, Stephen Marder, Seth R. Smith, Joel A. Snaith, Henry J. Ginger, David S. Department of Chemistry University of Washington SeattleWA98195 United States Department of Physics University of Oxford OxfordOX1 3PU United Kingdom Institute of Materials Science Technical University of Munich München85748 Germany Department of Chemistry University of Colorado-Boulder BoulderCO80309 United States Department of Bioengineering University of Washington SeattleWA98195 United States School of Materials Science and Engineering Georgia Institute of Technology North Ave NW AtlantaGA30332 United States Université Grenoble Alpes CEA Liten Campus Ines Le Bourget du Lac73375 France Renewable and Sustainable Energy Institute University of Colorado-Boulder BoulderCO80309 United States Department of Chemical and Biological Engineering and Materials Science Program University of Colorado-Boulder BoulderCO80309 United States Physical Sciences Division Physical and Computational Sciences Directorate Pacific Northwest National Laboratory RichlandWA99352 United States

We show that the use of 1,3-diaminopropane (DAP) as a chemical modifier at the perovskite/electron-transport layer (ETL) interface enhances the power conversion efficiency (PCE) of 1.7 eV bandgap FACs mixed-halide perovskite single-junction cells, primarily by boosting the open-circuit voltage (VOC) from 1.06 V to 1.15 V. Adding a post-processing annealing step after C60 evaporation, further improves the fill factor (FF) by 20% from the control to the DAP + post-annealing devices. Using hyperspectral photoluminescence microscopy, we demonstrate that annealing helps improve compositional homogeneity at the top and bottom interfaces of the solar cell, which prevents detrimental bandgap pinning in the devices and improves C60 adhesion. Using time-of-flight secondary ion mass spectrometry, we show that DAP reacts with formamidinium present near the surface of the perovskite lattice to form a larger molecular cation, 1,4,5,6-tetrahydropyrimidinium (THP) that remains at the interface. Combining the use of DAP and the annealing of C60 interface, we fabricate Si-perovskite tandems with PCE of 25.29%, compared to 23.26% for control devices. Our study underscores the critical role of chemical reactivity and thermal post-processing of the C60/Lewis-base passivator interface in minimizing device losses and advancing solar-cell performance of wide-bandgap mixed-cation mixed-halide perovskite for tandem application. © 2024, CC BY.

关键词： Perovskite

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Dynamic and Thermodynamic Origins of Motility-Induced Phase Separation

arXiv

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arXiv 2022年

作者： Su, Jie Cao, Zhiyu Wang, Jin Jiang, Huijun Hou, Zhonghuai Department of Chemical Physics & Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Anhui Hefei230026 China Center for Theoretical Interdisciplinary Sciences Wenzhou Institute University of Chinese Academy of Sciences Wenzhou325001 China Department of Chemistry and of Physics and Astronomy State University of New York of Stony Brook Stony BrookNY11794 United States

Active matter systems are inherently out of equilibrium and break the detailed balance (DB) at the microscopic scale, exhibiting vital collective phenomena such as motility-induced phase separation (MIPS). Here, we introduce a coarse-grained mapping method to probe DB breaking in the density-energy phase space, which allows us to reveal the dynamic and thermodynamic origins of MIPS based on nonequilibrium potential and flux landscape theory. Hallmarks of nonequilibrium properties are manifested by identifying the visible probability flux in the coarse-grained phase space. Remarkably, the flux for the system with the activity lower than the MIPS threshold tends to "tear up" the single potential well of the uniform-density phase to create two wells of phases with different densities, presenting directly that the nonequilibrium flux is the dynamic origin of MIPS. Moreover, we find that the obtained entropy production rate (EPR) of the system undergoes a transition from nearly independent of activity to increasing proportionally as activity increases after the single well is"teared up". The transition of EPR’s scaling behavior might provide a hint of the thermodynamic origin of MIPS in the coarse-grained space. Our findings propose a new route to explore the nonequilibrium nature of active systems, and provide new insights into dynamic and thermodynamic properties of MIPS. © 2022, CC BY.

关键词： Phase separation

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Ultrasensitive piezoelectric sensor based on two-dimensional Na2Cl crystals with periodic atom vacancies

arXiv

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arXiv 2024年

作者： Wang, Tao Fan, Yan Jiang, Jie Zhang, Yangyang Huang, Yingying Zhu, Liuyuan Zhan, Haifei Zhang, Chunli Peng, Bingquan Gu, Zhen Pan, Qiubo Wu, Junjie Chen, Junlang Li, Pei Zhang, Lei Chen, Liang Lü, Chaofeng Fang, Haiping School of Physical Science and Technology Ningbo University Ningbo315211 China Department of Optical Engineering Zhejiang A&F University Hangzhou311300 China Faculty of Mechanical Engineering & Mechanics Ningbo University Ningbo315211 China School of Physics East China University of Science and Technology Shanghai200237 China College of Civil Engineering and Architecture Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province Zhejiang University Hangzhou310027 China Department of Engineering Mechanics Zhejiang University Hangzhou310027 China Wenzhou Institute University of Chinese Academy of Sciences Zhejiang Wenzhou325000 China Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of Education East China University of Science and Technology Shanghai200237 China MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter School of Physics Xi’an Jiaotong University Xi’an710049 China School of Physics Zhejiang University Hangzhou310027 China

Pursuing ultrasensitivity of pressure sensors has been a long-standing goal. Here, we report a piezoelectric sensor that exhibits supreme pressure-sensing performance, including a peak sensitivity up to 3.5×106 kPa−1 in the pressure range of 1-100 mPa and a detection limit of less than 1 mPa, superior to the current state-of-the-art pressure sensors. These properties are attributed to the high percentage of periodic atom vacancies in the two-dimensional Na2Cl crystals formed within multilayered graphene oxide membrane in the sensor, which provides giant polarization with high stability. The sensor can even clearly detect the airflow fluctuations surrounding a flapping butterfly, which have long been the elusive tiny signals in the famous "butterfly effect". The finding represents a step towards next-generation pressure sensors for various precision applications. Copyright © 2024, The Authors. All rights reserved.

关键词： Pressure sensors

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Electrically tunable helicity of cholesteric heliconical superstructure [Invited]

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Chinese Optics Letters 2020年第8期18卷 22-27页

作者： Conglong Yuan Wenbin Huang Xiaoqian Wang Dong Shen Zhigang Zheng Department of Physics East China University of Science and TechnologyShanghai 200237China School of Optoelectronic Science and Engineering&Collaborative Innovation Center of Suzhou Nano Science and Technology Soochow UniversitySuzhou 215006China Advanced Materials and Liquid Crystal Institute and Chemical Physics Interdisciplinary Program Kent State UniversityKentOhio 44242USA

The dynamic manipulation of the helicity in a cholesteric helical superstructure could enable precise control over its physical and chemical properties, thus opening numerous possibilities for exploring multifunctional *** cholesteric material satisfies the sufficiently small bending elastic effect, an electrically induced deformation named the cholesteric heliconical superstructure is formed. Through theoretical and numerical analysis, we systematically studied the tunable helicity of the heliconical superstructure, including the evolution of the corresponding oblique angle and pitch length. To further confirm the optical properties, Berreman’s 4 × 4 matrix method was employed to numerically analyze the corresponding structure reflection under the dual stimuli of chirality and electric field.

关键词： cholesteric liquid crystal heliconical superstructure tunable reflection band electro-optical materials

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Metal-to-insulator transition inoxide semimetalsby anion doping

arXiv

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arXiv 2023年

作者： Hong, Haitao Zhang, Huimin Lin, Shan Dhas, Jeffrey A. Paudel, Binod Xu, Shuai Chen, Shengru Cui, Ting Fan, Yiyan Rong, Dongke Jin, Qiao Zhu, Zihua Du, Yingge Chambers, Scott A. Ge, Chen Wang, Can Zhang, Qinghua Jin, Kui-Juan Wang, Le Dong, Shuai Guo, Er-Jia Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China Department of Physics Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing100049 China Key Laboratory of Quantum Materials and Devices of Ministry of Education School of Physics Southeast University Nanjing211189 China Materials Science and Technology Division Oak Ridge National Laboratory Oak RidgeTN37831 United States Physical and Computational Sciences Directorate Pacific Northwest National Laboratory RichlandWA99354 United States School of Chemical Biological and Environmental Engineering Oregon State University CorvallisOR97331 United States Beijing Advanced Innovation Center for Materials Genome Engineering Department of Physical Chemistry University of Science and Technology Beijing Beijing100083 China Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory RichlandWA99354 United States Songshan Lake Materials Laboratory Dongguan Guangdong523808 China

Oxide semimetals exhibiting both nontrivial topological characteristics stand as exemplary parent compoundsand multiple degrees of freedom, offering great promise for the realization of novel electronic states. In this study, we present compelling evidence of profound structural and transport phase shifts in a recently uncovered oxide semimetal, SrNbO3,achieved through effective in-situanion ***, a remarkable increase in resistivity of more than threeorders of magnitude at room temperatureis observed uponnitrogen-doping. The extent of electronic modulation in SrNbO3is strongly correlated with the misfit strain, underscoring its phase instability to both chemical doping and crystallographic symmetry ***-principles calculations, we discern that elevating the level of nitrogen doping induces an upward shift in the conductive bands of SrNbO3-δNδ. Consequently, a transition from a metallic state to an insulating state becomes apparent as the nitrogen concentration reaches a threshold of 1/3. This investigation sheds light on the potential of anion engineering in oxide semimetals, offering pathways for manipulating their physical properties. These insights hold promise for future applications that harness these materials for tailored functionalities. © 2023, CC BY.

关键词： Degrees of freedom (mechanics)

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Anti-siting for stabilizing structure and modulating cationic/anionic redox reactions

引用

Energy Storage Materials 2024年 70卷

作者： Wang, Luyao Zhang, Chu Lin, Ting Chu, Hang Gao, Yurui Hu, Zhiwei Haw, Shu-Chih Chen, Chien-Te Kuo, Chang-Yang Li, Xiangfei Gai, Yuming Guo, Qinwen Meng, Ying Zhuang, Haoyu Shen, Xi Wang, Zhaoxiang Yu, Richeng Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China College of Material Science and Opto-Electronic Technology University of Chinese Academy of Sciences Beijing100190 China School of Physical Sciences University of Chinese Academy of Sciences Beijing100049 China Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and Technology Chinese Academy of Sciences Beijing100190 China Max Planck Institute for Chemical Physics of Solids Dresden01187 Germany National Synchrotron Radiation Research Center Hsinchu300092 Taiwan Department of Electrophysics National Yang Ming Chiao Tung University Hsinchu30010 Taiwan College of Electronic Engineering South China Agricultural University Guangzhou510642 China Songshan Lake Materials Laboratory Dongguan523808 China

The layered Mn-rich oxide cathode materials with oxygen redox activity are highly appealing in sodium-ion (Na-ion) batteries because of their high energy density and low cost. However, the applications of such materials are hindered by issues such as low Mn redox potential and irreversible phase transformation. Rational modulation of the ordering of the transition metal (TM) layer can inhibit the constraints and stabilize the anionic redox reactions. Herein we introduce stable Li/Mn anti-siting in the TM layer of P2-type Na0.6Li0.2Mn0.8O2 as a strategy to create abundant Mn sites and O sites that are inequivalent to the counterpart of each in the lattice, and thus to prompt the diverse Mn and O redox. The self-locking of the anti-siting energetically inhibits the P2-O2 phase transformation and the resultant structural degradations. In addition, such modulation activates more Mn in charge compensation at high potentials. As a result, this regulation increases the reversible capacity from 104.2 mAh g−1 to 153.7 mAh g−1 and enhances the cycling stability of Na0.6Li0.2Mn0.8O2. This anti-siting strategy offers a new solution to designing cathode materials with high structural stability and high energy density. © 2024 Elsevier B.V.

关键词： Sodium-ion batteries

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Experimental observation of one-dimensional motion of interstitial skyrmion in FeGe

arXiv

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arXiv 2022年

作者： Song, Dongsheng Wang, Weiwei Yu, Jie-Xiang Zhang, Peng Pershoguba, Sergey S. Yin, Gen Wei, Wensen Jiang, Jialiang Ge, Binghui Fan, Xiaolong Tian, Mingliang Rosch, Achim Zang, Jiadong Du, Haifeng Institutes of Physical Science and Information Technology Anhui University Hefei230601 China Anhui Key Laboratory of Condensed Matter Physics at Extreme Conditions High Magnetic Field Laboratory HFIPS Anhui Chinese Academy of Sciences Hefei230031 China School of Physical Science and Technology Soochow University Suzhou215006 China Key Laboratory for Magnetism and Magnetic Materials The Ministry of Education Lanzhou University Lanzhou730000 China Department of Physics and Astronomy University of New Hampshire DurhamNH03824 United States Department of Physics Georgetown University WashingtonDC20057 United States Science Island Branch of Graduate School University of Science and Technology of China Anhui Hefei230026 China School of Physics and Materials Science Anhui University Hefei230601 China Institute for Theoretical Physics University of Cologne Cologne50937 Germany Materials Science Program University of New Hampshire DurhamNH03824 United States

The interplay between dimensionality and topology manifests in magnetism via both exotic texture morphology and novel dynamics. A free magnetic skyrmion exhibits the skyrmion Hall effect under electric currents. Once it is confined in one-dimensional (1D) channels, the skyrmion Hall effect would be suppressed, and the current-driven skyrmion speed should be boosted by the non-adiabatic spin transfer torque β. Here, we experimentally demonstrate that stripes of a spatially modulated spin helix serve as natural 1D channels to restrict skyrmion. Using FeGe as a benchmark, an interstitial skyrmion is created by geometry notch and further moves steadily without the skyrmion Hall effect. The slope of the current-velocity curve for 1D skyrmion is enhanced almost by an order of magnitude owing to a large β in FeGe. This feature is also observed in other topological defects. Utilizing the 1D skyrmion dynamics would be a highly promising route to implement topological spintronic devices. © 2022, CC BY.

关键词： Germanium compounds

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Aggregation-induced emission luminogen for specific identification of malignant tumour in vivo

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science China Chemistry 2020年第3期63卷 393-397页

作者： Jianlei Shen Kun Tao Peilin Gu Chen Gui Dong Wang Zhenyu Tan Lihua Wang Zhiming Wang Anjun Qin Ben Zhong Tang Shisan Bao School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China Tongren Hospital School of MedicineShanghai Jiao Tong UniversityShanghai 200240China Discipline of Pathology Bosch Institute and School of Medical SciencesCharles Perkins CentreThe University of SydneyAustralia Division of Physical Biology CAS Key Laboratory of Interfacial Physics and TechnologyShanghai Synchrotron Radiation FacilityShanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800China Department of Chemistry HKUST Jockey Club Institute for Advanced StudyInstitute of Molecular Functional MaterialsDivision of Biomedical EngineeringState Key Laboratory of Molecular NeuroscienceDivision of Life ScienceThe Hong Kong University of Science and TechnologyHong KongChina State Key Laboratory of Luminescent Materials and Devices South China University of TechnologyGuangzhou 510640China

Colorectal cancer(CRC)is still a major killer,mainly due to the lack of early detection biomarker with sensitivity/*** histopathology is the gold standard approach in practice,but there are still some issues(false diagnosis and long waiting period).Aggregation-induced emission(AIE)is a novel photophysical phenomenon which has been widely utilized for biological imaging in vitro,including malignant cells,showing remarkable imaging contrast and enhanced emission in high concentrated ***,it is unclear if AIE dyes can identify malignant cells specifically in vivo.A great challenge for specific labeling of malignant cells is probably ascribed to the complex compositions in tumor ***,an AIE dye-based mitochondria-targeted histological staining strategy was employed to localize cancer and the metastatic track in the fresh colorectal *** novel approach holds great potential to revolutionize the clinical diagnosis and intervention for devastating malignancy.

关键词： aggregation-induced emission histological staining colorectal cancer

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