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Highly Dispersed Pd@ZIF-8 for Photo-Assisted Cross-Couplings and CO2to Methanol: Activity and Selectivity Insights

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Angewandte Chemie 2024年第48期136卷

作者： Vijay K. Velisoju Enrique V. Ramos-Fernández Rajesh Kancherla Rafia Ahmad Kuntal Pal Hend Mohamed Jose L. Cerrillo Mark J. Meijerink Luigi Cavallo Magnus Rueping Pedro Castaño Multiscale Reaction Engineering KAUST Catalysis Center (KCC) King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia KAUST Catalysis Center (KCC) King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia Laboratorio de Materiales Avanzados Departamento de Química Inorgánica—Instituto Universitario de Materiales de Alicante Universidad de Alicante Apartado 99 E-03080 Alicante Spain Chemical Engineering Program Physical Science and Engineering (PSE) Division KAUST Thuwal 23955-6900 Saudi Arabia

Our study unveils a pioneering methodology that effectively distributes Pd species within a zeolitic imidazolate framework-8 (ZIF-8). We demonstrate that Pd can be encapsulated within ZIF-8 as atomically dispersed Pd species that function as an excited-state transition metal catalyst for promoting carbon–carbon (C−C) cross-couplings at room temperature using visible light as the driving force. Furthermore, the same material can be reduced at 250 °C, forming Pd metal nanoparticles encapsulated in ZIF-8. This catalyst shows high rates and selectivity for carbon dioxide hydrogenation to methanol under industrially relevant conditions (250 °C, 50 bar): 7.46 mol methanol mol metal −1 h −1 and >99 %. Our results demonstrate the correlations of the catalyst structure with the performances at experimental and theoretical levels.

关键词： Pd@ZIF-8 CO2 hydrogenation Alkyl halide Excited-state Palladium Cross-coupling

Corrigendum to “Electric field emission in GdNiO 3 microflower” [Mater. Today Commun. 40 (2024) 109632]

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Materials Today Communications 2024年 41卷

作者： Subrata Karmakar Vanshree Parey Chetan D. Mistari Md Abdul Hamid Injamamul Hoque Emu Md Abdul Halim Gopal Sanyal Brahmananda Chakraborty M.A. More Ravi Droopad Ariful Haque Electrical Engineering Ingram School of Engineering Texas State University San Marcos TX 78666 USA Department of Chemical Engineering Indian Institute of Technology Kanpur Kanpur 208016 India Department of Physics Savitribai Phule Pune University Pune Maharashtra 411007 India Mechanical Metallurgy Division Bhabha Atomic Research Centre Trombay Mumbai 400085 India High Pressure and Synchrotron Radiation Physics Division Bhabha Atomic Research Centre Trombay Mumbai 400085 India Homi Bhabha National Institute Anushaktinagar Mumbai 400094 India Materials Science Engineering & Commercialization Program Texas State University San Marcos TX 78666 USA

Miniaturized Microarray-Format Digital ELISA Enabled by Lithographic Protein Patterning

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SSRN

SSRN 2023年

作者： Stephens, Andrew D. Song, Yujing McClellan, Brandon L. Su, Shiuan-Haur Xu, Sonnet Chen, Kevin Castro, Maria G. Singer, Benjamin H. Kurabayashi, Katsuo Department of Mechanical Engineering University of Michigan Ann ArborMI48109 United States Department of Neurosurgery University of Michigan Medical School Ann ArborMI48109 United States Department of Cell and Developmental Biology University of Michigan Medical School Ann ArborMI48109 United States Graduate Program in Immunology University of Michigan Medical School Ann ArborMI48109 United States Department of Biomedical Engineering University of Michigan Ann ArborMI48109 United States Rogel Cancer Center University of Michigan Ann ArborMI48109 United States Department of Internal Medicine Division of Pulmonary and Critical Care Medicine University of Michigan Ann ArborMI48109 United States Department of Electrical Engineering and Computer Science University of Michigan Ann ArborMI48109 United States Weil Institute for Critical Care Research and Innovation University of Michigan Ann ArborMI48109 United States

The search for reliable protein biomarker candidates is critical for early disease detection and treatment. However, current immunoassay technologies are failing to meet increasing demands for sensitivity and multiplexing. Here, the authors have created a highly sensitive protein microarray using the principle of single-molecule counting for signal amplification, capable of simultaneously detecting a panel of cancer biomarkers at sub-pg/mL levels. To enable this amplification strategy, the authors introduce a novel method of protein patterning using photolithography to subdivide addressable arrays of capture antibody spots into hundreds of thousands of individual microwells. This allows for the total sensor area to be miniaturized, increasing the total possible multiplex capacity. With the immunoassay realized on a standard 75x25 mm form factor glass substrate, sample volume consumption is minimized to © 2023, The Authors. All rights reserved.

关键词： Biomarkers

Discovery of a reversible redox-induced order-disorder transition in a 10-cation compositionally complex ceramic

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arXiv 2021年

作者： Zhang, Dawei Chen, Yan Feng, Tianshi Yu, Dunji An, Ke Chen, Renkun Luo, Jian Program of Materials Science and Engineering University of California San Diego La Jolla CA92093 United States Neutron Scattering Division Oak Ridge National Laboratory Oak RidgeTN38731 United States Department of Mechanical & Aerospace Engineering University of California San Diego La Jolla CA92093 United States Department of NanoEngineering University of California San Diego La Jolla CA92093 United States

This study discovers a reversible order-disorder transition (ODT) in a 10-cation compositionally complex ceramic, (Nd0.15Pr0.15Dy0.8Ho0.8Er0.8Ti0.2Yb0.1Hf0.1Zr0.1Nb0.8)O7-δ, induced via annealing in oxidized vs. reduced environments at 1600οC. Notably, the 10-cation oxide remains a homogenous single-phase high-entropy solid solution before and after the ODT in the pyrochlore vs. fluorite structure that can be quenched. In-situ neutron diffraction reveals the oxygen vacancy formation and atomic displacement during this ODT. The temperature dependence of thermal conductivity is altered by the ODT. This study reveals a new pathway to induce ODT via a redox transition to tailor the properties of compositionally complex fluorite-based oxides. © 2021, CC BY.

关键词： Entropy

Cavity-mediated superthermal phonon correlations in the ultrastrong coupling regime

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arXiv 2024年

作者： Kim, Dasom Hou, Jin Lee, Geon Agrawal, Ayush Kim, Sunghwan Zhang, Hao Bao, Di Baydin, Andrey Wu, Wenjing Tay, Fuyang Huang, Shengxi Chia, Elbert E.M. Kim, Dai-Sik Seo, Minah Mohite, Aditya D. Hagenmüller, David Kono, Junichiro Applied Physics Graduate Program Smalley–Curl Institute Rice University HoustonTX77005 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Department of Materials Science and NanoEngineering Rice University HoustonTX77005 United States Sensor System Research Center Korea Institute of Science and Technology Seoul02792 Korea Republic of Department of Physics and Astronomy Seoul National University Seoul08826 Korea Republic of Department of Chemical and Biomolecular Engineering Rice University Houston77005 United States Ulsan44919 Korea Republic of Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore637371 Singapore Smalley–Curl Institute Rice University HoustonTX77005 United States Rice Advanced Materials Institute Rice University HoustonTX77005 United States KU–KIST Graduate School of Converging Science and Technology Korea University Seoul02841 Korea Republic of Université de Strasbourg CNRS Strasbourg67200 France Department of Physics and Astronomy Rice University HoustonTX77005 United States

Phonons, or vibrational quanta, are behind some of the most fundamental physical phenomena in solids, including superconductivity, Raman processes, and broken-symmetry phases. It is therefore of fundamental importance to find ways to harness phonons for controlling these phenomena and developing novel quantum technologies. However, the majority of current phonon control techniques rely on the use of intense external driving fields or strong anharmonicities, which restricts their range of applications. Here, we present a scheme for controlling the intensity fluctuations in phonon emission at room temperature based on multimode ultrastrong light–matter coupling. The multimode ultrastrong coupling regime is achieved by coupling two optical phonon modes in lead halide perovskites to an array of nanoslots, which operates as a single-mode cavity. The extremely small mode volume of the nanoslots enables unprecedented coupling strengths in a cavity phonon-polariton system. In the far-detuned, low-cavity-frequency regime, we demonstrate that the nanoslot resonator mediates an effective coupling between the phonon modes, resulting in superthermal phonon bunching in thermal equilibrium, both within the same mode and between different modes. Experimental results are in good agreement with a multimode Hopfield model. Our work paves the way for the tailoring of phonons to modify charge and energy transport in perovskite materials, with potential applications in light-collecting or emitting devices. Copyright © 2024, The Authors. All rights reserved.

关键词： Perovskite

Gradient double-twisted Bouligand structural design for high impact resistance over a wide range of loading velocities

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science Advances 2025年第23期11卷 eadv2169页

作者： Shao-Meng Wen Weitao Gao Si-Chao Zhang Jun Pang Chen Cui Huai-Ling Gao Zhijun Zheng Si-Ming Chen Shu-Hong Yu New Cornerstone Science Laboratory Department of Chemistry Institute of Biomimetic Materials & Chemistry Anhui Engineering Laboratory of Biomimetic Materials Division of Nanomaterials & Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei 230026 China. CAS Key Laboratory of Mechanical Behavior and Design of Materials Department of Modern Mechanics University of Science and Technology of China Hefei 230027 China. Institute of Innovative Materials Department of Chemistry Department of Materials Science and Engineering Shenzhen Key Laboratory of Sustainable Biomimetic Materials Guangming Advanced Research Institute of Sustech Southern University of Science and Technology Shenzhen 518055 China.

Structural materials for protective applications are exposed to complex environments including impacts under a wide range of loading velocities. Bioinspired Bouligand-type structural materials show high impact resistance under quasi-static and low-velocity impacts. However, their protective performance under high-velocity impact is lacking investigation. Herein, we expand the Bouligand-type structure family by synergistically considering structural design and compositional regulation and highlight a double-twisted Bouligand structure with gradient composition (DT-Bou-G) for enhancing impact resistance under a wide range of loading velocities. As one demonstration, the DT-Bou-G structural material was fabricated by multimaterial fused deposition with stiff polylactic acid and soft thermoplastic polyurethane as raw materials. Experimental investigations show its superior impact-resistant capability under multiple loading velocities (0.5 millimeters per minute, 2.1 meters per second, 4.3 meters per second, and 120 meters per second). Finite element simulations further prove the mechanical result and reveal the underlying mechanisms. The DT-Bou-G structure will inspire the design of engineering protective materials capable of withstanding complex working conditions.

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Bipolar conduction and giant positive magnetoresistance in doped metallic titanium oxide heterostructures

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arXiv 2021年

作者： Huang, Ke Wang, Tao Jin, Mengjia Wu, Liang Wang, Junyao Floria Li, Shengyao Qi, Dong-Chen Cheng, Shuying Li, Yangyang Chen, Jingsheng He, Xiaozhong Li, Changjian Pennycook, Stephen J. Wang, X. Renshaw Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University 21 Nanyang Link 637371 Singapore Institute of Fluid Physics CAEP P. O. Box 919-106 Mianyang621900 China College of Physics and Information Engineering Institute of Micro-Nano Devices & Solar Cells Fuzhou University Fuzhou350108 China School of Material Science and Engineering Kunming University of Science and Technology Yunnan Kunming650093 China Singapore269734 Singapore ARC Centre of Excellence in Future Low-Energy Electronics Technologies School of Chemistry Physics Mechanical Engineering Queensland University of Technology BrisbaneQLD4001 Australia Department of Materials Science and Engineering National University of Singapore 117575 Singapore School of Electrical and Electronic Engineering Nanyang Technological University 50 Nanyang Ave 639798 Singapore

Empowering conventional materials with unexpected magnetoelectric properties is appealing to the multi-functionalization of existing devices and the exploration of future electronics. Recently, owing to its unique effect in modulating a matter's properties, ultra-small dopants, e.g. H, D, and Li, attract enormous attention in creating emergent functionalities, such as superconductivity, and metal-insulator transition. Here, we report an observation of bipolar conduction accompanied by a giant positive magnetoresistance in D-doped metallic Ti oxide (TiOxDy) films. To overcome the challenges in intercalating the D into a crystalline oxide, a series of TiOxDy were formed by sequentially doping Ti with D and surface/interface oxidation. Intriguingly, while the electron mobility of the TiOxDy increases by an order of magnitude larger after doping, the emergent holes also exhibit high mobility. Moreover, the bipolar conduction induces a giant magnetoresistance up to 900% at 6 T, which is ~6 times higher than its conventional phase. Our study paves a way to empower conventional materials in existing electronics and induce novel electronic phases. © 2021, CC BY.

关键词： Metal insulator boundaries

Corrigendum to “Reaction kinetics for high pressure hydrogen oxy-combustion in the presence of high levels of H 2 O and CO 2 ” [Combust. Flame 247 (2023) 112498]

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Combustion and Flame 2024年 266卷

作者： Ashkan Beigzadeh Mohammed Alabbad Dapeng Liu Khalid Aljohani Khaiyom Hakimov Touqeer Anwar Kashif Kourosh Zanganeh Eric Croiset Aamir Farooq Natural Resources Canada (NRCan) CanmetENERGY-Ottawa (CE-O) 1 Haanel Dr. Ottawa ON K1A 1M1 Canada Department of Chemical Engineering University of Waterloo 200 University Avenue West Waterloo ON N2L 3G1 Canada Clean Combustion Research Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Thuwal 23955 Saudi Arabia Department of Mechanical Engineering College of Engineering in Al-Kharj Prince Sattam Bin Abdulaziz University Al-Kharj 11942 Saudi Arabia

Bulk-plasmon-mediated free-electron radiation beyond the conventional formation time

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arXiv 2022年

作者： Tay, Fuyang Lin, Xiao Shi, Xihang Chen, Hongsheng Kaminer, Ido Zhang, Baile Interdisciplinary Center for Quantum Information State Key Laboratory of Modern Optical Instrumentation ZJUHangzhou Global Science and Technology Innovation Center College of Information Science and Electronic Engineering Zhejiang University Hangzhou310027 China Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Applied Physics Graduate Program Smalley–Curl Institute Rice University HoustonTX77005 United States International Joint Innovation Center The Electromagnetics Academy Zhejiang University Zhejiang University Haining314400 China Department of Electrical Engineering Technion-Israel Institute of Technology Haifa32000 Israel Jinhua Institute of Zhejiang University Zhejiang University Jinhua321099 China Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University 637371 Singapore Centre for Disruptive Photonic Technologies Nanyang Technological University 637371 Singapore

Free-electron radiation is a fundamental photon emission process that is induced by fast-moving electrons interacting with optical media. Historically, it has been understood that, just like any other photon emission process, free-electron radiation must be constrained within a finite time interval known as the "formation time", whose concept is applicable to both Cherenkov radiation and transition radiation, the two basic mechanisms describing radiation from a bulk medium and from an interface, respectively. Here we reveal an alternative mechanism of free-electron radiation far beyond the previously defined formation time. It occurs when a fast electron crosses the interface between vacuum and a plasmonic medium supporting bulk plasmons. While emitted continuously from the crossing point on the interface — thus consistent with the features of transition radiation — the extra radiation beyond the conventional formation time is supported by a long tail of bulk plasmons following the electron’s trajectory deep into the plasmonic medium. Such a plasmonic tail mixes surface and bulk effects, and provides a sustained channel for electron-interface interaction. These results also settle the historical debate in Ferrell radiation, regarding whether it is a surface or bulk effect, from transition radiation or plasmonic oscillation. Copyright © 2022, The Authors. All rights reserved.

关键词： Plasmonics