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Mapping the Complete Photocycle that Powers a Large Stokes Shift Red Fluorescent Protein

Angewandte Chemie 2022年第5期135卷

作者： Dr. Ziyu Wang Dr. Ya Zhang Dr. Cheng Chen Dr. Ruixue Zhu Dr. Jiaming Jiang Prof. Tsu-Chien Weng Prof. Quanjiang Ji Prof. Yifan Huang Prof. Chong Fang Prof. Weimin Liu School of Physical Science and Technology ShanghaiTech University 201210 Shanghai China Contribution: Data curation (equal) Formal analysis (lead) Investigation (equal) Methodology (equal) Resources (supporting) Visualization (lead) Writing - original draft (equal) Writing - review & editing (supporting) University of Chinese Academy of Sciences 100049 Beijing China Contribution: Data curation (supporting) Investigation (supporting) Methodology (equal) Resources (supporting) Writing - original draft (supporting) Department of Chemistry Oregon State University 153 Gilbert Hall 97331 Corvallis OR USA Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Validation (supporting) Visualization (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Validation (supporting) Contribution: Investigation (supporting) Validation (supporting) Contribution: Data curation (supporting) Resources (supporting) Supervision (supporting) Validation (supporting) Contribution: Data curation (supporting) Resources (equal) Supervision (supporting) Validation (supporting) Contribution: Data curation (supporting) Funding acquisition (supporting) Resources (equal) Software (lead) Validation (supporting) Visualization (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Funding acquisition (equal) Investigation (supporting) Project administration (supporting) Resources (supporting) Supervision (supporting) Validation (supporting) Visualization (equal) Writing - review & editing (lead) Contribution: Conceptualization (lead) Data curation (equal) Funding acquisition (lead) Investigation (supporting) Methodology (lead) Project administration (lead) Resources (equal) Supervision (lead) Validation (supporting) Writing - original draft (equal) Writing - review & editing (supporting)

Large Stokes shift (LSS) red fluorescent proteins (RFPs) are highly desirable for bioimaging advances. The RFP mKeima, with coexisting cis- and trans -isomers, holds significance as an archetypal system for LSS emission due to excited-state proton transfer (ESPT), yet the mechanisms remain elusive. We implemented femtosecond stimulated Raman spectroscopy (FSRS) and various time-resolved electronic spectroscopies, aided by quantum calculations, to dissect the cis - and trans -mKeima photocycle from ESPT, isomerization, to ground-state proton transfer in solution. This work manifests the power of FSRS with global analysis to resolve Raman fingerprints of intermediate states. Importantly, the deprotonated trans -isomer governs LSS emission at 620 nm, while the deprotonated cis -isomer's 520 nm emission is weak due to an ultrafast cis -to- trans isomerization. Complementary spectroscopic techniques as a table-top toolset are thus essential to study photochemistry in physiological environments.

关键词： Chromophore Isomerization Excited- and Ground-State Proton Transfer Femtosecond Raman Spectroscopy Large Stokes Shift Red Fluorescent Proteins

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Cover Image, Volume 140, Issue 9

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Journal of Applied Polymer Science 2023年第9期140卷

作者： Pirada Sudprasert Shotaro Kariya Kenji Ogino Suwabun Chirachanchai Shinji Kanehashi Contribution: Formal analysis (lead) Investigation (lead) Visualization (lead) Writing - original draft (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Supervision (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Supervision (supporting) Writing - original draft (supporting) Writing - review & editing (equal) Contribution: Conceptualization (lead) Funding acquisition (lead) Investigation (equal) Methodology (equal) Project administration (lead) Resources (lead) Supervision (lead) Writing - original draft (supporting) Writing - review & editing (lead)

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Distinguishing Protein Chemical Topologies Using Supercharging Ion Mobility Spectrometry-Mass Spectrometry

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Angewandte Chemie 2023年第51期135卷

作者： Jiyeon Lee Dahye Im Yajie Liu Jing Fang Xibao Tian Minsu Kim Prof. Wen-Bin Zhang Prof. Jongcheol Seo Department of Chemistry Pohang University of Science and Technology (POSTECH) 77 Cheongam-ro Nam-gu Pohang 37673 Gyeonsangbuk-do (Republic of Korea Contribution: Data curation (lead) Formal analysis (equal) Visualization (lead) Writing - original draft (lead) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (equal) Visualization (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry & Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University Beijing 100871 P. R. China Contribution: Resources (equal) Contribution: Data curation (supporting) Validation (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (equal) Project administration (supporting) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (lead) Project administration (lead) Validation (lead) Writing - review & editing (lead)

A technique combining ion mobility spectrometry-mass spectrometry (IMS-MS) and supercharging electrospray ionization (ESI) has been demonstrated to differentiate protein chemical topology effectively. Incorporating as many charges as possible into proteins via supercharging ESI allows the protein chains to be largely unfolded and stretched, revealing their hidden chemical topology. Different chemical topologies result in differing geometrical sizes of the unfolded proteins due to constraints in torsional rotations in cyclic domains. By introducing new topological indices, such as the chain-length-normalized collision cross-section (CCS) and the maximum charge state ( z M ) in the extensively unfolded state, we were able to successfully differentiate various protein chemical topologies, including linear chains, ring-containing topologies (lasso, tadpole, multicyclics, etc.), and mechanically interlocked rings, like catenanes.

关键词： Mass Spectrometry Protein Engineering Proteins

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Spin-Phonon Interactions Induced Anomalous Thermal Conductivity in Nickel (Ii) Oxide

SSRN

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SSRN 2023年

作者： Sun, Qiyang Hou, Songrui Wei, Bin Su, Yaokun Ortiz, Victor Sun, Bo Lin, Jiao Y.Y. Smith, Hillary Danilkin, Sergey Abernathy, Douglas L. Wilson, Richard Li, Chen Mechanical Engineering University of California Riverside RiversideCA92521 United States Materials Science and Engineering University of California Riverside RiversideCA92521 United States Henan Key Laboratory of Materials on Deep-Earth Engineering School of Materials Science and Engineering Henan Polytechnic University Jiaozuo454000 China Tsinghua-Berkeley Shenzhen Institute Guangdong Provincial Key Laboratory of Thermal Management Engineering and Materials TSIGS Tsinghua University Shenzhen518055 China Neutron Data Analysis and Visualization Division Oak Ridge National Laboratory Oak RidgeTN37830 United States Department of Physics and Astronomy Swarthmore College SwarthmorePA19081 United States Australian Centre for Neutron Scattering Australian Nuclear Science and Technology Organization Lucas HeightsNSW2234 Australia Neutron Scattering Division Oak Ridge National Laboratory Oak RidgeTN37830 United States

Nickel (II) oxide is a prominent candidate for spintronic and spin-caloritronic applications operating at room temperature. Although there are extensive studies on nickel oxide, the roles of magnon- and spin-phonon interactions on thermal transport are not well understood. In the present work, the relationship between spin-phonon interactions and thermal transport is investigated by performing inelastic neutron scattering, time-domain thermoreflectance thermal conductivity measurements, and atomistic thermal transport calculations. Inelastic neutron scattering measurements of the magnon lifetime imply that magnon thermal conductivity is trivial, and so heat is conducted only by phonons. Time-domain thermoreflectance measurements of the thermal conductivity vs. temperature follow T-1.47 in the antiferromagnetic phase. This temperature dependence cannot be explained by phonon-isotope and phonon-defect scattering or phonon softening. Instead, we attribute this to magnon-phonon scattering and spin-induced dynamic symmetry breaking. The spin-phonon interactions are saturated in the paramagnetic phase and lead to a weaker temperature dependence of T-1.00 at 550-700 K. These results reveal the importance of spin-phonon interactions on lattice thermal transport, shedding light on the engineering of functional antiferromagnetic spintronic and spin-caloritronic materials through these interactions. © 2023, The Authors. All rights reserved.

关键词： Nickel oxide

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Reversing Free-Electron Transfer of MoS2+xCocatalyst for Optimizing Antibonding-Orbital Occupancy Enables High Photocatalytic H2Evolution

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Angewandte Chemie 2023年第25期135卷

作者： Duoduo Gao Pinsi Deng Dr. Jianjun Zhang Prof. Liuyang Zhang Prof. Xuefei Wang Prof. Huogen Yu Prof. Jiaguo Yu State Key Laboratory of Silicate Materials for Architectures and School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology 430070 Wuhan P. R. China Contribution: Investigation (lead) Methodology (lead) Software (lead) Visualization (lead) Writing - original draft (lead) Contribution: Formal analysis (lead) Software (equal) Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 430074 Wuhan P. R. China Contribution: Data curation (lead) Project administration (lead) Contribution: Data curation (lead) Software (equal) Contribution: Conceptualization (lead) Funding acquisition (lead) Resources (lead) Supervision (lead) Validation (lead) Visualization (lead) Contribution: Conceptualization (lead) Resources (lead) Supervision (equal) Validation (lead)

The interaction between a co-catalyst and photocatalyst usually induces spontaneous free-electron transfer between them, but the effect and regulation of the transfer direction on the hydrogen-adsorption energy of the active sites have not received attention. Herein, to steer the free-electron transfer in a favorable direction for weakening S−H ads bonds of sulfur-rich MoS 2+ x , an electron-reversal strategy is proposed for the first time. The core–shell Au@MoS 2+ x cocatalyst was constructed on TiO 2 to optimize the antibonding-orbital occupancy. Research results reveal that the embedded Au can reverse the electron transfer to MoS 2+ x to generate electron-rich S (2+δ)− active sites, thus increasing the antibonding-orbital occupancy of S−H ads in the Au@MoS 2+ x cocatalyst. Consequently, the increase in the antibonding-orbital occupancy effectively destabilizes the H 1s-p antibonding orbital and weakens the S−H ads bond, realizing the expedited desorption of H ads to rapidly generate a lot of visible H 2 bubbles. This work delves deep into the latent effect of the photocatalyst carrier on cocatalytic activity.

关键词： Antibonding Orbitals Co-Catalysts Electron Reversal Photocatalysis Sulfur–Hydrogen Bonds

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Integrating Chemical Pre-Potassiation with Pre-Modulated KF-Rich Electrolyte Interfaces for Dual-Carbon Potassium Ion Hybrid Capacitor

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Angewandte Chemie 2023年第9期135卷

作者： Yong Qian Bei Wu Yang Li Zhen Pan Dr. Shuai Feng Dr. Ning Lin Prof. Yitai Qian Hefei National Laboratory for Physical Sciences at the Microscale Department of Applied Chemistry University of Science and Technology of China Hefei 230026 P. R. China Contribution: Conceptualization (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Contribution: Software (equal) Visualization (lead) Contribution: Data curation (equal) Resources (equal) College of Chemistry and Chemical Engineering Taishan University Shandong 271021 P. R. China Contribution: Resources (equal) Visualization (equal) Contribution: Funding acquisition (lead) Writing - review & editing (lead) Contribution: Funding acquisition (equal)

Herein, a chemical pre-potassiation strategy via simultaneously treating both glucose derived carbon (GDC) anode and commercial activated carbon (CAC) cathode in potassium-naphthalene-tetrahydrofuran solution is developed for potassium ion hybrid capacitor (PIHC). Combined with in situ and ex situ characterizations, a radical reaction between pre-potassiation reagent and carbon electrodes is confirmed, which not only deactivates electrochemical irreversible sites, but also promotes to pre-form a uniform and dense KF-rich electrolyte film on the electrodes. As a result, the pre-potassiation treatment presents multiple advantages: (I) the initial Coulombic efficiency (CE) of the GDC anode increases from 45.4 % to 84.0 % with higher rate capability; (II) the CAC cathode exhibits the improved cycling CEs and stability due to the enhanced resistance to electrolyte oxidation at 4.2 V; (III) the assembled PIHC achieves a high energy density of 172.5 Wh kg −1 with cycling life over 10000 cycles.

关键词： Chemical Pre-Potassiation Strategy Higher Rate Capability KF-Rich Electrolyte Interface Radical Reaction the Resistance to Electrolyte Oxidation

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Disparities in melanoma incidence and mortality in rural versus urban Michigan

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Cancer Reports 2022年第2期6卷

作者： Richard A. Shellenberger Timothy M. Johnson Fatima Fayyaz Bhanu Swamy Jeremy Albright Alan C. Geller St. Joseph Mercy Ann Arbor Hospital Ypsilanti Michigan USA Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Project administration (lead) Resources (lead) Software (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead) Ganger Dermatology and Departments of Dermatology Otolaryngology and Surgery Michigan Medicine Ann Arbor Michigan USA Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Northwell Health Cancer Institute Zucker School of Medicine New Hyde Park New York USA Contribution: Conceptualization (supporting) Data curation (equal) Formal analysis (supporting) Visualization (supporting) Writing - original draft (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (supporting) Software (supporting) Visualization (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Methods Consultants of Ann Arbor Ypsilanti Michigan USA Harvard TH Chen School of Public Health Cambridge M

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π–π Interaction-Induced Organic Long-wavelength Room-Temperature Phosphorescence forIn VivoAtherosclerotic Plaque Imaging

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Angewandte Chemie 2023年第2期136卷

作者： Yufan Zhang Jisen Li Jiliang Zhao Xuefei Li Zhimei Wang Yicheng Huang Prof. Hongkai Zhang Prof. Qian Liu Prof. Yunxiang Lei Prof. Dan Ding Frontiers Science Center for Cell Responses State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Bioactive Materials Ministry of Education College of Life Sciences Nankai University 300071 Tianjin China Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (lead) Writing - original draft (lead) Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Contribution: Investigation (equal) Methodology (equal) Contribution: Conceptualization (supporting) Software (equal) School of Chemistry and Materials Engineering Wenzhou University 325035 Wenzhou China Contribution: Investigation (supporting) Methodology (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Department of Urology Tianjin First Central Hospital 300192 Tianjin China Contribution: Data curation (supporting) Software (supporting) Contribution: Visualization (lead) Writing - review & editing (supporting) Contribution: Funding acquisition (lead) Writing - review & editing (lead)

Room-temperature phosphorescent (RTP) materials have great potential for in vivo imaging because they can circumvent the autofluorescence of biological tissues. In this study, a class of organic-doped long-wavelength (≈600 nm) RTP materials with benzo[c][1,2,5] thiadiazole as a guest was constructed. Both host and guest molecules have simple structures and can be directly purchased commercially at a low cost. Owing to the long phosphorescence wavelength of the doping system, it exhibited good tissue penetration (10 mm). Notably, these RTP nanoparticles were successfully used to image atherosclerotic plaques, with a signal-to-background ratio (SBR) of 44.52. This study provides a new approach for constructing inexpensive red organic phosphorescent materials and a new method for imaging cardiovascular diseases using these materials.

关键词： Atherosclerotic Plaque Imaging Benzo[c][1,2,5] Thiadiazole Guest Host-Guest Doped Systems Room Temperature Phosphorescence

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Tailoring Electrochemical CO2Reduction on Copper by Reactive Ionic Liquid and Native Hydrogen Bond Donors

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Angewandte Chemie 2023年第1期136卷

作者： Oguz Kagan Coskun Saudagar Dongare Brian Doherty Aidan Klemm Mark Tuckerman Burcu Gurkan Department of Chemical and Biomolecular Engineering Case Western Reserve University Cleveland OH 44106 USA Contribution: Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (equal) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Validation (supporting) Writing - review & editing (supporting) Department of Chemistry New York University New York NY 10003 USA Contribution: Data curation (supporting) Investigation (supporting) Methodology (supporting) Visualization (lead) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Validation (supporting) Writing - review & editing (supporting) Simons Center for Computational Physical Chemistry at New York University New York NY 10003 USA Contribution: Funding acquisition (supporting) Methodology (supporting) Resources (supporting) Software (equal) Supervision (supporting) Validation (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Formal analysis (supporting) Funding acquisition (lead) Investigation (equal) Methodology (equal) Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (equal)

Electrochemical CO 2 reduction (CO 2 RR) on copper (Cu) shows promise for higher-value products beyond CO. However, challenges such as the limited CO 2 solubility, high overpotentials, and the competing hydrogen evolution reaction (HER) in aqueous electrolytes hinder the practical realization. We propose a functionalized ionic liquid (IL) which generates ion-CO 2 adducts and a hydrogen bond donor (HBD) upon CO 2 absorption to modulate CO 2 RR on Cu in a non-aqueous electrolyte. As revealed by transient voltammetry, electrochemical impedance spectroscopy (EIS), and in situ surface-enhanced Raman spectroscopy (SERS) complemented with image charge augmented quantum-mechanical/molecular mechanics (IC-QM/MM) computations, a unique microenvironment is constructed. In this microenvironment, the catalytic activity is primarily governed by the IL and HBD concentrations; former controlling the double layer thickness and the latter modulating the local proton availability. This translates to ample CO 2 availability, reduced overpotential, and suppressed HER where C 4 products are obtained. This study deepens the understanding of electrolyte effects in CO 2 RR and the role of IL ions towards electrocatalytic microenvironment design.

关键词： CO2 Conversion Electrocatalysis Double Layer Interfacial Liquid Structure Electrolysis

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Organic Zinc-Ion Battery: Planar, π-Conjugated Quinone-Based Polymer Endows Ultrafast Ion Diffusion Kinetics

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Angewandte Chemie 2022年第51期134卷

作者： Dr. Fei Ye Qiang Liu Dr. Hongliang Dong Kailin Guan Zhaoyang Chen Na Ju Prof. Linfeng Hu School of Materials Science and Engineering Southeast University Nanjing 211189 China Contribution: Conceptualization (supporting) Data curation (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Software (lead) Center for High Pressure Science and Technology Advanced Research Shanghai 201203 P. R. China Contribution: Investigation (equal) Methodology (equal) Resources (equal) Validation (lead) Contribution: Formal analysis (equal) Investigation (lead) Methodology (equal) Contribution: Investigation (equal) Software (equal) Validation (lead) Visualization (lead) Contribution: Data curation (equal) Formal analysis (equal) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

A novel poly(phenazine-alt-pyromellitic anhydride) (PPPA) has been successfully designed and synthesized via a condensation polymerization strategy as promising cathode material in organic zinc-ion batteries. Electrochemical quartz crystal microbalance (EQCM), FTIR and XPS characterizations verify a reversible Zn 2+ -coordination mechanism in our PPPA cathode. Intriguingly, an ultrahigh Zn 2+ diffusion coefficient of 1.2×10 −7 cm 2 s −1 was found in this large π-conjugated system, which is the highest one among all organic cathode materials for zinc-ion batteries. Theoretical calculations reveal the extended π-conjugated plane in our PPPA sample results in a significant reduction on energy gap, effectively accelerating intramolecular electron transfer during charge/discharge process. Our finding provides insights to achieve high zinc-ion transport kinetics by a design strategy on planar polymer system.

关键词： Energy Gap Linear Polymer Organic Zinc-Ion Batteries Quinone-Based Polymer Zn2+ Diffusion Coefficient

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