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Synergistic Catalysis by Brønsted Acid/Carbodicarbene Mimicking Frustrated Lewis Pair-Like Reactivity

Angewandte Chemie 2021年第36期133卷

作者： Yi-Chen Chan Yuna Bai Dr. Wen-Ching Chen Prof. Hsing-Yin Chen Chen-Yu Li Dr. Ying-Yann Wu Dr. Mei-Chun Tseng Glenn P. A. Yap Prof. Lili Zhao Prof. Hsuan-Ying Chen Prof. Tiow-Gan Ong Institute of Chemistry Academia Sinica Taipei Taiwan R.O.C. Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu Taiwan R.O.C. Taiwan International Graduate Program (TIGP) Sustainable Chemical Science and Technology (SCST) Academia Sinica Taipei Taiwan R.O.C. Institute of Advanced Synthesis School of Chemistry and Molecular Engineering Nanjing Tech University Nanjing China Department of Medicinal and Applied Chemistry Drug Development and Value Creation Research Center Kaohsiung Medical University Kaohsiung 80708 Taiwan R.O.C. The Department of Chemistry and Biochemistry University of Delaware Newark DE USA Department of Medicinal Research Kaohsiung Medical University Hospital Kaohsiung 80708 Taiwan R.O.C. Department of Chemistry National (Taiwan) University Taipei Taiwan R.O.C.

Carbodicarbene (CDC), unique carbenic entities bearing two lone pairs of electrons are well-known for their strong Lewis basicity. We demonstrate herein, upon introducing a weak Brønsted acid benzyl alcohol (BnOH) as a co-modulator, CDC is remolded into a Frustrated Lewis Pair (FLP)-like reactivity. DFT calculation and experimental evidence show BnOH loosely interacting with the binding pocket of CDC via H-bonding and π-π stacking. Four distinct reactions in nature were deployed to demonstrate the viability of proof-of-concept as synergistic FLP/Modulator (CDC/BnOH), demonstrating enhanced catalytic reactivity in cyclotrimerization of isocyanate, polymerization process for L -lactide (LA), methyl methacrylate (MMA) and dehydrosilylation of alcohols. Importantly, the catalytic reactivity of carbodicarbene is uniquely distinct from conventional NHC which relies on only single chemical feature of nucleophilicity. This finding also provides a new spin in diversifying FLP reactivity with co-modulator or co-catalyst.

关键词： benzyl alcohol BnOH carbodicarbene frustrated Lewis pair

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Structural Degradations in the Bulk of Cathode Particles for Li-ion Batteries

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Microscopy and Microanalysis 2018年第S1期24卷 1504-1505页

作者： Hanlei Zhang Fredrick Omenya M. Stanley Whittingham Chongmin Wang Guangwen Zhou Materials Science and Engineering Program & Department of Mechanical Engineering State University of New York Binghamton New York13902 United States NorthEast Center for Chemical Energy Storage State University of New York Binghamton New York13902 United States Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland Washington99352 United States

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Predictable and precise template-free CRISPR editing of pathogenic variants (vol 563, pg 646, 2018)

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NATURE 2019年第7746期567卷 E1-E2页

作者： Shen, Max W. Arbab, Mandana Hsu, Jonathan Y. Worstell, Daniel Culbertson, Sannie J. Krabbe, Olga Cassa, Christopher A. Liu, David R. Gifford, David K. Sherwood, Richard I. Computational and Systems Biology Program Massachusetts Institute of Technology Cambridge USA Computer Science and Artificial Intelligence Laboratory Massachusetts Institute of Technology Cambridge USA Merkin Institute of Transformative Technologies in Healthcare Broad Institute of Harvard and MIT Cambridge USA Department of Chemistry and Chemical Biology Harvard University Cambridge USA Howard Hughes Medical Institute Harvard University Cambridge USA Department of Biological Engineering Massachusetts Institute of Technology Cambridge USA Molecular Pathology Unit Center for Cancer Research and Center for Computational and Integrative Biology Massachusetts General Hospital Charlestown USA Division of Genetics Department of Medicine Brigham and Women’s Hospital and Harvard Medical School Boston USA Hubrecht Institute for Developmental Biology and Stem Cell Research Royal Netherlands Academy of Arts and Sciences (KNAW) Utrecht The Netherlands Broad Institute of MIT and Harvard Cambridge USA Department of Electrical Engineering and Computer Science Massachusetts Institute of Technology Cambridge USA

In this Article, a data processing error affected Fig. 3e and Extended Data Table 2; these errors have been corrected online.

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Reconfigurable mid-infrared hyperbolic metasurfaces using phase-change materials

arXiv

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arXiv 2018年

作者： Folland, T.G. Fali, A. White, S.T. Matson, J.R. Liu, S. Aghamiri, N.A. Edgar, J.H. Haglund, R.F. Abate, Y. Caldwell, J.D. Department of Mechanical Engineering Vanderbilt University NashvilleTN37212 United States Department of Physics and Astronomy University of Georgia AthensGA30602-2451 United States Department of Physics and Astronomy Vanderbilt University NashvilleTN37235 United States Interdisciplinary Materials Science Program Vanderbilt University NashvilleTN37212 Department of Chemical Engineering Kansas State University ManhattanKS66506 United States

Metasurfaces offer the potential to control light propagation at the nanoscale for applications in both free-space and surface-confined geometries1-3. Existing metasurfaces frequently utilize metallic polaritonic4 elements with high absorption losses5, and/or fixed geometrical designs that serve a single function. Here we overcome these limitations by demonstrating a reconfigurable hyperbolic6 metasurface comprising of a heterostructure of isotopically enriched hexagonal boron nitride (hBN)7-10 in direct contact with the phase-change material (PCM) vanadium dioxide (VO2)11-14. Spatially localized metallic and dielectric domains in VO2 change the wavelength of the hyperbolic phonon polaritons (HPhPs) supported in hBN by a factor 1.6 at 1450cm-1. This induces in-plane launching, refraction and reflection of HPhPs in the hBN, proving reconfigurable control of in-plane HPhP propagation at the nanoscale15. These results exemplify a generalizable framework based on combining hyperbolic media and PCMs in order to design optical functionalities such as resonant cavities, beam steering, waveguiding and focusing with nanometric control. Copyright © 2018, The Authors. All rights reserved.

关键词： III-V semiconductors

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GWTC-3: Compact Binary Coalescences Observed by LIGO and Virgo during the Second Part of the Third Observing Run

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Physical Review X 2023年第4期13卷 041039-041039页

作者： R. Abbott T. D. Abbott F. Acernese K. Ackley C. Adams N. Adhikari R. X. Adhikari V. B. Adya C. Affeldt D. Agarwal M. Agathos K. Agatsuma N. Aggarwal O. D. Aguiar L. Aiello A. Ain P. Ajith S. Akcay T. Akutsu S. Albanesi A. Allocca P. A. Altin A. Amato C. Anand S. Anand A. Ananyeva S. B. Anderson W. G. Anderson M. Ando T. Andrade N. Andres T. Andrić S. V. Angelova S. Ansoldi J. M. Antelis S. Antier S. Appert Koji Arai Koya Arai Y. Arai S. Araki A. Araya M. C. Araya J. S. Areeda M. Arène N. Aritomi N. Arnaud M. Arogeti S. M. Aronson K. G. Arun H. Asada Y. Asali G. Ashton Y. Aso M. Assiduo S. M. Aston P. Astone F. Aubin C. Austin S. Babak F. Badaracco M. K. M. Bader C. Badger S. Bae Y. Bae A. M. Baer S. Bagnasco Y. Bai L. Baiotti J. Baird R. Bajpai M. Ball G. Ballardin S. W. Ballmer A. Balsamo G. Baltus S. Banagiri D. Bankar J. C. Barayoga C. Barbieri B. C. Barish D. Barker P. Barneo F. Barone B. Barr L. Barsotti M. Barsuglia D. Barta J. Bartlett M. A. Barton I. Bartos R. Bassiri A. Basti M. Bawaj J. C. Bayley A. C. Baylor M. Bazzan B. Bécsy V. M. Bedakihale M. Bejger I. Belahcene V. Benedetto D. Beniwal T. F. Bennett J. D. Bentley M. BenYaala F. Bergamin B. K. Berger S. Bernuzzi C. P. L. Berry D. Bersanetti A. Bertolini J. Betzwieser D. Beveridge R. Bhandare U. Bhardwaj D. Bhattacharjee S. Bhaumik I. A. Bilenko G. Billingsley S. Bini R. Birney O. Birnholtz S. Biscans M. Bischi S. Biscoveanu A. Bisht B. Biswas M. Bitossi M.-A. Bizouard J. K. Blackburn C. D. Blair D. G. Blair R. M. Blair F. Bobba N. Bode M. Boer G. Bogaert M. Boldrini L. D. Bonavena F. Bondu E. Bonilla R. Bonnand P. Booker B. A. Boom R. Bork V. Boschi N. Bose S. Bose V. Bossilkov V. Boudart Y. Bouffanais A. Bozzi C. Bradaschia P. R. Brady A. Bramley A. Branch M. Branchesi J. Brandt J. E. Brau M. Breschi T. Briant J. H. Briggs A. Brillet M. Brinkmann P. Brockill A. F. Brooks J. Brooks D. D. Brown S. Brunett G. Bruno R. Bruntz J. Bryant T. Bulik H. J. Bulten A. Buonanno R. Buscicchio D. Buskulic C. Buy R. L. Byer G. S. Cabourn Davies L. Cadonati G. Cagn LIGO Laboratory California Institute of Technology Pasadena California 91125 USA Louisiana State University Baton Rouge Louisiana 70803 USA Dipartimento di Farmacia Università di Salerno I-84084 Fisciano Salerno Italy INFN Sezione di Napoli Complesso Universitario di Monte S. Angelo I-80126 Napoli Italy OzGrav School of Physics & Astronomy Monash University Clayton 3800 Victoria Australia LIGO Livingston Observatory Livingston Louisiana 70754 USA University of Wisconsin-Milwaukee Milwaukee Wisconsin 53201 USA OzGrav Australian National University Canberra Australian Capital Territory 0200 Australia Max Planck Institute for Gravitational Physics (Albert Einstein Institute) D-30167 Hannover Germany Leibniz Universität Hannover D-30167 Hannover Germany Inter-University Centre for Astronomy and Astrophysics Pune 411007 India University of Cambridge Cambridge CB2 1TN United Kingdom Theoretisch-Physikalisches Institut Friedrich-Schiller-Universität Jena D-07743 Jena Germany University of Birmingham Birmingham B15 2TT United Kingdom Center for Interdisciplinary Exploration and Research in Astrophysics (CIERA) Northwestern University Evanston Illinois 60208 USA Instituto Nacional de Pesquisas Espaciais 12227-010 São José dos Campos São Paulo Brazil Gravity Exploration Institute Cardiff University Cardiff CF24 3AA United Kingdom INFN Sezione di Pisa I-56127 Pisa Italy International Centre for Theoretical Sciences Tata Institute of Fundamental Research Bengaluru 560089 India University College Dublin Dublin 4 Ireland Gravitational Wave Science Project National Astronomical Observatory of Japan (NAOJ) Mitaka City Tokyo 181-8588 Japan Advanced Technology Center National Astronomical Observatory of Japan (NAOJ) Mitaka City Tokyo 181-8588 Japan INFN Sezione di Torino I-10125 Torino Italy Università di Napoli “Federico II” Complesso Universitario di Monte S. Angelo I-80126 Napoli Italy Université de Lyon Université Claude Bernard Lyon 1 CNRS Institut L

The third Gravitational-Wave Transient Catalog (GWTC-3) describes signals detected with Advanced LIGO and Advanced Virgo up to the end of their third observing run. Updating the previous GWTC-2.1, we present candidate gravitational waves from compact binary coalescences during the second half of the third observing run (O3b) between 1 November 2019, 15∶00 Coordinated Universal Time (UTC) and 27 March 2020, 17∶00 UTC. There are 35 compact binary coalescence candidates identified by at least one of our search algorithms with a probability of astrophysical origin pastro>0.5. Of these, 18 were previously reported as low-latency public alerts, and 17 are reported here for the first time. Based upon estimates for the component masses, our O3b candidates with pastro>0.5 are consistent with gravitational-wave signals from binary black holes or neutron-star–black-hole binaries, and we identify none from binary neutron stars. However, from the gravitational-wave data alone, we are not able to measure matter effects that distinguish whether the binary components are neutron stars or black holes. The range of inferred component masses is similar to that found with previous catalogs, but the O3b candidates include the first confident observations of neutron-star–black-hole binaries. Including the 35 candidates from O3b in addition to those from GWTC-2.1, GWTC-3 contains 90 candidates found by our analysis with pastro>0.5 across the first three observing runs. These observations of compact binary coalescences present an unprecedented view of the properties of black holes and neutron stars.

关键词： Gravitational waves

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Toward the integration of speciation research

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Evolutionary Journal of the Linnean Society 2024年第1期3卷

作者： Stankowski, Sean Cutter, Asher D Satokangas, Ina Lerch, Brian A Rolland, Jonathan Smadja, Carole M Segami Marzal, J Carolina Cooney, Christopher R Feulner, Philine G D Domingos, Fabricius Maia Chaves Bicalho North, Henry L Yamaguchi, Ryo Butlin, Roger K Wolf, Jochen B W Coughlan, Jenn Heidbreder, Patrick Hernández-Gutiérrez, Rebeca Barnard-Kubow, Karen B Peede, David Rancilhac, Loïs Salvador, Rodrigo Brincalepe Thompson, Ken A Stacy, Elizabeth A Moyle, Leonie C Garlovsky, Martin D Maulana, Arif Kantelinen, Annina Cacho, N Ivalú Schneemann, Hilde Domínguez, Marisol Dopman, Erik B Lohse, Konrad Rometsch, Sina J Comeault, Aaron A Merrill, Richard M Scordato, Elizabeth S C Singhal, Sonal Pärssinen, Varpu Lackey, Alycia C R Kumar, Sanghamitra Meier, Joana I Barton, Nicholas Fraïsse, Christelle Ravinet, Mark Kulmuni, Jonna Institute of Science and Technology Austria (ISTA) Klosterneuburg Austria Department of Ecology and Evolution University of Sussex Brighton United Kingdom Ecology & Evolutionary Biology University of Toronto Toronto Canada Organismal and Evolutionary Biology Research Programme University of Helsinki Helsinki Finland Department of Biology University of North Carolina at Chapel Hill Chapel Hill NC United States Centre de Recherche sur la Biodiversité et l’Environnement (CRBE) Université de Toulouse CNRS IRD Toulouse INP Université Toulouse 3 – Paul Sabatier (UT3) Toulouse France Institut des Sciences de l’Evolution de Montpellier ISEM Univ. Montpellier CNRS IRD Montpellier France Department of Biology Duke University Durham NC United States Ecology and Evolutionary Biology School of Biosciences University of Sheffield Sheffield United Kingdom Department of Fish Ecology and Evolution Centre of Ecology Evolution and Biogeochemistry EAWAG Swiss Federal Institute of Aquatic Science and Technology Kastanienbaum Switzerland Division of Aquatic Ecology and Evolution Institute of Ecology and Evolution University of Bern Bern Switzerland Departamento de Zoologia Universidade Federal do Paraná Curitiba PR Brazil Department of Zoology University of Cambridge Cambridge United Kingdom Department of Advanced Transdisciplinary Sciences Hokkaido University Sapporo Japan Department of Zoology & Biodiversity Research Centre University of British Columbia Vancouver Canada Department of Marine Sciences University of Gothenburg Gothenburg Sweden Division of Evolutionary Biology LMU Munich Munich Germany Department of Ecology & Evolutionary Biology Yale University New Haven CT United States Department of Evolution Ecology and Organismal Biology University of California Riverside Riverside CA United States Department of Biology James Madison University Harrisonburg VA United States Department of Ecology Evolution and Organismal Biology Brown University Provi

Speciation research—the scientific field focused on understanding the origin and diversity of species—has a long and complex history. While relevant to one another, the specific goals and activities of speciation researchers are highly diverse, and scattered across a collection of different perspectives. Thus, our understanding of speciation will benefit from efforts to bridge scientific findings and the diverse people who do the work. In this paper, we outline two ways of integrating speciation research: (i) scientific integration, through the bringing together of ideas, data, and approaches; and (ii) social integration, by creating ways for a diversity of researchers to participate in the scientific process. We then discuss five challenges to integration: (i) the multidisciplinary nature of speciation research, (ii) the complex language of speciation; (iii) a bias toward certain study systems; (iv) the challenges of working across scales; and (v) inconsistent measures and reporting standards. We provide practical steps that individuals and groups can take to help overcome these challenges, and argue that integration is a team effort in which we all have a role to play.

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Ultramicroporous Building Units as a Path to Bi‐microporous Metal–Organic Frameworks with High Acetylene Storage and Separation Performance

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Angewandte Chemie 2019年第38期131卷

作者： Yong‐Peng Li Ying Wang Ying‐Ying Xue Hai‐Peng Li Quan‐Guo Zhai Shu‐Ni Li Yu‐Cheng Jiang Man‐Cheng Hu Xianhui Bu Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education School of Chemistry & Chemical Engineering Shaanxi Normal University Xi'an Shaanxi 710062 China Department of Chemistry and Biochemistry California State University Long Beach California 90840 USA

A strategy called ultramicroporous building unit (UBU) is introduced. It allows the creation of hierarchical bi‐porous features that work in tandem to enhance gas uptake capacity and separation. Smaller pores from UBUs promote selectivity, while larger inter‐UBU packing pores increase uptake capacity. The effectiveness of this UBU strategy is shown with a cobalt MOF (denoted SNNU‐45) in which octahedral cages with 4.5 Å pore size serve as UBUs. The C 2 H 2 uptake capacity at 1 atm reaches 193.0 cm 3 g −1 (8.6 mmol g −1 ) at 273 K and 134.0 cm 3 g −1 (6.0 mmol g −1 ) at 298 K. Such high uptake capacity is accompanied by a high C 2 H 2 /CO 2 selectivity of up to 8.5 at 298 K. Dynamic breakthrough studies at room temperature and 1 atm show a C 2 H 2 /CO 2 breakthrough time up to 79 min g −1 , among top‐performing MOFs. Grand canonical Monte Carlo simulations agree that ultrahigh C 2 H 2 /CO 2 selectivity is mainly from UBU ultramicropores, while packing pores promote C 2 H 2 uptake capacity.

关键词： C2H2-Aufnahme C2H2/CO2-Trennung Metall-organische Gerüstverbindungen Ultramikroporöse Bausteine

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Active-layer evolution and （CH3NH3）3Bi2l9-based solar substrate efficiency improvement of cell on TiO2-deposited ITO

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Nano Research 2016年第10期9卷 2921-2930页

作者： Xinqian Zhang Gang Wu Zhuowei Gu Bing Guo Wenqing Liu Shida Yang Tao Ye Chen Chen Weiwei Tu Hongzheng Chen State Key Laboratory of Silicon Materials MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China Department of Chemical Engineering Xinjiang Agriculture University Urumqi 830052 China

We systematically investigated the development of film morphology and crystallinity of methyl-ammonium bismuth （Ⅲ） iodide （MA3Bi2I9） through one- step spin-coating on TiO2-deposited indium tin oxide （ITO）/glass. The precursor solution concentration and substrate structure have been demonstrated to be critically important in the active-layer evolution of the MA3Bi2I9-based solar cell. This work successfully improved the cell efficiency to 0.42% （average： 0.38%） with the mesoscopic architecture of ITO/compact-TiOdmesoscopic-TiO2 （meso-TiO2）/ MA3Bi2I9/2,2＇,7,7＇-tetrakis（N,N-di-4-methoxyphenylamino）-9,9＇spiro-bifluorene （spiro-MeOTAD）/MoO3/Ag under a precursor concentration of 0.45 M, which provided the probability of further improving the efficiency of the BiB＋-based lead-free organic-inorganic hybrid solar cells.

关键词： methyl-ammonium bismuth （Ⅲ） iodide organic-inorganic hybridsolar cell TiO2-depostied indium tinoxide （FRO） substrate morphology and crystallinity precursor solution concentration

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Effect of particle shape and size distribution on dewatering and filtercake permeability

Effect of particle shape and size distribution on dewatering...

引用

Paper Conference and Trade Show: Renew, Rethink, Redefine the Future, PaperCon 2017

作者： Weeks, Lisa Bousfield, Doug W. Hayes, Peter Paper Surface Science Program Department of Chemical and Biological Engineering University of Maine OronoME04469 United States BASF 11501 Steele Creek Rd. CharlotteNC28273 United States

ISBN: (纸本)9781510847286

Excess dewatering of the coating upon contact with paper is one potential source for runnability problems. As the water penetrates the base sheet paper, the solids content of the coating increases. This increases in concentration can lead to operational problems such as scratches or excessive blade wear. The influence of the shape factor of the pigment on the dewatering properties of a coating has not been the subject of a systematic study in the literature. The effect of the particle shape and particle size distribution on the dewatering and the filtercake permeability were analyzed. The dewatering rates were measured with the common pressure filtration method called the gravimetric water retention (GWR) test, and with a Bristow absorption wheel. The pore size and porosity of the dried filtercakes were characterized with mercury porosimetry. The permeability of the filtercakes were obtained by fitting the data to a filtration equation and predicted by the Carman-Kozeny equation. The particle shape is found to influence the permeability, but the results do not simply follow the theory.

关键词： Coatings

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Super‐Resolution Microscopy: On‐Chip Super‐Resolution Imaging with Fluorescent Polymer Films (Adv. Funct. Mater. 27/2019)

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Advanced Functional Materials 2019年第27期29卷

作者： Chenlei Pang Jingxi Li Mingwei Tang Jianpu Wang Ioanna Mela Florian Ströhl Lisa Hecker Weidong Shen Qiulan Liu Xiaowei Liu Yinan Wang Hao Zhang Meng Xu Xinghong Zhang Xu Liu Qing Yang Clemens F. Kaminski State Key Laboratory of Modern Optical Instrumentation College of Optical Science and Engineering Zhejiang University Hangzhou 310027 China Institute of Advanced Materials Nanjing Tech University Nanjing 211816 China Department of Chemical Engineering and Biotechnology University of Cambridge Cambridge CB3 0AS United Kingdom MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China State Key Lab. of Modern Optical Instrumentation College of Optical Science and Engineering Zhejiang University Hangzhou 310027 China Collaborative Innovation Center of Extreme Optics Shanxi University Taiyuan 030006 China

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