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Pillar[5]arene-Containing Metallacycles and Host-Guest Interaction Caused Aggregation-Induced Emission Enhancement Platforms.

Wei Tuo, Yan Sun, Shuai Lu, Xiaopeng Li, Yao Sun, Peter J Stang,

Coordination-driven Pt metallacycles have shown potential in controllable modular self-assembly, which has made a vital contribution to biomedicine, catalysis, and multiresponsive materials. Herein, pillar[5]arene units were integrated into one skeleton through coordination-driven self-assembly, resulting in the formation of a hexagonal Pt(II) metallacycle decorated with six pillar[5]arenes. The host-guest interactions of ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Toward understanding optical properties of amyloids: a reaction path and nonadiabatic dynamics study.

Luca Grisanti, Marin Sapunar, Ali Hassanali, Nađa Došliċ,

Amyloids have unique structural, chemical and optical properties. Although much theoretical effort has been directed toward understanding amyloid nucleation, the understanding of their optical properties has remained rather limited. In particular, the photophysical mechanisms leading to near UV excitation and characteristic blue-green luminescence in amyloid systems devoid of aromatic amino ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Serine-Selective Bioconjugation.

Julien C Vantourout, Srinivasa Rao Adusumalli, Kyle W Knouse, Dillon T Flood, Antonio Ramirez, Natalia M Padial, Alena Istrate, Katarzyna Maziarz, Justine N deGruyter, Rohan R Merchant, Jennifer X Qiao, Michael A Schmidt, Michael J Deery, Martin D Eastgate, Philip E Dawson, Gonçalo J L Bernardes, Phil S Baran,

The first general method for the rapid, chemoselective, and modular functionalization of serine residues in native polypeptides is reported using a reagent platform based on P(V) oxidation state. This redox-economic approach can be used to append nearly any kind of cargo onto serine, generating a stable, benign, and hydrophilic phosphorothioate ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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All-Carboxylate-Protected Superatomic Silver Nanocluster with an Unprecedented Rhombohedral Ag8 Core.

Kuan-Guan Liu, Xue-Mei Gao, Tongyu Liu, Mao-Lin Hu, De-En Jiang,

We report the synthesis and structure of the first all-carboxylate-protected superatomic silver nanocluster. It was prepared by heating a dimethylformamide solution of perfluoroglutaric acid and AgNO3 under alkaline conditions, yielding a single crystal of [(CH3)2NH2]6[Ag8(pfga)6]. The [Ag8(pfga)6]6- cluster has a rhombohedral Ag86+ core, with each of its faces protected by ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Mechanistic Insight into Concerted Proton-Electron Transfer of a Ru(IV)-Oxo Complex: A Possible Oxidative Asynchronicity.

Hiroaki Kotani, Hinatsu Shimomura, Kei Ikeda, Tomoya Ishizuka, Yoshihito Shiota, Kazunari Yoshizawa, Takahiko Kojima,

We have thoroughly investigated the oxidation of benzyl alcohol (BA) derivatives by a RuIV(O) complex (RuIV(O)) in the absence or presence of Brønsted acids in order to elucidate the proton-coupled electron-transfer (PCET) mechanisms in C-H oxidation on the basis of a kinetic analysis. Oxidation of BA derivatives by RuIV(O) without ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Influence of Defects and H2O on the Hydrogenation of CO2 to Methanol over Pt Nanoparticles in UiO-67 Metal-Organic Framework.

Emil Sebastian Gutterød, Sri Harsha Pulumati, Gurpreet Kaur, Andrea Lazzarini, Bjørn Gading Solemsli, Anette Eleonora Gunnæs, Christian Ahoba-Sam, Maria Evangelou Kalyva, Johnny Andreas Sannes, Stian Svelle, Egill Skúlason, Ainara Nova, Unni Olsbye,

In catalysts for CO2 hydrogenation, the interface between metal nanoparticles (NPs) and the support material is of high importance for the activity and reaction selectivity. In Pt NP-containing UiO Zr-metal-organic frameworks (MOFs), key intermediates in methanol formation are adsorbed at open Zr-sites at the Pt-MOF interface. In this study, we ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Enhanced safety and anti-tumor efficacy of switchable dual chimeric antigen receptor-engineered T cell against solid tumor through a synthetic bifunctional PD-L1-blocking peptide.

Peiwei Yang, Ying Wang, Zheng Yao, Xinmei Gao, Chen Liu, Xinmin Wang, Hemin Wu, Xu Ding, Jialiang Hu, Bingjing Lin, Qian Li, Mengwei Li, Xin Li, Xiangying Chen, Weiyan Qi, Weiguang Li, Jianpeng Xue, Hanmei Xu,

Chimeric antigen receptor (CAR)-engineered T cells (CAR-Ts) therapy has excellent efficacy in cancer treatment especially its impressive results in hematological malignancies. Unfortunately, its application on solid tumors is challenged by the off-target effects caused by lacking of tumor specific antigens and the immunosuppression caused by tumor microenvironment. We constructed a ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Untangling the Mechanochromic Properties of Benzothiadiazole-Based Luminescent Polymorphs through Supramolecular Organic Framework Topology.

Marcelo Echeverri, Constanza Ruiz, Sergio Gámez-Valenzuela, Irene Martín, M Carmen Ruiz Delgado, Enrique Gutiérrez-Puebla, M Ángeles Monge, Lina M Aguirre-Díaz, Berta Gómez-Lor,

Two new luminophore polymorphs of 4-bromo-7-(4-nonylphenyl)benzo[c][1,2,5]thiadiazole (1α and 1β) exhibiting different color emissions, which switch into each other in response to shear force and solvent vapors, are presented and their X-ray structure is determined. Supramolecular organic framework topology (SOFT) studies on the two polymorphic structures led us to conclude that ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Photoresponsive Organic-Inorganic Hybrid Ferroelectric Designed at the Molecular Level.

Wei-Jian Xu, Konstantin Romanyuk, José M G Martinho, Ying Zeng, Xue-Wen Zhang, Andrei Ushakov, Vladimir Shur, Wei-Xiong Zhang, Xiao-Ming Chen, Andrei Kholkin, João Rocha,

Molecular ferroelectrics are becoming an important area of research due to their ability to form a variety of structures exhibiting the desired properties. However, the precise control over the assembly of molecular building blocks for the design and synthesis of photoresponsive molecular ferroelectrics remains a considerable challenge. Here, we report ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Intrinsic and Extrinsic Programming of Product Chain Length and Release Mode in Fungal Collaborating Iterative Polyketide Synthases.

Chen Wang, Xiaojing Wang, Liwen Zhang, Qun Yue, Qingpei Liu, Ya-Ming Xu, A A Leslie Gunatilaka, Xiaoyi Wei, Yuquan Xu, István Molnár,

Combinatorial biosynthesis with fungal polyketide synthases (PKSs) promises to produce unprecedented bioactive "unnatural" natural products (uNPs) for drug discovery. Genome mining of the dothideomycete Rhytidhysteron rufulum uncovered a collaborating highly reducing PKS (hrPKS)-nonreducing PKS (nrPKS) pair. These enzymes produce trace amounts of rare S-type benzenediol macrolactone congeners with a phenylacetate ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Evolution from tunneling to hopping mediated triplet energy transfer from quantum dots to molecules.

Zhiyuan Huang, Zihao Xu, Tingting Huang, Victor Gray, Kasper Moth-Poulsen, Tianquan Lian, Ming Lee Tang,

Efficient energy transfer is particularly important for multi-excitonic processes like singlet fission and photon upconversion. Observation of the transition from short-range tunneling to long-range hopping during triplet exciton transfer from CdSe nanocrystals to anthracene is reported here. This is firmly supported by steady-state photon upconversion measurements, a direct proxy for ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Interfacial Dipole in Organic and Perovskite Solar Cells.

Qi Chen, Cheng Wang, Yaowen Li, Liwei Chen,

Incorporating dipole interlayer has been one of the most crucial interfacial engineering strategies in organic and perovskite solar cells. Interfacial dipole brings steep shifts in electronic band structure across interfaces and thus effectively tunes charge carrier transport. However, the origin of interfacial dipole and its effects on device performance are ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Catalytic Asymmetric Synthesis of Chiral Covalent Organic Frameworks from Prochiral Monomers for Heterogeneous Asymmetric Catalysis.

Jian-Cheng Wang, Xuan Kan, Jin-Yan Shang, Hua Qiao, Yu-Bin Dong,

Direct synthesis, postsynthetic modification, and chiral induction have been recognized as three powerful methods to synthesize chiral covalent organic frameworks (CCOFs). However, catalytic asymmetric methodology, as the most important and effective synthetic approach to access chiral organics, has not been enabled for CCOFs synthesis thus far. Herein we report, for ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Mechanistic Insight into the Photoredox-Nickel-HAT Triple Catalyzed Arylation and Alkylation of α-Amino Csp3-H Bonds.

Bholanath Maity, Chen Zhu, Huifeng Yue, Long Huang, Moussab Harb, Yury Minenkov, Magnus Rueping, Luigi Cavallo,

We report here a comprehensive computational analysis of the mechanisms of the photoredox-nickel-HAT (HAT: hydrogen atom transfer) catalyzed arylation and alkylation of α-amino Csp3-H bonds developed by MacMillan and co-workers. Different alternatives for the three catalytic cycles were tested to identify unambiguously the operative reaction mechanism. Our analysis indicated that ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Methane Borylation Catalyzed by Ru, Rh, and Ir Complexes in Comparison with Cyclohexane Borylation: Theoretical Understanding and Prediction.

Rong-Lin Zhong, Shigeyoshi Sakaki,

Methane borylation catalyzed by Cp*M(Bpin)n (M = Ru or Rh; HBpin = pinacolborane; n = 2 or 3) and (TMPhen)Ir(Bpin)3 (TMPhen = 3,4,7,8-tetramethyl-1,10-phenanthroline) was investigated by DFT in comparison with cyclohexane borylation. Because Ru-catalyzed borylation has not been theoretically investigated yet, its reaction mechanism was first elucidated; Cp*Ru(Bpin)3 1-Ru is ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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The Radical SAM enzyme Spore Photoproduct Lyase: Properties of the Ω Organometallic Intermediate and Identification of Stable Protein Radicals Formed During Substrate-Free Turnover.

Adrien Pagnier, Hao Yang, Richard Jodts, Christopher James, Eric M Shepard, Stella Impano, William Broderick, Brian M Hoffman, Joan B Broderick,

Spore photoproduct lyase is a radical S-adenosyl-l-methionine (SAM) enzyme with the unusual property that addition of SAM to the [4Fe-4S]1+ enzyme absent substrate results in rapid electron transfer to SAM with accompanying homolytic S-C5' bond cleavage. Herein we demonstrate that this unusual reaction forms the organometallic intermediate, Ω, in which ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Invoking Side-Chain Functionality for the Mediation of Regioselectivity during Ring-Opening Polymerization of Glucose Carbonates.

Yue Song, Xin Yang, Yidan Shen, Mei Dong, Yen-Nan Lin, Michael B Hall, Karen L Wooley,

The extent of participation of side-chain functionalities during the 1,5,7-triazabicyclo[5.4.0]dec-5-ene (TBD) organobase-catalyzed ring-opening polymerizations (ROP) of six-membered cyclic d-glucose-based carbonates was found to result in significantly different regiochemical outcomes. High regioselectivity was observed for naturally derived poly(4,6-d-glucose carbonate)s (PGCs) containing carbonate side chain substituents in the 2- and 3-positions, whereas ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Reaction-Induced Strong Metal-Support Interactions between Metals and Inert Boron Nitride Nanosheets.

Jinhu Dong, Qiang Fu, Haobo Li, Jianping Xiao, Bing Yang, Bingsen Zhang, Yunxing Bai, Tongyuan Song, Rankun Zhang, Lijun Gao, Jun Cai, Hui Zhang, Zhi Liu, Xinhe Bao,

Encapsulation of metal nanocatalysts by support-derived materials is well known as a classical strong metal-support interaction (SMSI) effect that occurs almost exclusively with active oxide supports and often blocks metal-catalyzed surface reactions. In the present work this classical SMSI process has been surprisingly observed between metal nanoparticles, e.g., Ni, Fe, ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Distance-Selected Topochemical Dehydro-Diels-Alder Reaction of 1,4-Diphenylbutadiyne toward Crystalline Graphitic Nanoribbons.

Peijie Zhang, Xingyu Tang, Yida Wang, Xuan Wang, Dexiang Gao, Yapei Li, Haiyan Zheng, Yajie Wang, Xinxin Wang, Riqiang Fu, Mingxue Tang, Kazutaka Ikeda, Ping Miao, Takanori Hattori, Asami Sano-Furukawa, Christopher A Tulk, Jamie J Molaison, Xiao Dong, Kuo Li, Jing Ju, Ho-Kwang Mao,

Solid-state topochemical polymerization (SSTP) is a promising method to construct functional crystalline polymeric materials, but in contrast to various reactions that happen in solution, only very limited types of SSTP reactions are reported. Diels-Alder (DA) and dehydro-DA (DDA) reactions are textbook reactions for preparing six-membered rings in solution but are ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Correction to "Inorganic Halide Double Perovskites with Optoelectronic Properties Modulated by Sublattice Mixing".

Christopher J Bartel, Jacob M Clary, Christopher Sutton, Derek Vigil-Fowler, Bryan R Goldsmith, Aaron M Holder, Charles B Musgrave,

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Visible Circularly Polarized Luminescence of Octanuclear Eu(III) Circular Helicate.

Yan Bing Tan, Yoshinori Okayasu, Shohei Katao, Yoshiko Nishikawa, Fumio Asanoma, Mihoko Yamada, Junpei Yuasa, Tsuyoshi Kawai,

This work reports on the structural and photophysical characterizations of D4-point symmetrical octanuclear circular LnIII helicates, [(R)- or (S)-iPr-pybox]8(LnIII)8(THP)8 (where Ln = Eu and Tb, THP = tri-anionic tris-β-diketonate and iPr-pybox = chiral bis(4-isopropyl-2-oxazolinyl)pyridine). X-ray crystallographic analysis revealed that the octanuclear circular helicate possesses square antiprism architecture and consists of ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Insight into the Catalytic Mechanism of GH11 Xylanase: Computational Analysis of Substrate Distortion based on a Neutron Structure.

Toyokazu Ishida, Jerry M Parks, Jeremy C Smith,

The reaction mechanism of xylanase biomass decomposition enzymes has been the subject of debate. To clarify the mechanism we investigated the glycosylation step of GH11 xylanase, an enzyme that catalyzes the hydrolysis of lignocellulosic hemicellulose (xylan). Making use of a recent neutron structure, which identified the protonation states of relevant ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Precise Control of Pi-electron Magnetism in Metal-free Porphyrins.

Yan Zhao, Kaiyue Jiang, Can Li, Yufeng Liu, Chengyang Xu, Wenna Zheng, Dandan Guan, Yaoyi Li, Hao Zheng, Canhua Liu, Weidong Luo, Jinfeng Jia, Xiaodong Zhuang, Shiyong Wang,

The porphyrin macrocycle can stabilize a set of magnetic metal ions, thus introducing localized net spins near the center. However, it remains elusive but most desirable to introduce delocalized spins in porphyrins with wide implications, for example, for building correlated quantum spins. Here, we demonstrate that metal-free porphyrins host delocalized ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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TRPswitch - a step function chemo-optogenetic ligand for the vertebrate TRPA1 channel.

Pui-Ying Lam, Aditya Raymond Thawani, Enrique Balderas, Andrew J P White, Dipayan Chaudhuri, Matthew J Fuchter, Randall Peterson,

Chemo-optogenetics has produced powerful tools for optical control of cell activity, but current tools suffer from a variety of limitations including low unitary conductance, the need to modify the target channel, or the inability to control both on and off switching. Using a zebrafish behavior-based screening strategy, we discovered "TRPswitch", ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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Synthesis, Assembly and Sizing of Neutral, Lanthanide Substituted Molybdenum Blue Wheels {Mo90+2nLn10-n}.

Eduard Garrido Ribó, Nicola L Bell, Weimin Xuan, Jiancheng Luo, De-Liang Long, Tianbo Liu, Leroy Cronin,

Polyoxometalate Molybdenum blue (MBs) complexes typically exist as discrete multianionic clusters and are composed of repeating Mo building units. MB Wheels, such as {Mo176} and {Mo154} are made from pentagon-centered {Mo8} building blocks joined by equal number of {Mo1} units as loin, and {Mo2} dimer units as skirt along the ... Read more >>

J. Am. Chem. Soc. (Journal of the American Chemical Society)
[2020, :]

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