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Dynamic Nuclear Polarization Enables NMR of Surface Passivating Agents on Hybrid Perovskite Thin Films J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-12 Aditya Mishra, Michael A. Hope, Masaud Almalki, Lukas Pfeifer, Shaik Mohammed Zakeeruddin, Michael Grätzel, Lyndon Emsley
Surface and bulk molecular modulators are the key to improving the efficiency and stability of hybrid perovskite solar cells. However, due to their low concentration, heterogeneous environments, and low sample mass, it remains challenging to characterize their structure and dynamics at the atomic level, as required to establish structure–activity relationships. Nuclear magnetic resonance (NMR) spectroscopy
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Controlled Living Cascade Polymerization of Polycyclic Enyne Monomers: Leveraging Complete Degradability for a Stereochemical and Structural Investigation J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-12 Antonio Rizzo, Eunsong Jung, Hojoon Song, Yunhyeong Cho, Gregory I. Peterson, Tae-Lim Choi
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Collective wind farm operation based on a predictive model increases utility-scale energy production Nat. Energy (IF 67.439) Pub Date : 2022-08-11 Michael F. Howland, Jesús Bas Quesada, Juan José Pena Martínez, Felipe Palou Larrañaga, Neeraj Yadav, Jasvipul S. Chawla, Varun Sivaram, John O. Dabiri
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Filling of a water-free void explains the allosteric regulation of the β1-adrenergic receptor by cholesterol Nat. Chem. (IF 24.274) Pub Date : 2022-08-11 Layara Akemi Abiko, Raphael Dias Teixeira, Sylvain Engilberge, Anne Grahl, Tobias Mühlethaler, Timothy Sharpe, Stephan Grzesiek
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Different timescales during ultrafast stilbene isomerization in the gas and liquid phases revealed using time-resolved photoelectron spectroscopy Nat. Chem. (IF 24.274) Pub Date : 2022-08-11 Chuncheng Wang, Max D. J. Waters, Pengju Zhang, Jiří Suchan, Vít Svoboda, Tran Trung Luu, Conaill Perry, Zhong Yin, Petr Slavíček, Hans Jakob Wörner
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Climate change is making hundreds of diseases much worse Nature (IF 69.504) Pub Date : 2022-08-12
Heatwaves, droughts, floods and storms push up the number of cases, make diseases more severe and hamper people’s ability to cope.
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World’s largest ice sheet threatened by warm water surge Nature (IF 69.504) Pub Date : 2022-08-12
Shifting winds and ocean currents are pushing warm waters into East Antarctica, contributing to ice loss, an analysis finds.
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An Asymmetric sp3–sp3 Cross-Electrophile Coupling Using ‘Ene’-Reductases Nature (IF 69.504) Pub Date : 2022-08-11 Haigen Fu, Jingzhe Cao, Tianzhang Qiao, Yuyin Qi, Simon J. Charnock, Samuel Garfinkle, Todd K. Hyster
The catalytic asymmetric construction of Csp3–Csp3 bonds remains one of the foremost challenges in organic synthesis.1 Metal-catalyzed cross-electrophile couplings (XEC) have emerged as a powerful tool for C–C bond formation.2-5 However, coupling two distinct Csp3-electrophiles with high cross- and stereoselectivity continues as an unmet challenge. Here, we report a highly chemo- and enantioselective
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The geometry of life: when mathematics meets synthetic biology Nature (IF 69.504) Pub Date : 2022-08-11
How researchers created complex tiling patterns with bioengineered bacteria
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How does monkeypox spread? What scientists know Nature (IF 69.504) Pub Date : 2022-08-11
Prolonged contact, especially with a person’s skin lesions, is emerging as the top transmission route.
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Why thinking hard makes us feel tired Nature (IF 69.504) Pub Date : 2022-08-11
Difficult tasks can lead to build-up of a signalling molecule in the brain, triggering fatigue.
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Ultra-Low Voltage Bipolar Hydrogen Production from Biomass-Derived Aldehydes and Water in Membrane-Less Electrolyzers Energy Environ. Sci. (IF 39.714) Pub Date : 2022-08-12 Hengzhou Liu, Naveen Agrawal, Arna Ganguly, Yifu Chen, Jungkuk Lee, Jiaqi Yu, Wenyu Huang, Mark M Wright, Michael Janik, Wenzhen Li
Water electrolysis using renewable energy inputs is being actively pursued as a green route for hydrogen production. However, it is limited by the high energy consumption due to the sluggish anodic oxygen evolution reaction (OER) and safety issues associated with H2 and O2 mixing. Here, we replaced OER with an electrocatalytic oxidative dehydrogenation (EOD) of aldehydes for bipolar H2 production and
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Solid Additive Tuning Polymer Blend Morphology Enables Non-halogenated-solvent All-polymer Solar Cells with Efficiency over 17% Energy Environ. Sci. (IF 39.714) Pub Date : 2022-08-12 Ke Hu, Can Zhu, Lei Meng, Kan Ding, Shucheng Qin, Wenbin Lai, Jiaqi Du, Jianqi Zhang, Zhixiang Wei, Xiaojun Li, Zhanjun Zhang, Harald Ade, Yongfang Li
All-polymer solar cells (all-PSCs) have attracted considerable interests, owing to their superior device stability and mechanical robustness. Recently, all-PSCs have achieved high power conversion efficiency (PCE) over 17% benefitted from the development of polymerized small molecular acceptors. However, most of the all-PSCs are processed with halogenated solvents that are hazardous for environment
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Nonplanar porphyrins: synthesis, properties, and unique functionalities Chem. Soc. Rev. (IF 60.615) Pub Date : 2022-08-12 Tomoya Ishizuka, Nitika Grover, Christopher J. Kingsbury, Hiroaki Kotani, Mathias O. Senge, Takahiko Kojima
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CRISPR/Cas12a-Responsive Dual-Aptamer DNA Network for Specific Capture and Controllable Release of Circulating Tumor Cells Chem. Sci. (IF 9.969) Pub Date : 2022-08-12 Dong-Xia Wang, Jing Wang, Yaxin Wang, Jia-Yi Ma, Bo Liu, An-na Tang, Deming Kong
The separation and detection of circulating tumor cells (CTCs) have a significant impact on clinical diagnosis and treatment by providing a predictive diagnosis of primary tumors and tumor metastasis. But the responsive release and downstream analysis of live CTCs will provide more valuable information about molecular markers and functional properties. To this end, specific capture and controllable
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Aromatic Heterobicycle-Fused Porphyrins: Impact on Aromaticity and Excited State Electron Transfer Leading to Long-Lived Charge Separation Chem. Sci. (IF 9.969) Pub Date : 2022-08-12 Austen Moss, Youngwoo B. Jang, Jacob Arvidson, Vladimir Nesterov, Francis D'Souza, Hong Wang
A new synthetic method to fuse benzo[4,5]imidazo[2,1-a]isoindole to the porphyrin periphery through the β, β-positions has been developed, and its impact on the aromaticity and electronic structures is investigated. Reactivity investigation of the fused benzoimidazo-isoindole component reveals fluorescence quenching of zinc porphyrin (AMIm-2) upon treatment of Brønsted acid. The reaction of zinc porphyrin
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Nickel-Catalyzed Arylative Substitution of Homoallylic Alcohols Chem. Sci. (IF 9.969) Pub Date : 2022-08-12 Hai N. Tran, Chau Nguyen, Mason T. Koeritz, Dustin Youmans, Levi Stanley
Direct coupling of unactivated alcohols remains a challenge in synthetic chemistry. Current approaches to cross-coupling of alcohol-derived electrophiles often involve activated alcohols such as tosylates or carbonates. We report the direct arylative substitution of homoallylic alcohols catalyzed by a nickel-bisphosphine complex as a facile method to generate allylic arenes. These reactions proceed
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Unprecedented pairs of uranium (IV/V) hydroxido and (IV/V/VI) oxido complexes supported by a seven-coordinate cyclen-anchored tris-aryloxide ligand Chem. Sci. (IF 9.969) Pub Date : 2022-08-12 Sascha T. Löffler, Julian Hümmer, Andreas Scheurer, Frank Heinemann, Karsten Meyer
We present the synthesis and reactivity of a newly developed, cyclen-based tris-aryloxide ligand, namely cyclen(Me)(t-Bu,t-BuArOH)3, and its coordination chemistry to uranium. The corresponding uranium(III) complex [UIII((OArt-Bu,t-Bu)3(Me)cyclen)] (1) was characterized by 1H NMR analysis, CHN elemental analysis and UV/vis/NIR electronic absorption spectros¬copy. Since no single-crystals suitable for
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Unraveling hydridic-to-protonic dihydrogen bond predominance in monohydrated dodecaborate clusters Chem. Sci. (IF 9.969) Pub Date : 2022-08-12 Yanrong Jiang, Qinqin Yuan, Wenjin Cao, Zhubin Hu, Yan Yang, Cheng Zhong, Tao Yang, Haitao Sun, Xue-Bin Wang, Zhenrong Sun
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Radical defects modulate the photocatalytic response in 2D-graphitic carbon nitride Chem. Sci. (IF 9.969) Pub Date : 2022-08-12 Edoardo Raciti, Sai Manoj Gali, Michele Melchionna, Giacomo Filippini, Arianna Actis, Mario Chiesa, Manuela Bevilacqua, Paolo Fornasiero, Maurizio Prato, David Beljonne, Roberto Lazzaroni
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N-doped nonalternant aromatic belt via a six-fold annulative double N-arylation Chem. Sci. (IF 9.969) Pub Date : 2022-08-09 Hiroki Sato, Rie Suizu, Tomoki Kato, Akiko Yagi, Yasutomo Segawa, Kunio Awaga, Kenichiro Itami
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Iron catalyzed deconstructive alkylation through chlorine radical induced C-C single bond cleavage under visible light Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Qiang Wu, Wei Liu, Miao Wang, Yahao Huang, Peng Hu
Selective C-C single bond cleavage of simple compounds is a highly challenging and desired process. Herein, a chlorine radical-induced deconstructive C-C bond alkylation with alcohols and alkenes catalyzed by iron salts was reported for the first time. Readily available alcohols and various electron-deficient alkenes were tolerated. Late-stage and large-scale reactions proceed smoothly. This catalyst
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Reactive oxygen species-responsive Pre-PROTAC for tumor-specific protein degradation Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Haixia Liu, Chaowei Ren, Renhong Sun, Huihui Wang, Yuexiong Zhan, Xiaobao Yang, Biao Jiang, Hongli Chen
By introducing a Reactive oxygen species (ROS) triggered leaving group (arylboronic acid) to the parent PROTACs. ROS-responsive Pre-PROTACs were designed and evaluated. Pre-PROTAC (7) efficiently degrade the target proteins BRD3 according to ROS levels. Our research provides an effective approach to control PROTAC activation by endogenous ROS-related microenvironment.
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A Golgi-targeted viscosity rotor for monitoring early Alcohol-Induced Liver Injury Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Chuan hao Liu, Lin Zhou, Ying Zheng, Huizi Man, Zhiwei Ye, Xinfu Zhang, Lijuan Xie, Yi Xiao
We proposed to monitor the early stage of alcohol-induced liver injury through quantitatively detecting Golgi viscosity. Therefore, the first Golgi-targeted fluorescent rotor (GA-Vis) was developed. With the aid of GA-Vis, the changes in Golgi viscosity during alcohol-induced liver injury was quantitatively evaluated by fluorescence lifetime imaging in live cells and zebrafishes. GA-Vis was qualified
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Facile high-yield synthesis and purification of lysine-modified graphene oxide for enhanced drinking water purification Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Sebastiano Mantovani, Sara Khaliha, Tainah Dorina Marforio, Alessandro Kovtun, Laura Favaretto, Francesca Tunioli, Antonio Bianchi, Gaetana Petrone, Andrea Liscio, Vincenzo Palermo, Matteo Calvaresi, Maria Luisa Navacchia, Manuela Melucci
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Novel Polymer-based Thermoresponsive Photonic Crystal Sensors with Broad Wavelength Shifts Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Lu Li, Jingjing Xu, Xin Lyu, Zhanfang Liu, Zihe Song, Juan Wei
Novel broad wavelength-shifted thermoresponsive sensors were fabricated by introducing ferrocene groups into polymeric photonic crystals. They are more suitable thermosensors due to their advantages, such as simple preparation, broad wavelength shifts (up to 162 nm), visible color change, and strong anti-interference ability.
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General Synthesis Strategy of ZrO2 Nanofilms with Few-Atom Layered Thickness for Boosting Triethylamine Detection Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Jie Lu, xiang huang, Yuanyu Xie, Hongjie Liu, Shaopeng Wang, yongchang Chen, liwei wang
ZrO2, a traditional inert transition metal oxide (TMO), can be prepared into ZrO2 Nanofilms (NFs) with a single layer thickness of only 2.5 nm through the generally applicable two-dimensional TMO synthesis strategy reported by us, which has displayed remarkable sensitivity and selectivity properties for triethylamine gas detection.
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γ-Agostic interactions in (MesCCC)Fe–Mes(L) complexes Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Daniel C. Najera, Marconi N. Peñas-Defrutos, Max García-Melchor, Alison R. Fout
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Asymmetric organocatalytic sulfenylation for the construction of a diheteroatom-bearing tetrasubstituted carbon centre Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Qingfa Tan, Qianping Chen, Zitong Zhu, Xiaohua Liu
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Selective C(sp2)–H bond functionalization of olefins via visible-light-induced photoredox-quinuclidine dual catalysis Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Xintao Gu, Long-Hai Li, Yin Wei, Min Shi
The site selective C(sp2)–H bond functionalization of olefins has been achieved through a visible-light-induced photoredox-quinuclidine dual catalysis upon merging quinuclidinium radical cation addition to alkene strategy and the distal heteroaryl ipso-migration strategy. This synthetic protocol features a simple operation with readily available starting materials in good step-economy to access alkenylheteroaromatic
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Development of Catalysts for Electrochemical Nitrogen Reduction toward Ammonia: Theoretical and Experimental Advances Chem. Commun. (IF 6.065) Pub Date : 2022-08-12 Yuhuan Cui, ChangNing SUN, Yanbin Qu, Tianyi Dai, Hongyu Zhou, Zhili Wang, Qing Jiang
Ammonia (NH3) is essential for the production of fertilizers, pharmaceuticals, plastics, synthetic fibers, resins, and chemicals in industry and is also a promising carbon free energy carrier. The electrocatalytic nitrogen reduction reaction (eNRR) driven by renewable energy sources at ambient temperature and atmospheric pressure is an alternative approach to the Haber-Bosch process for NH3 synthesis
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Structurally characterised intermediate of the oxidative addition of a heteroleptic germylene to gallanediyle Chem. Commun. (IF 6.065) Pub Date : 2022-08-08 Anna Bücker, Christoph Wölper, Gebhard Haberhauer, Stephan Schulz
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Air-stable aryl derivatives of pentafluoroorthotellurate Chem. Commun. (IF 6.065) Pub Date : 2022-08-08 Daniel Wegener, Kurt F. Hoffmann, Alberto Pérez-Bitrián, Ilayda Bayindir, Amiera N. Hadi, Anja Wiesner, Sebastian Riedel
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Probing the Dynamics of Low-Overpotential CO2-to-CO Activation on Copper Electrodes with Time-Resolved Raman Spectroscopy J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Jim de Ruiter, Hongyu An, Longfei Wu, Zamorano Gijsberg, Shuang Yang, Thomas Hartman, Bert M. Weckhuysen, Ward van der Stam
Oxide-derived copper electrodes have displayed a boost in activity and selectivity toward valuable base chemicals in the electrochemical carbon dioxide reduction reaction (CO2RR), but the exact interplay between the dynamic restructuring of copper oxide electrodes and their activity and selectivity is not fully understood. In this work, we have utilized time-resolved surface-enhanced Raman spectroscopy
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Photoswitchable Diazocine-Based Estrogen Receptor Agonists: Stabilization of the Active Form inside the Receptor J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Julia Ewert, Linda Heintze, Mireia Jordà-Redondo, Jan-Simon von Glasenapp, Santi Nonell, Götz Bucher, Christian Peifer, Rainer Herges
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Ultrafast Symmetry-Breaking Charge Separation in a Perylene Bisimide Dimer Enabled by Vibronic Coupling and Breakdown of Adiabaticity J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Yongseok Hong, Felix Schlosser, Woojae Kim, Frank Würthner, Dongho Kim
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Identification of Single Amino Acid Chiral and Positional Isomers Using an Electrostatically Asymmetric Nanopore J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Jiajun Wang, Jigneshkumar Dahyabhai Prajapati, Fan Gao, Yi-Lun Ying, Ulrich Kleinekathöfer, Mathias Winterhalter, Yi-Tao Long
Chirality is essential in nearly all biological organizations and chemical reactions but is rarely considered due to technical limitations in identifying L/D isomerization. Using OmpF, a membrane channel from Escherichia coli with an electrostatically asymmetric constriction zone, allows discriminating chiral amino acids in a single peptide. The heterogeneous distribution of charged residues in OmpF
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Dynamical Study of Adsorbate-Induced Restructuring Kinetics in Bimetallic Catalysts Using the PdAu(111) Model System J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Chen Zhou, Hio Tong Ngan, Jin Soo Lim, Zubin Darbari, Adrian Lewandowski, Dario J. Stacchiola, Boris Kozinsky, Philippe Sautet, Jorge Anibal Boscoboinik
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Kinetically Controlled Structural Transitions in Layered Halide-Based Perovskites: An Approach to Modulate Spin Splitting J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Yi Xie, Ruyi Song, Akash Singh, Manoj K. Jana, Volker Blum, David B. Mitzi
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A Ribonucleotide ↔ Phosphoramidate Reaction Network Optimized by Computer-Aided Design J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Andreas Englert, Julian F. Vogel, Tim Bergner, Jessica Loske, Max von Delius
A growing number of out-of-equilibrium systems have been created and investigated in chemical laboratories over the past decade. One way to achieve this is to create a reaction cycle, in which the forward reaction is driven by a chemical fuel and the backward reaction follows a different pathway. Such dissipative reaction networks are still relatively rare, however, and most non-enzymatic examples
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Mechanistic Investigations of the Asymmetric Hydrogenation of Enamides with Neutral Bis(phosphine) Cobalt Precatalysts J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Lauren N. Mendelsohn, Ljiljana Pavlovic, Hongyu Zhong, Max R. Friedfeld, Michael Shevlin, Kathrin H. Hopmann, Paul J. Chirik
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Enantioselective Cobalt-Catalyzed Hydroboration of Fluoroalkyl-Substituted Alkenes to Access Chiral Fluoroalkylboronates J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Ming Hu, Boon Beng Tan, Shaozhong Ge
Selective defluoroborylation and asymmetric hydroboration reactions of fluoroalkyl-substituted terminal alkenes with pinacolborane (HBpin) have been developed with cobalt catalysts generated from Co(acac)2 and bisphosphine ligands. A variety of fluoroalkyl-substituted terminal alkenes undergo this enantioselective hydroboration, affording the corresponding chiral alkylboronates containing fluoroalkyl-substituted
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Passive Macromolecular Translocation Mechanism through Lipid Membranes J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Ekaterina Kostyurina, Jürgen Allgaier, Margarita Kruteva, Henrich Frielinghaus, Agnes Csiszár, Stephan Förster, Ralf Biehl
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Site- and Enantioselective Manganese-Catalyzed Benzylic C–H Azidation of Indolines J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Min Cao, Hongliang Wang, Yingang Ma, Chen-Ho Tung, Lei Liu
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Unprecedented Small Molecule-Based Uniform Two-Dimensional Platelets with Tailorable Shapes and Sizes J. Am. Chem. Soc. (IF 16.383) Pub Date : 2022-08-11 Yanjun Gong, Chuanqin Cheng, Hongwei Ji, Yanke Che, Ling Zang, Jincai Zhao, Yifan Zhang
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Two-Dimensional Nanoradiosensitizer Enhances Radiotherapy and Delivers STING Agonists to Potentiate Cancer Immunotherapy Adv. Mater. (IF 32.086) Pub Date : 2022-08-11 Taokun Luo, Geoffrey T. Nash, Xiaomin Jiang, Xuanyu Feng, Jianming Mao, Jianqiao Liu, Aditya Juloori, Alexander T. Pearson, Wenbin Lin
Despite potent preclinical antitumor activity, activation of stimulator of interferon genes (STING) has shown modest therapeutic effects in clinical studies. Many STING agonists including 2’,3’-cyclic guanosine monophosphate–adenosine monophosphate (cGAMP) show poor pharmacokinetic properties for sustaining STING activation in tumors and achieving optimal antitumor efficacy. Improved delivery of STING
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3D Printing Flexible Sodium Ion Micro-batteries with Ultrahigh Areal Capacity and Robust Rate Capability Adv. Mater. (IF 32.086) Pub Date : 2022-08-11 Jiaxin Ma, Shuanghao Zheng, Liping Chi, Yu Liu, Ying Zhang, Kai Wang, Zhong-Shuai Wu
Rechargeable sodium ion micro-batteries (NIMBs) constructed using low-cost and abundant raw materials in planar configuration with both cathode and anode on the same substrate, hold promises for powering coplanar microelectronics, but are hindered by the low areal capacity owing to thin microelectrodes. Here, a prototype of planar and flexible 3D-printed NIMBs is demonstrated with three-dimensionally
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Reductive Cross-Coupling of Unreactive Electrophiles Acc. Chem. Res. (IF 24.466) Pub Date : 2022-08-11 Xiaobo Pang, Pei-Feng Su, Xing-Zhong Shu
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Reactivation of chromia poisoned oxygen exchange kinetics in mixed conducting solid oxide fuel cell electrodes by serial infiltration of lithia Energy Environ. Sci. (IF 39.714) Pub Date : 2022-08-11 Han Gil Seo, Anna Friederike Staerz, Dennis S Kim, Dino Klotz, Clement Nicollet, Michael Xu, James M LeBeau, Harry L. Tuller
Solid oxide fuel cells have the potential to render the conversion from fuel to electrical energy more efficienct while lowering emissions. The technology, however, suffers from performance degradation due to cathode poisoning by chromia from metal interconnects. We confirm the deleterious impact of chromia on the performance of the model mixed conducting cathode material Pr0.1Ce0.9O2- by examining
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Coherent Ring-Current Migration of Mg-Phthalocyanine Probed by Time-Resolved X-Ray Circular Dichroism Chem. Sci. (IF 9.969) Pub Date : 2022-08-11 Shichao Sun, Haiwang Yong, Feng Chen, S. Mukamel
The coherent ring current of Mg-phthalocyanine created by a broad band UV-visible pump pulse shows variation with time, where the ring currents at the corner benzene rings, around the Mg cation and on the outer ring oscillate with different time periods and the current density migrates among these regions. The 7 pairs of Eu degenerate excited states populated upon photoexcitation, generate 21 distinct
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Investigating the role of the strong field ligands in [FeFe] hydrogenase: Spectroscopic and functional characterization of a semi-synthetic mono-cyanide active site Chem. Sci. (IF 9.969) Pub Date : 2022-08-11 Marco Lorenzi, Joe Gellett, Afridi Zamader, Moritz Senger, Zehui Duan, Patricia Rodriguez Macia, Gustav Berggren
Artificial maturation of hydrogenases provides a path towards generating new semi-synthetic enzymes with novel catalytic properties. Here enzymes featuring a synthetic asymmetric mono-cyanide cofactor have been prepared using two different hydrogenase scaffolds. Their structure and reactivity was investigated in order to elucidate the design rationale behind the native di-cyanide cofactor, and by extension
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Iron-catalysed Alkene and Heteroarene H/D Exchange by Reversible Protonation of Iron-hydride Intermediates Chem. Sci. (IF 9.969) Pub Date : 2022-08-11 Luke Britton, Jamie Docherty, Jan Sklyaruk, Jessica Cooney, Gary Stephen Nichol, Andrew Dominey, Stephen P. Thomas
C-H functionalisation reactions offer a sustainable method for molecular construction and diversification. These reactions however remain dominated by precious metal catalysis. While significant interest in iron-catalysed C-H activation reactions has emerged, the isolation, characterisation and mechanistic understanding of these processes remain lacking. Herein the iron-catalysed C(sp2)-H bond hydrogen/deuterium
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Collective Adaptability in a Replication Network of Minimal Nucleobase Sequences Chem. Sci. (IF 9.969) Pub Date : 2022-08-11 Sonia Vela, Zulay D. Pardo Botero, Cristian Moya, Andres De la Escosura
A major challenge for understanding the origins of life is to explore how replication networks can engage in an evolutionary process. Herein, we shed light on this problem by implementing a network constituted by two different types of extremely simple biological components: the amino acid cysteine and the canonical nucleobases adenine and thymine, connected through amide bonds to the cysteine amino
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Isolating elusive 'Al(μ-O)M' intermediates in CO2 reduction by bimetallic Al–M complexes (M = Zn, Mg) Chem. Commun. (IF 6.065) Pub Date : 2022-08-11 Matthew J Evans, George Iliffe, Samuel E Neale, Claire L. McMullin, J. Robin Fulton, Mathew David Anker, Martyn P Coles
The reaction of compounds containing Al–Mg and Al–Zn bonds with N2O enabled isolation of the corresponding Al(μ-O)M complexes. Electronic structure analysis identified largely ionic Al–O and O–M bonds, featuring an anionic μ-oxo centre. Reaction with CO2 confirmed that these species correspond to the proposed intermediates in the formation of μ-carbonate compounds.
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Regulation of coordination and doping environment via target molecular for boosting selective photocatalytic ability Chem. Commun. (IF 6.065) Pub Date : 2022-08-11 Guosheng Zhou, Yu Cheng, Zehui Yu, Xinlin Liu, Dehai Chen, Jiaqi Wang, Ying Hang, Yangrui Xu, Chunxiang Li, Ziyang Lu
Here, a novel transformed CdO with low coordination and N doping environment was simply synthesized through the involvement of the target molecule tetracycline (TC). The results showed that the shedding of surface hydroxyl groups led to low coordination environment, and N doping formed a new doping energy level, which increased the charge density and promoted the migration and separation of photo-generated
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Revival of Ferroelectric Memories Based on Emerging Fluorite-Structured Ferroelectrics Adv. Mater. (IF 32.086) Pub Date : 2022-08-11 Ju Yong Park, Duk-Hyun Choe, Dong Hyun Lee, Geun Taek Yu, Kun Yang, Se Hyun Kim, Geun Hyeong Park, Seung-Geol Nam, Hyun Jae Lee, Sanghyun Jo, Bong Jin Kuh, Daewon Ha, Yongsung Kim, Jinseong Heo, Min Hyuk Park
Over the last few decades, the research on ferroelectric memories has been limited due to their dimensional scalability and incompatibility with complementary metal-oxide-semiconductor (CMOS) technology. The discovery of ferroelectricity in fluorite-structured oxides revived interest in the research on ferroelectric memories, with inducing nanoscale nonvolatility in state-of-the-art gate insulators
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Technological breakthroughs in chip fabrication, transfer, and color conversion for high performance micro-LED display Adv. Mater. (IF 32.086) Pub Date : 2022-08-11 Jung-El Ryu, Sohyeon Park, Yongjo Park, Sang-Wan Ryu, Kyungwook Hwang, Ho Won Jang
The implementation of high efficiency and high-resolution displays has been the focus of considerable research interest. Recently, micro-LEDs, which are inorganic light-emitting diodes of size less than 100 μm2, have emerged as a promising display technology owing to their superior features and advantages over other displays like liquid crystal displays and organic light-emitting diodes. Although many
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Recent Progress in Strain Engineering on Van der Waals 2D Materials: Tunable Electrical, Electrochemical, Magnetic and Optical Properties Adv. Mater. (IF 32.086) Pub Date : 2022-08-11 Yaping Qi, Mohammad A. Sadi, Dan Hu, Ming Zheng, Zhenping Wu, Yucheng Jiang, Yong P. Chen
Strain engineering is a promising way to tune the electrical, electrochemical, magnetic, and optical properties of two-dimensional (2D) materials, with the potential to achieve high-performance 2D-material-based devices ultimately. This review discusses the experimental and theoretical results from recent advances in the strain engineering of 2D materials. We summarize some novel methods to induce
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Antiferromagnetic-Ferromagnetic Heterostructure-based Field-Free Terahertz Emitters Adv. Mater. (IF 32.086) Pub Date : 2022-08-11 Xiaojun Wu, Hanchen Wang, Haijiang Liu, Yizhan Wang, Xinhou Chen, Peng Chen, Peiyan Li, Xiufeng Han, Jungang Miao, Haiming Yu, Caihua Wan, Jimin Zhao, Sai Chen
Recently, ferromagnetic heterostructure spintronic terahertz (THz) emitters have been recognized as one of the most promising candidates for the next-generation THz sources, owing to their peculiarities of high efficiency, high stability, low cost, ultrabroad bandwidth, controllable polarization, and high scalability. Despite the substantial efforts, they rely on external magnetic fields to initiate
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Balanced interfacial ion concentration and migration steric hindrance promoting high-efficiency deposition/dissolution battery chemistry Adv. Mater. (IF 32.086) Pub Date : 2022-08-11 Zhexuan Liu, Lanyan Li, Liping Qin, Shan Guo, Guozhao Fang, Zhigao Luo, Shuquan Liang
Solid-liquid transition reaction lays the foundation of many electrochemical energy storage systems with high capacity, but realizing high efficiency of this reaction remain a challenge. Herein, in terms of thermodynamics and dynamics, this work demonstrates the significant role of both interfacial H+ ion concentration and Mn2+ ion migration steric hindrance for the high-efficiency deposition/dissolution