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Chromium Nitride Umpolung Tuned by the Locus of Oxidation J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Diego Martelino, Samyadeb Mahato, Warren VandeVen, Nicholas M. Hein, Ryan M. Clarke, Gregory A. MacNeil, Fabrice Thomas, Tim Storr
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Continuous-Flow Reactor Synthesis for Homogeneous 1 nm-Sized Extremely Small High-Entropy Alloy Nanoparticles J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Hiroki Minamihara, Kohei Kusada, Dongshuang Wu, Tomokazu Yamamoto, Takaaki Toriyama, Syo Matsumura, Loku Singgapulige Rosantha Kumara, Koji Ohara, Osami Sakata, Shogo Kawaguchi, Yoshiki Kubota, Hiroshi Kitagawa
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Templating Bicarbonate in the Second Coordination Sphere Enhances Electrochemical CO2 Reduction Catalyzed by Iron Porphyrins J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Jeffrey S. Derrick, Matthias Loipersberger, Sepand K. Nistanaki, Aila V. Rothweiler, Martin Head-Gordon, Eva M. Nichols, Christopher J. Chang
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An Artificial Metalloenzyme Based on a Copper Heteroscorpionate Enables sp3 C–H Functionalization via Intramolecular Carbene Insertion J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Corentin Rumo, Alina Stein, Juliane Klehr, Ryo Tachibana, Alessandro Prescimone, Daniel Häussinger, Thomas R. Ward
The selective functionalization of sp3 C–H bonds is a versatile tool for the diversification of organic compounds. Combining attractive features of homogeneous and enzymatic catalysts, artificial metalloenzymes offer an ideal means to selectively modify these inert motifs. Herein, we report on a copper(I) heteroscorpionate complex embedded within streptavidin that catalyzes the intramolecular insertion
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Oxygen Vacancy-Mediated Selective C–N Coupling toward Electrocatalytic Urea Synthesis J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Xiaoxiao Wei, Xiaojian Wen, Yingying Liu, Chen Chen, Chao Xie, Dongdong Wang, Mengyi Qiu, Nihan He, Peng Zhou, Wei Chen, Jun Cheng, Hongzhen Lin, Jianfeng Jia, Xian-Zhu Fu, Shuangyin Wang
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Palladium Mediated Synthesis of Protein–Polyarene Conjugates J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Jacob Rodriguez, Heemal H. Dhanjee, Bradley L. Pentelute, Stephen L. Buchwald
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Intrinsically Re-curable Photopolymers Containing Dynamic Thiol-Michael Bonds J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Connor J. Stubbs, Anissa L. Khalfa, Viviane Chiaradia, Joshua C. Worch, Andrew P. Dove
The development of photopolymers that can be depolymerized and subsequently re-cured using the same light stimulus presents a significant technical challenge. A bio-sourced terpenoid structure, l-carvone, inspired the creation of a re-curable photopolymer in which the orthogonal reactivity of an irreversible thioether and a dynamic thiol-Michael bond enables both photopolymerization and thermally driven
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Reversible Structural Isomerization of Nature’s Water Oxidation Catalyst Prior to O–O Bond Formation J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Yu Guo, Johannes Messinger, Lars Kloo, Licheng Sun
Photosynthetic water oxidation is catalyzed by a manganese–calcium oxide cluster, which experiences five “S-states” during a light-driven reaction cycle. The unique “distorted chair”-like geometry of the Mn4CaO5(6) cluster shows structural flexibility that has been frequently proposed to involve “open” and “closed”-cubane forms from the S1 to S3 states. The isomers are interconvertible in the S1 and
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Structural Basis for Dityrosine-Mediated Inhibition of α-Synuclein Fibrillization J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Cagla Sahin, Eva Christina Østerlund, Nicklas Österlund, Joana Costeira-Paulo, Jannik Nedergaard Pedersen, Gunna Christiansen, Janni Nielsen, Anne Louise Grønnemose, Søren Kirk Amstrup, Manish K. Tiwari, R. Shyama Prasad Rao, Morten Jannik Bjerrum, Leopold L. Ilag, Michael J. Davies, Erik G. Marklund, Jan Skov Pedersen, Michael Landreh, Ian Max Møller, Thomas J. D. Jørgensen, Daniel Erik Otzen
α-Synuclein (α-Syn) is an intrinsically disordered protein which self-assembles into highly organized β-sheet structures that accumulate in plaques in brains of Parkinson’s disease patients. Oxidative stress influences α-Syn structure and self-assembly; however, the basis for this remains unclear. Here we characterize the chemical and physical effects of mild oxidation on monomeric α-Syn and its aggregation
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Inherent Minor Conformer of Bordetella Effector BteA Directs Chaperone-Mediated Unfolding J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Adi Yahalom, Hadassa Shaked, Sharon Ruthstein, Jordan H. Chill
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Ultralow-Loading Pt/Zn Hybrid Cluster in Zeolite HZSM-5 for Efficient Dehydroaromatization J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Genwei Chen, Lingzhe Fang, Tao Li, Yizhi Xiang
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Conformational Flexibility as a Tool for Enabling Site-Selective Functionalization of Unactivated sp3 C–O Bonds in Cyclic Acetals J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Ciro Romano, Laura Talavera, Enrique Gómez-Bengoa, Ruben Martin
A dual catalytic manifold that enables site-selective functionalization of unactivated sp3 C–O bonds in cyclic acetals with aryl and alkyl halides is reported. The reaction is triggered by an appropriate σ*–p orbital overlap prior to sp3 C–O cleavage, thus highlighting the importance of conformational flexibility in both reactivity and site selectivity. The protocol is characterized by its excellent
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Synergistic Stimulation of Metal–Organic Frameworks for Stable Super-cooled Liquid and Quenched Glass J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Zheng Yin, Yingbo Zhao, Shuang Wan, Jian Yang, Zhaolin Shi, Si-Xu Peng, Ming-Zhu Chen, Tian-Yi Xie, Teng-Wu Zeng, Osamu Yamamuro, Masami Nirei, Hiroshi Akiba, Yue-Biao Zhang, Hai-Bin Yu, Ming-Hua Zeng
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In Situ Mechanistic Insights for the Oxygen Reduction Reaction in Chemically Modulated Ordered Intermetallic Catalyst Promoting Complete Electron Transfer J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Soumi Mondal, Debabrata Bagchi, Mohd Riyaz, Shreya Sarkar, Ashutosh Kumar Singh, C. P. Vinod, Sebastian C. Peter
The well-known limitation of alkaline fuel cells is the slack kinetics of the cathodic half-cell reaction, the oxygen reduction reaction (ORR). Platinum, being the most active ORR catalyst, is still facing challenges due to its corrosive nature and sluggish kinetics. Many novel approaches for substituting Pt have been reported, which suffer from stability issues even after mighty modifications. Designing
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Structural Basis of Pyridostatin and Its Derivatives Specifically Binding to G-Quadruplexes J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Liu-Yi Liu, Tian-Zhu Ma, You-Liang Zeng, Wenting Liu, Zong-Wan Mao
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Ligand-Field Spectroscopy of Co(III) Complexes and the Development of a Spectrochemical Series for Low-Spin d6 Charge-Transfer Chromophores J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-24 Jonathan T. Yarranton, James K. McCusker
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Detection of Few Hydrogen Peroxide Molecules Using Self-Reporting Fluorescent Nanodiamond Quantum Sensors J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-23 Yingke Wu, Priyadharshini Balasubramanian, Zhenyu Wang, Jaime A. S. Coelho, Mateja Prslja, Reiner Siebert, Martin B. Plenio, Fedor Jelezko, Tanja Weil
Hydrogen peroxide (H2O2) plays an important role in various signal transduction pathways and regulates important cellular processes. However, monitoring and quantitatively assessing the distribution of H2O2 molecules inside living cells requires a nanoscale sensor with molecular-level sensitivity. Herein, we show the first demonstration of sub-10 nm-sized fluorescent nanodiamonds (NDs) as catalysts
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Identifying the Real Chemistry of the Synthesis and Reversible Transformation of AuCd Bimetallic Clusters J. Am. Chem. Soc. (IF 15.419) Pub Date : 2022-06-23 Huixin Xiang, Hao Yan, Jiaohu Liu, Ranran Cheng, Cong-Qiao Xu, Jun Li, Chuanhao Yao
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Artificial Intelligence in Meta-optics Chem. Rev. (IF 60.622) Pub Date : 2022-06-24 Mu Ku Chen, Xiaoyuan Liu, Yanni Sun, Din Ping Tsai
Recent years have witnessed promising artificial intelligence (AI) applications in many disciplines, including optics, engineering, medicine, economics, and education. In particular, the synergy of AI and meta-optics has greatly benefited both fields. Meta-optics are advanced flat optics with novel functions and light-manipulation abilities. The optical properties can be engineered with a unique design
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Engineering van der Waals Materials for Advanced Metaphotonics Chem. Rev. (IF 60.622) Pub Date : 2022-06-24 Han Lin, Zhenfang Zhang, Huihui Zhang, Keng-Te Lin, Xiaoming Wen, Yao Liang, Yang Fu, Alan Kin Tak Lau, Tianyi Ma, Cheng-Wei Qiu, Baohua Jia
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Recent Advances in Microscale Electroporation Chem. Rev. (IF 60.622) Pub Date : 2022-06-23 Sung-Eun Choi, Harrison Khoo, Soojung Claire Hur
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X-ray Raman Scattering: A Hard X-ray Probe of Complex Organic Systems Chem. Rev. (IF 60.622) Pub Date : 2022-06-23 Rafaella Georgiou, Christoph J. Sahle, Dimosthenis Sokaras, Sylvain Bernard, Uwe Bergmann, Jean-Pascal Rueff, Loïc Bertrand
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Water vapour induced reversible switching between a 1-D coordination polymer and a 0-D aqua complex Chem. Commun. (IF 6.222) Pub Date : 2022-06-24 Michael Zaworotko, Ming Deng, Soumya Mukherjee, Yu-Jie Liang, Xiao-Dan Fang, Ai-Xin Zhu
[Zn(3-tba)2], 1, a 1-D coordination polymer synthesised as 1·DMA, 1α, transformed to a nonporous form, 1β upon activation. 1β underwent further transformation to the dimeric complex [Zn(3-tba)2(H2O)2], 2, above 40% RH. The reverse transformations, 2 to 1β and 1β to 1α, were accomplished by heating and exposure to DMA, respectively, and were single-crystal-to-single-crystal phase changes. Single crystal
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Native Mass Spectrometry at the Convergence of Structural Biology and Compositional Proteomics Acc. Chem. Res. (IF 22.384) Pub Date : 2022-06-24 Kevin Jooß, John P. McGee, Neil L. Kelleher
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Superconducting Material Based Maglev Generator Used for Outer-Space Adv. Mater. (IF 30.849) Pub Date : 2022-06-24 Zheng Ma, Qi Wang, Zhenhua Wu, Dezhi Chen, Chunze Yan, Yusheng Shi, Michael D. Dickey, Bin Su
Solar cells are conventionally used to harvest energy in outer space, but they are ineffective in dark locations. Here, we show that superconducting materials – which work best in cold environments, such as those found in outer space—provide a mechanism to harvest energy that does not require light. A superconducting maglev (magnetic levitation) magnetoelectric generator (SMMG) can convert mechanical
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Turbostratic Boron-Carbon-Nitrogen and Boron-Nitride by Flash Joule Heating Adv. Mater. (IF 30.849) Pub Date : 2022-06-24 Weiyin Chen, John Tianci Li, Chang Ge, Zhe Yuan, Wala A. Algozeeb, Paul A. Advincula, Guanhui Gao, Jinhang Chen, Kexin Ling, Chi Hun Choi, Emily A. McHugh, Kevin M. Wyss, Duy Xuan Luong, Zhe Wang, Yimo Han, James M. Tour
Turbostratic layers in 2D materials have an interlayer misalignment. The lack of alignment expands the intrinsic interlayer distances and weakens the optical and electronic interactions between adjacent layers. This introduces properties distinct from those structures with well-aligned lattices and strong coupling interactions. However, direct, and rapid synthesis of turbostratic materials remains
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Composition Engineering of Amorphous Nickel Boride Nanoarchitectures Enabling Highly Efficient Electrosynthesis of Hydrogen Peroxide Adv. Mater. (IF 30.849) Pub Date : 2022-06-23 Jie Wu, Meilin Hou, Ziliang Chen, Weiju Hao, Xuelei Pan, Hongyuan Yang, Wanglai Cen, Yang Liu, Hui Huang, Prashanth W. Menezes, Zhenhui Kang
Developing advanced electrocatalysts with exceptional two electron (2e–) selectivity, activity and stability are crucial for driving oxygen reduction reaction (ORR) to produce hydrogen peroxide (H2O2). Herein, a composition engineering strategy has been adapted to flexibly regulate the intrinsic activity of amorphous nickel boride nanoarchitectures for efficient 2e– ORR by oriented reduction of Ni2+
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Dinitrogen Binding at a Trititanium Chloride Complex and Its Conversion to Ammonia under Ambient Conditions Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Carlos Yelamos, Estefania del Horno, Jesus Jover, Miguel Mena, Adrian Perez-Redondo
Reaction of [TiCp*Cl3] (Cp* = η5-C5Me5) with one equivalent of magnesium in tetrahydrofuran at room temperature affords the paramagnetic trinuclear complex [{TiCp*(μ-Cl)}3(μ3-Cl)], which reacts with dinitrogen under ambient conditions to give the diamagnetic derivative [{TiCp*(μ-Cl)}3(μ3-η1:η2:η2-N2)] and the titanium(III) dimer [{TiCp*Cl(μ-Cl)}2]. The structure of the trinuclear mixed-valence complexes
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Explaining Regio-Divergent Vinylations with Vinylbenziodoxolones Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Ester Maria Di Tommaso, Per-Ola Norrby, Berit Olofsson
Vinylbenziodoxolones have recently been identified as efficient hypervalent iodine(III) reagents for electrophilic vinylations under transition metal-free conditions. Their unique reactivity allows synthesis of either internal or terminal alkenes, depending on the nucleophile class. This paper constitutes the first mechanistic investigation of VBX vinylations, and makes use of NMR studies, deuterium
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Enhanced promotion of Ru-based ammonia catalysts by in situ dosing of Cs Energy Environ. Sci. (IF 38.532) Pub Date : 2022-06-24 Vahid Shadravan, ANG CAO, Vanessa Jane Bukas, Mette K. Grønborg, Christian Danvand Damsgaard, Zhenbin Wang, Jakob Kibsgaard, Jens Kehlet Norskov, Ib Chorkendorff
Ammonia synthesis via the high-temperature and -pressure Haber-Bosch (HB) process at large centralized facilities has a significant contribution to the global CO2 emission. Radically new catalysts should be discovered to enable sustainable ammonia synthesis processes that can operate at much lower temperatures to relax the demand for the high pressure in the current HB process. In this manner, the
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Single-Molecule Magnets beyond a Single Lanthanide Ion: The Art of Coupling Chem. Sci. (IF 9.825) Pub Date : 2022-06-24 Yan-Cong Chen, Ming-Liang Tong
The promising future of storing and processing quantized information at the molecular level has been attracting the study of Single-Molecule Magnets (SMMs) for almost three decades. Although some recent breakthroughs are mainly about the SMMs containing only one lanthanide ion, we believe SMMs can tell much deeper story than the single-ion anisotropy. Here in this Perspective, we will try to draw a
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Enzyme-photo-coupled catalysis in gas-sprayed microdroplets Chem. Sci. (IF 9.825) Pub Date : 2022-06-24 Yunxiu Bai, Pengqian Luan, Yunpeng Bai, Richard N. Zare, Jun Ge
Enzyme-photo-coupled catalysis produces fine chemicals by combining the high selectivity of an enzyme with the green energy input of sunlight. Operating a large-scale system, however, remains challenging because of the significant loss of enzyme activity caused by continuous illumination and the difficulty in utilizing solar energy with high efficiency at large scale. We present a large-scale enzyme-photo-couple
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Revealing Hydrogen Spillover Pathways in Reducible Metal Oxides Chem. Sci. (IF 9.825) Pub Date : 2022-06-24 Kazuki Shun, Kohsuke Mori, Shinya Masuda, Naoki Hashimoto, Yoyo Hinuma, Hisayoshi Kobayashi, Hiromi Yamashita
Hydrogen spillover, the migration of dissociated hydrogen atoms from noble metal to their support materials, is a ubiquitous phenomenon and is widely utilized in heterogeneous catalysis and hydrogen storage materials. However, in-depth understanding of the migration of spilled hydrogen over different types of supports is still lacking. Herein, hydrogen spillover in typical reducible metal oxides, such
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Substrate access path-guided engineering of L-threonine aldolase for improving diastereoselectivity Chem. Commun. (IF 6.222) Pub Date : 2022-06-24 Wenlong Zheng, Zhongji Pu, Lanxin Xiao, Gang Xu, Li-Rong Yang, Haoran Yu, Jianping Wu
The L-threonine aldolase from Leishmania major was engineered to improve diastereoselectivity by a CAST/ISM strategy, providing insights into the relationship between physico -chemical properties of substrate access path and diastereoselectivity. The steric hindrance, hydrophobic interaction and π-π interaction cooperated to improve diastereoselectivity of the enzyme, with a diastereomeric excess (de)
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A Top-down Strategy to Engineer Active Layer Morphology for Highly Efficient and Stable All-polymer Solar Cells Adv. Mater. (IF 30.849) Pub Date : 2022-06-24 Huiting Fu, Zhengxing Peng, Qunping Fan, Francis R. Lin, Feng Qi, Yixin Ran, Ziang Wu, Baobing Fan, Kui Jiang, Han Young Woo, Guanghao Lu, Harald Ade, Alex K.-Y. Jen
A major challenge hindering the further development of all-polymer solar cells (all-PSCs) employing polymerized small-molecule acceptors is the relatively low fill factor (FF) due to the difficulty in controlling active layer morphology. The issues typically arise from oversized phase separation resulting from the thermodynamically unfavorable mixing between two macromolecular species, and disordered
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Promoting Dinuclear-Type Catalysis in Cu1-C3N4 Single Atom Catalyst Adv. Mater. (IF 30.849) Pub Date : 2022-06-24 Jingting Song, Zhongxin Chen, Xiangbin Cai, Xin Zhou, Gaolei Zhan, Runlai Li, Pingping Wei, Ning Yan, Shibo Xi, Kian Ping Loh
Reducing particle size in supported metal catalyst to single atom level isolates the active metal sites and maximizes the atomic utilization efficiency. However, the large inter-atom distance, particularly in low-loading single atom catalyst (SAC), is not favourable for a complex reaction where two (or more) reactants have to be activated. A key question is how to control the inter-atom distances to
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Switchable unipolar-barrier van der Waals heterostructures with natural anisotropy for full linear polarimetry detection Adv. Mater. (IF 30.849) Pub Date : 2022-06-24 Wenjie Deng, Mingjin Dai, Chongwu Wang, Congya You, Wenduo Chen, Song Han, Jiayue Han, Fakun Wang, Ming Ye, Song Zhu, Jieyuan Cui, Qi Jie Wang, Yongzhe Zhang
Polarization-resolved photodetection in a compact footprint is of great interests for ultra-miniaturized polarimeter to be used in a wide range of applications. However, states of polarization (SOP) probing in natural anisotropy materials are usually weak, limited by material's natural dichroism or diattenuation. Here, we report a twisted unipolar-barrier van der Waals heterostructure (vdWH) to construct
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Necklace-like Nanostructures: from Fabrication, Properties to Applications Adv. Mater. (IF 30.849) Pub Date : 2022-06-24 Lei Zhang, Gill M. Biesold, Chunyan Zhao, Hui Xu, Zhiqun Lin
The shape-controlled synthesis of nanocrystals remains a hot research topic in nanotechnology. Particularly, the fabrication of one-dimensional (1D) structures such as wires, rods, belts, and tubes has been an interesting and important subject within nanoscience in the last few decades. 1D necklace-like micro/nano-structures are a sophisticated geometry that has attracted increasing attention due to
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Brain Codelivery of Temozolomide and Cisplatin for Combinatorial Glioblastoma Chemotherapy Adv. Mater. (IF 30.849) Pub Date : 2022-06-23 Yan Zou, Yibin Wang, Sen Xu, Yanjie Liu, Jinlong Yin, David B. Lovejoy, Meng Zheng, Xing-Jie Liang, Jong Bae Park, Yuri M. Efremov, Ilya Ulasovand, Bingyang Shi
Glioblastoma (GBM) is an intractable malignancy with high recurrence and mortality. Temozolomide (TMZ) and cisplatin (CDDP) based combinational therapy shows promising potential for GBM therapy in clinical trials. However, significant challenges include limited blood-brain-barrier (BBB) penetration, poor targeting of GBM tissue/cells and systemic side effect which hinder its efficacy in GBM therapy
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Dynamic Surface Evolution of Metal Oxides for Autonomous Adaptation to Catalytic Reaction Environments Adv. Mater. (IF 30.849) Pub Date : 2022-06-23 Jun Kyu Kim, Sangwoo Kim, Seunghyun Kim, Hyung Jun Kim, Kyeounghak Kim, WooChul Jung, Jeong Woo Han
Metal oxides possessing distinctive physical/chemical properties due to different crystal structures and stoichiometries play a pivotal role in numerous current technologies, especially heterogeneous catalysis for production/conversion of high-valued chemicals and energy. To date, many researchers have investigated the effect of the structure and composition of these materials on their reactivity to
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Spontaneous Construction of Nucleophilic Carbonyl-Containing Interphase towards Ultra-Stable Zinc Metal Anodes Adv. Mater. (IF 30.849) Pub Date : 2022-06-23 Pinji Wang, Shuquan Liang, Chen Chen, Xuesong Xie, Jiawen Chen, Zhenhan Liu, Yan Tang, Bingan Lu, Jiang Zhou
Multifunctional interfacial engineering on Zn anode to conquer the dendrite growth, hydrogen evolution and sluggish kinetics associated with Zn deposition is highly desirable for boosting the commercialization of aqueous zinc-ion batteries. Herein, a spontaneous construction of carbonyl-containing layer on Zn anode (Zn@ZCO) is rationally designed as an ion redistributor and functional protective interphase
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Formulating High-Rate and Long-Cycle Heterostructured Layered Oxide Cathodes by Local Chemistry and Orbital Hybridization Modulation for Sodium-ion Batteries Adv. Mater. (IF 30.849) Pub Date : 2022-06-23 Yao Xiao, Hong-Rui Wang, Hai-Yan Hu, Yan-Fang Zhu, Shi Li, Jia-Yang Li, Xiong-Wei Wu, Shu-Lei Chou
It is still very urgent and challenging to simultaneously develop high-rate and long-cycle oxide cathodes for sodium-ion batteries (SIBs) because of its sluggish kinetics and complex multiphase evolution during cycling. Here, we report the concept of accurately manipulating structural evolution and formulating high-performance heterostructured biphasic layered oxide cathodes by local chemistry and
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Binary Organic Solar Cells Breaking 19% via Manipulating Vertical Component Distribution Adv. Mater. (IF 30.849) Pub Date : 2022-06-23 Yanan Wei, Zhihao Chen, Guanyu Lu, Na Yu, Congqi Li, Jinhua Gao, Xiaobin Gu, Xiaotao Hao, Guanghao Lu, Zheng Tang, Jianqi Zhang, Zhixiang Wei, Xin Zhang, Hui Huang
The variation of vertical component distribution can significantly influence photovoltaic performance of organic solar cells (OSCs), mainly due to its impact on the exciton dissociation, and the charge carrier transport and recombination. Herein, the binary devices are fabricated via sequential deposition (SD) of D18 and L8-BO materials in a two-step process. Upon independently regulating the spin-coating
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Spontaneous Ammonia Activation Through Coordination Induced Bond Weakening in Molybdenum Complexes of a Dianionic Pentadentate Ligand Platform Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 C. Christopher Almquist, Nicole Removski, Thayalan Rajeshkumar, Benjamin Gelfand, Warren Piers, Laurent Maron
Ammonia oxidation catalyzed by molecular compounds is of current interest as a carbon free source of dihydrogen. Activation of N-H bonds through coordination to transition metal centers is a key reaction in this process. We report the substantial activation of ammonia via reaction with low valent molybdenum complexes of a diborate pentadentate ligand system. Spontaneous loss of hydrogen atoms from
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Redox-Active Crystalline Coordination Catalyst for Hybrid Electrocatalytic Full Reaction Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Sheng-Nan Sun, Long-Zhang Dong, Jia-Ru Li, Jing-Wen Shi, Jiang Liu, Yi-Rong Wang, Qing Huang, Ya-Qian Lan
Hybrid CO 2 electroreduction in which carbon dioxide reduction reaction (CO 2 RR) is coupled with a thermodynamically more favorable anodic oxidation reaction is recognized as a very important strategy to improve the total value of redox products and energy conversion efficiency. In this work, a coordination catalyst model system for hybrid electrocatalytic full reaction, including Ni 8 -TET with active
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Fast A-Site Cation Cross-exchange at Room Temperature: Single-to Double- and Triple-Cation Halide Perovskite Nanocrystals Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Clara Otero-Martínez, Muhammad Imran, Nadine J. Schrenker, Junzhi Ye, Kangyu Ji, Akshay Rao, Samuel D. Stranks, Robert L. Z. Hoye, Sara Bals, Liberato Manna, Jorge Pérez-Juste, Lakshminarayana Polavarapu
We report here fast A-site cation cross-exchange between APbX 3 perovskite nanocrystals (NCs) made of different A-cations (Cs (Cesium), FA (formamidinium), and MA (methylammonium)) at room temperature. Surprisingly, the A-cation cross-exchange proceeds as fast as the halide (X=Cl, Br, or I) exchange with the help of free A-oleate complexes present in the freshly prepared colloidal perovskite NC solutions
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Solvent-Dependent Supramolecular Host-Guest Assemblies of Platinum(II) Tweezers and a Guest System: From Discrete Molecules to High-Ordered Oligomers Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Jenny Yuk-Wa Yeung, Fred Ka-Wai Kong, Franky Ka-Wah Hau, Michael Ho-Yeung Chan, Maggie Ng, Ming-Yi Leung, Vivian W. W. Yam
A series of platinum(II) calix[4]arene-based molecular tweezers was synthesized. The studies of the host-guest association with a charge-neutral cyclometalated platinum(II) complex showed a drastic color change and the turning on of near-infrared emission resulting from Pt⋯Pt and π−π interactions. Control of the host-guest assembly process by varying the solvent composition can lead to a change from
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The Impact of Boron Hybridisation on Photocatalytic Processes Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Alessandro Marotta, Callum E. Adams, John Molloy
Recently the fruitful merger of organoboron chemistry and photocatalysis has come to the forefront of organic synthesis resulting in the development of new technologies to access complex (non)borylated frameworks. Central to the success of this combination is control of boron hybridisation. Contingent on the photoactivation mode, boron as its neutral planar form or tetrahedral boronate can be used
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Luminescence and Length Control in Nonchelated d8-Metallosupramolecular Polymers through Metal-Metal Interactions Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Jonas Matern, Ivan Maisuls, Cristian A. Strassert, Gustavo Fernandez
Supramolecular polymers (SPs) of d 8 transition metal complexes have received considerable attention by virtue of their rich photophysical properties arising from metal-metal interactions. However, thus far, the molecular design is restricted to complexes with chelating ligands due to their advantageous preorganization and strong ligand fields. Herein, we demonstrate unique pathway-controllable me
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Magneto-Orientation of Magnetic Double Stacks for Patterned Anisotropic Hydrogels with Multiple Responses and Modulable Motions Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Chen Fei Dai, Olena Khoruzhenko, Chengqian Zhang, Qing Li Zhu, Dejin Jiao, Miao Du, Josef Breu, Peng Zhao, Qiang Zheng, Zi Liang Wu
Reported here is a multi-response anisotropic poly(N-isopropylacrylamide) hydrogel developed by using a rotating magnetic field to align magnetic double stacks (MDSs) that are fixed by polymerization. The magneto-orientation of MDSs originates from the unique structure with g-Fe2O3 nanoparticles sandwiched by two silicate nanosheets. The resultant gels not only exhibit anisotropic optical and mechanical
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Cis-Trans Reisomerization Precedes Reprotonation of the Retinal Chromophore in the Photocycle of Schizorhodopsin 4 Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Kouhei Hayashi, Misao Mizuno, Hideki Kandori, Yasuhisa Mizutani
Recent discoveries of light-driven inward proton-pumping rhodopsins have opened new avenues to exploring the mechanism of unidirectional transport because these proteins transport protons in the opposite direction to conventional proton-pumping rhodopsins, despite their similar protein structure and membrane topology. Schizorhodopsin (SzR) is a newly discovered rhodopsin family of light-driven inward
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One-Step Thermophoretic AND Gate Operation on Extracellular Vesicles Improves Diagnosis of Prostate Cancer Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Jinqi Deng, Shuai Zhao, Junhong Li, Yangchang Cheng, Chao Liu, Zheng Liu, Lele Li, Fei Tian, Bo Dai, Jiashu Sun
Circulating extracellular vesicles (EVs) have emerged as a valuable source of cancer biomarkers. However, the high degree of EV heterogeneity and the complexity of clinical samples pose a challenge in the sensitive identification of tumor-derived EVs. Here we introduce a one-step thermophoretic AND gate operation (Tango) assay that integrates polyethylene glycol (PEG)-enhanced thermophoretic accumulation
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Amine-directed Formation of B–N Bonds for BN-fused Polycyclic Aromatic Multiple Resonance Emitters with Narrowband Emission Angew. Chem. Int. Ed. (IF 15.336) Pub Date : 2022-06-24 Guoyun Meng, Hengyi Dai, Tianyu Huang, Jinbei Wei, Jianping Zhou, Xiao Li, Xiang Wang, Xiangchen Hong, Chen Yin, Xuan Zeng, Yuewei Zhang, Dezhi Yang, Dongge Ma, Guomeng Li, Dongdong Zhang, Lian Duan
Despite the remarkable multiple resonances (MR) optoelectronic properties of organic nanographenes with boron and nitrogen atoms disposed para to each other, the synthetic procedures are sophisticated with low yields and the molecular skeletons are limited. Here, a new paradigm of easy-to-access MR emitter is constructed by simplifying the multiborylation through the amine-directed formation of B-N
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Why you should love wasps, and what is emotion? Books in brief Nature (IF 49.962) Pub Date : 2022-06-24
Andrew Robinson reviews five of the week’s best science picks.
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Into high gear: material made of cogs stiffens or flexes on command Nature (IF 49.962) Pub Date : 2022-06-24
A strong material becomes more rigid or more relaxed when its constituent gears are spun.
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Daily briefing: Rare ‘triple-dip’ La Niña climate event looks likely Nature (IF 49.962) Pub Date : 2022-06-23
A long-running La Niña climate event could persist into 2023. Plus, breast cancer cells are more likely to go rogue at night, and research to quantify and reduce inequality.
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What Omicron’s BA.4 and BA.5 variants mean for the pandemic Nature (IF 49.962) Pub Date : 2022-06-23
The lineages’ rise seems to stem from their ability to infect people who were immune to earlier forms of Omicron and other variants.
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Largest bacterium ever found is surprisingly complex Nature (IF 49.962) Pub Date : 2022-06-23
‘Microorganism’ is a misnomer when it comes to centimetre-long Thiomargarita magnifica.
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Separating molecules by their shapes can purify natural gas Nature (IF 49.962) Pub Date : 2022-06-22
Membranes with methane-excluding pores can remove nitrogen and carbon dioxide from natural gas in an energy-efficient and cost-effective way.
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Hijacked-journal tracker helps researchers to spot scam websites Nature (IF 49.962) Pub Date : 2022-06-22
Scientists can now check whether a journal website has been cloned before submitting their manuscript.