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Ligand-Mediated Revival of Degraded α-CsPbI3to Stable Highly Luminescent Perovskite

Angewandte Chemie 2023年第22期135卷

作者： Arup Ghorai Somnath Mahato Sudarshan Singh Shaona Bose Baidyanath Roy Unyong Jeong Samit Kumar Ray School of Nano Science and Technology Indian Institute of Technology Kharagpur 721302 Kharagpur India Department of Materials Science and Engineering Pohang University of Science and Technology (POSTECH) 77 Cheongam-ro Nam-gu 37673 Pohang Republic of Korea Current address: Łukasiewicz Research Network— PORT Polish Center for Technology Development Stabłowicka 147 54-066 Wrocław Poland Department of Physics Indian Institute of Technology Kharagpur 721302 Kharagpur India

Although α-CsPbI 3 is regarded as an attractive optical luminophore, it is readily degraded to the optically inactive δ-phase under ambient conditions. Here, we present a simple approach to revive degraded (“optically sick”) α-CsPbI 3 through “medication” with thiol-containing ligands. The effect of different types of thiols is systematically studied through optical spectroscopy. The structural reconstruction of degraded α-CsPbI 3 nanocrystals to cubic crystals in the presence of thiol-containing ligands is visualized through high-resolution transmission electron microscopy and supported by X-ray diffraction analysis. We found that 1-dodecanethiol (DSH) effectively revives degraded CsPbI 3 and results in high immunity towards moisture and oxygen, hitherto unreported. DSH facilitates the passivation of surface defects and etching of degraded Cs 4 PbI 6 phase, thus reverting them back to the cubic CsPbI 3 phase, leading to enhanced PL and environmental stability.

关键词： Atomic Resolution TEM Caesium Lead Halide Perovskites Density Functional Theory Ligand Mediated Revival Structural Reconstruction

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Hemin as a General Static Dark Quencher for Constructing Heme Oxygenase-1 Fluorescent Probes

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Angewandte Chemie 2023年第21期135卷

作者： Fan Chen Dr. Baoxin Zhang Dr. Zhenjiang Ding Miao Zhong Dr. Yanan Hou Fang Zhang Dr. Guodong Hu Prof. Jianguo Fang State Key Laboratory of Applied Organic Chemistry and College of Chemistry and Chemical Engineering Lanzhou University Lanzhou Gansu 730000 China Current address: Beijing Key Laboratory of the Innovative Development of Functional Staple and Nutritional Intervention for Chronic Diseases China National Research Institute of Food and Fermentation Industries Beijing 100015 China School of Chemistry and Chemical Engineering Nanjing University of Science & Technology Nanjing Jiangsu 210094 China

The development of small-molecule probes suitable for live-cell applications remains challenging yet highly desirable. We report the first fluorescent probe, RBH, for imaging the heme oxygenase-1 (HO-1) activity in live cells after discovering hemin as a universal dark quencher. Hemin works via a static quenching mechanism and shows high quenching efficiency (>97 %) with fluorophores across a broad spectrum ( λ ex =400–700 nm). The favorable properties of RBH (e.g. long excitation/emission wavelengths, fast response rate and high magnitude of signal increase) enable its use for determining HO-1 activity in complex biological samples. As HO-1 is involved in regulating antioxidant defence, iron homeostasis and gasotransmitter carbon monoxide production, we expect RBH to be a powerful tool for dissecting its functions. Also, the discovery of hemin as a general static dark quencher provides a straightforward strategy for constructing novel fluorescent probes for diverse biological species.

关键词： Dark Quencher Fluorescent Probe Heme Oxygenase-1 Hemin Static Quenching

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Publicly funded exome sequencing for outpatients with neurodevelopmental disorders demonstrates a high rate of unexpected findings impacting medical management

Genetics in Medicine Open

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Genetics in Medicine Open 2023年第1期1卷 100828-100828页

作者： Nakhleh Francis, Yara Hershkovitz, Tova Ekhilevitch, Nina Habib, Clair Ravid, Sarit Tal, Galit Schertz, Mitchell Mory, Adi Zinger, Amihood Baris Feldman, Hagit Zaid, Rinat Paperna, Tamar Weiss, Karin Department of obstetrics and gynecology Galilee medical center Nahariya Israel The Faculty of Medicine in the Galilee Bar-Ilan University Safed Israel The Genetics Institute Rambam Health Care Campus Haifa Israel The Ruth and Bruce Rappaport Faculty of Medicine Technion-Israel Institute of Technology Haifa Israel Pediatric neurology unit Rambam Health Care Campus Haifa Israel Metabolic Clinic Ruth Rappaport Children's Hospital Rambam Health Care Campus Haifa Israel Child Development and Pediatric Neurology Service Meuhedet Tel Aviv Israel Current address: The Genetics Institute Tel Aviv Sourasky Medical Center Tel Aviv Israel Community Genetics Public Health Services Ministry of Health Jerusalem Israel Sackler Faculty of Medicine Tel Aviv University Tel Aviv Israel

Purpose: Exome sequencing (ES) is a powerful tool that facilitates the diagnosis of patients with rare Mendelian syndromes. In 2018 the Israeli Ministry of Health initiated a national pilot program that funds ES for outpatients with global developmental delay (GDD). Here, we describe the 3-year impact of this program on patient care in a single tertiary hospital. Methods: From 2018 to 2020, trio ES was performed on 170 participants fulfilling Israeli Ministry of Health criteria: (1) moderate to severe GDD and (2) mild GDD with epilepsy or a major congenital anomaly. We retrospectively analyzed this cohort. Results: A diagnosis was achieved in 74 individuals (43%). There were 82 clinically significant variants, the majority being novel. Consanguinity was reported in 22% and was not associated with a higher diagnostic rate. The presence of autism spectrum was associated with a lower diagnostic rate of 8/33 (24%). Autosomal dominant inheritance was identified in 14% of participants, and the parental phenotype ranged between fully affected and asymptomatic. Among the diagnosed participants, 16% had an unexpected diagnosis that did not fit the typical clinical presentation. In 9%, the diagnosis changed short-term active clinical management, in 19%, the surveillance recommendations, and in 23%, the family-focused outcomes. Conclusion: The introduction of a national program that funds ES for GDD has transformed patient care, leading to a significant effect on medical management and treatment. The high rate of an unexpected inheritance mode and variable phenotypes emphasizes the diagnostic complexity of neurodevelopmental disorders and the strength of a non-targeted approach. © 2023 The Authors

关键词： Autism Clinical management Consanguinity Exome sequencing Global developmental delay

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Titelbild: Entropy-Mediated Stable Structural Evolution of Prussian White Cathodes for Long-Life Na-Ion Batteries (Angew. Chem. 7/2024)

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Angewandte Chemie 2024年第7期136卷

作者： Yueyue He Sören L. Dreyer Yin-Ying Ting Prof. Yuan Ma Dr. Yang Hu Dr. Damian Goonetilleke Dr. Yushu Tang Dr. Thomas Diemant Bei Zhou Dr. Piotr M. Kowalski Prof. Maximilian Fichtner Prof. Horst Hahn Prof. Jasmin Aghassi-Hagmann Dr. Torsten Brezesinski Dr. Ben Breitung Prof. Yanjiao Ma Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) Hermann-von-Helmholtz Platz 1 76344 Eggenstein-Leopoldshafen Germany Institute of Energy and Climate Research (IEK-13) Forschungszentrum Jülich GmbH Wilhelm-Johnen-Str. 52428 Jülich Germany Chair of Theory and Computation of Energy Materials Faculty of Georesources and Materials Engineering RWTH Aachen University 52062 Aachen Germany Helmholtz Institute Ulm (HIU) for Electrochemical Energy Storage Helmholtzstr. 11 89081 Ulm Germany Current address: Corporate Research and Development Umicore Watertorenstraat 33 2250 Olen Belgium Jülich Aachen Research Alliance JARA Energy & Center for Simulation and Data Science (CSD) 52425 Jülich Germany School of Chemical Biological and Materials Engineering The University of Oklahoma Norman OK 73019 USA Current address: School of Energy and Mechanical Engineering Jiangsu Key Laboratory of New Power Batteries Nanjing Normal University Nanjing 210023 China

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Cover Picture: Entropy-Mediated Stable Structural Evolution of Prussian White Cathodes for Long-Life Na-Ion Batteries (Angew. Chem. Int. Ed. 7/2024)

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Angewandte Chemie International Edition 2024年第7期63卷

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Innenrücktitelbild: Synthesis of Topological Gels by Penetrating Polymerization Using a Molecular Net (Angew. Chem. 11/2024)

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Angewandte Chemie 2024年第11期136卷

作者： Prof. Dr. Yuichi Ohya Ryota Dohi Fumika Seko Yuto Nakazawa Ken-ichiro Mizuguchi Kosei Shinzaki Takahiko Yasui Hiroaki Ogawa Shizuka Kato Dr. Yuta Yoshizaki Dr. Nobuo Murase Prof. Dr. Akinori Kuzuya Department of Chemistry and Materials Engineering Faculty of Chemistry Materials and Bioengineering Kansai University 3-3-35 Yamate Suita Osaka 564-8680 Japan Kansai University Medical Polymer Research Center Kansai University 3-3-35 Yamate Suita Osaka 564-8680 Japan Organization for Research & Development of Innovative Science & Technology (ORDIST) Kansai University 3-3-35 Yamate Suita Osaka 564-8680 Japan Current address: Graduate School of Pharmaceutical Sciences Tohoku University 6-3 Aoba Aramaki Aoba-ku Sendai Miyagi 980-8578 Japan

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Synthesis of Topological Gels by Penetrating Polymerization Using a Molecular Net

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Angewandte Chemie 2024年第11期136卷

Topological gels possess structures that are cross-linked only via physical constraints; ideally, no attractive intermolecular interactions act between their components, which yields interesting physical properties. However, most reported previous topological gels were synthesized based on supramolecular interlocked structures such as polyrotaxane, for which attractive intermolecular interactions are essential. Here, we synthesize a water-soluble “molecular net” (MN) with a large molecular weight and three-dimensional network structure using poly(ethylene glycol). When a water-soluble monomer ( N -isopropylacrylamide) is polymerized in the presence of the MNs, the extending polymer chains penetrates the MNs to form an ideal topological MN gel with no specific attractive interactions between its components. The MN gels show unique physical properties as well a significantly high degree of swelling and high extensibility due to slipping of the physical cross-linking. We postulate this method to yield a new paradigm in gel science with unprecedented physical properties.

关键词： Mechanical Property Molecular Net Penetrating Polymerization Temperature-Responsive Topological Gel

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Inside Back Cover: Synthesis of Topological Gels by Penetrating Polymerization Using a Molecular Net (Angew. Chem. Int. Ed. 11/2024)

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Angewandte Chemie International Edition 2024年第11期63卷

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Entropy-Mediated Stable Structural Evolution of Prussian White Cathodes for Long-Life Na-Ion Batteries

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Angewandte Chemie 2023年第7期136卷

The high-entropy approach is applied to monoclinic Prussian White (PW) Na-ion cathodes to address the issue of unfavorable multilevel phase transitions upon electrochemical cycling, leading to poor stability and capacity decay. A series of Mn-based samples with up to six metal species sharing the N-coordinated positions was synthesized. The material of composition Na 1.65 Mn 0.4 Fe 0.12 Ni 0.12 Cu 0.12 Co 0.12 Cd 0.12 [Fe(CN) 6 ] 0.92 □ 0.08 ⋅ 1.09H 2 O was found to exhibit superior cyclability over medium/low-entropy and conventional single-metal PWs. We also report, to our knowledge for the first time, that a high-symmetry crystal structure may be advantageous for high-entropy PWs during battery operation. Computational comparisons of the formation enthalpy demonstrate that the compositionally less complex materials are prone to phase transitions, which negatively affect cycling performance. Based on data from complementary characterization techniques, an intrinsic mechanism for the stability improvement of the disordered PW structure upon Na + insertion/extraction is proposed, namely the dual effect of suppression of phase transitions and mitigation of gas evolution.

关键词： High-Entropy Materials Outgassing Phase Transitions Prussian White Sodium-Ion Cathode

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Author Correction: Trans-ancestral genome-wide association study of longitudinal pubertal height growth and shared heritability with adult health outcomes

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Genome biology 2024年第1期25卷 129页

作者： Jonathan P Bradfeld Rachel L Kember Anna Ulrich Zhanna Balkhiyarova Akram Alyass Izzuddin M Aris Joshua A Bell K Alaine Broadaway Zhanghua Chen Jin-Fang Chai Neil M Davies Dietmar Fernandez-Orth Mariona Bustamante Ruby Fore Amitavo Ganguli Anni Heiskala Jouke-Jan Hottenga Carmen Íñiguez Sayuko Kobes Jaakko Leinonen Estelle Lowry Leo-Pekka Lyytikainen Anubha Mahajan Niina Pitkänen Theresia M Schnurr Christian Theil Have David P Strachan Elisabeth Thiering Suzanne Vogelezang Kaitlin H Wade Carol A Wang Andrew Wong Louise Aas Holm Alessandra Chesi Catherine Choong Miguel Cruz Paul Elliott Steve Franks Christine Frithiof-Bøjsøe W James Gauderman Joseph T Glessner Vicente Gilsanz Kendra Griesman Robert L Hanson Marika Kaakinen Heidi Kalkwarf Andrea Kelly Joseph Kindler Mika Kähönen Carla Lanca Joan Lappe Nanette R Lee Shana McCormack Frank D Mentch Jonathan A Mitchell Nina Mononen Harri Niinikoski Emily Oken Katja Pahkala Xueling Sim Yik-Ying Teo Leslie J Baier Toos van Beijsterveldt Linda S Adair Dorret I Boomsma Eco de Geus Mònica Guxens Johan G Eriksson Janine F Felix Frank D Gilliland Torben Hansen Rebecca Hardy Marie-France Hivert Jens-Christian Holm Vincent W V Jaddoe Marjo-Riitta Järvelin Terho Lehtimäki David A Mackey David Meyre Karen L Mohlke Juha Mykkänen Sharon Oberfeld Craig E Pennell John R B Perry Olli Raitakari Fernando Rivadeneira Seang-Mei Saw Sylvain Sebert John A Shepherd Marie Standl Thorkild I A Sørensen Nicholas J Timpson Maties Torrent Gonneke Willemsen Elina Hypponen Chris Power Mark I McCarthy Rachel M Freathy Elisabeth Widén Hakon Hakonarson Inga Prokopenko Benjamin F Voight Babette S Zemel Struan F A Grant Diana L Cousminer Center for Applied Genomics Children's Hospital of Philadelphia Philadelphia PA 19104 USA. Center for Spatial and Functional Genomics Children's Hospital of Philadelphia Philadelphia PA 19104 USA. Department of Psychiatry Perelman School of Medicine University of Pennsylvania Philadelphia USA. Department of Clinical & Experimental Medicine University of Surrey Guildford UK. Department of Metabolism Digestion and Reproduction Imperial College London London UK. People-Centred Artifcial Intelligence Institute University of Surrey Guildford UK. Department of Health Research Methods Evidence and Impact McMaster University Hamilton Canada. Division of Chronic Disease Research Across the Lifecourse Department of Population Medicine Harvard Medical School and Harvard Pilgrim Health Care Institute Boston MA 02215 USA. MRC Integrative Epidemiology Unit at the University of Bristol Bristol UK. Department of Genetics University of North Carolina Chapel Hill NC USA. Department of Population and Public Health Sciences University of Southern California Los Angeles CA 90032 USA. Saw Swee Hock School of Public Health National University of Singapore and National University Health System Singapore Singapore. Bristol Medical School Population Health Sciences University of Bristol Bristol UK. K.G. Jebsen Center for Genetic Epidemiology Department of Public Health and Nursing NTNU Norwegian University of Science and Technology Trondheim Norway. ISGlobal Barcelona Spain. Center for Life Course Health Research University of Oulu Oulu Finland. Department of Biological Psychology Vrije Universiteit Amsterdam Amsterdam The Netherlands. Department of Statistics and Computational Research Universitat de València Valencia Spain. CIBER Epidemiología y Salud Pública (CIBERESP) Madrid Spain. Epidemiology and Environmental Health Joint Research Unit FISABIO-Universitat Jaume I-Universitat de València Valencia Spain. Phoenix Epidemiology and Clinical Research Center NIDDK

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