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In-Situ Formation of Three-Dimensional Network Intrinsic Microporous Ladder Polymer Membranes with Ultra-High Gas Separation Performance and Anti-Trade-Off Effect

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Angewandte Chemie 2025年第6期137卷

作者： Luxin Sun Wei Xu Prof. Hongjun Zhang Jiachen Chu Mengtao Wang Kai Song Wenjie Wu Prof. Jianxin Li Dr. Yingge Wang Prof. Ingo Pinnau Prof. Xiaohua Ma State Key Laboratory of Separation Membranes and Membrane Processes School of Materials Science and Engineering Tiangong University Tianjin 300387 P. R. China State Key Laboratory of Particle Detection and Electronics & Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 P.R. China Advanced Membranes and Porous Materials Center Chemical Engineering Program Physical Science and Engineering Division King Abdullah University of Science and Technology Thuwal 23955-6900 Saudi Arabia

The global quest for clean energy and sustainable processes makes advanced membrane extremely attractive for energy-intensive industrial gas separations. Here, we disclose a series of ultra-high-performance gas separation membranes (PIM-3D-TB) from novel network polymers of intrinsic microporosity (PIM) that combine the advantages of solution processible PIM and small pore size distribution (PSD) of porous organic polymers (POP), which was synthesized by in situ copolymerization of triptycene-2,6-diamine as linear part and triptycene-2,6,13(14)-triamine (TTA) as crosslinker. The resulting PIM-3D-TB membranes demonstrated outstanding separation properties that outperformed the latest trade-off lines for H 2 /CH 4 and O 2 /N 2 . They also showed an anti-trade-off effect by simultaneously enhancing gas permeability and gas-pair selectivity with increasing TTA content. The TTA crosslinking node increased the microporosity, and, shifted the PSD from the ultramicropore (<7 Å) toward the more size sieving submicropore (<4 Å) region. The post-treated TTA-75 displayed an exceptional H 2 permeability of 8000 Barrer and H 2 /CH 4 selectivity of 208. These PIM-3D-TB membranes and their design protocol have unparalleled potential in the next generation of membranes for hydrogen purification and air separations.

关键词： Polymers of intrinsic microporosity 3D network membrane gas separation molecular sieving

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Diamine Surface Passivation and Post-Annealing Enhance Performance of Silicon-Perovskite Tandem Solar Cells

arXiv

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arXiv 2024年

作者： Taddei, Margherita Contreras, Hannah Doan, Hai-Nam McCarthy, Declan P. Seo, Seongrok Westbrook, Robert J.E. Graham, Daniel J. Datta, Kunal Carroy, Perrine Muñoz, Delfina Correa-Baena, Juan-Pablo Barlow, Stephen Marder, Seth R. Smith, Joel A. Snaith, Henry J. Ginger, David S. Department of Chemistry University of Washington SeattleWA98195 United States Department of Physics University of Oxford OxfordOX1 3PU United Kingdom Institute of Materials Science Technical University of Munich München85748 Germany Department of Chemistry University of Colorado-Boulder BoulderCO80309 United States Department of Bioengineering University of Washington SeattleWA98195 United States School of Materials Science and Engineering Georgia Institute of Technology North Ave NW AtlantaGA30332 United States Université Grenoble Alpes CEA Liten Campus Ines Le Bourget du Lac73375 France Renewable and Sustainable Energy Institute University of Colorado-Boulder BoulderCO80309 United States Department of Chemical and Biological Engineering and Materials Science Program University of Colorado-Boulder BoulderCO80309 United States Physical Sciences Division Physical and Computational Sciences Directorate Pacific Northwest National Laboratory RichlandWA99352 United States

We show that the use of 1,3-diaminopropane (DAP) as a chemical modifier at the perovskite/electron-transport layer (ETL) interface enhances the power conversion efficiency (PCE) of 1.7 eV bandgap FACs mixed-halide perovskite single-junction cells, primarily by boosting the open-circuit voltage (VOC) from 1.06 V to 1.15 V. Adding a post-processing annealing step after C60 evaporation, further improves the fill factor (FF) by 20% from the control to the DAP + post-annealing devices. Using hyperspectral photoluminescence microscopy, we demonstrate that annealing helps improve compositional homogeneity at the top and bottom interfaces of the solar cell, which prevents detrimental bandgap pinning in the devices and improves C60 adhesion. Using time-of-flight secondary ion mass spectrometry, we show that DAP reacts with formamidinium present near the surface of the perovskite lattice to form a larger molecular cation, 1,4,5,6-tetrahydropyrimidinium (THP) that remains at the interface. Combining the use of DAP and the annealing of C60 interface, we fabricate Si-perovskite tandems with PCE of 25.29%, compared to 23.26% for control devices. Our study underscores the critical role of chemical reactivity and thermal post-processing of the C60/Lewis-base passivator interface in minimizing device losses and advancing solar-cell performance of wide-bandgap mixed-cation mixed-halide perovskite for tandem application. © 2024, CC BY.

关键词： Perovskite

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Front Cover: Ethylene Oligomerization: Unraveling the Roles of Ni Sites, Acid Sites, and Zeolite Pore Topology through Continuous and Pulsed Reactions (ChemCatChem 5/2024)

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ChemCatChem 2024年第5期16卷

作者： Omar Abed Dr. Hend Omar Mohamed Dr. Idoia Hita Dr. Vijay Velisoju Dr. Natalia Morlanés Dr. Omar El Tall Prof. Pedro Castaño Multiscale Reaction Engineering KAUST Catalysis Center (KCC) King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia KAUST Catalysis Center King Abdullah University of Science and Technology Thuwal 23955-6900 Saudi Arabia KAUST Core Labs King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia Chemical Engineering Program Physical Science and Engineering (PSE) Division King Abdullah University of Science and Technology Thuwal 23955-6900 Saudi Arabia

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Inverse Vulcanization of Aziridines: Enhancing Polysulfides for Superior Mechanical Strength and Adhesive Performance

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Angewandte Chemie 2024年第6期137卷

作者： Jieai Fan Changzheng Ju Songjie Fan Xia Li Zhen Zhang Nikos Hadjichristidis School of Chemical Engineering and Light Industry Guangdong University of Technology 510006 Guangzhou China Analysis and Test Center Guangdong University of Technology 510006 Guangzhou China Polymer Synthesis Laboratory Chemistry Program KAUST Catalysis Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology (KAUST) 23955 Thuwal Saudi Arabia

This study introduces a novel approach to inverse vulcanization by utilizing a commercially available triaziridine crosslinker as an alternative to conventional olefin-based crosslinkers. The model reactions reveal a self-catalyzed ring-opening of “unactivated” aziridine with elemental sulfur, forming oligosulfide-functionalized diamines. The triaziridine-derived polysulfides exhibit impressive mechanical properties, achieving a maximum stress of ~8.3 MPa and an elongation at break of ~107 %. The incorporation of silicon dioxide (20 wt %) enhances the composite's rigidity, yielding a Young's modulus of ~0.94 GPa. Furthermore, these polysulfides display excellent adhesion strength on various substrates, such as aluminum (~7.0 MPa), walnut (~9.6 MPa), and steel (~11.0 MPa), with substantial retention of adhesion strength (~3.3 MPa on steel) at −196 °C. The straightforward synthetic process, combined with the accessibility of the triaziridine crosslinker, emphasizes the potential for further innovations in sulfur polymer chemistry.

关键词： elemental sulfur aziridines inverse vulcanization polysulfides adhesive

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Cover Picture: Zeolite–Water Chemistry: Characterization Methods to Unveil Zeolite Structure (Chem. Methods 4/2025)

Chemistry–Methods

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Chemistry–Methods 2025年第4期5卷

作者： José Nuno Almeida Lu Song Sohrab Askarli Sang-Ho Chung Javier Ruiz-Martínez Catalysis Nanomaterials and Spectroscopy Group King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia Department of Carbon Neutrality Soonchunhyang University (SCH University) 22 Soonchunhyang-ro Sinchang-myeon Asan-si Chungcheongnam-do 31538 South Korea Chemical Engineering Program Physical Science and Engineering (PSE) Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia

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Isomeric 1,4-Dihydropentalene-Containing Building Blocks for High Mobility Ladder-Type Conjugated Polymers

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Angewandte Chemie 2025年

作者： Shengnan Zhang Yuqian Liu Hao Dong Yanru Li Kai Zhang Kaihu Xian Prof. Yang Han Prof. Long Ye Prof. Martin Heeney Prof. Zhuping Fei Institute of Molecular Plus Department of Chemistry and Haihe Laboratory of Sustainable Chemical Transformations Key Laboratory of Organic Integrated Circuits Ministry of Education Tianjin University Tianjin 300072 China School of Materials Science & Engineering Tianjin Key Laboratory of Molecular Optoelectronic Sciences and Collaborative Innovation Center of Chemical Science and Engineering Tianjin University Tianjin 300350 China Institute for Electric Light Sources School of Information Science and Technology Fudan University Shanghai 200433 China Division of Physical Sciences & Engineering Chemistry Program King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia

Nearly amorphous conjugated polymers, though lacking long-range order, can exhibit high charge carrier mobility and enhanced flexibility, making them ideal for flexible or stretchable OFET applications. However, research on novel structural blocks for this class of materials remains limited. We report the synthesis of two derivatives of the 5,10-dihydroindeno[2,1- a ]indene (DHI) core, where two thieno groups are appended to each end to reduce torsional disorder with adjacent comonomers. The two 1,4-dihydropentalene containing isomers, anti-C16DHIT-Br and syn-C16DHIT-Br, feature distinct thieno group orientations, leading to differences in their electronic properties. The anti-isomer shows a fully delocalized conjugation pathway, whereas the syn isomer exhibits cross-conjugation, limiting delocalization along the polymer backbone. These monomers were copolymerized with benzothiadiazole (BT) to form two conjugated polymers, anti-C16DHIT-BT and syn-C16DHIT-BT, both with highly planar backbones, good solubility, and solution processability. Morphological studies reveal that anti-C16DHIT-BT exhibits more ordered stacking and higher crystallinity than syn-C16DHIT-BT. Devices based on anti-C16DHIT-BT show significantly better performance, with a hole mobility of 2.38 cm 2 V −1 s −1 , slightly higher than the widely studied pIDTBT under identical conditions.

关键词： Conjugated polymers High mobility Isomerization effect Novel building blocks Organic field-effect transistors

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Nanoslot-Induced Ultrastrong Phonon-Photon and Phonon-Phonon Coupling in Hybrid Organic-Inorganic Perovskites

Nanoslot-Induced Ultrastrong Phonon-Photon and Phonon-Phonon...

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Pacific Rim Conference on Lasers and Electro-Optics (CLEO/Pacific Rim)

作者： Dasom Kim Jin Hou Geon Lee Ayush Agrawal Sunghwan Kim Hao Zhang Di Bao Andrey Baydin Wenjing WU Fuyang Tay Shengxi Huang Daivd Hagenmüller Elbert E. M. Chia Dai-Sik Kim Minah Seo Aditya D. Mohite Junichiro Kono Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston TX USA Department of Electrical and Computer Engineering Rice University Houston TX USA Department of Materials Science and NanoEngineering Rice University Houston TX USA Sensor System Research Center Korea Institute of Science and Technology Seoul Republic of Korea Department of Physics and Astronomy Seoul National University Seoul Republic of Korea Department of Chemical and Biomolecular Engineering Rice University Houston TX USA Department of Physics Long-wavelength Nanotechnology Laboratory Quantum Photonics Institute Ulsan National Institute of Science and Technology (UNIST) Ulsan Republic of Korea Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore Smalley-Curl institute Rice University Houston TX USA CESQ-ISIS (UMR 7006) Universite de Strasbourg and CNRS Strasbourg France KU-KIST Graduate School of Converging Science and Technology Korea University Seoul Republic of Korea Department of Physics and Astronomy Rice University Houston TX USA

Methods for harnessing vibrational states are desired for phonon-based technologies. We realized ultrastrong coupling of two phonon modes in perovskite materials induced by ultrastrong coupling with a common photonic ... 详细信息

ISBN: (数字)9798350372076

ISBN: (纸本)9798350372083

关键词： Couplings Phonons Laser modes Perovskites Electro-optical waveguides Photonics

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Transforming Red Phosphorus Photocatalysis: Dual Roles of Pre-Anchored Ru Single Atoms in Defect and Interface engineering

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Angewandte Chemie 2024年第45期136卷

作者： Junwei Bian Wei Zhang Prof. Yun Hau Ng Prof. Zhuofeng Hu Prof. Zhen Wei Yuxi Liu Prof. Jiguang Deng Prof. Hongxing Dai Prof. Lin Jing Beijing Key Laboratory for Green Catalysis and Separation College of Materials Science and Engineering Beijing University of Technology Beijing 100124 China School of Energy and Environment City University of Hong Kong Tat Chee Avenue Kowloon 999077 Hong Kong S.A.R. China Chemical Engineering Program Physical Science and Engineering Division King Abdullah University of Science and Technology Thuwal 23955-6900 Kingdom of Saudi Arabia School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510275 China

Crystalline red phosphorus (CRP), known for its promising photocatalytic properties, faces challenges in photocatalytic hydrogen evolution (PHE) due to undesired inherent charge deep trapping and recombination effects induced by defects. This study overcomes these limitations through an innovative strategy in integrating ruthenium single atoms (Ru 1 ) within CRP to simultaneously repair the intrinsic undesired vacancy defects and serve as the uniformly distributed anchoring sites for a controllable growth into ruthenium nanoparticles (Ru NP ). Hence, a highly functionalized CRP with Ru 1 and Ru NP (Ru 1-NP /CRP) with concerted effects in regulating electronic structures and promoting interfacial charge transfer has been achieved. Advanced characterizations unveil the pioneering dual role of pre-anchored Ru 1 (analogous to the “Tai Chi” principle) in transforming CRP photocatalysis. The regulations of vacancy defects on the surface of CRP minimize the detrimental deep charge trapping, resulting in the prolonged lifetime of active charges. With the well-distributed in situ growth of Ru NP on Ru 1 sites, the constructed robust “bridge” that connects CRP and Ru NP facilitates constructive interfacial charge transfer. Ultimately, the synergistic effect induced by the pre-anchored Ru 1 endows Ru 1-NP /CRP with an exceptional PHE rate of 3175 μmol h −1 g −1 , positioning it as one of the most efficient elemental-based photocatalysts available. This breakthrough underscores the crucial role of pre-anchoring metal single atoms at defect sites of catalysts in enhancing sustainable hydrogen production.

关键词： photocatalytic hydrogen evolution red phosphorus ruthenium single atom defect engineering interface engineering

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Synthesis of α,ω-End Functionalized Polydienes: Allylic-Bearing Heteroleptic Aluminums for Selective Alkylation and Transalkylation in Coordinative Chain Transfer Polymerization

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Angewandte Chemie 2023年第5期136卷

作者： Dr. Pibo Liu Xiao Yang Dr. He Li Dr. Songbo Zhang Prof. Yanming Hu Prof. Guangyuan Zhou Prof. Nikos Hadjichristidis Division of Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian Liaoning 116023 China Physical Sciences and Engineering Division KAUST Catalysis Center Chemistry Program Polymer Synthesis Laboratory King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Kingdom of Saudi Arabia

There are still challenges in the preparation of difunctional stereoregular polydienes, especially for the construction of initiating chain-end functionalization. Coordinative chain transfer polymerization (CCTP) provides a way to achieve the goal but usually requires sophisticated functionalized catalysts as well as expensive chain transfer agents (CTAs). In this work, heteroleptic aluminum with oligo(dienyl) substituents (oligo-Al agents) were readily prepared by living anionic polymerization (LAP) technique. The oligo-Al agents used in Nd-mediated CCTPs of dienes exhibit highly selective alkylation and transalkylation features. Kinetics and transfer efficiency studies using 1 H NMR, 13 C NMR, 1 H- 13 C HSQC, and Dosy NMR analyses revealed that the resulting polydienes possess substituents at the initiating chain-end that have transferred from the oligo-Al agents. The functionalization efficiency of the initiating chain-end is up to 99 %, and the molar mass regulation efficiency of heteroleptic aluminum is higher than that of the traditional CTA Al i Bu 2 H (0.608 vs. 0.410). Based on the experimental results and density functional theory (DFT) calculations, we propose a mechanism in which allylic-Al acts as an efficient alkylating moiety in catalyst preformation and also as an effective transfer agent in polymerization. Taking advantage of these features, di-functionalized polyisoprene, polybutadiene, and poly(isoprene-co-butadiene) can be facilely synthesized.

关键词： Aluminum Chain Transfer Polymerization End-Functionalization Neodymium Polydiene

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Cover Picture: Transforming Red Phosphorus Photocatalysis: Dual Roles of Pre-Anchored Ru Single Atoms in Defect and Interface engineering (Angew. Chem. Int. Ed. 45/2024)

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Angewandte Chemie International Edition 2024年第45期63卷

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