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Periodically Interrupting Bonding Behavior to Reformat Delocalized Electronic States of Graphdiyne for Improved Electrocatalytic Hydrogen Evolution

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Angewandte Chemie 2022年第42期134卷

作者： Kaikai Ma Jing Wu Xin Wang Yu Sun Zhaozhao Xiong Fulong Dai Haokun Bai Yong Xie Zhuo Kang Yue Zhang Academy for Advanced Interdisciplinary Science and Technology Beijing Advanced Innovation Center for Materials Genome Engineering University of Science and Technology Beijing Beijing 100083 P. R. China Beijing Key Laboratory for Advanced Energy Materials and Technologies School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Project administration (lead) Contribution: Conceptualization (lead) Data curation (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Project administration (lead) Resources (lead) Software (lead) Supervision (lead)

π electron configuration plays a pivotal role in metal-free carbon catalysts, and its delocalization degree overwhelmingly dominates catalytic activity. However, precise and targeted regulation of inherent π electrons still remain challenging. Here, one chemical-bond-targeted physical clipping strategy is proposed and effectively adopted in the cutting-edge carbon material system of graphdiyne (GDY) as a concept-of-proof. The delocalized electrons are expected to be periodically reformatted for substantially enhancing π electron delocalization. Via theoretical screening and well-designed experiments, periodical interruption of Csp−Csp 2 bonds in GDY can render sp−C sites with decent activity, ultimately yielding top-ranking electrocatalytic performance without intentionally introducing external decoration. The as-proposed concept endows a universal prescription to push the limit of delocalization degree, thus shedding novel light on the rational design of decent metal-free catalysts.

关键词： Bonding Behavior Delocalization Degree Graphdiyne Hydrogen Evolution π Electron State

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Active Sites Decorated Nonpolar Pore-Based MOF for One-step Acquisition of C2H4and Recovery of C3H6

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Angewandte Chemie 2023年第43期135卷

作者： Dr. Gang-Ding Wang Dr. Yong-Zhi Li Dr. Wen-Juan Shi Prof. Lei Hou Prof. Yao-Yu Wang Prof. Zhonghua Zhu Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry & Materials Science Northwest University Xi'an 710069 P. R. China Contribution: Data curation (lead) Investigation (lead) Methodology (equal) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Writing - review & editing (supporting) Contribution: Formal analysis (equal) Software (equal) Contribution: Software (lead) Supervision (lead) Writing - review & editing (lead) Contribution: Formal analysis (equal) Resources (equal) School of Chemical Engineering The University of Queensland Brisbane 4072 Australia

Herein, a 2-fold interpenetrated metal-organic framework (MOF) Zn-BPZ-TATB with accessible N/O active sites in nonpolar pore surfaces was reported for one-step C 2 H 4 purification from C 2 H 6 or C 3 H 6 mixtures as well as recovery of C 3 H 6 from C 2 H 6 /C 3 H 6 /C 2 H 4 mixtures. The MOF exhibits the favorable C 2 H 6 and C 3 H 6 uptakes (>100 cm 3 g −1 at 298 K under 100 kPa) as well as selective adsorption of C 2 H 6 and C 3 H 6 over C 2 H 4 . The C 3 H 6 - and C 2 H 6 -selective feature were investigated detailedly by experimental tests as well as sorption kinetic studyies. Molecular modelling revealed the multiple interactions between C 3 H 6 or C 2 H 6 molecules and methyl groups as well as triazine rings in pores. Zn-BPZ-TATB not only can directly generate 323.4 L kg −1 and 15.4 L kg −1 of high-purity (≥99.9 %) C 2 H 4 from C 3 H 6 /C 2 H 4 and C 2 H 6 /C 2 H 4 mixtures, but also provide a large high-purity (≥99.5 %) C 3 H 6 recovery capacity of 60.1 L kg −1 from C 3 H 6 /C 2 H 4 mixtures. More importantly, the high-purity C 3 H 6 (≥99.5 %) and C 2 H 4 (≥99.9 %) with the productivities of 38.2 and 12.7 L kg −1 can be simultaneously obtained from C 2 H 6 /C 3 H 6 /C 2 H 4 mixtures through a single adsorption/desorption cycle.

关键词： Crystal Structure Ethylene Purification Gas Adsorption and Separation Metal–Organic Framework Microporous Materials

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Defect-Free Synthesis of a Fully π-Conjugated Helical Ladder Polymer and Resolution into a Pair of Enantiomeric Helical Ladders**

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Angewandte Chemie 2023年第20期135卷

作者： Dr. Tomoyuki Ikai Sayaka Miyoshi Dr. Kosuke Oki Dr. Ranajit Saha Dr. Yuh Hijikata Prof. Eiji Yashima Department of Molecular and Macromolecular Chemistry Graduate School of Engineering Nagoya University Chikusa-ku Nagoya 464-8603 Japan Precursory Research for Embryonic Science and Technology (PRESTO) Japan Science and Technology Agency (JST) Kawaguchi Saitama 332-0012 Japan Contribution: Conceptualization (lead) Funding acquisition (supporting) Project administration (equal) Supervision (equal) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Data curation (lead) Formal analysis (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Institute for Chemical Reaction Design and Discovery (WPI-ICReDD) Hokkaido University Sapporo 001-0021 Japan Contribution: Data curation (supporting) Software (supporting) Contribution: Data curation (supporting) Software (lead) Contribution: Conceptualization (supporting) Funding acquisition (lead) Project administration (equal) Supervision (equal) Writing - review & editing (equal)

Fully π-conjugated ladder polymers with a spiral geometry represent a new class of helical polymers with great potential for organic nanodevices, but there is no precedent for an optically active helical ladder polymer totally composed of achiral units. We now report the defect-free synthesis and resolution of a fully π-conjugated helical ladder polymer with a rigid helical cavity, which has been achieved by quantitative and chemoselective acid-promoted alkyne benzannulations of a rationally designed, random-coil achiral polymer followed by chromatographic enantioseparation. Because of a sufficiently high helix-inversion barrier, the isolated excess one-handed helical ladder polymer with a degree of polymerization of more than 15 showed a strong circular dichroism with a dissymmetry factor of up to 1.7×10 −2 and is thermally stable, maintaining its optical activity in solution even at 100 °C, as well-supported by molecular dynamics simulation.

关键词： Defect-Free Enantioseparation Fully π-Conjugation Helical Ladder Polymers

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One-Handed Helical Tubular Ladder Polymers for Chromatographic Enantioseparation**

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Angewandte Chemie 2023年第11期135卷

作者： Dr. Wei Zheng Dr. Kosuke Oki Dr. Ranajit Saha Dr. Yuh Hijikata Prof. Eiji Yashima Dr. Tomoyuki Ikai Department of Molecular and Macromolecular Chemistry Graduate School of Engineering Nagoya University Chikusa-ku Nagoya 464-8603 Japan Contribution: Data curation (lead) Formal analysis (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Institute for Chemical Reaction Design and Discovery (WPI-ICReDD) Hokkaido University Sapporo 001-0021 Japan Contribution: Data curation (supporting) Software (supporting) Contribution: Data curation (supporting) Software (lead) Contribution: Conceptualization (supporting) Funding acquisition (lead) Project administration (equal) Supervision (equal) Writing - review & editing (equal) Precursory Research for Embryonic Science and Technology (PRESTO) Japan Science and Technology Agency (JST) Kawaguchi Saitama 332-0012 Japan Contribution: Conceptualization (lead) Funding acquisition (supporting) Project administration (equal) Supervision (equal) Writing - original draft (lead) Writing - review & editing (equal)

Defect-free one-handed contracted helical tubular ladder polymers with a π-electron-rich cylindrical helical cavity were synthesized by alkyne benzannulations of the random-coil precursor polymers containing 6,6′-linked-1,1′-spirobiindane-7,7′-diol-based chiral monomer units. The resulting tightly-twisted helical tubular ladder polymers showed remarkably high enantioseparation abilities toward a variety of chiral hydrophobic aromatics with point, axial, and planar chiralities. The random-coil precursor polymer and analogous rigid-rod extended helical ribbon-like ladder polymer with no internal helical cavity exhibited no resolution abilities. The molecular dynamics simulations suggested that the π-electron-rich cylindrical helical cavity formed in the tightly-twisted tubular helical ladder structures is of key importance for producing the highly-enantioseparation ability, by which chiral aromatics can be enantioselectively encapsulated by specific π-π and/or hydrophobic interactions.

关键词： Alkyne Benzannulations Chiral Recognition Helical Cavities Ladder Formation Spiro Structures

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Organic Zinc-Ion Battery: Planar, π-Conjugated Quinone-Based Polymer Endows Ultrafast Ion Diffusion Kinetics

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Angewandte Chemie 2022年第51期134卷

作者： Dr. Fei Ye Qiang Liu Dr. Hongliang Dong Kailin Guan Zhaoyang Chen Na Ju Prof. Linfeng Hu School of Materials Science and Engineering Southeast University Nanjing 211189 China Contribution: Conceptualization (supporting) Data curation (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Software (lead) Center for High Pressure Science and Technology Advanced Research Shanghai 201203 P. R. China Contribution: Investigation (equal) Methodology (equal) Resources (equal) Validation (lead) Contribution: Formal analysis (equal) Investigation (lead) Methodology (equal) Contribution: Investigation (equal) Software (equal) Validation (lead) Visualization (lead) Contribution: Data curation (equal) Formal analysis (equal) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

A novel poly(phenazine-alt-pyromellitic anhydride) (PPPA) has been successfully designed and synthesized via a condensation polymerization strategy as promising cathode material in organic zinc-ion batteries. Electrochemical quartz crystal microbalance (EQCM), FTIR and XPS characterizations verify a reversible Zn 2+ -coordination mechanism in our PPPA cathode. Intriguingly, an ultrahigh Zn 2+ diffusion coefficient of 1.2×10 −7 cm 2 s −1 was found in this large π-conjugated system, which is the highest one among all organic cathode materials for zinc-ion batteries. Theoretical calculations reveal the extended π-conjugated plane in our PPPA sample results in a significant reduction on energy gap, effectively accelerating intramolecular electron transfer during charge/discharge process. Our finding provides insights to achieve high zinc-ion transport kinetics by a design strategy on planar polymer system.

关键词： Energy Gap Linear Polymer Organic Zinc-Ion Batteries Quinone-Based Polymer Zn2+ Diffusion Coefficient

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Edge-centric functional network reveals new spatiotemporal biomarkers of early mild cognitive impairment

Brain‐X

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Brain‐X 2023年第3期1卷

作者： Weiping Wang Ruiying Du Zhen Wang Xiong Luo Haiyan Zhao Ping Luan Jipeng Ouyang Song Liu School of Computer and Communication Engineering University of Science and Technology Beijing Beijing China Shunde Graduate School Beijing University of Science and Technology Shunde Guangdong China Beijing Key Laboratory of Knowledge Engineering for Materials Science Beijing China Contribution: Investigation Writing - original draft Writing - review & editing The Center for Optical Imagery Analysis and Learning and School of Mechanical Engineering Northwestern Polytechnical University Xi'an Shaanxi China Weiping Wang Zhen Wang and Haiyan Zhao. Contribution: Conceptualization Formal analysis Contribution: Formal analysis Supervision Department of Neurology Peking University Third Hospital Beijing China Contribution: Data curation Formal analysis Guangdong Second People's Hospital Guangzhou Guangdong China Department of Neurology Shunde Hospital Southern Medical University Shunde Guangdong China Contribution: Conceptualization Data curation Southeast Asia Project Manager Department of China Petroleum Pipeline Engineering Co. Ltd. Langfang Hebei China Contribution: Software Supervision

Most neuroimaging studies of the pathogenesis of early mild cognitive impairment (EMCI) rely on a node-centric network model, which only calculates correlations between brain regions. Considering the interaction of low-order correlations between pairs of brain regions, we use an edge-centric network model to study high-order functional network correlations. Here, we compute edge time series (eTS) to obtain overlapping communities and study the relationship between subnetworks and communities in space. Then, based on the overlapping communities, we calculate the normalized entropy to measure the diversity of each node. Next, we compute the high-amplitude co-fluctuation of the eTS to explore the pattern of brain activity with temporal precision. Our results show that the normal control and EMCI patients differ in brain regions, subnetworks, and the whole brain. In particular, entropy values show a gradual decrease, and brain network co-fluctuation increases with disease progression. Our study is the first to investigate the pathogenesis of EMCI from the perspective of spatiotemporal flexibility and cognitive diversity based on high-order edge connectivity, further characterizing brain dynamics and providing new insights into the search for biomarkers of EMCI.

关键词： co-fluctuation edge-centric functional flexibility overlapping community spatiotemporal

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π–π Interaction-Induced Organic Long-wavelength Room-Temperature Phosphorescence forIn VivoAtherosclerotic Plaque Imaging

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Angewandte Chemie 2023年第2期136卷

作者： Yufan Zhang Jisen Li Jiliang Zhao Xuefei Li Zhimei Wang Yicheng Huang Prof. Hongkai Zhang Prof. Qian Liu Prof. Yunxiang Lei Prof. Dan Ding Frontiers Science Center for Cell Responses State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Bioactive Materials Ministry of Education College of Life Sciences Nankai University 300071 Tianjin China Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (lead) Writing - original draft (lead) Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Contribution: Investigation (equal) Methodology (equal) Contribution: Conceptualization (supporting) Software (equal) School of Chemistry and Materials Engineering Wenzhou University 325035 Wenzhou China Contribution: Investigation (supporting) Methodology (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Department of Urology Tianjin First Central Hospital 300192 Tianjin China Contribution: Data curation (supporting) Software (supporting) Contribution: Visualization (lead) Writing - review & editing (supporting) Contribution: Funding acquisition (lead) Writing - review & editing (lead)

Room-temperature phosphorescent (RTP) materials have great potential for in vivo imaging because they can circumvent the autofluorescence of biological tissues. In this study, a class of organic-doped long-wavelength (≈600 nm) RTP materials with benzo[c][1,2,5] thiadiazole as a guest was constructed. Both host and guest molecules have simple structures and can be directly purchased commercially at a low cost. Owing to the long phosphorescence wavelength of the doping system, it exhibited good tissue penetration (10 mm). Notably, these RTP nanoparticles were successfully used to image atherosclerotic plaques, with a signal-to-background ratio (SBR) of 44.52. This study provides a new approach for constructing inexpensive red organic phosphorescent materials and a new method for imaging cardiovascular diseases using these materials.

关键词： Atherosclerotic Plaque Imaging Benzo[c][1,2,5] Thiadiazole Guest Host-Guest Doped Systems Room Temperature Phosphorescence

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Unsupervised Learning-Guided Accelerated Discovery of Alkaline Anion Exchange Membranes for Fuel Cells

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Angewandte Chemie 2023年第19期135卷

作者： Dr. Xiuyang Zou Guodong Xu Pengda Fang Dr. Weizheng Li Zhiyu Jin Dr. Siyu Guo Yin Hu Prof. Meisheng Li Ji Pan Prof. Zhe Sun Prof. Feng Yan Jiangsu Engineering Laboratory of Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Negative Carbon Technologies College of Chemistry Suzhou Key Laboratory of Soft Material and New Energy College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Contribution: Data curation (supporting) Contribution: Formal analysis (equal) Contribution: Formal analysis (supporting) Contribution: Validation (equal) Contribution: Methodology (supporting) School of Chemistry and Chemical Engineering Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials Huaiyin Normal University Huaian 223300 China Contribution: Software (equal) Contribution: Software (supporting) Contribution: Conceptualization (equal) Contribution: Conceptualization (lead)

Without insight into the correlation between the structure and properties, anion exchange membranes (AEMs) for fuel cells are developed usually using the empirical trial and error method or simulation methods. Here, a virtual module compound enumeration screening (V-MCES) approach, which does not require the establishment of expensive training databases and can search the chemical space containing more than 4.2×10 5 candidates was proposed. The accuracy of the V-MCES model was considerably improved when the model was combined with supervised learning for the feature selection of molecular descriptors. Techniques from V-MCES, correlating the molecular structures of the AEMs with the predicted chemical stability, generated a ranking list of potential high stability AEMs. Under the guidance of V-MCES, highly stable AEMs were synthesized. With understanding of AEM structure and performance by machine learning, AEM science may enter a new era of unprecedented levels of architectural design.

关键词： Alkaline Stability Anion Exchange Membranes Degradation Prediction Machine Learning Material Genomics

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Unlocking the Interfacial Adsorption-Intercalation Pseudocapacitive Storage Limit to Enabling All-Climate, High Energy/Power Density and Durable Zn-Ion Batteries

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Angewandte Chemie 2023年第27期135卷

作者： Ming Yang Dr. Yanyi Wang Dr. Dingtao Ma Jianhui Zhu Hongwei Mi Prof. Zuotai Zhang Buke Wu Prof. Lin Zeng Minfeng Chen Prof. Jizhang Chen Prof. Peixin Zhang College of Chemistry and Environmental Engineering Shenzhen University Shenzhen 518060 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (equal) Writing - original draft (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Project administration (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Project administration (supporting) Supervision (supporting) Writing - review & editing (lead) Contribution: Formal analysis (supporting) Resources (supporting) Software (supporting) Contribution: Resources (supporting) Supervision (supporting) School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen 518055 China Contribution: Investigation (supporting) Resources (supporting) Department of Mechanical and Energy Engineering Southern University of Science and Technology Ministry of Education Shenzhen 518055 China Contribution: Writing - review & editing (supporting) College of Materials Science and Engineering Nanjing Forestry University Nanjing 210037 China Contribution: Data curation (supporting) Investigation (supporting) Contribution: Funding acquisition (lead) Project administration (lead) Resources (lead) Supervision (equal) Writing - review & editing (supporting)

Sluggish storage kinetics and insufficient performance are the major challenges that restrict the transition metal dichalcogenides (TMDs) applied for zinc ion storage, especially at the extreme temperature conditions. Herein, a multiscale interface structure-integrated modulation concept was presented, to unlock the omnidirectional storage kinetics-enhanced porous VSe 2− x ⋅ n H 2 O host. Theory research indicated that the co-modulation of H 2 O intercalation and selenium vacancy enables enhancing the interfacial zinc ion capture ability and decreasing the zinc ion diffusion barrier. Moreover, an interfacial adsorption-intercalation pseudocapacitive storage mechanism was uncovered. Such cathode displayed remarkable storage performance at the wide temperature range (−40–60 °C) in aqueous and solid electrolytes. In particular, it can retain a high specific capacity of 173 mAh g −1 after 5000 cycles at 10 A g −1 , as well as a high energy density of 290 Wh kg −1 and a power density of 15.8 kW kg −1 at room temperature. Unexpectedly, a remarkably energy density of 465 Wh kg −1 and power density of 21.26 kW kg −1 at 60 °C also can be achieved, as well as 258 Wh kg −1 and 10.8 kW kg −1 at −20 °C. This work realizes a conceptual breakthrough for extending the interfacial storage limit of layered TMDs to construct all-climate high-performance Zn-ion batteries.

关键词： All-Climate Interfacial Adsorption-Intercalation Pseudocapacitive Storage Multiscale Interface Structure Omnidirectional Storage Kinetics Zn-Ion Batteries

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Regulating the Mechanical and Optical Properties of Polymer-based Nanocomposites by Sub-Nanowires

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Angewandte Chemie 2022年第5期135卷

作者： Feng Yuan Dr. Chen Ouyang Minzheng Yang Prof. Wenxiong Shi Dr. Weibin Ren Prof. Yang Shen Prof. Yan Wei Prof. Xuliang Deng Prof. Xun Wang Institute of Medical Technology Peking University Health Science Center Beijing 100191 China Beijing Laboratory of Biomedical Materials Department of Geriatric Dentistry Peking University School and Hospital of Stomatology Beijing 100081 China Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University Beijing 100084 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (supporting) Formal analysis (supporting) State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China Contribution: Software (supporting) Contribution: Formal analysis (supporting) Contribution: Formal analysis (supporting) Supervision (supporting) Contribution: Conceptualization (equal) Formal analysis (lead) Supervision (lead) Contribution: Conceptualization (lead) Supervision (lead) Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Methodology (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Sub-nanowires (SNWs) exhibit great potential applications in nanocomposites owing to their high specific surface area, high flexibility, and similarity to polymer chains in dimension, which are a good entry point to bridge inorganic materials and polymer materials. Herein, we synthesized hydroxyapatite sub-nanowires (HAP SNWs) and engineered hydroxyapatite sub-nanowires/polyimide (HSP) gels and films by simple mixing of HAP SNWs and polyimide (PI). Benefiting from the interactions between HAP SNWs and PI, these nanocomposites were a continuous hybrid network. As the increase of HAP SNWs contents, the viscosity and modulus of HSP gels were greatly improved by one or two orders of magnitude compared with PI gel. HSP films not only maintained high transparency but also gained high haze, as well as exhibited enhanced Young's modulus. Thus, both HSP gels and films developed in this work are promising for various applications in coatings and high-performance films.

关键词： Gels Nanocomposites Nanowires Thin Films

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