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Metal-Organic Frameworks for Practical Separation of Cyclic and Linear Polymers

Angewandte Chemie 2021年第21期133卷

作者： Taku Sawayama Yubo Wang Tomohisa Watanabe Prof. Masayoshi Takayanagi Prof. Takuya Yamamoto Dr. Nobuhiko Hosono Prof. Takashi Uemura Department of Advanced Materials Science Graduate School of Frontier Sciences The University of Tokyo 5-1-5 Kashiwanoha Kashiwa Chiba 277-8561 Japan Graduate School of Chemical Sciences and Engineering Hokkaido University Sapporo Hokkaido 060-8628 Japan The Center for Data Science Education and Research Shiga University Hikone Shiga 522-8522 Japan RIKEN Center for Advanced Intelligence Project 1-4-1 Nihonbashi Chuo-ku Tokyo 103-0027 Japan Division of Applied Chemistry Faculty of Engineering Hokkaido University Sapporo Hokkaido 060-8628 Japan Department of Applied Chemistry Graduate School of Engineering The University of Tokyo 7-3-1 Hongo Bunkyo-ku Tokyo 113-8656 Japan

The purification step in the manufacturing of cyclic polymers is difficult as complete fractionation to eliminate linear impurities requires considerable effort. Here, we report a new polymer separation methodology that uses metal-organic frameworks (MOFs) to discriminate between linear and cyclic polyethylene glycols (PEGs) via selective polymer insertion into the MOF nanopores. Preparation of a MOF-packed column allowed analytical and preparative chromatographic separation of these topologically distinct pairs. In addition, gram-scale PEGs with only cyclic structures were successfully obtained from a crude reaction mixture by using MOF as an adsorbent.

关键词： column chromatography cyclic polymers macromolecular recognition metal-organic frameworks separation

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Author Correction: Exploration of natural red-shifted rhodopsins using a machine learning-based Bayesian experimental design

Communications biology

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Communications biology 2021年第1期4卷 532页

作者： Keiichi Inoue Masayuki Karasuyama Ryoko Nakamura Masae Konno Daichi Yamada Kentaro Mannen Takashi Nagata Yu Inatsu Hiromu Yawo Kei Yura Oded Béjà Hideki Kandori Ichiro Takeuchi The Institute for Solid State Physics The University of Tokyo Kashiwa Japan. inoue@issp.u-tokyo.ac.jp. RIKEN Center for Advanced Intelligence Project Tokyo Japan. inoue@issp.u-tokyo.ac.jp. Department of Life Science and Applied Chemistry Nagoya Institute of Technology Nagoya Japan. inoue@issp.u-tokyo.ac.jp. OptoBioTechnology Research Center Nagoya Institute of Technology Nagoya Japan. inoue@issp.u-tokyo.ac.jp. PRESTO Japan Science and Technology Agency Kawaguchi Japan. inoue@issp.u-tokyo.ac.jp. PRESTO Japan Science and Technology Agency Kawaguchi Japan. Department of Computer Science Nagoya Institute of Technology Nagoya Japan. Department of Life Science and Applied Chemistry Nagoya Institute of Technology Nagoya Japan. The Institute for Solid State Physics The University of Tokyo Kashiwa Japan. Graduate School of Humanities and Sciences Ochanomizu University Tokyo Japan. Center for Interdisciplinary AI and Data Science Ochanomizu University Tokyo Japan. School of Advanced Science and Engineering Waseda University Tokyo Japan. Faculty of Biology Technion-Israel Institute of Technology Haifa Israel. RIKEN Center for Advanced Intelligence Project Tokyo Japan. OptoBioTechnology Research Center Nagoya Institute of Technology Nagoya Japan. RIKEN Center for Advanced Intelligence Project Tokyo Japan. takeuchi.ichiro@nitech.ac.jp. OptoBioTechnology Research Center Nagoya Institute of Technology Nagoya Japan. takeuchi.ichiro@nitech.ac.jp. Department of Computer Science Nagoya Institute of Technology Nagoya Japan. takeuchi.ichiro@nitech.ac.jp.

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Biaxially-Strained Phthalocyanine at Polyoxometalate@Carbon Nanotube Heterostructure Boosts Oxygen Reduction Catalysis

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Angewandte Chemie 2023年第42期135卷

作者： Prof. Sheng Zhu Lingtong Ding Xuehuan Zhang Kun Wang Prof. Xiao Wang Prof. Feng Yang Prof. Gaoyi Han Institute of Molecular Science Key Lab of Materials for Energy Conversion and Storage of Shanxi Province Key Laboratory of Chemical Biology and Molecular Engineering of Education Ministry Shanxi University Taiyuan 030006 China Institute for Carbon-Based Thin Film Electronics Peking University Shanxi (ICTFE-PKU) Taiyuan 030012 China Contribution: Formal analysis (lead) Funding acquisition (lead) Methodology (lead) Resources (lead) Writing - original draft (lead) Writing - review & editing (lead) Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China Contribution: Data curation (equal) Methodology (equal) Validation (equal) Visualization (equal) Contribution: Formal analysis (supporting) Investigation (supporting) Department of Chemistry Southern University of Science and Technology Shenzhen 518055 China Contribution: Formal analysis (equal) Funding acquisition (supporting) Methodology (supporting) Visualization (equal) Writing - review & editing (supporting) Contribution: Funding acquisition (supporting) Investigation (equal) Methodology (equal) Writing - review & editing (supporting) Contribution: Project administration (supporting) Supervision (equal)

Iron phthalocyanine (FePc) with unique FeN 4 site has attracted increasing interests as a promising non-precious catalyst. However, the plane symmetric structure endows FePc with undesired catalytic performance toward the oxygen reduction reaction (ORR). Here, we report a novel one-dimensional heterostructured ORR catalyst by coupling FePc at polyoxometalate-encapsulated carbon nanotubes (FePc-{PW 12 }@NTs) using host-guest chemistry. The encapsulation of polyoxometalates can induce a local tensile strain of single-walled NTs to strengthen the interactions with FePc. Both the strain and curvature effects of {PW 12 }@NT scaffold tune the geometric structure and electronic localization of FeN 4 centers to enhance the ORR catalytic performance. As expected, such a heterostructured FePc-{PW 12 }@NT electrocatalyst exhibits prominent durability, methanol tolerance, and ORR activity with a high half-wave potential of 0.90 V and a low Tafel slope of 30.9 mV dec −1 in alkaline medium. Besides, the assembled zinc-air battery demonstrates an ultrahigh power density of 280 mW cm −2 , excellent charge/discharge ability and long-term stability over 500 h, outperforming that of the commercial Pt/C+IrO 2 cathode. This study offers a new strategy to design novel heterostructured catalysts and opens a new avenue to regulate the electrocatalytic performance of phthalocyanine molecules.

关键词： Carbon Nanotubes Electrocatalyst Oxygen Reduction Phthalocyanine Polyoxometalates

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Living cell-laden hydrogels: Unleashing the future of responsive biohybrid systems

Responsive Materials

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Responsive Materials 2023年第1期1卷

作者： Xuejia Hu Bing Lei Sen-Sen Li Lu-Jian Chen Quan Li Department of Electronic Engineering School of Electronic Science and Engineering Fujian Key Laboratory of Ultrafast Laser Technology and Applications Xiamen University Xiamen China Contribution: Conceptualization (equal) Data curation (equal) Funding acquisition (supporting) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Formal analysis (supporting) Visualization (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Funding acquisition (supporting) Visualization (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (lead) Project administration (equal) Resources (lead) Writing - original draft (equal) Writing - review & editing (equal) Institute of Advanced Materials and School of Chemistry and Chemical Engineering Southeast University Nanjing China Lu-Jian Chen and Quan Li. Contribution: Conceptualization (equal) Validation (supporting) Writing - original draft (supporting) Writing - review & editing (supporting)

Responsive biohybrid systems have the potential to overcome limitations of both natural and artificial machines in terms of efficiency, accuracy, and functionality. As functional units, living cells act as bricks for building biohybrid machines, where the extracellular matrix mimics hydrogels to act as ideal biological concrete. Combining living cells with hydrogels offers unique advantages in simulating human tissues or organs, which unleashes the future of biohybrid systems, and thus has attracted extensive attention. Herein, recent progress in cell-laden hydrogel-based responsive biohybrid systems is summarized to provide a basic understanding of how these systems are built from the bottom up and how to achieve the complex functions. This review focuses on advanced manufacturing technologies for responsive biohybrid systems, including laden cells in hydrogel matrices, three-dimensional bioprinting, and microfluidic manufacturing. Subsequently, the innovative applications of these works, including actuators, sensors, and engineered functional materials, are presented, along with different triggering mechanisms that are highlighted. Finally, the current challenges and future opportunities in the field are addressed. This review provides a unique perspective and is hoped to inspire fields such as biohybrid technologies, soft robots, and tissue engineering.

关键词： hydrogel living cell responsive biohybrid system soft robot

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Computer-Aided Discovery of Potent Broad-Spectrum Vaccine Adjuvants

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Angewandte Chemie 2023年第18期135卷

作者： Juan Ma Shenqing Wang Chuanfang Zhao Xiliang Yan Quanzhong Ren Zheng Dong Jiahuang Qiu Yin Liu Qing'e Shan Ming Xu Bing Yan Sijin Liu State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 P. R. China School of Environmental Sciences University of Chinese Academy of Sciences Beijing 100049 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Funding acquisition (supporting) Investigation (lead) Methodology (equal) Visualization (equal) Writing - original draft (lead) Institute of Environmental Research at Greater Bays Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of Education Guangzhou University Guangzhou 510006 P. R. China Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (supporting) Investigation (supporting) Methodology (lead) School of Chemical Sciences University of Chinese Academy of Sciences Beijing 100049 P. R. China Contribution: Methodology (supporting) Software (lead) Visualization (lead) Contribution: Methodology (supporting) Software (lead) Visualization (supporting) Department of toxicology and sanitary chemistry School of public health Capital Medical University Beijing 100069 P. R. China Contribution: Data curation (supporting) Investigation (supporting) School of Environment Hangzhou Institute for Advanced Study University of Chinese Academy of Sciences Hangzhou 330106 P. R. China Contribution: Formal analysis (supporting) Methodology (supporting) Medical Science and Technology Innovation Center Shandong First Medical University & Shandong Academy of Medical Sciences Jinan Shandong 250117 P. R. China Contribution: Investigation (supporting) Contribution: Supervision (supporting) Contribution: Conceptualization (equal) Funding acquisition (supporting) Methodology (supporting) Project administration (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

Adjuvants stimulate the immune system to vigorously respond to a vaccine. While current adjuvants such as aluminum salts and oil-in-water emulsions have been used for decades, they do not generate broad and long-lasting responses in many vaccines. Consequently, more potent adjuvants are needed. Here, using computer-aided molecule design and machine learning, we discovered 2 new, broad-spectrum adjuvants that can boost vaccine responses. Our library containing 46 toll-like receptor (TLR)-targeting agonist ligands were assembled on Au nanoparticles. Comprehensive in vitro , ex vivo and in vivo studies showed both leads promoted dendritic cell activation via multiple TLRs and enhanced antigen presentation to T cells. When used together with tumor-specific antigens to immunize mice against B16-OVA melanoma and 4T1-PD1 breast cancer, both adjuvants unleashed strong immune responses that suppressed tumor growth and lung metastases. Our results show computer-aided design and screening can rapidly uncover potent adjuvants for tackling waning immunity in current vaccines.

关键词： Cancer Immunotherapy Computer-Aided Design Dendritic Cell Nano Adjuvant Pattern Recognition Receptor

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Leveraging legacy data to accelerate materials design via preference learning

arXiv

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arXiv 2019年

作者： Sun, Xiaolin Hou, Zhufeng Sumita, Masato Ishihara, Shinsuke Tamura, Ryo Tsuda, Koji Graduate School of Frontier Sciences University of Tokyo 5-1-5 Kashiwa-no-ha Kashiwa Chiba277-8561 Japan Research and Services Division of Materials Data and Integrated System National Institute for Materials Science 1-2-1 Sengen Tsukuba Ibaraki305-0047 Japan Fuzhou Fujian350002 China National Institute for Materials Science 1-1 Namiki Tsukuba Ibaraki305-0044 Japan Center for Advanced Intelligence Project RIKEN 1-4-1 Nihombashi Chuo-ku Tokyo103-0027 Japan

Machine learning applications in materials science are often hampered by shortage of experimental data. Integration with legacy data from past experiments is a viable way to solve the problem, but complex calibration is often necessary to use the data obtained under different conditions. In this paper, we present a novel calibration-free strategy to enhance the performance of Bayesian optimization with preference learning. The entire learning process is solely based on pairwise comparison of quantities (i.e., higher or lower) in the same dataset, and experimental design can be done without comparing quantities in different datasets. We demonstrate that Bayesian optimization is significantly enhanced via addition of legacy data for organic molecules and inorganic solid-state materials. Copyright © 2019, The Authors. All rights reserved.

关键词： data integration

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Sample efficient stochastic gradient iterative hard thresholding method for stochastic sparse linear regression with limited attribute observation 18

Sample efficient stochastic gradient iterative hard threshol...

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Proceedings of the 32nd International Conference on Neural Information Processing Systems

作者： Tomoya Murata Taiji Suzuki NTT DATA Mathematical Systems Inc. Tokyo Japan Department of Mathematical Informatics Graduate School of Information Science and Technology The University of Tokyo Tokyo Japan and Center for Advanced Intelligence Project RIKEN Tokyo Japan

We develop new stochastic gradient methods for efficiently solving sparse linear regression in a partial attribute observation setting, where learners are only allowed to observe a fixed number of actively chosen attributes per example at training and prediction times. It is shown that the methods achieve essentially a sample complexity of O (1/ε) to attain an error of ε under a variant of restricted eigenvalue condition, and the rate has better dependency on the problem dimension than existing methods. Particularly, if the smallest magnitude of the non-zero components of the optimal solution is not too small, the rate of our proposed Hybrid algorithm can be boosted to near the minimax optimal sample complexity of full information algorithms. The core ideas are (i) efficient construction of an unbiased gradient estimator by the iterative usage of the hard thresholding operator for configuring an exploration algorithm; and (ii) an adaptive combination of the exploration and an exploitation algorithms for quickly identifying the support of the optimum and efficiently searching the optimal parameter in its support. Experimental results are presented to validate our theoretical findings and the superiority of our proposed methods.

关键词：

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Impact of Strain Relaxation on 2D Ruddlesden–Popper Perovskite Solar Cells

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Angewandte Chemie 2022年第36期134卷

作者： Qian Cheng Boxin Wang Gaosheng Huang Yanxun Li Dr. Xing Li Dr. Jieyi Chen Shengli Yue Kang Li Dr. Hong Zhang Prof. Yuan Zhang Prof. Huiqiong Zhou CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Beijing 100191 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Contribution: Investigation (supporting) Supervision (supporting) Contribution: Investigation (supporting) Software (supporting) Contribution: Methodology (supporting) School of Chemistry Beijing Advanced Innovation Center for Biomedical Engineering Beihang University Beijing 100191 China Contribution: Investigation (supporting) Contribution: Investigation (supporting) Methodology (supporting) Contribution: Investigation (supporting) Writing - review & editing (supporting) Contribution: Funding acquisition (supporting) Supervision (supporting) Writing - review & editing (supporting) Contribution: Funding acquisition (lead) Project administration (lead) Writing - review & editing (lead)

Although the photovoltaic performance of perovskite solar cells (PSCs) has reached the commercial standards, the unsatisfactory stability limits their further application. Hydrophobic interface and encapsulation can block the damage of water and oxygen, while the instability induced by intrinsic residual strain remains inevitable. Here, the residual strain in a two-dimensional (2D) Ruddlesden–Popper (RP) perovskite film is investigated by X-ray diffraction and atomic force microscopy. It's found that the spacer cations contribute to the residual strain even though they are not in the inorganic cages. Benefited from strain relaxation, the film quality is improved, leading to suppressed recombination, promoted charge transport and enhanced efficiency. More significantly, the strain-released devices maintain 86 % of the initial efficiency after being kept in air with 85 % relative humidity (RH) for 1080 h, 82 % under maximum power point (MPP) tracking at 50 °C for 804 h and 86 % after continuous heating at 85 °C for 1080 h.

关键词： Perovskites Ruddlesden–Popper Solar Cells Stability Strain Relaxation

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Zincophilic Electrode Interphase with Appended Proton Reservoir Ability Stabilizes Zn Metal Anodes

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Angewandte Chemie 2022年第5期135卷

作者： Zhenyue Xing Yanyan Sun Xuesong Xie Yan Tang Prof. Guofu Xu Prof. Junwei Han Prof. Bingan Lu Prof. Shuquan Liang Ass. Prof. Gen Chen Prof. Jiang Zhou School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University Changsha Hunan 410083 P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Contribution: Formal analysis (equal) Investigation (supporting) Writing - review & editing (equal) Contribution: Conceptualization (supporting) Investigation (supporting) Contribution: Writing - review & editing (supporting) Contribution: Supervision (supporting) Writing - review & editing (supporting) School of Minerals Processing and Bioengineering Central South University Changsha Hunan 410083 P. R. China Contribution: Funding acquisition (equal) Validation (lead) Writing - review & editing (supporting) School of Physics and Electronics Hunan University Changsha Hunan 410082 P. R. China Contribution: Investigation (supporting) Writing - review & editing (supporting) Contribution: Project administration (supporting) Writing - review & editing (supporting) Contribution: Formal analysis (equal) Investigation (equal) Project administration (equal) Writing - review & editing (equal) College of Chemistry and Chemical Engineering Jishou University Jishou Hunan 416000 P. R. China Contribution: Conceptualization (lead) Funding acquisition (lead) Investigation (equal) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

The rampant dendrites and hydrogen evolution reaction (HER) resulting from the turbulent interfacial evolution at the anode/electrolyte are the main culprits of short lifespan and low Coulombic efficiency of Zn metal batteries. In this work, a versatile protective coating with excellent zincophilic and amphoteric features is constructed on the surface of Zn metal (ZP@Zn) as dendrite-free anodes. This kind of protective coating possesses the advantages of reversible proton storage and rapid desolvation kinetics, thereby mitigating the HER and facilitating homogeneous nucleation concomitantly. Furthermore, the space charge polarization effect promotes charge redistribution to achieve uniform Zn deposition. Accordingly, the ZP@Zn symmetric cell manifests excellent reversibility at an ultrahigh cumulative plating capacity of 4700 mAh cm −2 and stable cycling at 80 % depth of discharge (DOD). The ZP@Zn//V 6 O 13 pouch cell also reveals superior cycling stability with a high capacity of 326.6 mAh g −1 .

关键词： Amphoteric Group Aqueous Zn Ion Batteries Dendrite-Free Zn Anode Hydrogen Evolution Interfacial Modification

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Sample efficient stochastic gradient iterative hard thresholding method for stochastic sparse linear regression with limited attribute observation

arXiv

引用

arXiv 2018年

作者： Murata, Tomoya Suzuki, Taiji NTT DATA Mathematical Systems Inc. Tokyo Japan Department of Mathematical Informatics Graduate School of Information Science and Technology University of Tokyo Tokyo Japan Japan Center for Advanced Intelligence Project RIKEN Tokyo Japan

We develop new stochastic gradient methods for efficiently solving sparse linear regression in a partial attribute observation setting, where learners are only allowed to observe a fixed number of actively chosen attributes per example at training and prediction times. It is shown that the methods achieve essentially a sample complexity of O(1/Ε) to attain an error of Ε under a variant of restricted eigenvalue condition, and the rate has better dependency on the problem dimension than existing methods. Particularly, if the smallest magnitude of the non-zero components of the optimal solution is not too small, the rate of our proposed Hybrid algorithm can be boosted to near the minimax optimal sample complexity of full information algorithms. The core ideas are (i) efficient construction of an unbiased gradient estimator by the iterative usage of the hard thresholding operator for configuring an exploration algorithm;and (ii) an adaptive combination of the exploration and an exploitation algorithms for quickly identifying the support of the optimum and efficiently searching the optimal parameter in its support. Experimental results are presented to validate our theoretical findings and the superiority of our proposed methods. Copyright © 2018, The Authors. All rights reserved.

关键词： Eigenvalues and eigenfunctions

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