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Cobalt-catalyzed migratory carbon-carbon cross-coupling of borabicyclo[3.3.1]nonane(9-BBN)borates

Chinese Chemical Letters 2025年第4期36卷 139-143页

作者： Peng Guo Shicheng Dong Xiang-Gui Zhang Bing-Bin Yang Jun Zhu Ke-Yin Ye College of Chemistry Fuzhou UniversityFuzhou 350108China School of Science and Engineering The Chinese University of Hong KongShenzhen 518172China State Key Laboratory of Physical Chemistry of Solid Surfaces and Collaborative Innovation Center of Chemistry for Energy Materials(iChEM) Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryDepartment of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

In most Suzuki–Miyaura carbon-carbon cross-coupling reactions,the borabicyclo[3.3.1]nonane scaffold(9-BBN)only serves as an auxiliary facilitating the transmetalation step and thus is transformed into *** are rare examples where the 9-BBN derivatives serve as the potentially diverse C8 building blocks in cross-coupling ***,we report a cobalt-catalyzed migratory carboncarbon cross-coupling reaction of the in situ formed 9-BBN ate complexes to afford diverse aryl-and alkyl-functionalized *** mechanistic studies suggest the oxidation-induced cisbicyclo[3.3.0]oct-1-ylborane is the key intermediate in this migratory cross-coupling reaction,which promotes the development of other diverse migratory cross-coupling of borate complexes.

关键词： Cobalt Cross-coupling Borate Rearrangement Cyclooctene

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An artificial chaperone serves a dual role in regulating the assembly of peptides through phase separation

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Aggregate 2024年第2期5卷 473-481页

作者： Wang Li Yang Zhou Sheng He Tianyi Tong Congsen Wang Peichen Shi Suixu Li Xinchang Wang Liulin Yang Xiaoyu Cao Zhong-Qun Tian State Key Laboratory of Physical Chemistry of Solid Surface Key Laboratory of Chemical Biology of Fujian ProvinceCollaborative Innovation Center of Chemistry for Energy Materials(iChEM)Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM)Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenChina School of Electronic Science and Engineering(National Model Microelectronics College) Xiamen UniversityXiamenChina

In biological systems,molecular assembly primarily relies on the assistance of molecular *** by nature,strategies like‘chaperone-assisted assembly’and‘catalyzed assembly’have been proposed for the sophisticated control of molecular ***,significant challenges remain in the rational design of such systems,calling for a deep understanding of underlying ***,we demonstrate an artificial chaperone serves a dual role,that is catalyst in low dosages and inhibitor in high dosages,in regulating the supramolecular polymerization of *** dosages of carboxymethyl cellulose,as the chaperones,catalyze the assembly of Aβ_(16-22) peptides into fibrils through multi-step phase separation,while high dosages trap the peptides into coacervate intermediates and therefore inhibit the ***,the quantity of chaperones does not follow the intuition that‘more is better’for catalyzing assembly but instead has an optimal molar *** reveals that the interplay and evolution of electrostatic and hydrophobic interactions are the keys to achieving these *** study provides insights into the multifaceted roles artificial chaperones may play in a dosage-dependent manner and enriches the toolkit for efficient and controllable construction of complex assembly systems.

关键词： artificial chaperone catassembly dosage effect peptide assembly supramolecular polymerization

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Networking retinomorphic sensor with memristive crossbar for brain-inspired visual perception

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National science Review 2021年第2期8卷 74-82页

作者： Shuang Wang Chen-Yu Wang Pengfei Wang Cong Wang Zhu-An Li Chen Pan Yitong Dai Anyuan Gao Chuan Liu Jian Liu Huafeng Yang Xiaowei Liu Bin Cheng Kunji Chen Zhenlin Wang Kenji Watanabe Takashi Taniguchi Shi-Jun Liang Feng Miao National Laboratory of Solid State Microstructures School of PhysicsCollaborative Innovation Center of Advanced MicrostructuresNanjing University School of Electronic Science and Engineering Nanjing University National Institute for Materials Science

Compared to human vision, conventional machine vision composed of an image sensor and processor suffers from high latency and large power consumption due to physically separated image sensing and processing. A neuromorphic vision system with brain-inspired visual perception provides a promising solution to the problem. Here we propose and demonstrate a prototype neuromorphic vision system by networking a retinomorphic sensor with a memristive crossbar. We fabricate the retinomorphic sensor by using WSe2/h-BN/Al2O3van der Waals heterostructures with gate-tunable photoresponses, to closely mimic the human retinal capabilities in simultaneously sensing and processing images. We then network the sensor with a large-scale Pt/Ta/Hf O2/Ta one-transistor-one-resistor（1 T1 R） memristive crossbar,which plays a similar role to the visual cortex in the human brain. The realized neuromorphic vision system allows for fast letter recognition and object tracking, indicating the capabilities of image sensing, processing and recognition in the full analog regime. Our work suggests that such a neuromorphic vision system may open up unprecedented opportunities in future visual perception applications.

关键词： van der Waals heterostructure retinomorphic sensor memristive crossbar brain-inspired visual perception neuromorphic computing

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The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO_(2) single-atom catalysts

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Nano Research 2024年第1期17卷 397-406页

作者： Danfeng Wu Shuyun Zhou Congcong Du Juan Li Jianyu Huang Hong-xia Shen Abhaya K.Datye Shan Jiang Jeffrey T.Miller Sen Lin Haifeng Xiong State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350002China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China College of Biology and Chemical Engineering Jiaxing UniversityJiaxing 314000China Department of Chemical&Biological Engineering University of New MexicoAlbuquerqueNM 8731-0001USA Davidson School of Chemical Engineering Purdue UniversityWest LafayetteIN 47907-2100USA Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China Fujian Key Laboratory of Rare-earth Functional Materials Fujian Shanhai Collaborative Innovation Center of Rare-earth Functional MaterialsLongyan 366300China

The local structure of the metal single-atom site is closely related to the catalytic activity of metal single-atom catalysts(SACs).However,constructing SACs with homogeneous metal active sites is a challenge due to the surface heterogeneity of the conventional ***,we prepared two Rh1/CeO_(2)SACs(0.5Rh1/r-CeO_(2)and 0.5Rh1/c-CeO_(2),respectively)using two shaped CeO_(2)(rod and cube)exposing different facets,i.e.,CeO_(2)(111)and CeO_(2)(100).In CO oxidation reaction,the T100 of 0.5Rh1/r-CeO_(2)SACs is 120°C,while the T100 of 0.5Rh1/c-CeO_(2)SACs is as high as 200°*** in-situ CO diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS),we found that the proximity between OH group and Rh single atom on the plane surface plays an important role in the catalytic activity of Rh1/CeO_(2)SAC system in CO *** Rh single atom trapped at the CeO_(2)(111)crystal surface forms the Rh1(OH)adjacent species,which is not found on the CeO_(2)(100)crystal surface at room ***,during CO oxidation,the OH group far from Rh single atom on the 0.5Rh1/c-CeO_(2)disappears and forms Rh1(OH)adjacent species when the temperature is above 150°*** formation of Rh1(OH)adjacentCO intermediate in the reaction is pivotal for the excellent catalytic activity,which explains the difference in the catalytic activity of Rh single atoms on two different CeO_(2)*** formed Rh1(OH)adjacent-O-Ce structure exhibits good stability in the reducing atmosphere,maintaining the Rh atomic dispersion after CO oxidation even when pre-reduced at high temperature of 500°*** functional theory(DFT)calculations validate the unique activity and reaction path of the intermediate Rh1(OH)adjacentCO species *** work demonstrates that the proximity between metal single atom and hydroxyl can determine the formation of active intermediates to affect the catalytic performances in catalysis.

关键词： crystal plane Rh1/CeO_(2)single-atom catalyst proximity of Rh and hydroxyl coordination structure CO oxidation

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Photothermal-chemical synthesis of P-S-H ternary hydride at high pressures

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Chinese Physics B 2022年第6期31卷 650-655页

作者： Tingting Ye Hong Zeng Peng Cheng Deyuan Yao Xiaomei Pan Xiao Zhang Junfeng Ding Key Laboratory of Materials Physics Institute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031China University of Science and Technology of China Hefei 230026China Frontiers Science Center for Transformative Molecules School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The recent discovery of room temperature superconductivity(283 K)in carbonaceous sulfur hydride(C-S-H)has attracted much interest in ternary hydrogen rich *** this report,ternary hydride P-S-H was synthesized through a photothermal-chemical reaction from elemental sulfur(S),phosphorus(P)and molecular hydrogen(H_(2))at high pressures and room *** spectroscopy under pressure shows that H_(2)S and PH_(3) compounds are synthesized after laser heating at 0.9 GPa,and a ternary van der Waals compound P-S-H is synthesized with further compression to 4.6 *** P-S-H compound is probably a mixed alloy of PH_(3) and(H_(2)S)_(2)H_(2) with a guest-host structure similar to the C-S-H *** ternary hydride can persist up to 35.6 GPa at least and shows two phase transitions at approximately 23.6 GPa and 32.8 GPa,respectively.

关键词： hydride superconductor high pressure Raman spectroscopy

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Functional LiTaO_(3)filler with tandem conductivity and ferroelectricity for PVDF-based composite solid-state electrolyte

Energy Materials and Devices

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Energy materials and Devices 2023年第1期1卷 95-105,94页

作者： Yu Yuan Likun Chen Yuhang Li Xufei An Jianshuai Lv Shaoke Guo Xing Cheng Yang Zhao Ming Liu Yan-Bing He Feiyu Kang Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center Institute of Materials Research(IMR)Tsinghua Shenzhen International Graduate SchoolShenzhen 518055China School of Materials Science and Engineering Tsinghua UniversityBeijing 100084China

Composite solid-state electrolytes have received significant attention due to their combined advantages as inorganic and polymer ***,conventional ceramic fillers offer limited ion conductivity enhancement for composite solid-state electrolytes due to the space-charge layer between the polymer matrix and ceramic *** this study,we develop a ferroelectric ceramic ion conductor(LiTaO_(3))as a func-tional filler to simultaneously alleviate the space-charge layer and provide an extra Li+transport *** obtained composite solid-state electrolyte comprising LiTaO_(3)filler and poly(vinylidene difluoride)matrix(P-LTO15)achieves an ionic conductivity of 4.90×10^(−4)S cm−1 and a Li+transference number of *** polar-ized ferroelectric LiTaO_(3)creates a uniform electric field and promotes homogenous Li plating/stripping,providing the Li symmetrical batteries with an ultrastable cycle life for 4000 h at 0.1 mA cm^(−2)and a low polar-ization overpotential(~50 mV).Furthermore,the solid-state NCM811/P-LTO15/Li full batteries achieve an ultralong cycling performance(1400 cycles)at 1 C and a high discharge capacity of 102.1 mAh g^(−1)at 5 *** work sheds light on the design of functional ceramic fillers for composite solid-state electrolytes to effec-tively enhance ion conductivity and battery performance.

关键词： ferroelectric ion conductor composite solid-state electrolytes space charge layer Li deposition

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Large upper critical fields and dimensionality crossover of superconductivity in the infinite-layer nickelate La0.8Sr0.2NiO2

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Physical Review B 2023年第22期107卷 L220503-L220503页

作者： Wei Wei Wenjie Sun Yue Sun Yongqiang Pan Gangjian Jin Feng Yang Yueying Li Zengwei Zhu Yuefeng Nie Zhixiang Shi Department of Physics Southeast University Nanjing 211189 China National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional Materials College of Engineering and Applied Sciences Nanjing University Nanjing 210093 People's Republic of China Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 People's Republic of China Key Laboratory of Materials Physics Institute of Solid State Physics Chinese Academy of Sciences Hefei 230031 China School of Electrical and Electronic Engineering Huazhong University of Science and Technology Wuhan 430074 China School of Physics Huazhong University of Science and Technology Wuhan 430074 China Wuhan National High Magnetic Field Center and School of Physics Huazhong University of Science and Technology Wuhan 430074 China

The recently emerging superconductivity in infinite-layer nickelates with the isostructural and isoelectronic characteristics of cuprates provides a new platform to explore the pairing mechanism of high-temperature superconductors. In this work, we studied the upper critical field (Hc2) of a high-quality La0.8Sr0.2NiO2 thin film with superconducting transition temperature, Tconset=18.8 K, using high magnetic field up to 56 T. A very large Hc2, ∼40 T for H∥c and ∼52 T for H⊥c, was confirmed, which suggests that infinite-layer nickelates also have great application potential. The anisotropy of Hc2 monotonically decreases from ∼10(γ=Hc2ab/Hc2c) near Tc to ∼1.5 at 2 K. Angle dependence of Hc2 confirms the crossover of superconductivity from two-dimensional to three-dimensional as the temperature decreases. We discussed that the interstitial orbital effect causes the weakening of anisotropy. The observed abnormal upturning of Hc2 at low temperatures is found to be a universal behavior independent of film quality and rare-earth elements. Therefore, it should not be the Fulde-Ferrell-Larkin-Ovchinnikov state due to the fact that it is in the dirty limit and insensitive to disorder.

关键词： High magnetic fields Multiband superconductivity Superconductivity High-temperature superconductors Type-II superconductors Unconventional superconductors Critical field Resistivity measurements

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Two-dimensional capillaries assembled by van der Waals heterostructures

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Nano Research 2023年第3期16卷 4119-4129页

作者： Jiaojiao Ma Kaiwen Guan Yu Jiang Yang Cao Sheng Hu State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Pen-Tung Sah Institute of Micro-Nano Science and Technology Xiamen UniversityXiamen 361005China

Research on two-dimensional materials in the past decades has brought many insights of low-dimensional science on a wide range of related *** a novel two-dimensional structure,the atomic-scale capillaries which can conceptually be seen as the empty space left by removing few layers of two-dimensional materials from their bulk van der Waals crystals offer a unique platform of investigating physical and chemical processes of ions,molecules,and atoms under two-dimensional *** of many important problems,such as capillary condensation and water network structure that are difficult to be explored experimentally in other confinement structures,has now been accessible;two-dimensional migration of ions,water,and gases shows abnormal transport properties beyond conventional theory prediction;influence of quantum effect to molecule permeation is observable even at room *** these discoveries greatly extend our fundamental understandings of nano-science,and stimulate the development of potential *** review the fabrication of these two-dimensional capillaries which are created by the assembly of van der Waals heterostructures,and discuss the ultimate steric effects in the smallest possible *** interactions between capillary interior and confined particles are also *** coupled with external stimuli,these channels exhibit tunable mass transport behaviors,which not only gives feedback to the mechanism understanding but in turn guides the channel structure optimization.

关键词： atomic-scale capillaries van der Waals heterostructures two-dimensional materials smallest confinement mass transport

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非化学计量比Ba_(0.9)(Fe_(0.5)Nb_(0.5))O_(3-δ)薄膜中晶格畸变诱导的铁电性

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science China materials 2023年第9期66卷 3681-3686页

作者：杨明迪李姗王艺霖籍伟花李天宇吕宗霖陈昕李强苗君邢献然 Beijing Advanced Innovation Center for Materials Genome Engineering Institute of Solid State ChemistryDepartment of Physical ChemistryUniversity of Science and Technology BeijingBeijing 100083China College of Materials Science and Engineering Nanjing Tech UniversityNanjing 211816China Beijing Advanced Innovation Center for Materials Genome Engineering Department of Physical ChemistryUniversity of Science and Technology BeijingBeijing 100083China

实现材料的顺电-铁电相变可以丰富铁电材料的多样性.本文通过设计和引入A位非化学计量缺陷,在Ba_(0.9)(Fe_(0.5)Nb_(0.5))O_(3-δ)薄膜中实现了晶格畸变,诱导出室温铁电.薄膜中引入的四方畸变和局部位错促进了结构的对称性破缺以及自发... 详细信息

实现材料的顺电-铁电相变可以丰富铁电材料的多样性.本文通过设计和引入A位非化学计量缺陷,在Ba_(0.9)(Fe_(0.5)Nb_(0.5))O_(3-δ)薄膜中实现了晶格畸变,诱导出室温铁电.薄膜中引入的四方畸变和局部位错促进了结构的对称性破缺以及自发极化的出现.在这里我们成功实现了室温下剩余极化Pr约为8μC cm^(-2)的铁电性和高达450℃的相稳定性温度我们的研究工作为通过缺陷工程发现和调节新型铁电材料提供了一种实用的方法.

关键词：对称性破缺铁电材料非化学计量比晶格畸变缺陷工程自发极化铁电相变相稳定性

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AI for organic and polymer synthesis

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science China Chemistry 2024年第8期67卷 2461-2496页

作者： Xin Hong Qi Yang Kuangbiao Liao Jianfeng Pei Mao Chen Fanyang Mo Hua Lu Wen-Bin Zhang Haisen Zhou Jiaxiao Chen Lebin Su Shuo-Qing Zhang Siyuan Liu Xu Huang Yi-Zhou Sun Yuxiang Wang Zexi Zhang Zhunzhun Yu Sanzhong Luo Xue-Feng Fu Shu-Li You Center of Chemistry for Frontier Technologies Department of ChemistryZhejiang UniversityHangzhou 310027China Center of Basic Molecular Science Department of ChemistryTsinghua UniversityBeijing 100084China Guangzhou National Laboratory Guangzhou 510005China Center for Quantitative Biology Academy for Advanced Interdisciplinary StudiesPeking UniversityBeijing 100871China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China School of Materials Science and Engineering Peking UniversityBeijing 100871China Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China AI for Science(AI4S)-Preferred Program Shenzhen Graduate SchoolPeking UniversityShenzhen 518055China State Key Laboratory of Chemical Biology Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China Department of Chemical Sciences National Natural Science Foundation of ChinaBeijing 100085China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Recent years have witnessed the transformative impact from the integration of artificial intelligence with organic and polymer synthesis. This synergy offers innovative and intelligent solutions to a range of classic problems in synthetic chemistry. These exciting advancements include the prediction of molecular property, multi-step retrosynthetic pathway planning, elucidation of the structure-performance relationship of single-step transformation, establishment of the quantitative linkage between polymer structures and their functions, design and optimization of polymerization process, prediction of the structure and sequence of biological macromolecules, as well as automated and intelligent synthesis platforms. Chemists can now explore synthetic chemistry with unprecedented precision and efficiency, creating novel reactions, catalysts, and polymer materials under the datadriven paradigm. Despite these thrilling developments, the field of artificial intelligence(AI) synthetic chemistry is still in its infancy, facing challenges and limitations in terms of data openness, model interpretability, as well as software and hardware support. This review aims to provide an overview of the current progress, key challenges, and future development suggestions in the interdisciplinary field between AI and synthetic chemistry. It is hoped that this overview will offer readers a comprehensive understanding of this emerging field, inspiring and promoting further scientific research and development.

关键词： organic synthesis polymer synthesis machine learning prediction chemical database automated synthesis

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