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AI for organic and polymer synthesis

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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Photochromic radical states in 3D covalent organic frameworks with zyg topology for enhanced photocatalysis

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National Science Review 2024年第7期11卷 177-188页

作者： Tian-Tian Ma Guo-Zhang Huang Xiao-Han Wang Yan Liang Run-Han Li Bin Wang Su-Juan Yao Jia-Peng Liao Shun-Li Li Yong Yan Ya-Qian Lan School of chemistry South China Normal University department of chemistry Guangdong Provincial Key Laboratory of Catalytic Chemistry Southern University of Science and Technology

Covalent-organic frameworks（COFs） with photoinduced donor-acceptor（D-A） radical pairs show enhanced photocatalytic activity in principle. However, achieving long-lived charge separation in COFs proves challenging due to the rapid charge recombination. Here, we develop a novel strategy by combining[6 + 4] nodes to construct zyg-type 3D COFs, first reported in COF chemistry. This structure type exhibits a fused Olympic-rings-like shape, which provides a platform for stabilizing the photoinduced D-A radical pairs. The zyg-type COFs containing catalytically active moieties such as triphenylamine and phenothiazine（PTZ） show superior photocatalytic production rates of hydrogen peroxide（H2O2）. Significantly, the photochromic radical states of these COFs show up to 400% enhancement in photocatalytic activity compared to the parent states, achieving a remarkable H2O2synthesis rate of 3324 μmol g-1h-1, which makes the PTZ-COF one of the best crystalline porous photocatalysts in H2O2production. This work will shed light on the synthesis of efficient 3D COF photocatalysts built on topologies that can facilitate photogenerating D-A radical pairs for enhanced photocatalysis.

关键词： 3D covalent-organic frameworks photochromic radical states donor and acceptor hydrogen peroxide photocatalysis

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Stereoselective recognition of morphine enantiomers by μ-opioid receptor

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National Science Review 2024年第3期11卷 183-191页

作者： Yibo Wang Van A.Ngo Xiaohui Wang Laboratory of Chemical Biology Changchun Institute of Applied ChemistryChinese Academy of Sciences Advanced Computing for Life sciences and Engineering Group Science Engagement Section National Center for Computational Sciences Oak Ridge National Lab School of Applied chemistry and Engineering University of Science and Technology of China Beijing National Laboratory for Molecular sciences

Stereospecific recognition of chiral molecules plays a crucial role in biological systems. The μ-opioid receptor（MOR） exhibits binding affinity towards（-）-morphine, a well-established gold standard in pain management, while it shows minimal binding affinity for the（+）-morphine enantiomer, resulting in a lack of analgesic activity. Understanding how MOR stereoselectively recognizes morphine enantiomers has remained a puzzle in neuroscience and pharmacology for over half-a-century due to the lack of direct observation techniques. To unravel this mystery, we constructed the binding and unbinding processes of morphine enantiomers with MOR via molecular dynamics simulations to investigate the thermodynamics and kinetics governing MOR's stereoselective recognition of morphine enantiomers. Our findings reveal that the binding of（-）-morphine stabilizes MOR in its activated state, exhibiting a deep energy well and a prolonged residence time. In contrast,（+）-morphine fails to sustain the activation state of ***, the results suggest that specific residues, namely D1142.50and D1473.32, are deprotonated in the active state of MOR bound to（-）-morphine. This work highlights that the selectivity in molecular recognition goes beyond binding affinities, extending into the realm of residence time.

关键词： stereoselective recognition thermodynamics and kinetics residence time morphine enantiomers μ-opioid receptor

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SO_(2)-Insertion induced enantioselective oxysulfonylation to access β-chiral sulfones with quaternary carbon stereocenters

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Science China chemistry 2024年第3期67卷 908-913页

作者： Jun Zhang Xuefeng Wang Peiqi Wang Jiayuan Fang Shaoyu Li Jie Wu School of Pharmaceutical and Chemical Engineering&Institute for Advanced Studies Taizhou UniversityShanghai 200438China department of chemistry Fudan UniversityShanghai 200438China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007China

β-Chiral sulfones are structural motifs widely found in natural products and bioactive molecules, while also serving as important intermediates for the synthesis of valuable chiral scaffolds. In contrast to the rapid growth of sulfur dioxide insertion chemistry over the last decade, enantioselective catalytic variants for accessing β-chiral sulfones, especially those bearing a quaternary carbon stereocenter, remain rare. Herein, we report an enantioselective copper/bisoxazoline catalyzed oxysulfonylation of alkenes to yield isoxazolinyl-containing β-chiral sulfones bearing quaternary carbon stereocenters with moderate to excellent yields and up to 96:4 er. The advantage and irreplaceability of this sulfur dioxide insertion catalytic system have been demonstrated by achieving transformations clearly unavailable with the previously reported sulfonyl chloride system. Additionally,the recoverability of the new-developed bisoxazoline ligand L9 and its reusability without any erosion of the catalytic activity and enantioselectivity further demonstrate the usefulness of the protocol.

关键词： β-chiral sulfones sulfur dioxide insertion oxysulfonylation copper catalysis enantioselectivity

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Coordination-driven self-assembly of a molecular 818knot and molecular borromean rings

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Science China chemistry 2024年第11期67卷 3652-3656页

作者： Xiang Gao Dong Liu Hai-Ning Zhang Guo-Xin Jin department of chemistry Fudan University

We report the facile construction of a molecular 818knot and a molecular Borromean rings assembly through self-assembly directed by Cp*Rh corner units. Two curved ligands of similar size and shape were used in this study. The slight steric differences between the two ligands induce the formation of distinctly different topologies of the assembled products. The structures were confirmed by single-crystal X-ray analysis and nuclear magnetic resonance spectroscopy.

关键词： coordination-driven Cp*Rh 818 knot Borromean rings

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Selective control of secondary alcohols upgrading using Ir-catalyzed cross-coupling strategy

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Science China chemistry 2024年第3期67卷 914-921页

作者： Siqi Yang Zeye Lu Jiale Ji Qingshu Zheng Tao Tu Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China Frontiers Science Center for Transformative Molecules School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

The selective coupling of alcohols is a fascinating yet challenging approach for upgrading alcohols. Herein, we accomplished the controlled production of β-disubstituted ketones or upgraded secondary alcohols via the Ir-catalyzed cross-coupling of secondary alcohols in excellent yields with broad substrate scopes. This selective control was achieved by using an in-situ generated monoNHC-Ir or a tris-NHC-Ir complex as the catalysts, respectively. Mechanistic studies revealed that the delicate balance between dehydrogenation and hydrogenation abilities of these bifunctional catalysts is crucial for achieving different selectivity. The tris-NHC-Ir complex effectively facilitated dehydrogenation of alcohols and hydrogenation of intermediates, leading to the desired upgraded secondary alcohols. Conversely, the high dehydrogenation ability of the mono-NHC-Ir complex promoted the conversion of formed secondary alcohols back to ketones.

关键词： cross-coupling hydrogen-borrowing NHC-Ir complexes selectivity control upgrading of alcohols

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Access to Versatile Functionalized Cu(Ⅲ) Complexes Enabled by Direct Transmetalation to Well-Defined Copper(Ⅲ) Fluoride Complex Me_(4)N^(+)[Cu(CF_(3))_(3)F]^(-)

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Chinese Journal of chemistry 2024年第10期42卷 1107-1113页

作者： Guangyu Wang Huaiyuan Li Xuebing Leng Long Lu Qilong Shen Key Laboratory of Fluorine and Nitrogen chemistry and Advanced Materials Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling LuShanghai 200032China

The invention of a well-defined Cu(Ⅲ)fluoride complex Me_(4)N^(+)[Cu(CF_(3))_(3)(F)]^(-)1 enabled to access a versatile of functionalized Cu(Ⅲ)complexes[Me_(4)N]^(+)[Cu(X)(CF_(3))_(3)]^(-)(X=C_(6)F_(5),C_(6)F_(5)C≡C,CN,Cl,N_(3),^(t)BuOO,SCN,OAc,SAr),many of them for the first *** availability of these complexes allowed us to evaluate the trans-influence order of ligand in Cu(Ⅲ)complexes:Bn>CF_(3)^(-)>C_(6)F_(5)^(-)>N_(3)^(-)>py~CH_(3)^(-)~C_(6)F_(5)C≡C>NO_(2)PhO^(-)~^(t)BuOO^(-)~CH_(3)COO^(-)>F^(-).

关键词： Fluorine Copper Cu(Ⅲ) Cu(Ⅲ)fluoride Trifluoromethyl

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Pd-catalyzed intermolecular Si–O formation via Si–C activation

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Science China chemistry 2024年第8期67卷 2661-2669页

作者： Shuang Liu Yu-Shu Chen Yichen Wu Peng Wang State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesShanghai 200032China School of chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China College of Material chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistryand Material Technology of Ministry of EducationHangzhou Normal UniversityHangzhou 311121China

The development of efficient Si–O bond formation reaction with 100% atom-economy, excellent functional group tolerance, and broad scope under mild conditions is highly desired due to the prevalence of silanol, silyl ether, and their derivatives in synthetic chemistry and materials science. Here, we have realized the Pd-catalyzed Si–O formation reaction via a Si–C activation approach with 100% atom-economy by employing silacyclobutanes(SCBs) and various hydroxy-containing substrates, including water,alcohols, phenols, and silanols. This protocol features a broad substrate scope, remarkable functional compatibility and mild conditions, providing a series of silanols, silyl ethers in high efficiency. Notably, this protocol could also be used for selective protection of hydroxy functionalities, and for the access of a class of novel polymers containing Si–O main chain. Preliminary mechanistic studies unveiled that this reaction underwent a Pd-catalyzed concerted ring-opening mechanism.

关键词： Si–O formation Si–C activation palladium silacyclobutane silanol silyl ether

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Solid-state atomic hydrogen as a broad-spectrum RONS scavenger for accelerated diabetic wound healing

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National Science Review 2024年第2期11卷 196-206页

作者： Man Luo Qin Wang Gang Zhao Wei Jiang Cici Zeng Qingao Zhang Ruyu Yang Wang Dong Yunxi Zhao Guozhen Zhang Jun Jiang Yucai Wang Qing Zhu Key Laboratory of Precision and Intelligent chemistry School of Chemistry and Materials Science University of Science and Technology of China department of Radiology The First Affiliated Hospital of University of Science and Technology of China Division of Life Sciences and Medicine University of Science and Technology of China Shenzhen Senior High School Institute of Intelligent Innovation Henan Academy of Sciences

Hydrogen therapy shows great promise as a versatile treatment method for diseases associated with the overexpression of reactive oxygen and nitrogen species（RONS）. However, developing an advanced hydrogen therapy platform that integrates controllable hydrogen release, efficient RONS elimination, and biodegradability remains a giant technical challenge. In this study, we demonstrate for the first time that the tungsten bronze phase H0.53WO3（HWO） is an exceptionally ideal hydrogen carrier, with salient features including temperature-dependent highly-reductive atomic hydrogen release and broad-spectrum RONS scavenging capability distinct from that of molecular hydrogen. Moreover, its unique p H-responsive biodegradability ensures post-therapeutic clearance at pathological sites. Treatment with HWO of diabetic wounds in an animal model indicates that the solid-state atomic H promotes vascular formation by activating M2-type macrophage polarization and anti-inflammatory cytokine production, resulting in acceleration of chronic wound healing. Our findings significantly expand the basic categories of hydrogen therapeutic materials and pave the way for investigating more physical forms of hydrogen species as efficient RONS scavengers for clinical disease treatment.

关键词： atomic hydrogen RONS scavenger inflammatory regulation diabetic wound healing hydrogen therapy

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Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li Meiling Xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor *** the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient ***,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)*** lattice disorder in HEOs is believed to increase migration energy barrier of lattice *** a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) *** work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction

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