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Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China Chemistry 2025年第1期 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie State key laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University Green Catalysis Center College of Chemistry Zhengzhou University State key laboratory of Natural Medicines China Pharmaceutical University

Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis. A wide range of structurally diverse primary, secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with the α-C(sp3)–H in glycine residue of peptides. This protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups. A series of relay transformations to construct cyclic peptides, to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic practicality. In addition, mechanistic studies and density functional theory(DFT) calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET) mechanism.

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Orbitronics for energy-efficient magnetization switching

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Science China(Information Sciences) 2025年第1期 398-399页

作者： Yuxuan YAO Daoqian ZHU Qingtao XIA Jianing LIANG Yuhao JIANG Zhiyang PENG Jiaxu LI Chen XIAO Renyou XU Wenwen WANG Xiantao SHANG Shiyang LU Dapeng ZHU Hong-Xi LIU Kaihua CAO Weisheng ZHAO Fert Beijing Institute School of Integrated Circuit Science and Engineering Beihang University National key Lab of Spintronics Institute of International Innovation Beihang University Qingdao Research Institute Beihang University Truth Memory Corporation

Spin-orbit torque （SOT）,as a promising writing method for magnetic random-access memory （MRAM）,has garnered widespread interest for over a decade [1].Heavy metals,such as β-W,have been broadly adopted as spin current sources,but suffer from phase change at a limited thickness,resulting in a dramatic reduction of the charge-tospin conversion efficiency θSH[2].The thickness limitation leads to stringent etching conditions and large distribution among devices,posing challenges for simultaneously satisfying SOT efficiency,etching-stop margins,and back-end-ofline （BEOL） compatibility.

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Cobalamin-dependent radical S-adenosyl-L-methionine protein functions with a partner to successively methylate tricyclic indole alkaloid for chuangxinmycin maturation and derivatization

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Science China Chemistry 2025年第1期 308-316页

作者： Sili Wang Jiancheng Huang Yanan Du Wei Huang Yufeng Xue Xiaokun Xu Guannan Zhong Yuanyuan Shi Bin Hong Xiaoying Bian Wen Liu State key laboratory of Chemical Biology Shanghai Institute of Organic Chemistry University of Chinese Academy of SciencesChinese Academy of Sciences State key laboratory of Microbial Technology Shandong University National Health Commission (NHC) key laboratory of Biotechnology for Microbial Drugs Institute of Medicinal BiotechnologyChinese Academy of Medical Science & Peking Union Medical College

Cobalamin(Cbl)-dependent radical S-adenosyl-L-methionine(SAM) proteins constitute the largest collection of the radical SAM superfamily that has hundreds of thousands of individual members. Many of these proteins are involved in the biosynthesis of pharmaceutically important natural products to catalyze chemically demanding reactions. In the biosynthetic pathway of chuangxinmycin(CXM), a unique indole alkaloid antibiotic with potent anti-infective activity, functionalization of the characteristic thiopyrano[4,3,2-cd]indole scaffold by regio-and stereoselective C3-methylation is believed to rely on a Cbl-dependent radical process, which, however, remained to be reconstituted biochemically. We here report the dissection of this enzymatic process, which requires the incorporation of Cxm8, a Cbl-dependent radical SAM protein, with Cxm9, a DUF5825family protein that shares no homology to any proteins of known functions. Cxm8 and Cxm9 function together by forming an unexpected heterodimeric complex that selectively catalyzes C3-methylation of the tricyclic indole-S-hetero ring system in a successive manner, achieving CXM and a recently identified, C3-dimethylated congener. Detailed biochemical characterization,isotope labeling, structural simulation and bioinformatics analysis rationalized the catalysis of the Cxm8/Cxm9 complex and particularly the necessity of the DUF5825 protein for C3-methylase activity. This is the first example that a Cbl-dependent protein acts with a partner to exhibit radical SAM activity.

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Cyano migration-mediated radical-polar crossover cyclopropanation

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Science China Chemistry 2025年第01期 241-248页

作者： Ziqiang Wang Yasu Chen Jie Li Chen Zhu key laboratory of organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials ScienceSoochow University Frontiers Science Center for Transformative Molecules Zhangjiang Institute for Advanced Study and Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Shanghai Jiao Tong University

We report a novel cyano migration-mediated radical-polar crossover process, whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently achieved. This transformation yields a diverse array of multisubstituted cyclopropanes under mild photocatalytic conditions. Mechanistic studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution, leading to the formation of the cyclopropane derivatives.

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调控串联三金属AuAgCu异质结上*CO中间体的吸附构型,促进CO2通过不对称C-C耦合电还原为乙醇（英文）

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Science China Materials 2025年第1期 173-179页

作者：石永霞李俊俊闵志雯王鑫亿侯曼马昊庄泽超秦毓辰孙源淼王定胜张志成 key laboratory of organic integrated circuit Ministry of Education & Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of Chemistry School of Science Tianjin University Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Department of Chemistry Tsinghua University College of Sciences Henan Agricultural University

在电化学CO2还原反应中,合理调节关键中间体*CO的吸附构型可以促进碳-碳（C–C）偶联生成多碳产物.在这项工作中,理论计算表明,通过顶式吸附的*CHO和三重位吸附的*CO在Cu位点上进行C–C耦合是一种能量有利的途径.作为概念验证,制备了串...

在电化学CO2还原反应中,合理调节关键中间体*CO的吸附构型可以促进碳-碳（C–C）偶联生成多碳产物.在这项工作中,理论计算表明,通过顶式吸附的*CHO和三重位吸附的*CO在Cu位点上进行C–C耦合是一种能量有利的途径.作为概念验证,制备了串联三金属AuAgCu异质结（Au@Ag/Cu）,其中Au@Ag位点上顶式吸附的*CO溢流到Cu位点后转变为三重位吸附,然后该三重位吸附的*CO和Cu位点上顶式吸附的*CHO进行不对称C–C偶联,促进了乙醇产物的形成.在-0.3 V ***的低电位下,乙醇法拉第效率最高为65.9%.我们的工作通过调节中间产物的吸附构型,为串联催化的内在机制提供了新的见解.

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Dynamic Regulation of Hydrogen Bonding Networks and Solvation Structures for Synergistic Solar‑Thermal Desalination of Seawater and Catalytic Degradation of organic Pollutants

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Nano-Micro Letters 2025年第2期17卷 548-565页

作者： Ming‑Yuan Yu Jing Wu Guang Yin Fan‑Zhen Jiao Zhong‑Zhen Yu Jin Qu Beijing key laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China State key laboratory of organic‑Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Although solar steam generation strategy is efficient in desalinating seawater,it is still challenging to achieve continuous solar-thermal desalination of seawater and catalytic degradation of organic ***,dynamic regulations of hydrogen bonding networks and solvation structures are realized by designing an asymmetric bilayer membrane consisting of a bacterial cellulose/carbon nanotube/Co_(2)(OH)_(2)CO_(3)nanorod top layer and a bacterial cellulose/Co_(2)(OH)_(2)CO_(3)nanorod(BCH)bottom ***,the hydrogen bonding networks inside the membrane can be tuned by the rich surface–OH groups of the bacterial cellulose and Co_(2)(OH)_(2)CO_(3)as well as the ions and radicals in situ generated during the catalysis ***,both SO_(4)^(2−)and HSO_(5)−can regulate the solvation structure of Na^(+)and be adsorbed more preferentially on the evaporation surface than Cl^(−),thus hindering the de-solvation of the solvated Na^(+)and subsequent nucleation/growth of ***,the heat generated by the solar-thermal energy conversion can accelerate the reaction kinetics and enhance the catalytic degradation *** work provides a flow-bed water purification system with an asymmetric solar-thermal and catalytic membrane for synergistic solar thermal desalination of seawater/brine and catalytic degradation of organic pollutants.

关键词： Solar steam generation Seawater desalination Catalytic degradation Bacterial cellulose Cobalt hydroxycarbonate nanorods

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A Rapid Adaptation Approach for Dynamic Air‑Writing Recognition Using Wearable Wristbands with Self‑Supervised Contrastive Learning

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Nano-Micro Letters 2025年第2期17卷 417-431页

作者： Yunjian Guo Kunpeng Li Wei Yue Nam‑Young Kim Yang Li Guozhen Shen Jong‑Chul Lee Department of Electronic Convergence Engineering Kwangwoon UniversitySeoul 01897South Korea Radio Frequency integrated circuit(RFIC)Bio Centre Kwangwoon UniversitySeoul 01897South Korea Department of Electronic Engineering Kwangwoon UniversitySeoul 01897South Korea School of Microelectronics Shandong UniversityJinan 250101People’s Republic of China State key laboratory of integrated Chips and Systems Fudan UniversityShanghai 200433People’s Republic of China School of integrated circuits and Electronics Beijing Institute of TechnologyBeijing 100081People’s Republic of China

Wearable wristband systems leverage deep learning to revolutionize hand gesture recognition in daily *** existing approaches that often focus on static gestures and require extensive labeled data,the proposed wearable wristband with selfsupervised contrastive learning excels at dynamic motion tracking and adapts rapidly across multiple *** features a four-channel sensing array composed of an ionic hydrogel with hierarchical microcone structures and ultrathin flexible electrodes,resulting in high-sensitivity capacitance *** wireless transmission from a Wi-Fi module,the proposed algorithm learns latent features from the unlabeled signals of random wrist ***,only few-shot labeled data are sufficient for fine-tuning the model,enabling rapid adaptation to various *** system achieves a high accuracy of 94.9%in different scenarios,including the prediction of eight-direction commands,and air-writing of all numbers and *** proposed method facilitates smooth transitions between multiple tasks without the need for modifying the structure or undergoing extensive task-specific *** utility has been further extended to enhance human–machine interaction over digital platforms,such as game controls,calculators,and three-language login systems,offering users a natural and intuitive way of communication.

关键词： Wearable wristband Self-supervised contrastive learning Dynamic gesture Air-writing Human-machine interaction

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Bifunctional bridging capping layer enables 24.5% efficiency of perovskite solar cells with polymer-based hole transport materials

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Science China Chemistry 2025年第1期 350-359页

作者： Can Zhu Yiyang Wang Lei Meng Beibei Qiu Jing Li Shucheng Qin Ke Hu Xin Jiang Wenbin Lai Minchao Liu Zhe Liu Chenxing Lu Jinyuan Zhang Yongfang Li Beijing National laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences School of Chemical Science University of Chinese Academy of Sciences key laboratory of Solid State Optoelectronic Devices of Zhejiang Province College of Physics and Electronic Information Engineering Zhejiang Normal University key laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of Sciences laboratory of Advanced Optoelectronic Materials College of Chemistry Chemical Engineering and Materials ScienceSoochow University

Developing a bridge capping layer between perovskite and hole transport layer materials（HTMs） in the n-i-p perovskite solar cells（pero-SCs） is an effective approach to modify the morphology of HTMs and passivate the perovskite ***, we select the quinoxaline-based bifunctional passivation agent, quinoxalin-6-yl-methylamine hydrochloride（Qx MACl）,as the bridging layer, and a D-A copolymer PBQ12 containing the same quinoxaline unit as an HTM for the n-i-p pero-SCs. Due to the π-π stacking among the common quinoxaline units in the bridge layer and HTM, Qx MACl induces the π-π stacking of the PBQ12 film and improves the film morphology of HTMs with better conductivity. Additionally, Qx MACl can effectively passivate the perovskite surface, and PBQ12 possesses appropriate energy levels and high hole mobility. The pero-SCs based on FAPbI3with PBQ12/Qx MACl treatment showed a higher power conversion efficiency（PCE） of 24.05% and outstanding stability, maintaining 95.4% and 92.1% of its initial PCE after 750 h of storage and after over 800 h of thermal annealing at 85 °C, respectively. To further enhance the PCE of the PBQ12/Qx MACl-based devices, we developed a non-metal ion dopant for the PBQ12 HTM. Through trace doping of PBQ12 HTM by the non-metal ion dopant, the PCE of the PBQ12/Qx MACl-based devices reached 25.24%（the calibrated PCE of 24.55% by the National Institute of Metrology, China）.

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De novo synthesis of atropisomeric benzofurans via Cu/SPDO complex catalyzed asymmetric formal [3 + 2] annulation

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Science China Chemistry 2025年第1期 174-180页

作者： Fan-Xiao Meng Xing-Yu Wang Ka Lu Ju-Song Yang Fu-Min Zhang Ai-Jun Ma Bao Du Yong-Qiang Tu State key laboratory of Applied organic Chemistry College of Chemistry and Chemical Engineering Lanzhou University School of Chemistry and Chemical Engineering Shanghai Jiao Tong University School of Biotechnology and Health Sciences Wuyi University

Herein, the de novo synthesis of atropisomeric benzofurans through the Cu/spirocyclic-pyrrolidine-oxazoline(SPDO) complex catalyze asymmetric formal [3 + 2] cycloaddition between quinones and ynamides is explored, producing a range of structurally diverse axially chiral benzofurans in satisfactory yields with good to excellent enantioselectivities. Furthermore, density functional theory calculations were applied to explain the possible reaction mechanism.

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