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Photosynthetic reaction pathways of natural and artificial systems

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Science China Chemistry 2025年

作者： Shixing Lei Liting Bi Lingxuan Chen Zhanting Li Jia Tian State Key Laboratory of Organometallic Chemistry and Shanghai Hong Kong Joint Laboratory in Chemical synthesis Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences

Photosynthesis converts solar energy into chemical energy through highly coordinated photosynthetic *** by natural systems,artificial photosynthesis aims to develop an efficient,sustainable,and cost-effective pathway for solar-tochemical *** review examines natural photosynthetic pathways,including retinal/rhodopsin-,bacteriochlorophyll-,and chlorophyll-based systems,highlighting their key components and ***,we outline reaction pathways in artificial photosynthetic systems constructed via heterogeneous,homogeneous,self-assembly,and semi-artificial strategies,focusing on water splitting,carbon fixation,and nitrogen ***,we offer insights into future directions for artificial photosynthesis,emphasizing the importance of using self-assembly strategies and the potential of using primitive phototrophic microorganisms as models.

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Enantioselective β-alkenylation of α,β-unsaturated aldehydes via chiral biphosphine ligand modified dirhodium(II) catalysis

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Science China Chemistry 2025年

作者： Guangli Xu Hongda Chen Xiaoming Wang State Key Laboratory of Organometallic Chemistry and Shanghai Hongkong Joint Laboratory in Chemical synthesis Center for Excellence in Molecular Synthesis Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences School of Chemistry and Materials Science Hangzhou Institute for Advanced Study University of Chinese Academy of Sciences School of Chemistry and Chemical Engineering Henan Normal University

Dirhodium(II) complexes have achieved great success in organic synthesis,and fine-tuning their catalytic properties with various bridging ligands is well-investigated in carbene ***,combining dirhodium(II) with a sophisticated ligand as a catalyst in other reactions is still extremely challenging,especially for the asymmetric synthesis of valuable chiral ***,we report a dirhodium(II)/(S)-MeO-BIPHEP catalytic system for the challenging asymmetric β-alkenylation of α,β-unsaturated aldehydes,affording the corresponding chiral conjugate addition products in good yields with high enantioselectivities.A couple of drug-derived substrates were also compatible with the protocol,which has been successfully used to prepare biologically relevant pyranochromene *** mechanistic studies suggested that the dirhodium core might remain intact over the catalytic cycle,and the chiral diphosphine ligand plays a key role in this novel reactivity and determining the high enantioselectivities of the asymmetric conjugate addition.

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Effect of Ti Additions on Mechanical and Thermodynamic Properties of W-Ti Alloys: A First-principles Study

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Journal of Wuhan University of Technology(Materials Science) 2025年第1期40卷 246-257页

作者： ZHANG Jian NIE Wei HUANG Jin ZHU Ke LIU Ruxia ZHANG Ruizhi LUO Guoqiang SHEN Qiang State Key Laboratory of Advanced Technology for Materials synthesis and Processing Wuhan University of TechnologyWuhan 430070China institute for Carbon Neutrality University of Science and Technology BeijingBeijing 100083China

The mechanical and thermodynamic properties of W-Ti alloys(including W_(15)Ti_(1),W_(14)Ti_(2),W_(12)Ti_(4) and W_(8)Ti_(8) alloys)were investigated by the first-principles approach based on density functional *** results indicate that W-Ti alloys except W_(8)Ti_(8) are thermodynamically *** modulus and hardness of W-Ti alloys are smaller than those of pure tungsten and gradually decrease with increasing Ti ***,their B/G ratios and Poisson's ratios exceed those of pure tungsten,suggesting that the introduction of Ti decreases the mechanical strength while enhancing the ductility of W-Ti *** thermal expansion coefficients for W-Ti alloys all surpass those of pure tungsten,indicating that the introduction of titanium exacerbates the thermal expansion behavior of W-Ti ***,elevated pressure has the capacity to suppress the thermal expansion tendencies in titanium-doped tungsten *** study offers theoretical insights for the design of nuclear materials by exploring the mechanical and thermodynamic properties of W-Ti alloys.

关键词： first-principles mechanical properties thermodynamic properties tungsten-titanium alloys

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Enantio-divergent C–H borylation with two different ligands from a single chiral source

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Science China Chemistry 2025年第1期68卷 226-232页

作者： Rongrong Du Senmiao Xu State Key Laboratory for Oxo synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of Material Chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of Education Hangzhou Normal University University of Chinese Academy of Sciences

Reported here is an iridium-catalyzed enantio-divergent C（sp3）–H borylation of α-gem-dimethyl groups of trifluoromethyl ketone-derived hydrazones to construct a series of acyclic all-carbon quaternary stereocenters with a high level of chiral induction. Two different chiral bidentate boryl ligands from a common chiral source not only can switch the enantioselectivity but also are complementary in terms of the substrate scope.

关键词： asymmetric catalysis C–H borylation all-carbon quaternary stereocenters synthetic methods

CoTCPP integrates with BiOBr microspheres for improved solar-driven CO_(2)reduction performance

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Green Energy & Environment 2025年第1期10卷 193-202页

作者： Lina Li Yi Zhang Gaopeng Liu Tiange Wei Junze Zhao Bin Wang Mengxia Ji Yuanbin She Jiexiang Xia Huaming Li School of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu University301 Xuefu RoadZhenjiang212013China State Key Laboratory Breeding Base of Green Chemistry-synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou310014China

CO_(2) photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse ***,the 5,10,15,20-tetra(4-carboxyphenyl)porphyrin cobalt(II)(CoTCPP)has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr *** as-prepared CoTCPP/BiOBr-2 composite shows optimized photocatalytic performance for CO_(2) conversion into CO and CH_(4) upon irradiation with 300 W Xe lamp,which is 2.03 and 2.58 times compared to that of BiOBr,*** introduced CoTCPP significantly enhanced light absorption properties,promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO_(2) *** metal Co^(2+) at the center of the porphyrin molecules also acts as adsorption center for CO_(2) molecules,accelerating the CO_(2) conversion into CO and *** possible mechanism of CO_(2) photoreduction was explored by in-situ FT-IR *** work offers a new possibility for the preparation of advanced photocatalysts.

关键词： BiOBr CoTCPP CO_(2)photoreduction Carriers transfer CO_(2)adsorption-activation

synthesis of chiral phosphine derivatives through a copper（I）-catalyzed desymmetric SNAr reaction

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Science China Chemistry 2025年

作者： Shuai Zhang Pei-Zhi Liu Yan-Bo Li Qi Zhang Jun-Zhao Xiao Yi-Fan Wang Tian-Yu Wei Jia-Wei Jiang Ye Wang Qian Peng Liang Yin Key Laboratory of Fluorine and Nitrogen Chemistry and Advanced Materials Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences State Key Laboratory of Elemento-organic Chemistry and Tianjin Key Laboratory of Biosensing and Molecular Recognition College of Chemistry Frontiers Science Center for New Organic Matter Nankai University Haihe Laboratory of Sustainable Chemical Transformations

Axially chiral phosphines are a class of extremely important ligands in asymmetric catalysis. Herein, an unprecedented copper（I）-catalyzed asymmetric SNAr reaction with HP（S）R2is uncovered, which delivers a series of axially chiral phosphine derivatives in high yields with excellent enantioselectivity. Furthermore, the diastereoselective reaction with the kinetic resolution of racemic HP（S）ArR proceeds smoothly, providing the products with moderate diastereoselectivity and excellent enantioselectivity. Control experiments indicate that HP（S）Ph2is much more active than HPPh2and HP（O）Ph2as the pronucleophile in the present reaction. It is found that the SNAr reaction （the first SNAr） proceeds in a desymmetric manner, providing the desired chiral products while a continued SNAr reaction （the second SNAr） slightly occurs in a kinetic resolution manner in the present catalytic system, which enhances the ee of the desired chiral products. DFTcalculations support a concerted reaction pathway rather than a step-wise mechanism. Finally, axially chiral olefin-phosphines produced by the present method work as suitable ligands in Pdcatalyzed asymmetric allylic substitution with C-, N-, and O-nucleophiles and Rh-catalyzed asymmetric addition of arylboronic acid to benzil.

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Regulating crystallization and retarding oxidation in Sn-Pb perovskite via 1D cation engineering for high performance all-perovskite tandem solar cells

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Journal of Energy Chemistry 2025年第1期100卷 646-652页

作者： Ranran Liu Xin Zheng Zaiwei Wang Miaomiao Zeng Chunxiang Lan Shaomin Yang Shangzhi Li Awen Wang Min Li Jing Guo Xuefei Weng Yaoguang Rong Xiong Li Michael Gr?tzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences School of Physics and Optoelectronic Engineering Hainan University Suzhou institute of Nano-Tech and Nano-Bionics (SINANO) Chinese Academy of Sciences School of Chemistry Chemical Engineering and Life Sciences State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

All-perovskite tandem solar cells have the potential to surpass the theoretical efficiency limit of single junction solar cells by reducing thermalization ***,the challenges encompass the oxidation of Sn2+to Sn4+and uncontrolled crystallization kinetics in Sn-Pb perovskites,leading to nonradiative recombination and compositional heterogeneity to decrease photovoltaic efficiency and operational ***,we introduced an ionic liquid additive,1-ethyl-3-methylimidazolium iodide （EMIMI） into Sn-Pb perovskite precursor to form low-dimensional Sn-rich/pure-Sn perovskites at grain boundaries,which mitigates oxidation of Sn2+to Sn4+and regulates the film-forming dynamics of Sn/Pb-based perovskite *** optimized single-junction Sn-Pb perovskite devices incorporating EMIMI achieved a high efficiency of 22.87%.Furthermore,combined with wide-bandgap perovskite sub-cells in tandem device,we demonstrate 2-terminal all-perovskite tandem solar cells with a power conversion efficiency of 28.34%,achieving improved operational stability.

关键词： All-perovskite tandem solar cells Sn-Pb perovskite 1D Regulated crystallization Antioxidation

ZnCdS-BiFeO3异质结负载钴催化剂促进光电催化产氢（英文）

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Science China Materials 2025年

作者：王玲娄青钱海霞尹晓爽刘瑛杨文忠徐晖 institute of Advanced synthesis School of Chemistry and Molecular EngineeringNanjing Tech University

Z-型光电化学（PEC）系统在氢气生产和水分解方面的发展,对解决日益严重的全球能源危机具有重要意义.在这项研究中,使用了一种三元Co-ZnCdS-BiFeO3Z-型复合光催化剂.通过优化BiFeO3/ZnCdS的比例,不仅增强了材料的光催化活性,还提升了电...

Z-型光电化学（PEC）系统在氢气生产和水分解方面的发展,对解决日益严重的全球能源危机具有重要意义.在这项研究中,使用了一种三元Co-ZnCdS-BiFeO3Z-型复合光催化剂.通过优化BiFeO3/ZnCdS的比例,不仅增强了材料的光催化活性,还提升了电子传输效率,并增强了光电阴极的稳定性.选择Co（dmgBF2）2（H2O）2作为助催化剂,以进一步提高电子-空穴分离效率和光腐蚀抵抗力.在可见光照射下,光电化学系统的产氢速率可达到4.03 mmol g-1h-1.在最佳条件下,施加-0.1 V vs. RHE的偏压可产生-38.5μA cm-2的电流密度.其光催化电流密度比纯ZnCdS高出13倍,大大提高了光催化剂的产氢效率和稳定性.本研究为设计用于水分解的高效Z-型光催化剂树立了新的标杆,并通过PEC分析提供了关于内在阻力的全新见解.

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An efficient synthetic approach towards new 5,5'-diaryl-2,2'-bipyridine-based fluorophores

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Chinese Chemical Letters 2017年第5期28卷 1099-1103页

作者： Alexey P.Krinochkin Dmitry S.Kopchuk Nikolay V.Chepchugov Grigory A.Kim Igor S.Kovalev Matiur Rahman Grigory V.Zyryanov Adinath Majee Vladimir L.Rusinov Oleg N.Chupakhin Ural Federal University Yekaterinburg 620002Russian Federation postovsky institute of organic synthesis of RAS(Ural Division) Yekaterinhurg 620990Russian Federation Department of Chemistry Visva-Bharati(A Central University)Santiniketan 731235India

An efficient approach has been developed for the synthesis of 5,5＇-diaryl-2,2＇-bipyridines via their 1,2,4-triazine *** notable advantages of the present method are：The possibility of varying the aromatic substituents in the positions 5 and 5＇ of bipyridine core and the possibility for obtaining 2,2＇-bipyridines bearing a fused cyclopentene core to increase the solubility in organic *** 5,5＇-diaryl-2,2＇-bipyridines exhibited an intense emission in a range of ca.422-521 nm in acetonitrile solution;depending on the nature of the aromatic substituents and the presence of annulated cyclopentene *** from that,the significant bathochromic shifts of the both absorption and emission maxima were observed in comparison with a number of previously described similar *** some cases the significant increasing of the fluorescence quantum yields took place.

关键词： 2 2'-Bipyridines 1 2 4-Triazines Aza-Diels-Alder reaction Fluorescence

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