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Synergistic enhancement of ion/electron transport by ultrafine nanoparticles and graphene in Li2FeTiO4/C/G nanofibers for symmetric Li-ion batteries

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Journal of Energy chemistry 2025年第02期101卷 42-51页

作者： Wenjie Ma Yakun Tang Yue Zhang Xiaohui Li Lang Liu Xueting Wang Yuliang Cao State Key laboratory of chemistry and Utilization of Carbon Based Energy Resources Key Laboratory of Energy Materials Chemistry Ministry of Education College of Chemistry Xinjiang University College of chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University

Low-cost Fe-based disordered rock salt（DRX） Li2FeTiO4is capable of providing high capacity(295 mA h g-1) by redox activity of cations(Fe2+/Fe4+and Ti3+/Ti4+) and anionic ***,DRX structures lack transport channels for ions and electrons,resulting in sluggish kinetics,poor electrochemical activity,and ***,graphene conductive carbon network permeated Li2FeTiO4（LFT/C/G） nanofibers are successfully prepared by a facile sol-gel assisted electrospinning *** Li2FeTiO4nanoparticles（2 nm） and one-dimensional（1D） structure provide abu ndant active sites and unobstructed diffu sion channels,accelerating ion *** addition,introducing graphene reduces the band gap and Li+diffusion barrier and improves the dynamic properties of Li2FeTiO4,thus achieving a relatively mild interfacial reaction and reversible redox *** expected,the LFT/C/1.0G cathode delivers a remarkable discharge capacity(238.5 mA h g-1),high energy density(508.8 Wh kg-1),and excellent rate capability(51.2 mA hg-1at 1.0 A g-1).Besides,the LFT/C/1.0G anode also displays a high capacity(514.5 mA h g-1at 500 mA g-1) and a remarkable rate capability(243.9 mA h g-1at 8 A g-1).Moreover,the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g-1after 100 cycles at 50 mA *** study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.

关键词： 1D structure Disordered rock salt Li2FeTiO4 Graphene Lithium-ion battery electrode Rapid ion/electron transport

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High-throughput experimentation and machine learning-promoted synthesis of α-phosphoryloxy ketones via Ru-catalyzed P(O)O–H insertion reactions of sulfoxonium ylides

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Science China chemistry 2025年第2期68卷 679-686页

作者： An Lin Jingyuan Liu Yougen Xu Haiting Wu Yating Chen Yan Zhang Lebin Su Xiaodan Zhao Kuangbiao Liao Institute of Organic chemistry&MOE Key laboratory of Bioinorganic and Synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510006China Guangzhou National laboratory Guangzhou 510005China Bioland laboratory Guangzhou 510005China

Herein,we report a novel and highly efficient method for the synthesis ofα-phosphoryloxy carbonyl compounds via Rucatalyzed P(O)O–H insertion reactions of sulfoxonium ylides and phosphinic acids,with the assistance of high-throughput experimentation(HTE)and machine learning(ML).A variety of P(O)O−H derivatives,including diarylphosphates,alkyl phosphates,and alkoxyphosphates,are competent candidates to react with sulfoxonium ylides in this transformation,and variousα-phosphoryloxy carbonyls and propylene phosphates are directly *** approach utilizes readily available sulfoxonium ylide as a carbene precursor,and features mild conditions,operational simplicity,and broad functional groups tolerance,and could be used for late-stage functionalization of structurally complex bioactive ***,a conducive exploration of the reaction space is also conducted(756 reactions)and a machine learning model for reaction yield prediction has been developed and applied,showcasing the practical application of this newly workflow(HTE-ML)in the field of synthetic chemistry.

关键词： α-phosphoryloxy ketones high-throughput experimentation machine learning P(O)O-H insertion sulfoxonium ylides

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Alumina supported platinum-ceria catalyst for reverse water gas shift reaction

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Journal of Rare Earths 2025年第2期43卷 284-294页

作者： Na Jiang Weiwei Wang Haoxin Liu Meiyao Wu Chunjiang Jia Key laboratory for Colloid and Interface chemistry Key Laboratory of Special Aggregated MaterialsSchool of Chemistry and Chemical EngineeringShandong University

The activation of CO2molecules is a fundamental step for their effective *** highdensity oxygen vacancies on the surface of reducible oxides is pivotal for the activation of *** this work,we prepared a series of 0.5PtxCe/Al2O3（x=1,5,10,or 20） catalysts with varying Ce loading and 0.5 wt% of Pt for the reverse water gas shift（RWGS） *** size of CeO2particle increases with Ce ***,the 0.5Pt5Ce/Al2O3catalyst with an average CeO2particle size of 5.5 nm exhibits a very high CO2conversion rate(116.4×10-5molCO2/(gcat·s)) and CO selectivity（96.1%） at 600℃.Our experimental findings reveal that the small-size CeO2in 0.5Pt5Ce/Al2O3possesses a greater capacity to generate reactive oxygen vacancies,promoting the adsorption and activation of *** addition,the oxygen vacancies are cyclically generated and consumed during the reaction,which contributes to the elevated catalytic performance of the *** work provides a general strategy to construct rich oxygen vacancies on CeO2for designing high-performance catalysts in C1chemistry.

关键词： CO 2 activation Ceria Oxygen vacancies Size-effect Reverse water gas shift reaction Rare earths

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Enantioselective reductive conjugate alkenylation ofα,β-enones with keto alkenyl acetates by nickel catalysis

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Science China chemistry 2025年第1期68卷 157-162页

作者： Rong-De He Yun-Lei Luo Qiu-Quan Pan Qi-Wei Yao Xing-Zhong Shu State Key laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China

Reactions involving alkenyl acetates offer cost-effective and environmentally friendly routes for alkene synthesis,yet their asymmetric variant remains ***,asymmetric conjugate alkenylation predominantly centered on nucleophilic addition using alkenyl–*** manuscript presents an asymmetric reductive conjugate alkenylation reaction involving alkenyl *** method facilitates the enantioselective addition of keto alkenyl groups toα,β-enones,resulting in the formation of unsaturated diketones—a class of useful structural motifs that are challenging to access *** use of electron-rich Pyroxy ligand is essential for achieving both high reaction efficiency and enantioselectivity.

关键词： nickel alkenylation asymmetric cross-coupling alkenes

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Critical new insights into the interactions of hexafluoropropylene oxide-dimer acid(GenX or HFPO-DA)with albumin at molecular and cellular levels

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Journal of Environmental Sciences 2025年第3期149卷 88-98页

作者： Shi-Ya Peng Ya-Di Yang Rong Tian Naihao Lu Jiangxi Key laboratory of Green chemistry College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022China

A key characteristic to be elucidated,to address the harmful health risks of environmental perfluorinated alkyl substances(PFAS),is their binding modes to serum albumin,the most abundant protein in *** oxide-dimer acid(GenX or HFPO-DA)is a new industrial replacement for the widespread linear long-chain ***,the detailed interaction of new-generation short-chain PFAS with albumin is still ***,the binding characteristics of bovine serum albumin(BSA)to GenX were explored at the molecular and cellular *** found that this branched short-chain GenX could bind to BSA with affinity lower than that of legacy linear long-chain perfluorooctanoic acid(PFOA).Site marker competitive study and molecular docking simulation revealed that GenX interacted with subdomain IIIA to form BSA-GenX *** with its weaker affinity to albumin protein,the cytotoxicity of branched short-chain GenX was less susceptible to BSA binding compared with that of the linear long-chain *** contrast to the significant effects of strong BSA-PFOA interaction,the weak affinity of BSA-GenX binding did not influence the structure of protein and the cytotoxicity of *** detailed characterization and direct comparisons of serum albumin interaction with new generation short-chain GenX will provide a better understanding for the toxicological properties of this new alternative.

关键词： GenX Protein binding Albumin Cytotoxicity Risk assessment

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Tandem asymmetric dearomatized functionalization reaction of phenols with Evans-ynamides enabled by divergent electrophiles

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Science China chemistry 2025年第2期68卷 649-660页

作者： Ying-Qi Zhang Gan-Lu Qian Yun Liu Jia-Hui Li Xin Hong Zhou Xu Bo Zhou Long-Wu Ye State Key laboratory of Physical chemistry of Solid Surfaces Key Laboratory of Chemical Biology of Fujian Provinceand College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Center of chemistry for Frontier Technologies Department of ChemistryState Key Laboratory of Clean Energy UtilizationZhejiang UniversityHangzhou 310027China Jiangsu Key laboratory of New Drug Research and Clinical Pharmacy School of PharmacyXuzhou Medical UniversityXuzhou 221004China State Key laboratory of Elemento-Organic chemistry Nankai UniversityTianjin 300071China State Key laboratory of Organometallic chemistry Chinese Academy of SciencesShanghai 200032China

Herein,we disclose a highly regio-/chemoselective tandem asymmetric dearomatized halofunctionalization reaction of phenoltethered ynamides with diverse electrophilic halogenation sources in a catalyst-free manner for the practical and rapid assembly of a series of halogenated spirocyclic ***,the related dearomatized selenation and protonation are also achieved,affording the corresponding selenated and protonated spirocycles in high ***,the enantioselectivities of these products can be perfectly induced by Evans auxiliaries(99%ees).Significantly,this protocol not only represents the first tandem asymmetric halofunctionalization reaction of phenol derivatives,but also constitutes the first asymmetric halogenation/selenation of *** calculations indicate a remote induction model of Evans chiral auxiliary-attached keteniminium.

关键词： alkynes cyclization dearomatization Evans chiral auxiliary spirocycles

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The transformation of nor-seco-cucurbit[10]uril to cucurbit[5]uril and cucurbit[8]uril controlled by its own concentration

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Chinese Chemical Letters 2025年第2期36卷 373-377页

作者： Shaojie Deng Peihua Ma Qinghong Bai Xin Xiao Key laboratory of Macrocyclic and Supramolecular chemistry of Guizhou Province Department of Chemistry Guizhou University

Nor-seco-cucurbit[10]uril(ns-CB[10]) is a kinetic product with unique structure. The single bridged methylene in its structure makes the molecular cavity of ns-CB[10] more deformable when compared to ordinary cucurbit[n]uril, reducing its structural stability. Repeated experiments showed that ns-CB[10] gradually cracks in an acidic solution and changes the specificity of cucurbit[5]uril(CB[5]) and cucurbit[8]uril(CB[8]) under more robust acidic solutions and when heated. A series of experiments were designed to study the transformation behavior of ns-CB[10]. It was found that the concentration of ns-CB[10] was correlated with the content distribution of CB[5] and CB[8]. This study explores the influencing factors and mechanisms of the transformation of ns-CB[10] to CB[5] and CB[8]. The results are of great significance for the application of ns-CB[10], understanding the formation mechanism of cucurbit[n]urils. Furthermore,it provides a new pathway for synthesizing new cucurbit[n]urils.

关键词： Concentration control Cracking Mechanism Nor-seco-cucurbituril Transformation

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Construction of N-doped copper metal-organic frameworks for promoting photocatalytic carbon dioxide reduction to ethylene

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Science China chemistry 2025年第2期68卷 601-609页

作者： Fan Guo Zong-Zheng He Peng Wang Xiao-Yu Zhang Hongjian Yu Qin-Chao Wang Wei-Yin Sun School of chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China Coordination chemistry Institute State Key Laboratory of Coordination ChemistrySchool of Chemistry and Chemical EngineeringNanjing National Laboratory of MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China

Engineering nonmetallic atom-doped metal-organic framework(MOF)catalyst to promote C−C coupling and realize conversion of CO_(2) into C_(2 )multi-carbon hydrocarbon products is still ***,with 2-methylimidazole as a dopant of N element,an N-doped NH_(2)-CuBDC catalyst was obtained via a facile and simple stirring *** illumination,compared with catalytic CO_(2) reduction to C1 product of CO by original MOF,N-doped NH_(2)-CuBDC can motivate generation of C_(2)H_(4),which is difficult to achieve in photocatalytic system by MOF-based *** transfer rates of photo-generated charges have been expedited due to the high electron density around Cu catalytic sites after *** importantly,C–C coupling intermediate CO–CHO*was identified by in situ Fourier transform infrared spectroscopy during the catalytic CO_(2) reduction reaction process,which further indicates the presence of Cu–N sites in the NH_(2)-CuBDC can facilitate the formation of C2H_(4) *** work uncovers a new paradigm to design photocatalysts for enhancing the reduction of CO_(2) to C_(2) products.

关键词： metal-organic frameworks C-C coupling doping photocatalytic CO_(2) reduction Cu-based catalysts

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Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China chemistry 2025年第1期68卷 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 MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China State Key laboratory of Natural Medicines China Pharmaceutical UniversityNanjing 211198China

Selective modification of peptides has always been a challenging *** selective alkylation of peptides can alter the biological activity and physical properties of molecules,and it has gained significant research *** 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 theα-C(sp^(3))–H in glycine residue of *** 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 *** addition,mechanistic studies and density functional theory(DFT)calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET)mechanism.

关键词： gold catalysis peptide alkylation C-C coupling radical

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Pyrimidine derivative as eco-friendly corrosion inhibitor for nickel−aluminum bronze in seawater

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Transactions of Nonferrous Metals Society of China 2025年第1期35卷 207-224页

作者： Jin-yu PI Qi WANG Chao-yang FU Key laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Materials Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

A pyrimidine derivative,6-phenyl-2-thiouracil(PT),was synthesized for developing a corrosion inhibitor(CI)applied in the protection of the nickel−aluminum bronze(NAB)in *** anti-corrosion effect of PT was evaluated by the mass loss experiment,electrochemical tests and surface *** results show that PT exhibits excellent inhibition performance and the maximum inhibition efficiency of PT reaches 99.6%.The interaction mechanism was investigated through X-ray photoelectron spectroscopy(XPS)and molecule dynamics simulation based on the density functional theory(DFT).The S-Cu,Al-N and Cu-N bonds are formed by the chemical interactions,leading to the adsorption of PT on the NAB *** diffusion of corrosive species is hindered considerably by the protective PT film with composition of(PT-Cu)_(ads)and(PT-Al)_(ads)on the PT/NAB *** degree of suppression is increased with the addition of more PT molecules.

关键词： nickel−aluminum bronze corrosion inhibitor diffusion coefficient adsorption seawater

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