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Encapsulated Fe(IV)Molecular Complex for Photoacoustic Imaging

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CCS chemistry 2024年第5期6卷 1184-1197页

作者： Ye Xu Chao Li Zhong-Yu Yu Jiamin Wang Zhaoyang Liu Chao Jiang Zhen-Feng Chen Xiaoyu Wu Ming-Xing Li Hong Yang Zhao-Xi Wang Jonathan L.Sessler Department of chemistry Center for Supramolecular Chemistry and CatalysisInnovative Drug Research CenterShanghai UniversityShanghai 200444 College of chemistry and Materials Science Shanghai Key Laboratory of Rare Earth Functional MaterialsShanghai Frontiers Science Center of Biomimetic CatalysisShanghai Normal UniversityShanghai 200234 Sijing Community Health Service center of Songjiang District Shanghai 201601 Key Laboratory for chemistry and Molecular Engineering of Medicinal Resources Guangxi Normal UniversityGuilin 541004 Department of chemistry The University of Texas at AustinAustinTexas 78712-1224

stable neutral Fe(IV)complex(Fe-HDCL),readily accessible on the g scale,was found to possess high water solubility and good stability(<5%degradation over 4 h upon photoirradiation).Fe-HDCL is green and absorbs light effectively in the visible region(500–800 nm)with aλmax at 650 nm(ɛ=7830 M^(−1)cm^(−1)).Fe-HDCL also exhibits photothermal(PT)behavior comparable to single-wall carbon nanotubes in the solid *** aqueous solution,high PT conversion(η=72.6%)is achieved,and a strong hyperthermia-based inhibition of cell growth is observed upon subjecting Fe-HDCL to near-infrared 730 nm laser *** biological studies in vitro and in vivo confirmed that Fe-HDCL is biocompatible,clears readily,and allows the visual detection of blood *** subjecting mice to intravenous injection at low doses(e.g.,50μmol·kg^(−1)),Fe-HDCL also permits the photoacoustic(PA)imaging of kidneys and the evaluation of renal fibrosis in mouse *** addition,Fe-HDCL allows PA-based imaging of brain tissues,presumably reflecting its ability to pass through the blood-brain *** thus propose that Fe-HDCL has a role to play as PT agent and as a photodiagnostic.

关键词： stable Fe(IV)complex blood-brain barrier molecular cage photoacoustic imaging renal fibrosis

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

A weakly-solvated ether-based electrolyte for fast-charging graphite anode

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Chinese Chemical Letters 2024年第8期35卷 526-532页

作者： Xiao Zhu Yanbing Mo Jiawei Chen Gaopan Liu Yonggang Wang Xiaoli Dong Department of chemistry and shanghai Key Laboratory of Molecular catalysis and Innovative Materials Institute of New EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan UniversityShanghai 200433China

Weakly-solvated electrolytes(WSEs)utilizing solvents with weak coordination ability offer advantages for low-potential graphite anode owing to their facile desolvation process and anions-derived inorganic-rich solid electrolyte interphase(SEI)***,these electrolytes face challenges in achieving a balance between the weak solvation affinity and high ionic conductivity,as well as between rigid inorganic-rich SEI and flexible SEI for long-term ***,we introduce 1,3-dioxolane(DOL)and lithium bis(trifluoromethanesulfonyl)-imide(LiTFSI)as functional additives into a WSE based on nonpolar cyclic ether(1,4-dioxane).The well-formulated WSE not only preserves the weakly solvated features and anion-dominated solvation sheath,but also utilizes DOL to contribute organic species for stabilizing the SEI *** from these merits,the optimized electrolyte enables graphite anode with excellent fast-charging performance(210 mAh/g at 5 C)and outstanding cycling stability(600 cycles with a capacity retention of 82.0%at room temperature and 400 cycles with a capacity retention of 80.4%at high temper-ature).Furthermore,the fabricated LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||graphite full cells demonstrate stable operation for 140 cycles with high capacity retention of 80.3%.This work highlights the potential of tailoring solvation sheath and interphase properties in WSEs for advanced electrolyte design in graphite-based lithium-ion batteries.

关键词： Weakly-solvated solvent Bisalt ether-based electrolyte Graphite anode NCM||graphite battery Interfacial optimization

Recent advances in the synthesis and application of N-heterocyclic carbene-based molecular cages

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Science China chemistry 2024年第5期67卷 1510-1523页

作者： Qiongjie Chai Lixin Duan Yanzhe Ma Tianheng Hou Tao Tu shanghai Key Laboratory of Molecular catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

N-Heterocyclic carbene(NHC)-based cages have emerged as a prominent and dynamic research area within the research field of chemistry. Leveraging the distinctive electronic and steric properties of NHC ligands, the design, synthesis, and application of these corresponding cages have garnered substantial scholarly interest. In recent years, we have witnessed the successful fabrication of diverse NHC-based cages through a range of synthetic methodologies, which hold significant potential for applications in molecular recognition and catalysis. In this review, we delve into the foundational synthetic strategies that underlie the creation of NHC-based cages, employing approaches encompassing metal–NHC chelation, coordination assembly,and covalent bonding. Additionally, we compile the diverse applications of these cages within catalytic processes and molecular recognition. Lastly, we shed light on the current limitations of synthesis and outline future trends in the development of NHCbased cages.

关键词： N-heterocyclic carbene molecular cages supramolecular chemistry synthetic strategies applications

Highly selective and efficient photocatalytic NO removal:Charge carrier kinetics and interface molecular process

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Nano Research 2024年第3期17卷 1003-1026页

作者： Huan Shang Hongbao Jia Pengpeng Li Hao Li Wenbin Zhang Shuangjun Li Qing Wang Shuning Xiao Ding Wang Guisheng Li Dieqing Zhang School of Materials and chemistry University of Shanghai for Science and TechnologyShanghai 200093China The Education Ministry Key Lab of Resource chemistry Joint International Research Laboratory of Resource Chemistry of Ministry of EducationShanghai Key Laboratory of Rare Earth Functional Materialsand Shanghai Frontiers Science Center of Biomimetic CatalysisShanghai Normal UniversityShanghai 200234China School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China

The widespread nitrogen oxides(NOx,mainly in NO)in the atmosphere have threatened human health and ecological *** dilute NO(ppb)is difficult to efficiently remove via the traditional process due to its characteristics of low concentration,wide range,large total amount,*** can utilize solar energy to purify NO pollutants under mild conditions,but its application is limited due to the low selectivity of nitrate and poor activity of NO *** underlying reason is that the interface mechanism of NO oxidation is not clearly understood,which leads to the inability to accurately regulate the NO oxidation ***,the recent advances in the photocatalytic oxidation of NO are ***,the common strategies to effectively regulate carrier dynamics such as morphology control,facet engineering,defect engineering,plasma coupling,heterojunction and single-atom catalysts are ***,the progress of enhancing the adsorption and activation of reactants such as NO and O_(2) during NO oxidation is described in detail,and the corresponding NO oxidation mechanisms are ***,the challenges and prospects of photocatalytic NO oxidation are presented in term of nanotechnology for air pollution *** review can shed light on the interface mechanism of NO oxidation and provide illuminating information on designing novel catalysts for efficient NOx control.

关键词： nitrogen oxide(NO)oxidation photocatalysis NO/O_(2)activation charge carrier kinetics interfacial mechanism

Revealing the specific role of sulfide and nano-alumina in composite solid-state electrolytes for performance-reinforced ether-nitrile copolymers

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Journal of Energy chemistry 2024年第4期91卷 628-636页

作者： Haoyang Yuan Changhao Tian Mengyuan Song Wenjun Lin Tao Huang Aishui Yu Department of chemistry Collaborative Innovation Center of Chemistry for Energy MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsInstitute of New EnergyFudan UniversityShanghai 200438China Laboratory of Advanced Materials Fudan UniversityShanghai 200438China

Composite solid-state electrolytes represent a critical pathway that balances the interface compatibility and lithium-ion conductivity in all-solid-state *** quest for stable and highly ion-conductive combinations between polymers and fillers is vital,but blind attempts are often made due to a lack of understanding of the mechanisms involved in the interaction between polymers and ***,we employ in-situ polymerization to prepare a polymer based on an ether-nitrile copolymer with high cathode stability as the foundation and discuss the performance enhancement mechanisms of argyrodite and *** 1%content of sulfide interacting with the polymer at the two-phase interface,the local enhancement of lithium-ion migration capability can be achieved,avoiding the reduction in capacity due to the low ion conductivity of the passivation layer during *** capacity retention after 50cycles at 0.5 C increases from 83.5%to 94.4%.Nano-alumina,through anchoring the anions and interface inhibition functions,eventually poses an initial discharge capacity of 136.8 m A h g^(-1)at 0.5 C and extends the cycling time to 1000 h without short-circuiting in lithium metal *** the combined action of dual fillers on the composite solid-state electrolyte,promising insights are provided for future material design.

关键词： Composite solid-state electrolytes Lithium metal anode Dual fillers Interfacial ionic conduction Inert nano-alumina

Nitrite-catalyzed economic and sustainable bromocyclization of tryptamines/tryptophols to access hexahydropyrrolo[2,3-b]indoles/tetrahydrofuroindolines in batch and flow

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Chinese Chemical Letters 2024年第7期35卷 247-252页

作者： Xiao Xiao Biao Chen Jia-Wei Li Jun-Bo Zheng Xu Wang Hang Zhao Fen-Er Chen Institute of Pharmaceutical Science and Technology Collaborative Innovation Center of Yangtze River Delta Region Green PharmaceuticalsZhejiang University of TechnologyHangzhou 310014China College of chemistry and Chemical Engineering Jiangxi Normal UniversityNanchang 330022China Engineering center of catalysis and Synthesis for Chiral Molecules Department of ChemistryFudan UniversityShanghai 200433China shanghai Engineering center of Industrial Asymmetric catalysis for Chiral Drugs Shanghai 200433China

A highly efficient and concise bromocyclization has been successfully achieved,in which tryptamine/tryptophol derivates can be transformed to valuable HPI/TFI scaffolds with economic and green ***,a controllable cascade transformation of bromocyclization and aromatic bromination has also been smoothly achieved to form dibrominated HPIs and *** could be successfully scaled up under both the batch process and a continuous flow *** most remarkable peculiarity of our process over all previous methods is that the generated water is the major ***,successful application of this new protocol has been demonstrated by the pharmaceutical and natural products syntheses.

关键词： Tryptamines and tryptophols Nitrite Economic and sustainable bromocyclization HPI and TFI structures Bath and flow

Binding SnO2 Nanoparticles with MoS2 Nanosheets Toward Highly Reversible and Cycle-Stable Lithium/Sodium Storage

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Energy & Environmental Materials 2024年第4期7卷 135-142页

作者： Deliang Cheng Wenbiao Zhang Yi Tang Qingsheng Gao Renzong Hu Lichun Yang Min Zhu Institute of Advanced Materials Jiangxi Normal University School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials South China University of Technology College of chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications Jinan University Department of chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials Fudan University

SnO2,with its high theoretical capacity,abundant resources,and environmental friendliness,is widely regarded as a potential anode material for lithium-ion batteries （LIBs）.Nevertheless,the coarsening of the Sn nanop... 详细信息

关键词： 1 T-MoS2 heterostructure lithium-ion batteries Sn coarsening SnO2

Disentangling distinct Cu surface sites for electrocatalytic CO_(2)-to-CO and CO-to-C_(2+)conversion

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Science China chemistry 2024年第4期67卷 1047-1048页

作者： Kun Jiang Wen-Bin Cai Interdisciplinary Science Research Centre School of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China shanghai Key Laboratory of Molecular catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Electrochemical CO_(2)reduction reaction(CO_(2)RR)is a promising strategy to curb anthropogenic carbon emissions,for which intermittent renewable electricity could be stored as chemical energy within carbon-based fuel... 详细信息

关键词： carbon Electrochemical surface