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Fluorescent carbon dots synthesized in solid phase and air for application in LEDs

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Nano Research 2024年第9期17卷 8495-8503页

作者： Wei-Jie Zheng Zhao-Nan Sun Yi-Ming Wang Huan-Ming Xiong Department of Chemistry and shanghai key laboratory of molecular catalysis and innovative materials Fudan UniversityShanghai 200438China

Carbon dots(CDs)have been widely adopted as optical materials because of their excellent luminescent ***,most of the reported synthetic methods are conducted in solvents,especially hydrothermal/solvothermal reactions,leading to intractable problems such as toxic and flammable solvents,complex and inseparable by-products,and dangerously high pressures and ***-phase synthesis of CDs in air is an effective solution to overcome the above issues,but solid reactions always result in uncontrolled growth and agglomeration of *** this study,some inorganic salts are selected as catalysts for synthesizing CDs in solid states and air,which also play as dispersants to hinder CDs *** the meantime,some aromatic derivatives containing hydroxyl and amino groups are chosen as carbon sources,ground with the optimized catalyst,and then heated together in *** production yields are affected by the reaction time and reactant ratio,while the graphitization degrees of the CDs are determined by the reaction *** IG/ID value of their Raman spectra increases from 0.59 to 0.85,and the particle size decreases from 2.5 to 1.4 nm when the synthesis temperature is increased from 200 to 280℃.The as-prepared CDs show emission peaks ranging from 366 to 606 nm,with the photoluminescence(PL)quantum yield up to 53%.Their emission color variation mainly results from different carbon sources,which can be ascribed to the differences in the element composition,functional groups,and graphitic nitrogen content of these *** dispersing CDs of different concentrations into polyvinyl alcohol(PVA)and combining them with blue LEDs,cold,standard,and warm white light emitting devices(WLEDs)are prepared,with a color rendering index(CRI)up to *** the as-prepared CDs have antioxidant ability at high temperature,the as-prepared WLEDs have long lifespans,remaining the effective white luminescence after 72 h continuous work.

关键词： carbon dot solid-phase synthesis white LED photoluminescence inorganic salt catalysis

taBOX: A water-soluble tetraanionic rectangular molecular container for conjugated molecules and taste masking for berberine and palmatine

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Chinese Chemical Letters 2024年第5期35卷 175-178页

作者： Qihan Lin Jiabin Xing Yue-Yang Liu Gang Wu Shi-Jia Liu Hui Wang Wei Zhou Zhan-Ting Li Dan-Wei Zhang Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200438China

A water-soluble macrocycle that bears four carboxylate anions has been designed and prepared,which forms a rectangular cavity that can efficiently encapsulate discrete electron-deficient aromatic compounds,including berberine and *** macrocycle is revealed to be highly biocompatible and able to inhibit the bitter taste of the two drugs.

关键词： Macrocycle Multianion molecular container molecular recognition Bitter taste masking

Revisiting the sodium-ion storage capability of hard carbon in carbonate-based electrolytes via a sodium-metal-free protocol

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Science China Chemistry 2024年第7期67卷 2240-2247页

作者： Gaopan Liu Yanbing Mo Jiawei Chen Yu Peng Xiao Zhu Fei Wang Xiaoli Dong Yongyao Xia Department of Chemistry and shanghai key laboratory of molecular catalysis and innovative materials Institute of New EnergyLaboratory of Advanced MaterialsFudan UniversityShanghai 200438China

Common evaluation methodology of sodium(Na)-containing two-electrode or three-electrode configurations overlooks the interference from highly reactive Na metal,leading to the underestimation or inconsistent performance of low-potential hard carbon(HC)***,the trap of Na metal was systematically investigated with or without applied current,uncovering its inadequacy as the reference or counter electrode in different configurations.A Na-metal-free three-electrode protocol is proposed for evaluating the actual Na^(+)-storage capability of the typical low-potential HC *** avoiding Na crosstalk and precisely controlling the working electrode's potential,the actual electrochemical performance of HC in the carbonate esterbased electrolyte can be recognized with high capacity of 222 mAh g^(-1)at 2 C and 113 mAh g^(-1)at 5 C,correcting the misunderstanding of the inferior performance of HC in coin-type half cells(68%and 50%undervaluation at 2 C and 5 C,respectively).The advanced protocol is expected to reduce misunderstandings or underestimation due to evaluation methods and to guide the development of high-performance battery materials.

关键词： highly reactive sodium potential drift carbonate ester sodium-metal-free protocol sodium storage capability

Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of Chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State key laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

Amphipathicity mediated endocytosis of mesoporous silica nanoparticles with tunable frameworks

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Nano Research 2024年第9期17卷 8350-8359页

作者： Runfeng Lin Tiancong Zhao Liang Chen Minchao Liu Hongyue Yu Ruicong Wang Minjia Yuan Xiaomin Li Dongyuan Zhao Department of Chemistry State Key Laboratory of Molecular Engineering of PolymersiChemShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200433China shanghai Qiran Biotechnology Co. Ltd.Shanghai 201702China

Due to the amphiphilic nature of phospholipids in the cell membrane,the amphipathicity of the nanomedicine plays a crucial role in the ***,limited biological characterization methods restrict the study of the state of nanoparticles with different amphiphilicities on cell *** understanding of interaction of amphiphilic particle with cell membrane is still ***,by combining the dissipative particle dynamics(DPD)with the framework construction of mesoporous silica nanoparticles(MSNs),we demonstrate the enhanced endocytosis induced by the *** results confirm that the presence of hydrophobic groups on the surface of nanoparticles can disturb the integrity of 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine(POPC)membrane and induce activation of phospholipids to a higher energy level,thereby facilitating the wrapping of *** validate the simulation findings,uniform MSNs with hydrophilic pure silica framework and two types of amphiphilic MSNs with varying hydrophilic organic groups in the framework are rationally synthesized by using different silane *** obtained three kinds of MSNs show similar diameter(~100 nm)and mesopores(~2 nm),but distinct hydrophobicity/hydrophilicity *** phenyl-bridged MSN with a carbon content of 27.1%exhibits enhanced cellular uptake,consistent with the theoretical simulation *** work sheds light on how the surface amphipathicity influences endocytosis through the interaction with cell membrane.

关键词： mesoporous silica nanoparticles mesoporous organosilica endocytosis cell membrane amphipathicity

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

Solar-assisted selective separation and recovery of precious group metals from deactivated air puriﬁcation catalysts

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Science Bulletin 2024年第15期69卷 2379-2386页

作者： Meijun Wu Yao Chen Zhenpeng Guo Xinru Wang Hanyun Zhang Ting Zhang Shuhui Guan Zhenfeng Bian Ministry of Education key laboratory of Resource Chemistry and shanghai key laboratory of Rare Earth Functional materials Shanghai Normal UniversityShanghai 200234China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200438China shanghai YK Pao School Shanghai 201620China

The mitigation of environmental and energy crises could be advanced by reclaiming platinum group precious metals(PGMs) from decommissioned air purification catalysts. However, the complexity of catalyst composition and the high chemical inertness of PGMs significantly impede this process. Consequently,recovering PGMs from used industrial catalysts is crucial and challenging. This study delves into an environmentally friendly approach to selectively recover PGMs from commercial air purifiers using photocatalytic redox technology. Our investigation focuses on devising a comprehensive strategy for treating three-way catalysts employed in automotive exhaust treatment. By meticulously pretreating and modifying reaction conditions, we achieved noteworthy results, completely dissolving and separating rhodium(Rh), palladium(Pd), and platinum(Pt) within a 12-h time frame. Importantly, the solubility selectivity persists despite the remarkably similar physicochemical properties of Rh, Pd, and Pt. To bolster the environmental sustainability of our method, we harness sunlight as the energy source to activate the photocatalysts, facilitating the complete dissolution of precious metals under natural light irradiation. This ecofriendly recovery approach demonstrated on commercial air purifiers, exhibits promise for broader application to a diverse range of deactivated air purification catalysts, potentially enabling implementation on a large scale.

关键词： Photocatalysis Air purification catalysts Platinum group precious metals Selective recovery

Highly dispersed Ru nanospecies on N-doped carbon/MXene composite for highly efficient alkaline hydrogen evolution

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Chinese Chemical Letters 2024年第4期35卷 153-159页

作者： Minying Wu Xueliang Fan Wenbiao Zhang Bin Chen Tong Ye Qian Zhang Yuanyuan Fang Yajun Wang Yi Tang Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materialsand Laboratory of Advanced MaterialsFudan UniversityShanghai 200438China College of Chemistry&materials Engineering Wenzhou UniversityWenzhou 325027China

Hydrogen has emerged as a promising environmentally friendly energy source. The development of lowcost, highly active, stable, and easily synthesized catalysts for hydrogen evolution reactions(HER) remains a significant challenge. This study explored the synthesis of nitrogen-doped MXene-based composite catalysts for enhanced HER performance. By thermally decomposing RuCl_(3) coordinated with melamine and formaldehyde resin, we successfully introduced nitrogen-doped carbon(N–C) with highly dispersed ruthenium(Ru) onto the MXene surface. The calcination temperature played a crucial role in controlling the size of Ru nanoparticles(Ru NPs) and the proportion of Ru single-atom(Ru SA), thereby facilitating the synergistic enhancement of HER performance by Ru NPs and Ru SA. The resulting catalyst prepared with a calcination temperature of 600℃, Ti_(3)C_(2)T_x-N/C-Ru-600(TNCR-600), exhibited exceptional HER activity(η10= 17 m V) and stability(160 h) under alkaline conditions. This work presented a simple and effective strategy for synthesizing composite catalysts, offering new insights into the design and regulation of high-performance Ru-based catalysts for hydrogen production.

关键词： HER activity Highly dispersed Ru-based catalysts MXene Alkaline condition

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