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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

Brønsted-acid sites induced photocatalytic cracking of low-polarity polyethylene plastics

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Journal of Energy chemistry 2024年第9期96卷 509-515页

作者： Qianyou Wen Quan Zhang Zhengzheng Liu Huining Wang Shuya Hao Fan Zhang Lijuan Zhang Qing Han Gengfeng Zheng laboratory of Advanced materials Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200438China

Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern ***,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards ***,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline *** to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via *** addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of *** a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes.

关键词： Photocatalytic cracking Polyethylene Surface phosphorylation Bronsted-acid site Carbon conversion

Access to High-molecular-Weight Polyethylenes through High Temperature Ethylene Polymerization Catalysed by Ethylene-Bridged ansa-(3-R-Cyclopentadienyl)(Fluorenyl) Zirconocene Complexes

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Chinese Journal of Polymer Science 2024年第1期42卷 42-51,I0007页

作者： Bo Li Haiyan Ma Jiling Huang Shanghai Key laboratory of Functional materials chemistry and laboratory of Organometallic chemistry School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

A series of C1-symmetric ethylene-bridged ansa-(3-R-cyclopentadienyl)(fluorenyl) metallocene complexes(Zr: 1-5;Hf: 6) have been synthesized, characterized and investigated as catalyst precursors for the high temperature ethylene polymerization. Using methylaluminoxane(MAO) as the cocatalyst, zirconium complexes 1-5 bearing a bulky substituent on the 3-position of the cyclopendienyl ring showed high catalytic activities up to 1.48×10^(7) g PE·mol_(Zr)^(-1)·h^(-1) toward the polymerization of ethylene and afforded polyethylenes with high molecular weights(1.49×10^(5)-6.31×10^(5) g/mol), meanwhile exhibting great thermal stability at high temperatures up to 120 ℃ together with a long catalytic life time up to 2 h. By adopting low Al/Zr ratios, such as 125, polyethylenes with ultra high molecular weights up to 2.86×106 g/mol were obtained. It is worthy of noting that zirconium complexes 1-4 bearing a substituent with an aryl pendant showed temperature-dependent activities, which increased rapidly with the increase of polymerization temperature, thus weak interaction of the pendent aryl group with the cationic active center is proposed to account for the very low activities displayed at low temperatures. In contrast to zirconocene complexes 1-5, hafnocene complex 6 only displayed very low catalytic activities toward the polymerization of ethylene and afforded polyethylenes with molecular weights ten times smaller than those obtained by zirconocene complexes 1-5. Zirconocene complexes 1-5 were also able to catalyse the polymerization of propylene at high temperatures, but only afforded waxes with low molecular weights.

关键词： ansa-Metallocene Ethylene Propylene Polymerization High temperature

Strong metal-support interactions between highly dispersed Cu^(+) species and ceria via mix-MOF pyrolysis toward promoted water-gas shift reaction

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Journal of Energy chemistry 2024年第4期91卷 475-483页

作者： Xiao-Chen Sun Xing-Chi Li Ze-Wei Xie Chen-Yue Yuan De-Jiu Wang Qian Zhang Xiao-Yu Guo Hao Dong Hai-Chao Liu Ya-Wen Zhang Beijing National laboratory for molecular Sciences(BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing National laboratory for molecular Sciences(BNLMS) College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing National laboratory for molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Stable and Unstable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported ***,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)*** obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 *** on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction *** Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,*** collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported *** study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.

关键词： Cu-based catalyst MOF derivative Water-gas shift reaction Metal-support interaction

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

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

Preparation of three-dimensional nanoporous copper foil with high specific surface area

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Rare Metals 2024年第7期43卷 3430-3437页

作者： Ning Song Li-Juan Wang Jun-Feng Wang Juan Liao Jian Huang Peng-Kang Du Yun-Zhi Tang Yu-Hui Tan Xiao-Wei Fan Jiangxi Provincial Key laboratory of Functional molecular materials chemistry School of Chemistry and Chemical EngineeringJiangxi University of Science and Technology

The porous copper foil material has the advantages of ultralight and ultra-thin,and can prevent dangers such as thermal runaway and battery fire,which could be regarded as a prospective material for lithium battery **... 详细信息

关键词： Pore structure

Thiazoloisoindigo-based Polymer Semiconductors: Synthesis,Structure-Property Relationship, Charge Carrier Polarity, and Field-Effect Transistor Performance

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Chinese Journal of Polymer Science 2024年第1期42卷 24-31,I0006页

作者： Bo-Wen Li Miao Xiong Mei-Hua Liu Zhi-Gao Li Long Sang Zi-Han Xiong Biao Xiao Jian Pei Xiao-Bo Wan Key laboratory of Optoelectronic Chemical materials and Devices Ministry of EducationSchoolofOptoelectronic Materials&TechnologyJianghan UniversityWuhan430056China Bejing National laboratoryfor molecular Sciences the Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Developing new polymeric semiconductors with excellent device performance is essential for organic electronics. Herein, we synthesized two new thiazoloisoindigo(Tz II)-based polymers, namely, P(Tz II-d Th-d Th) and P(Tz II-d Th-d Tz), by copolymerizing thiophene-flanked Tz II with bithiophene and bithiazole, respectively. Owing to the more electron-deficient nature of bithiazole than bithiophene, P(Tz II-d Th-d Tz)possesses deeper LUMO/HOMO levels of-3.45/-5.47 e V than P(Tz II-d Th-d Th)(-3.34/-5.32 e V). The organic field-effect transistor(OFET) devices based on P(Tz II-d Th-d Th) exhibited p-type behaviors with an average hole mobility value as high as 1.43 cm^(2)·V^(-1)·s^(-1), while P(Tz II-d Th-d Tz)showed typical ambipolar characteristics with average hole and electron mobilities of 0.38 and 0.56 cm^(2)·V^(-1)·s^(-1). In addition, we compared the performances of both polymers with other Tz II-based polymers reported in our previous work, and showed that the charge carrier polarity can be manipulated by adjusting the number of the thiophene units between the acceptor unit. As the increase of the number of thiophene rings,charge carrier polarity shifts from electron-dominated ambipolar transport to hole-dominated ambipolar transport and then to unipolar hole transport in OFETs, which provides an effective molecular design strategy for further optimization of polymer OFET performance.

关键词： Field-effect transistor Charge carrier polarity Thiazoloisoindigo

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

Efficient wide-bandgap perovskite solar cells with open-circuit voltage deficit below 0.4 V via hole-selective interface engineering

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Science China chemistry 2024年第6期67卷 2102-2110页

作者： Xiaoyu Ji Shuo Zhang Furong Yu Huidong Zhang Liqing Zhan Yue Hu Wei-Hong Zhu Yongzhen Wu Key laboratory for Advanced materials and Joint International Research laboratory of Precision chemistry and molecular Engineering Shanghai Key Laboratory of Functional Materials ChemistryFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China School of chemistry University of EdinburghKing’s BuildingsEdinburghEH93FJUK

Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low ***,the open-circuit voltage(V_(OC))of WBG-PSCs is still unsatisfactory as the V_(OC)-deficit is generally larger than 0.45 ***,we report a buried interface engineering strategy that substantially improves the V_(OC)of WBG-PSCs by inserting amphiphilic molecular hole-selective materials featuring with a cyanovinyl phosphonic acid(CPA)anchoring group between the perovskite and *** assembly and redistribution of CPA-based amphiphilic molecules at the perovskite-substrate buried interface not only promotes the growth of a low-defect crystalline perovskite thin film,but also suppresses the photo-induced halide phase *** energy level alignment between wide-bandgap perovskite and the hole-selective layer is further improved by modulating the substituents on the triphenylamine donor moiety(methoxyls for MPA-CPA,methyls for Me PA-CPA,and bare TPA-CPA).Using a 1.68 e V bandgap perovskite,the Me PA-CPA-based devices achieved an unprecedentedly high V_(OC)of 1.29 V and PCE of 22.3%under standard AM 1.5 *** V_(OC)-deficit(<0.40 V)is the lowest value reported for *** work not only provides an effective approach to decreasing the V_(OC)-deficit of WBG-PSCs,but also confirms the importance of energy level alignment at the charge-selective layers in PSCs.

关键词： cyanovinyl phosphonic acid energy level alignment hole-selective material open-circuit voltage wide-bandgap perovskite