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Durable poly(binaphthyl-co-p-terphenyl piperidinium)-based anion exchange membranes with dual side chains

Journal of Energy chemistry 2024年第2期89卷 324-335,I0008页

作者： Weiting Gao Xuelang Gao Qiugen Zhang Aimei Zhu Qinglin Liu department of Chemical&Biochemical Engineering Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryThe College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina department of chemistry Pohang University of Science and Technology(POSTECH)Pohang 790-784South Korea

Building well-developed ion-conductive highways is highly desirable for anion exchange membranes(AEMs).Grafting side chain is a highly effective approach for constructing a well-defined phaseseparated morphological structure and forming unblocked ion pathways in AEMs for fast ion *** of side chains can further enhance phase separation due to the superhydrophobic nature of fluorine ***,their electronic effect on the alkaline stability of side chains and membranes is rarely ***,fluorine-containing and fluorine-free side chains are introduced into the polyaromatic backbone in proper configuration to investigate the impact of the fluorine terminal group on the stability of the side chains and membrane *** poly(binaphthyl-co-p-terphenyl piperidinium)AEM(QBNp TP)has the highest molecular weight and most dimensional stability due to its favorable backbone arrangement among ortho-and meta-terphenyl based ***,by introducing both a fluorinated piperidinium side chain and a hexane chain into the p-terphenyl-based backbone,the prepared AEM(QBNp TP-QFC)presents an enhanced conductivity(150.6 m S cm^(-1))and a constrained swelling at 80℃.The electronic effect of fluorinated side chains is contemplated by experiments and *** results demonstrate that the presence of strong electro-withdrawing fluorine groups weakens the electronic cloud of adjacent C atoms,increasing OH^(-)attack on the C atom and improving the stability of piperidinium *** QBNp TP-QFC possesses a robust alkaline stability at 80℃(95.3%conductivity retention after testing in 2 M Na OH for 2160 h).An excellent peak power density of 1.44 W cm^(-2)and a remarkable durability at 80℃(4.5%voltage loss after 100 h)can be observed.

关键词： Anion exchange membranes Backbone structure Fluorinated side chain Alkaline stability

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Making topological protein links using enzymatic reactions

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National Science Review 2024年第03期11卷 50-51页

作者： Roger Castells-Graells Todd O.Yeates department of chemistry and Biochemistry University of California UCLA-DOE Institute for Genomics and Proteomics

Proteins are exceedingly complex molecules though, at their heart, they are essentially linear polymers. Pull at their ends and one obtains an extended backbone. While that is true in most cases, some natural proteins... 详细信息

关键词： DESIGN

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Polypyride intercalation boosting the kinetics and stability of V3O7·H2O cathodes for aqueous zinc-ion batteries

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Journal of Energy chemistry 2024年第10期97卷 361-370页

作者： Qingqing He Jie Bai Mengda Xue Yanxin Liao Huayu Wang Mujun Long Lingyun Chen department of Applied chemistry School of Chemistry and Chemical Engineering Chongqing University Laboratory of Materials and Metallurgy College of Materials Science and Engineering Chongqing University

V3O7·H2O（VO） is a high capacity cathode material in the field of aqueous zinc ion batteries（AZIBs）,but it is limited by slow ion migration and low electrical *** this paper,polypyridine（PPyd） intercalated VO with nanoribbon structure was prepared by a simple in-situ pre-intercalation,which is noted *** total density of states（TDOS） shows that after the pre-intercalation of PPyd,an intermediate energy level appears between the valence band and conduction band,which provides a step that can effectively reduce the band gap and enhance the electron ***,the density functional theory（DFT） results found that Zn2+is more easily de-intercalated from the V-O skeleton,which proves that the embeddedness of PPyd improves the diffusion kinetics of Zn2+.Electrochemical studies have shown that VO-PPyd cathode materials exhibit excellent rate performance(high specific capacity of 465 and 192 mA h g-1at 0.2 and 10 A g-1,respectively) and long-term cycling performance（92.7%capacity retention rate after 5300 cycles）,due to their advantages in structure and *** importantly,the energy density of VO-PPyd//Zn at 581 and 5806 W kg-1is 375 and 247 W h kg-1,***-PPyd exhibits excellent electrochemical properties compared to previously reported vanadium based cathodes,which makes it highly competitive in the field of high-performance cathode materials of AZIBs.

关键词： Aqueous zinc ion batteries DFT calculation Electrical conductivity Ion migration Polypyridine V3O7·H2O

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Amphiphilic amino-acid derivatives promote gram-scale single-crystal COFs synthesis

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Science China chemistry 2024年第2期67卷 415-416页

作者： Yijia Yuan Kian Ping Loh department of chemistry National University of SingaporeSingapore117543Singapore

Covalent organic frameworks(COFs) are crystalline organic compounds synthesized from covalently linked building blocks that extend in space to form a framework structure with periodic pores. The covalent linkages used... 详细信息

关键词： synthesis correction reversible

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Molecular solid solution of lanthanide-titanium-oxo clusters with enhanced photocatalytic hydrogen evolution

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Science China chemistry 2024年第2期67卷 529-535页

作者： Rong Chen Chao-Long Chen Hui Zhang Zi-Han Wang Fu-Li Sun Ming-Hao Du Gui-Lin Zhuang Cheng Wang La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Centre of chemistry for Energy Materials State Key Laboratory of Physical chemistry of Solid Surfaces and department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China College of Chemical Engineering Zhejiang University of TechnologyHangzhou310032China

Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely ***,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium *** light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_*** time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_*** studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.

关键词： molecular solid solution lanthanide-titanium-oxo clusters photocatalytic hydrogen evolution

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Effects of length alteration of OPE-containing mono- and dinuclear alkynylplatinum(II) terpyridine complexes on photophysical, structural and morphological properties

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Nano Research 2024年第10期17卷 8893-8903页

作者： Jason Koon-Lam Poon Sammual Yu-Lut Leung Eric Ka-Ho Wong Vivian Wing-Wah Yam Institute of Molecular Functional Materials State Key Laboratory of Synthetic Chemistry and Department of ChemistryThe University of Hong KongHong Kong 999077China

A series of mononuclear complexes and unsymmetric dinuclear alkynylplatinum(II)terpyridine complexes with oligo(paraphenylene ethynylene)(OPE)-derived backbone with a variation of the lengths of alkoxy chains and OPE backbones was *** morphological properties,packing lattice and gelation behaviors of the mononuclear complexes were systematically studied,and the thermodynamic parameters and packing lattices of the dinuclear complexes were also investigated,providing further insights into the roles of the non-covalent interactions and their delicate balance in constructing sophisticated supramolecular *** and nanotube formation have been observed upon a delicate control of the intermolecular interactions by altering the lengths and structural dimensions of the complexes.

关键词： supramolecular chemistry self-assembled nanostructures platinum(II)complexes metallogel

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How interfacial electron-donating defects influence the structure and charge of gold nanoparticles on TiO_(2)support

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Nano Research 2024年第7期17卷 5965-5974页

作者： Guang-Jie Xia Yu Fu Wei Cao Jun Li Yang-Gang Wang department of chemistry and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055China School of Physical Sciences Great Bay UniversityDongguan 523000China department of chemistry Tsinghua UniversityBeijing 100084China

The reduction degree of TiO_(2)support is critical to the performances of metal *** many previous theoretical calculations,only the bridge oxygen vacancy(Ov)was considered as the electron-donating defect on reduced rutile TiO_(2)(r-TiO_(2−x))***,titanium adatoms(Tiad.),oxidized titanium islands(***),and acid hydroxyls(ObrH)also exist at the metal/support *** conducting density functional theory(DFT)calculations and ab initio molecular dynamics(AIMD)simulations,we compared r-TiO_(2−x)surfaces with Ov,Tiad.,***,and ObrH sites loaded with Au nanoparticles(NPs).The results showed the Au NPs were oxygen-phobic but titanium-philic,resulting in wetting of Ov and *** short contact with *** and *** Bader charges of Au NPs(QM)showed a good linear relationship with the ideal number of donating electrons(Ne)from the defective sites(QM=−KeNe+QM,S),demonstrating the intrinsic electron allocation at the *** Ov,Tiad.,and *** exhibited similar slopes(Ke),relatively steeper than that of *** means in the scope of Au NP charge state,the *** *** have a close electron-donating ability with Ov,but the ObrH donates relatively fewer *** linear relationship can be extended approximately to other *** higher the metal work function,the steeper the Ke for easier electron donation from defective *** stronger the metal oxygen affinity,the more positive the intercept(QM,S).That explains the easy generation of metallic or negative Pt and Au NPs on r-TiO_(2−x),but hard for Cu and Zn in *** provides theoretical guidance for regulating the charge of metal NPs over TiO_(2−x)supports.

关键词： metal-support interaction titanium oxide oxygen vacancy surface hydroxyl titanium adatom

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Enhanced charge separation by incomplete calcination modified co-doped TiO_(2)nanoparticle for isothiazolinone photocatalytic degradation

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Nano Research 2024年第6期17卷 4834-4843页

作者： Zhiren Guo Xiao Zhang Xinyuan Li Chang Cui Zilei Zhang Hansheng Li Dongxiang Zhang Jinying Li Xiyan Xu Jiatao Zhang School of chemistry and Chemical Engineering Beijing Institute of TechnologyBeijing 102488China department of chemistry MSU-BIT UniversityShenzhen 517182Chin

Photocatalytic oxidation techniques are promising for degradation of the highly ecotoxic and refractory isothiazolinone bactericides in relevant industrial ***,low charge separation and directional transport efficiency under solar light radiation restrain their practical ***,we report a nanostructured photocatalyst doped with Gd and B in TiO_(2)with carbon incorporation and defect formation through incomplete *** specific surface area,grain size,and hydrophilicity of TiO_(2)are improved,which is beneficial for the interfacial reaction between the photocatalyst and *** reduction of the bandgap,the broadening of the photo-absorption range,and the retarded electron-hole recombination promote the photocatalytic performance due to the improved oxygen vacancies based on the electron distribution *** difference in partial density of states(ΔPDOS)between the current catalyst and raw TiO_(2)indicates that the co-doping of Gd and B with incomplete calcination changes the electronic hybridization of conduction band and valence band near the Fermi level,and affects the band gap *** improved charge separation and directional transport efficiency and benefited the formation of main active species,including•OH and O_(2)•−,for the pollutant *** rate of photocatalytic removal of benzisothiazolinone(BIT)by the current photocatalyst reaches 1.25 h^(−1),being 4.31 times that of TiO_(2).The current work offers a constructive approach to the design and synthesis of nanostructured photocatalysts for the photocatalytic degradation of refractory organic pollutants.

关键词： TiO_(2)nanoparticle charge separation oxygen vacancies electron distribution modification photocatalytic degradation

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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key Laboratory of Advanced Energy Material chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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The influence of various grease compositions and silver nanoparticle additives on electrically induced rolling-element bearing damage

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Friction 2024年第4期12卷 796-811页

作者： Samuel BOND Robert L.JACKSON German MILLS department of chemistry and Biochemistry Auburn UniversityAuburn 36849-5412USA department of Mechanical Engineering Auburn UniversityAuburn 36849-5412USA

Leakage currents accelerate surface degradation of metal contacts via small scale arcing across lubricating films,but recent observations suggest that metallic nanoparticle additives in lubricants may be useful to improve contact *** findings prompted a study that examined electrically induced surface pitting of steel contacts in the presence of several lubricating greases including some containing nanometer-sized colloidal silver(Ag)*** rolling sphere-on-disk experiments were conducted under electro-tribological loads employing polyurea greases derived from mineral and synthetic base oils with and without *** forces and electrical resistance were monitored continuously during the tests;surface changes were characterized by means of optical spectroscopy,stylus profilometry,and scanning electron microscopy(SEM)including compositional analysis using energy dispersive spectroscopy(EDS).The observations demonstrate that surface pitting induced by arcing occurs mainly at the points were the rolling motion changes direction and that eroded metal is deposited along the wear ***-sized pits are formed which contain carbon and oxygen indicating that arcing causes decomposition of the hydrocarbon *** findings indicate a significant inhibition of pitting is induced by the Ag nanoparticles;some greases containing other additives exhibit a similar,although less pronounced,effect.

关键词： electric motor bearings wheel bearings electric vehicles arcing electrically induced bearing damage pitting leakage current stray current

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