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Dual-single-atoms of Pt-Co boost sulfur redox kinetics for ultrafast Li-S batteries

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Carbon Energy 2024年第3期6卷 53-63页

作者： Hanyan Wu Xuejie Gao Xinyang Chen Weihan Li Junjie Li Lei Zhang Yang Zhao Ming Jiang Runcang Sun Xueliang Sun Center for Lignocellulosic chemistry and Biomaterials College of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalianChina department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada Institute of physical Science and Information Technology Anhui UniversityHefeiChina

Applications of lithium-sulfur(Li-S)batteries are still limited by the sluggish conversion kinetics from polysulfide to Li_(2)*** various single-atom catalysts are available for improving the conversion kinetics,the sulfur redox kinetics for Li-S batteries is still not ***,in this work,a catalyst with dual-single-atom Pt-Co embedded in N-doped carbon nanotubes(Pt&Co@NCNT)was proposed by the atomic layer deposition method to suppress the shuttle effect and synergistically improve the interconversion kinetics from polysulfides to Li_(2)*** X-ray absorption near edge curves indicated the reversible conversion of Li_(2)Sx on the S/Pt&Co@NCNT ***,density functional theory demonstrated that the Pt&Co@NCNT promoted the free energy of the phase transition of sulfur species and reduced the oxidative decomposition energy of Li_(2)*** a result,the batteries assembled with S/Pt&Co@NCNT electrodes exhibited a high capacity retention of 80%at 100 cycles at a current density of 1.3 mA cm^(−2)(S loading:2.5 mg cm^(−2)).More importantly,an excellent rate performance was achieved with a high capacity of 822.1 mAh g^(−1) at a high current density of 12.7 mA cm^(−2).This work opens a new direction to boost the sulfur redox kinetics for ultrafast Li-S batteries.

关键词： DFT calculation dual-single-atoms of Pt-Co fast Li-sulfur batteries sulfur redox kinetics XANES analysis

Bright dual-color electrochemiluminescence of a structurally determined Pt1Ag18 nanocluster

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Aggregate 2024年第1期5卷 345-352页

作者： Bing Yin Lirong Jiang Xiaojian Wang Ying Liu Kaiyang Kuang Mengmeng Jing Chunmin Fang Chuanjun Zhou Shuang Chen Manzhou Zhu Institutes of physical Science and Information Technology and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationDepartment of Chemistry and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefeiChina

Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1Ag18 nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic ***^(1)Ag_(18)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,*** the presence of tripropylamine(TPrA)as a coreactant,solid Pt1Ag18 shows unprecedented ECL efficiency,which is more than nine times higher than that of 1 mM Ru(bpy)32+with the same TPrA ***-resolved ECL spectra reveal two ECL emission bands in the presence of *** ECL emission centered at 650 nm is assigned to the solid Pt_(1)Ag_(18)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid *** ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon *** electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 180 in comparison to that without *** on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1Ag18 and CDs are *** findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.

关键词： AIECLE AIEE electrochemiluminescence nanocluster photoluminescence structure

Evolution of Monkeypox C9L RNA G-Quadruplex Elevates the Translation of Its Only Kelch-like Protein by Accelerating G-Quadruplex Unfolding Kinetics

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CCS chemistry 2024年第4期6卷 953-963页

作者： Yicong Dai Xucong Teng Difei Hu Qiushuang Zhang Jinghong Li department of chemistry Center for Bioanalytical ChemistryKey Laboratory of Bioorganic Phosphorus Chemistry and Chemical BiologyTsinghua UniversityBeijing 100084 New Cornerstone Science Laboratory Shenzhen 518054 Beijing Life Science Academy Beijing 102209 Center for Bioanalytical chemistry Hefei National Laboratory of Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026

Genomic surveillance of monkeypox virus(MPXV)is essential to explore the reason of its unusual *** phylogenomic analysis of the MPXV genome mainly focuses on the effect of amino acid ***,we explore the evolutionary variation of RNA G-quadruplex(RG4)of MPXV and find that the genome evolution of MPXV can also produce new effects through changes in the RG4 *** RG4 is located in MPXV’s only Kelch-like C9L gene,which encodes for an antagonist of the innate immune *** evolution of this virus increases the unfolding kinetic constant of C9L RG4 and promotes the C9 protein level in living ***,all reported MPXV genomes in 2022 carry the C9L-RG4-5 pattern with the highest unfolding kinetic ***,the RG4 ligand,RGB-1,can impede the unfolding of C9L-RG4-5 and thereby reduce the C9 protein *** findings carve out a new path to comprehensively understanding MPXV virology.

关键词： G-quadruplex RNA secondary structure unfolding kinetics monkeypox virus genomic evolution immune evasion

Development of biomedical hydrogels for rheumatoid arthritis treatment

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Asian Journal of Pharmaceutical Sciences 2024年第1期19卷 35-48页

作者： Mirza Muhammad Faran Ashraf Baig Lee KiWong Abdul Wasy Zia Hongkai Wu department of chemistry Hong Kong University of Science and TechnologyHong Kong 999077China Institute of Mechanical Process and Energy Engineering(IMPEE)School of Engineering and Physical SciencesHeriot-Watt UniversityEdinburghUnited Kingdom

Rheumatoid Arthritis(RA)is an autoimmune disorder that hinders the normal functioning of bones and joints and reduces the quality of human *** year,millions of people are diagnosed with RA worldwide,particularly among elderly individuals and ***,there is a global need to develop new biomaterials,medicines and therapeutic methods for treating *** will improve the Healthcare Access and Quality Index and also relieve administrative and financial burdens on healthcare service providers at a global *** are soft and cross-linked polymeric materials that can store a chunk of fluids,drugs and biomolecules for hydration and therapeutic *** are biocompatible and exhibit excellent mechanical properties,such as providing elastic cushions to articulating joints by mimicking the natural synovial ***,hydrogels create a natural biological environment within the synovial cavity to reduce autoimmune reactions and *** also lubricate the articulating joint surfaces to prevent degradation of synovial surfaces of bones and cartilage,thus exhibiting high potential for treating *** work reviews the progress in injectable and implantable hydrogels,synthesis methods,types of drugs,advantages and ***,it discusses the role of hydrogels in targeted drug delivery,mechanistic behaviour and tribological performance for RA treatment.

关键词： Rheumatoid arthritis Orthopeadic joints Hydrogel Therapeutics Mechanical properties Medicine

Relationship between physical activity and specific working memory indicators of depressive symptoms in university students

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World Journal of Psychiatry 2024年第1期14卷 148-158页

作者： Qun Zhao Xing Wang Shu-Fan Li Peng Wang Xiang Wang Xin Xin Suo-Wang Yin Zhao-Song Yin Li-Juan Mao School of physical Education Shanghai University of SportShanghai 200438China department of physical Education Donghua UniversityShanghai 201620China

BACKGROUND The detection rate of depression among university students has been increasing in recent years,becoming one of the main psychological diseases that endangers their physical and mental *** to statistics,self-harm and suicide,for which there is no effective intervention,are the second leading causes of *** To explore the relationship between different elements and levels of physical activity and college students’depression-symptom-specific working memory *** Of 143 college students were analyzed using the Beck Depression Self-Rating Scale,the physical Activity Rating Scale,and the Working Memory *** There was a significant difference between college students with depressive symptoms and healthy college students in completing verbal and spatial working memory(SWM)tasks correctly(all Pphysical Activity Scale-3 scores were significantly and positively correlated with the correct rate of the verbal working memory task(r=0.166)and the correct rate of the SWM task(r=0.210)(all P0.05).CONCLUSION An increase in physical exercise among college students,particularly medium-and high-intensity exercise and exercise of 30 min or more,can improve the correct rate of completing working memory tasks.

关键词： physical activity Depression symptoms University students Working memory

Simple chemical synthesis and isotropic negative thermal expansion in MHfF_(6)(M=Ca,Mn,Fe,and Co)

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Nano Research 2024年第3期17卷 2195-2203页

作者： Yongqiang Qiao Sen Zhang Peixian Zhang Juan Guo Andrea Sanson Xi Zhen Kaiyue Zhao Qilong Gao Jun Chen Key Laboratory of Materials Physics of Ministry of Education and School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450052China department of Physics and Astronomy University of PadovaPadova I-35131Italy Beijing Advanced Innovation Center for Materials Genome Engineering Department of Physical ChemistryUniversity of Science and Technology BeijingBeijing 100083China

The rapid progress of modern technologies has accelerated the prominence of thermal expansion mismatch between materials,and tunable thermal expansion materials will be a powerful safeguard against this ***,isotropic MHfF_(6)(M=Ca,Mn,Fe,and Co)compounds with tunable thermal expansion have been produced via a low-cost synthetic method and *** utilizing temperature dependent X-ray diffraction(XRD)and Raman spectroscopy,combined with first principles calculations,it was revealed that the transverse thermal vibrations of the F atoms are dominated by low-frequency phonons with negative Grüneisen parameters and are therefore the origin of the negative thermal expansion(NTE).Very interestingly,with the increase of the M atomic number,the metal…F atomic linkages become stiffer,reducing the number of vibrational modes with negative Grüneisen parameters,so that the strong NTE can be gradually adjusted to moderate NTE and to near zero thermal *** present study achieves the tunable thermal expansion in a new compound family and shed light on the internal mechanism from the perspective of lattice vibrational dynamics.

关键词： negative thermal expansion fluorides chemical synthesis nanosheet structure first principles calculations

Photoinduced Radical-Ionic Transfer of Various Chlorofluorocarbons to Alkenes from Oxime-Based Surrogates

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CCS chemistry 2024年第5期6卷 1222-1230页

作者： Jinghui Zhang Muliang Zhang Martin Oestreich Institut für Chemie Technische Universität Berlin10623 Berlin Hefei National Laboratory for physical Sciences at the Microscale and department of chemistry University of Science and Technology of ChinaHefei 230026

Functional-group-transfer strategies that avoid the use of unsustainable chemicals are attractive for the development of green ***(CFCs)not only contribute to the depletion of the stratospheric ozone layer,but their gaseous nature also poses a serious threat in scientific ***,the design of effective and sustainable alternatives to CFCs is highly ***,a practical CFC transfer platform for the addition of both a fluoroalkyl group and a chlorine substituent across alkenes by a photomediated redox-neutral manifold using bench-stable and easy-to-handle oxime-based surrogates is *** distinct reactivity of these tunable reagents allows for their single-electron reduction to trigger fragmentation driven by benzonitrile formation and loss of carbon *** other fragments released in that step,namely an electrophilic fluoroalkyl radical and a nucleophilic chloride anion,are subsequently transferred onto alkenes by a radical-ionic mechanism to deliver the desired chlorofluorocarbon products.

关键词： alkenes chlorofluorocarbons functionalgroup transfer radical-ionic crossover photoredox catalysis

Low cost and low density chloride solid electrolyte for all solid state cathode with high active material ratio

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Nano Research 2024年第10期17卷 8826-8833页

作者： Hao-Yuan Tan Mei-Yu Zhou Zhongyuan Huang Jin-Da Luo Jing-Tian Yang Jian-Ping Wang Ye-Chao Wu Xiao-Bin Cheng Zi-Wei Wang Xu-Dong Hao Linjun Wang Ke Gong Yi-Chen Yin Yinguo Xiao Hong-Bin Yao Hefei National Research Center for physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China department of Applied chemistry University of Science and Technology of ChinaHefei 230026China School of Advanced Materials Peking University Shenzhen Graduate SchoolShenzhen 518055China

Chloride solid electrolytes(SEs)have attracted widespread attention due to their high room-temperature ionic conductivity and excellent cathode ***,the conventionally selected central metal elements(e.g.,In,Y and Ta)are usually rare and heavy,inevitably causing the high cost and high density of the obtained chloride ***,by choosing abundant and light Mg and Al as central metal elements,we develop a cheap and low density Li_(1.2)Mg_(0.95)Al_(0.3)Cl_(4)SE for high active material ratio in all solid state *** replacement of Mg^(2+)by Al^(3+)in the framework yields vacancies and lowers the non-lithium metal ions occupancy at Mg/Li co-occupied 16d site,effectively relieving the blocking effects by Mg^(2+)in the pristine spinel Li_(2-2x)Mg_(1+x)Cl_(4).Thus,a significantly improved room-temperature conductivity of 3.08×10^(-4)S·cm^(-1)is achieved,two orders of magnitude higher than that of Li_(1.2)Mg_(1.4)Cl_(4).More attractively,its low density of only 1.98 g·cm-3 enables low SE mass ratio in cathodes(only 16 wt.%)with still effective electrolyte/cathode contact and lithium-ion conduction *** charged to potential of 4.30 V,the asfabricated Li_(1.2)Mg_(0.95)Al_(0.3)Cl_(4)-based solid lithium battery with uncoated NCM523 cathode can be cycled for over 100 cycles with a capacity retention of 86.68%at room temperature.

关键词： chloride solid electrolytes low cost low density Li+conductivities

Molecular engineering binuclear copper catalysts for selective CO_(2) reduction to C_(2) products

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Journal of Energy chemistry 2024年第6期93卷 166-173,I0005页

作者： Qi Zhao Kai Lei Bao Yu Xia Rachel Crespo-Otero Devis Di Tommaso department of chemistry School of Physical and Chemical SciencesQueen Mary University of LondonLondonE14NSUK Key Laboratory of Material chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureState Key Laboratory of Materials Processing and Die&Mould TechnologySchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074HubeiChina department of chemistry University College LondonLondonWC1H 0AJUK Digital Environment Research Institute Queen Mary University of LondonEmpire HouseLondon E11HHUK

Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal *** investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular *** modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)*** findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R *** rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular *** placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) *** research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products.

关键词： Molecular catalyst design Selective CO_(2)reduction C_(2)products Density functional theory calculations