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Slow magnetic relaxation behaviors and diamagnetic dilution studies of a carboxyl bridged dinuclear dysprosium(Ⅲ) complex

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Journal of Rare Earths 2024年第11期42卷 2088-2096页

作者： Wenting Liu Yibo Qiu Weiqin Xu Manli Cao Xin Deng Weiquan Lin School of chemistry and Materials Science Guangdong University of Education School of chemistry and Chemical Engineering/institute of Clean Energy and Materials Guangzhou University

By using a rigid bulky carboxylic ligand a-cyanocinnamic acid（CCA）,a dinuclear dysprosium（Ⅲ） complex [Dy2（CCA）6（MeOH）4]（1） was *** crystal X-ray crystallography reveals that the two eight-coordinate dysprosium ions are bridged by four deprotonated carboxyl groups,forming a centrosymmetric paddle-wheel-1ike *** magnetic property measurements indicate that complex 1 displays field-induced slow magnetic *** temperature-dependent relaxation times can be fitted using Orbach and Raman processes with parameters of n=2.8（2）,C=27（8） s-1/K~n,τ0=5（2） × 10-10s and Ueff=40（3） *** studies on the diamagnetic YⅢ-diluted analogue[Dy0.206Y1.794（CCA）6（MeOH）4]（2） reveal its slow magnetic relaxation behavior without external dc field and the antiferromagnetic coupling between the DyⅢions in *** on the obtained relaxation times of 2lead to the parameters of n=4.5（3）,C=0.7（2） s-1/K~n,τ0=2.8（2） × 10-9s and Ueff=38（2） *** results suggest that slow magnetic relaxation originates from the single-ion relaxation of DyⅢ***,the diamagnetic dilution can suppress other fast relaxation pathways at low temperature,on account of the elimination of magnetic coupling and dipolar *** initio calculations were then performed on the single DyⅢion species {YDy} and indicate that the first excited Kramers doublets（KDs）lie at ca.76 cm-1,which is slightly higher than the experimental *** intramolecular magnetic interactions were also calculated and indicate a weak ferromagnetic dipole-diploe magnetic interaction and an antiferromagnetic exchange coupling.

关键词： Diamagnetic dilution Dilanthanide complexes Rare earths Single-molecule magnets

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Layered oxide cathodes for sodium-ion batteries:microstructure design,local chemistry and structural unit

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Science China chemistry 2024年第1期67卷 191-213页

作者： Ling-Yi Kong Han-Xiao Liu Yan-Fang Zhu Jia-Yang Li Yu Su Hong-Wei Li Hai-Yan Hu Yi-Feng Liu Ming-Jing Yang Zhuang-Chun Jian Xin-Bei Jia Shu-Lei Chou Yao Xiao institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China

Because of the low price and abundant reserves of sodium compared with lithium,the research of sodium-ion batteries(SIBs)in the field of large-scale energy storage has returned to the research *** oxides distinguish themselves from the mains cathode materials of SIBs owing to their advantages such as high specific capacity,simple synthesis route,and environmental ***,the commercial development of the layered oxides is limited by sluggish kinetics,complex phase transition and poor air *** on the research ideas from macro-to micro-scale,this review systematically summarizes the current optimization strategies of sodium-ion layered oxide cathodes(SLOC)from different dimensions:microstructure design,local chemistry regulation and structural unit *** the dimension of microstructure design,the various structures such as the microspheres,nanoplates,nanowires and exposed active facets are prepared to improve the slow kinetics and electrochemical ***,from the view of local chemistry regulation by chemical element substitution,the intrinsic electron/ion properties of SLOC have been enhanced to strengthen the structural ***,the optimization idea of endeavors to regulate the physical and chemical properties of cathode materials essentially is put forward from the dimension of structural unit *** opinions and strategies proposed in this review will provide some inspirations for the design of new SLOC in the future.

关键词： sodium-ion batteries layered oxide cathodes microstructure design local chemistry structural unit

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Printable oil-NiO_(X)hole transport layer enables efficient n-i-p perovskite solar cells with a high thermal stability

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Science China chemistry 2024年第7期67卷 2335-2340页

作者： Yazhou Xu Zhaoyang Chu Hongyu Wang Zhi Xing Baojin Fan Xiaotian Hu Yiwang Chen College of chemistry and Chemical Engineering/institute of Polymers and Energy chemistry(IPEC)/Film Energy chemistry for Jiangxi Provincial Key Laboratory(FEC) Nanchang UniversityNanchang 330031China Key Lab of Fluorine and Silicon for Energy Materials and chemistry of Ministry of Education Jiangxi Normal University Nanchang 330022China Peking University Yangtze Delta institute of Optoelectronics Nantong 226010China

Currently,highly efficient n-i-p perovskite solar cells rely on an organic interface layer for high efficiency,especially 2,2',7,7'-tetrakis[N,N-bis(4-methoxyphenyl)ami-no]-9,9′-spirobifluorene(spiro-OMeTAD),but the instability of organic materials in the photothermal field compromises device *** this study,we employ the oleic acid(YS)/oleamine(YA)end-sealing method to achieve uniform dispersion of NiO_(X)nanoparticles,effectively mitigating coagulation resulting from high local concentration and secondary motion ***,the conductivity of the hole transport layer and its energy level alignment with perovskite is enhanced by the additional 2,3,5,6-tetrafluoro-7,7',8,8'-tetracyanodimethyl-p-benzoquinone(F4TCNQ),leading to a remarkable improvement of open-circuit voltage and fill factor,thus the high efficiency of 25.17%and 24.36%on 0.1 and 1.01cm2,***,by realizing an all-inorganic interface layer,an initial efficiency exceeding 90%is maintained even after 2,800 h of heating at 85℃.

关键词： oil-NiO_(X) perovskite solar cells printing technology high efficiency thermal stability

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Catechol-Formaldehyde Resin Coated CdS Core-Shell Composite as Robust Photocatalyst for Long-Term Sustainable Artificial Photosynthesis of H_(2)O_(2)

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Chinese Journal of chemistry 2024年第17期42卷 1975-1985页

作者： Yuexin Xiang Zhinan Xia Wanchao Hu Cuiyan Tong Yang Xiao Changli Lu institute of chemistry Northeast Normal UniversityChangchunJilin130024China

Catechol-formaldehyde resin(CFR)is very attractive for H_(2)O_(2) production via the catalytic ***,the H2O2 formation is accompanied by the oxidation of catechol groups to o-benzoquinone groups on CFR,which will cause irreversible damage to CFR and greatly limit its long-term stable catalytic ***,CdS/CFR composite photocatalyst with a core-shell structure was synthesized by hydrothermal *** photogenerated electrons of Cds are used as a powerful driving force for the reversible redox conversion between catechol groups and o-benzoquinone groups on the CFR.

关键词： Hydrogen peroxide Photocatalysis Catechol-formaldehyde resin Cds Core-shell structures Oxygen reduction reaction Charge transfer Heterogeneous catalysis

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Ce-modified USY zeolite catalysts for catalytic oxidation of chlorinated VOCs:Effect of the location of CeO2 and its synergistic effect with USY zeolite

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Journal of Rare Earths 2024年第11期42卷 2068-2077页

作者： Xiaolin Guo Zhiming Li Ang Zhou Yijun Shi Yong Wang Renxian Zhou institute of Catalysis Zhejiang University College of Materials and chemistry China Jiliang University

The catalytic behavior of a catalyst for chlorine-containing volatile organic compounds（CVOCs） oxidation largely depends on the synergistic interaction between the oxidizing and acidic *** the present work,two catalysts with different distributions of CeO2on the inner and outer surfaces of 4.0Ce-USY-ex and 4.0Ce-USY-dp（USY zeolite） were prepared respectively by ion exchange and deposition methods,with a purpose of finding out how the location of the oxidation sites（CeO2） influence its synergistic effect with the acidic sites of *** results show that 4.0Ce-USY-ex is much more active for catalytic degradation of 1,2-dichloroethane（DCE）,while 4.0Ce-USY-dp catalyst exhibit higher catalytic degradation activity for other structured CVOCs(dichloromethane（DCM）,trichloroethylene（TCE）,chlorobenzene（CB）).CeO2in 4.0Ce-USY-ex catalyst mainly disperses in the pore channels of USY zeolite,and there are many strong acid centers on the surface,which is conducive to the dechlorination conversion of ***,CeO2in 4.0Ce-USY-dp catalyst is mainly distributed on the outer surface of USY and has strong oxidation ability,which contributes to the deep oxidation of ***,the presence of a large number of strong acid centers on the catalyst surface of 4.0Ce-USY-ex catalysts leads to severe accumulation of surface carbon species and significantly decreases its stability towards ***,a large number of active oxygen species on the surface of 4.0Ce-USY-dp and CeO2catalysts are beneficial to the deep oxidation of DCE,reducing the formation of surface carbon and thus improving the stability of the ***,the influence of the location of the oxidation sites on its synergistic effect with the acidic sites was established in the present work,which could provide some new ideas for the rational design of CVOCs degradation catalyst with appropriate distribution of active sites.

关键词： CeO2 CVOCs oxidation Location Rare earths Synergistic effect USY

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Electrochemical CO_(2)reduction to C_(2+)products over Cu/Zn intermetallic catalysts synthesized by electrodeposition

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Frontiers in Energy 2024年第1期18卷 80-88页

作者： Ting DENG Shuaiqiang JIA Shitao HAN Jianxin ZHAI Jiapeng JIAO Xiao CHEN Cheng XUE Xueqing XING Wei XIA Haihong WU Mingyuan HE Buxing HAN School of chemistry and Molecular Engineering East China Normal UniversityShanghai 200062China institute of Eco-Chongming Shanghai 202162China institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China institute of chemistry Chinese Academy of SciencesBeijing 100190China

Electrocatalytic CO_(2)reduction(ECR)offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO_(2)as the ***,the lack of cost-effective electrocatalysts with better performances has seriously hindered its ***,a one-step co-electrodeposition method was used to introduce Zn,a metal with weak^(*)CO binding energy,into Cu to form Cu/Zn intermetallic catalysts(Cu/Zn IMCs).It was shown that,using an H-cell,the high Faradaic efficiency of C_(2+)hydrocarbons/alcohols()could be achieved in ECR by adjusting the surface metal components and the applied *** suitable conditions,FEC_(2+)and current density could be as high as 75%and 40 mA/cm^(2),*** with the Cu catalyst,the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area(ECSA),which accelerate the ***,the^(*)CO formed on Zn sites can move to Cu sites due to its weak binding with*CO,and thus enhance the C–C coupling on the Cu surface to form C_(2+)products.

关键词： carbon dioxide electroreduction electrochemistry co-electrodeposition intermetallic catalysts value-added chemicals

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Atomic-level coupled RuO_(2)/BaRuO_(3) heterostructure for efficient alkaline hydrogen evolution reaction

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Journal of Energy chemistry 2024年第1期88卷 356-362,I0009页

作者： Yueying Yan Tian Meng Yuting Chen Yang Yang Dewen Wang Zhicai Xing Xiurong Yang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina

The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of *** this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of *** RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water *** research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.

关键词： Heterostructure Hydrogen evolution reaction Interfacial electron transfer Oxygen vacancies

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Illuminating spin-crossover octanuclear metal-organic cages

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Science China chemistry 2024年第4期67卷 1208-1215页

作者： Zhi-Kun Liu Alyona A.Starikova Yu-Xia Li Ke Sun Meng Yu Zi-Shuo Yao Jun Tao Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China institute of Physical and Organic chemistry Southern Federal UniversityRostov-on-Don 344090Russia

Spin-crossover(SCO)materials that reversibly switch between high-and low-spin states have potential for the storage of spin state-relative information,and have gained much attention incorporating secondary physical properties,such as fluorescence and magneto-optical *** this study,we synthesized three octanuclear metal-organic cages(MOCs)using tetraphenylethylene-based luminophores,aldehydes,and Fe^(Ⅱ)salts,by subcomponent self-assembly approach,namely[Fe1]-[Fe3].By controlling the ligand-field strength and guest encapsulation,we finely tuned their SCO *** them,MOC[Fe2]displayed nearly complete SCO behavior in the solid state,which is rare for high-nuclearity *** also demonstrated the coupling of SCO with fluorescence emission in these MOCs by using isostructural Zn^(Ⅱ)complexes([Zn1]-[Zn3])as control experiments,for the first *** calculations revealed the energy-transfer mechanism between fluorophores and SCOactive centers,which emphasizes the significant contribution of d-d transitions in the interplay between the occurrence of SCO and fluorescence emission.

关键词： metal-organic cages spin crossover fluorescence switching materials DFT calculation

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Anion-induced differential assembly and structural transformation of supramolecular coordination cages

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Chinese Chemical Letters 2024年第3期35卷 268-272页

作者： Shao-Ping Zheng Yao-Wei Xu Pei-Yang Su Chen-Hui Liu Yin-Hui Huang Yu-Lin Lu Zhang-Wen Wei Zhiwei Jiao Hai-Sen Xu Cheng-Yong Su MOE Laboratory of Bioinorganic and Synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510006China institute of Environmental Research at Greater Bay Area Guangzhou UniversityGuangzhou 510006China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

The intimate host-anion interactions will regulate thermodynamics and kinetics in the self-assembly of cationic cages mimicking biological ***,we report construction and transformation of three Pd(Ⅱ)-based metal-organic cages(MOCs)depending on different *** conversions of the lantern-shaped MOC-34 into either octahedral MOC-35 or tricapped trigonal prism MOC-36 are induced by BF_(4)^(–)or NO_(3)^(–),***-36 is kinetically favored and can undergo quantitative conversion to the thermodynamically preferred MOC-35 upon heating,accelerated by excess BF_(4)^(–)to motivate dissociative dynamics of Pd-vertices and lower activation barrier of cage *** guest encapsulation behaviors of MOC-35 and MOC-36 have also been *** results manifest a significance of host-anion dynamics beyond complementary anion template,shedding light on the understanding of intricate anion recognition in nature.

关键词： Supramolecular coordination cage Dynamic host-anion interactions Structural transformation Anion receptor Guest inclusion

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Copper-catalyzed asymmetric dearomatizing amination of 2-naphthols:Csp^(2)–N coupling via 1,3-reductive elimination

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Science China chemistry 2024年第8期67卷 2694-2700页

作者： Aying Yihuo Maoping Pu Zheng Tan Jibang Liao Jiuqi Tan Qi-Lin Zhou Xiaohua Liu Xiaoming Feng Key Laboratory of Green chemistry&Technology Ministry of EducationCollege of ChemistrySichuan UniversityChengdu 610064China Key Laboratory and institute of Elemento-Organic chemistry College of Chemistry Frontiers Science Centerfor New Organic MatterNankai UniversityTianjin300071China

An efficient catalytic asymmetric dearomatizing amination of 2-naphthols and phenols catalyzed by N,N′-dioxide-copper(I)complex as a chiral catalyst was presented.A variety of optically activeβ-naphthalenone compounds with a nitrogen-containing quaternary carbon stereocenter were obtained with high yield and enantioselectivity under mild reaction *** studies indicated that this Csp^(2)–N dearomatizing coupling proceeds via 1,3-reductive elimination of phenolate-Cu~Ⅲ-amino intermediate in five-membered ring transition *** origin of enantioselectivity has also been elucidated based on density functional theory calculations.

关键词： asymmetric catalysis amination dearomatization copper catalysis coupling reaction

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