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Cucurbit[8]uril-regulated face-to-face dimerization assembly enhanced photosensitization and photocatalysis

Science China Chemistry 2024年第5期67卷 1605-1612页

作者： Haigen Nie Die Hu Zhiyao Zeng Yan Fan Yaxin Zhai xin-long Ni Key Laboratory of Chemical Biology and Traditional Chinese Medicine Ministry of Educational of ChinaKey Laboratory of the Assembly and Application of Organic Functional Molecules of Hunan ProvinceCollege of Chemistry and Chemical EngineeringHunan Normal UniversityChangsha 410081China Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education Department of PhysicsHunan Normal UniversityChangsha 410081China

In water, N,N′-diarylpyridinium thiazolo[5,4-d]thiazole guests(G1.G3) were encapsulated by cucurbit[8]uril(Q[8]) to construct Q[8]_(3)/G_(2) complexes, in which the encapsulated G molecules exist as an exact face-to-face dimer. These complexation behaviors have been indicated by proton nuclear magnetic resonance(~1. NMR) spectroscopy and isothermal titration calorimetry(ITC),and have been confirmed by X-ray single crystal structural analysis of Q[8]_(3)/G2_(2). While free guests G1.G3 have no ability to sensitize singlet oxygen, they all become effective singlet oxygen sensitizers when complexed with Q[8]. By irradiation of white light, Q[8]_(3)/G_(2) complexes induced selective oxidation of aryl sulfide to aryl sulfoxide in good yields and selective oxidation of dimethyl sulfide(DMS) to dimethyl sulfoxide(DMSO) in excellent yields without over-oxidation to dimethyl sulfone(DMSO_(2))even for elongated irradiation. High-yield photo-oxidation of DMS to DMSO_(2) was only achieved by irradiation of blue light in the presence of Q[8]_(3)/G1.(2), which was also effective in photobleaching of Rhodamine B in water. The higher photo-oxidation power of Q[8]_(3)/G1.(2) has been ascribed to an additional generation of reactive oxygen species besides singlet oxygen.

关键词： host-guest interaction dimerization macrocycles photosensitization

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A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China Chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-xin Li Wei-Chao Chen Kui-Zhan Shao xin-long Wang Chao Qin Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction *** we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(1.)(NH_(4))_(4)H_(1.)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(1.)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton ***,high proton conductivity(2.04×1.^(-2)S cm^(-1.) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting *** result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

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Association between stress hyperglycemia ratio and in-hospital outcomes:findings from the improving Care for Cardiovascular Disease in China-Acute Coronary Syndrome(CCC-ACS)Project

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Journal of Geriatric Cardiology 2024年第6期21卷 658-668页

作者： Wen-Jie WANG Ke-xin WANG Jia-{1. NIU Yi-Xuan LIU Hai-{1. GE Hua SHEN On behalf of CCC-ACS investigators Department of Cardiology Beijing Anzhen HospitalCapital Medical UniversityBeijingChina

BACKGROUND Stress hyperglycemia ratio(SHR)could provide accurate information on the acute status of *** relationship between SHR and acute coronary syndrome(ACS)prognosis remains *** study was conducted to identity the association between SHR and in-hospital outcomes in patients with *** A total of 1.,01. patients were eventually enrolled in the *** relationship between SHR and in-hospital major adverse cardiovascular events(MACEs)was then modeled by restricted cubic spline(RCS)curves,and all patients were divided into three groups according to the *** multivariate logistic regression analysis was used to determine the associations between the SHR and in-hospital outcomes,described as odds ratios(ORs)and 95%confidence intervals(CIs).Subgroup analyses were also performed on different *** The median age of this cohort was 63(54,71.years old,and 8942(74.5%)were *** 1.was defined as SHR1.n=5821.,and Group 3 was defined as SHR>1.n=5763).Compared with Group 2,Group 1.OR=1.891.95%CI:1.028-3.479,P1.and Group 3(OR=1.868,95%CI:1.434-2.434,P1.had higher risks of suffering from in-hospital *** was associated with higher risks of in-hospital MACEs in the subgroups of DM[OR=2.282,95%CI:1.477-3.524).CONCLUSIONS Both low and high SHR levels were independently associated with in-hospital *** males with DM,hypertension,and decreased renal function had much higher risks of suffering from SHR-correlated MACEs.

关键词： acute cardiovascular finding

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Constructing S-scheme charge separation in cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4) heterojunction with enhanced photothermal-assisted photocatalytic H_(2) evolution

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Rare Metals 2024年第1期43卷 198-211页

作者： Wei-long Shi Zheng Xu Yu-{1.g Shi Ling-Ling Li Jia-Lin Lu {1.-Hai Sun {1. Du Feng Guo Chang-Yu Lu School of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003JiangsuChina College of Chemistry Zhengzhou UniversityZhengzhou 450001China School of Water Resource and Environment Hebei Province Key Laboratory of Sustained Utilization and Development of Water RecourseHebei Center for Ecological and Environmental Geology ResearchHebei Geo UniversityShijiazhuang 050031China

Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific ***,cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4)(CoPc/OCN) S-scheme heterojunction photocatalyst was designed by coupling multi-step calcination with solvothermal method for enhanced photothermal-assisted photocatalytic H_(2) *** multistep calcined g-C_(3)N_(4) is easier for O-doping formation,and the ethanol solvothermal strategy is utilized to enhance the dispersion of CoPc on OCN nano sheet surface and forms sufficient S-scheme heterojunction through *** addition,the active sites and excellent photothermal properties of CoPc itself further improve the integrated photocatalytic activity of CoPc/OCN S-scheme *** optimal photocatalytic hydrogen evolution rate of CoPc/OCN S-scheme heterojunction photocatalyst reached 9.56 mmol·g^(-1.·h^(-1.,which is 2.69 and 1.23 times higher than that of CN and OCN,*** work provides a valuable design idea and scheme for enhancing the multi-factor co-assisted photocatalytic H_(2) evolution performance.

关键词： Photothermal Photocatalytic H_(2)evolution Cobalt phthalocyanine Oxygen-doped g-C_(3)N_(4) Sscheme heterojunction

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Heteroatom tuning in agarose derived carbon aerogel for enhanced potassium ion multiple energy storage

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Carbon Energy 2024年第3期6卷 239-254页

作者： Kaijun Xie xin Liu Haolin Li {1. Fang Kai Xia Dongjiang Yang Yihui Zou Xiaodong Zhang State Key Laboratory of Bio-fibers and Eco-textiles Shandong Collaborative Innovation Center of Marine Biobased Fibers and Ecological TextilesInstitute of Marine Biobased MaterialsCollege of Chemistry and Chemical EngineeringCollege of Environmental Science and EngineeringQingdao UniversityQingdaoChina

The incorporation of heteroatoms into carbon aerogels(CAs)can lead to structural distortions and changes in active sites due to their smaller size and electronegativity compared to pure ***,the evolution of the electronic structure from single-atom doping to heteroatom codoping in CAs has not yet been thoroughly investigated,and the impact of codoping on potassium ion(K+)storage and diffusion pathways as electrode material remains *** this study,experimental and theoretical simulations were conducted to demonstrate that heteroatom codoping,composed of multiple heteroatoms(O/N/B)with different properties,has the potential to improve the electrical properties and stability of CAs compared to single-atom *** states near the Fermi level have revealed that doping with O/N/B generates a greater number of active centers on adjacent carbon atoms than doping with O and O/N *** a result of synergy with enhanced wetting ability(contact angle of 9.26°)derived from amino groups and hierarchical porous structure,ON-CA has the most optimized adsorption capacity(−1.62 eV)and diffusion barrier(0.1. eV)of K^(+).The optimal pathway of K^(+)in ON-CA is along the carbon ring with N or O *** K^(+)storage material for supercapacitors and ion batteries,it shows an outstanding specific capacity and capacitance,electrochemical stability,and rate ***,the assembled symmetrical K^(+)supercapacitor demonstrates an energy density of 51.8 Wh kg^(−1.,an ultrahigh power density of 443Wkg^(−1.,and outstanding cycling stability(maintaining 83.3%after 1.,000 cycles in 1. KPF6 organic electrolyte).This research provides valuable insights into the design of highperformance potassium ion storage materials.

关键词： agarose carbon aerogels O/N/B codoping potassium-ion battery potassium-ion supercapacitor

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Lignin-reinforced PVDF electrolyte for dendrite-free quasi-solid-state Li metal battery

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Rare Metals 2024年第3期43卷 1006-1016页

作者： xin-Yang Chen Xue-Jie Gao Han-Yan Wu Yu-{1. Liu Xiao-Fei Yang Run-Cang Sun Center for Lignocellulosic Chemistry and Biomaterials College of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalian116034China Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China School of Chemistry Northeast Normal UniversityChangchun130024China

Quasi-solid-state lithium metal batteries(QSSLMBs)assembled with polyvinylidene fluoride(PVDF)are a promising class of next-generation rechargeable batteries due to their safety,high energy density,and superior interfacial ***,PVDF has a series of inherent drawbacks such as low ionic conductivity,ease of crystallization,and hydrophobic character that leading to poor cell *** tackle these issues,a lignin-reinforced PVDF electrolyte is proposed in this work to solve these drawbacks of PVDF and enhance the comprehensive performance of *** lithophilic polar groups of lignin can promote uniform deposition of Li on the *** with the improved mechanical properties can efficiently prevent Li dendrites penetration through the *** addition,more active sites provided by lignin can also enhance Li^(+)transport and lead to a faster electrochemical reaction *** from the ingenious design,Li symmetric cells with 5%lignin-PVDF quasi-solid-state electrolyte can operate for 900 h at a high current density/capacity of 5 mA·cm^(-2)/5 mAh·cm^(-2),while shortcircuiting occurs after 56 h for the counterpart(pure PVDF).Moreover,a full cell of Li/5%lignin-PVDF/LFP cell demonstrates a high capacity of 96.2 mAh·g^(-1.after 2000 cycles at 1. *** work is expected to open up promising opportunities to develop other high-energy/power-density QSSLMBs.

关键词： Quasi-solid-state electrolyte Lignin PVDF Dendrite-free Li metal battery

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Hybrid bimetallic cluster ZrO2/Rh@N,S co-doped porous carbon nanosheets for efficient hydrogen evolution in acid electrolytes

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Tungsten 2024年第4期6卷 657-662页

作者： xin-Yi Zhang Igor V.Zatovsky Jun-Ming Cao xing-long Wu Faculty of Chemistry Northeast Normal University F.D.Ovcharenko Institute of Biocolloidal Chemistry NAS Ukraine MOE Key Laboratory for UV Light-Emitting Materials and Technology Northeast Normal University

Acid hydrogen evolution reaction (HER) is a critical energy conversion process,which is significantly important in hydrogen energy manufacturing and storage [1..Although the performance of noble metal platinum (Pt)-based catalysts in acidic HER is well known,the challenges are high cost,limited reserves,poor stability,and susceptibility to toxic substances [2].Therefore,it is urgent to design and manufacture acidic HER catalysts with high reactivity,high stability,and low cost.

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Geochemical identification of a source rock affected by migrated hydrocarbons and its geological significance:Fengcheng Formation,southern Mahu Sag,Junggar Basin,NW China

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Petroleum Science 2024年第1期21卷 100-114页

作者： Wen-long Dang Gang Gao {1.-Cai You Ke-Ting Fan Jun Wu De-Wen Lei Wen-Jun He Yong Tang State Key Laboratory of Petroleum Resource and Prospecting China University of Petroleum(Beijing)Beijing102249China School of GeoSciences China University of Petroleum(Beijing)Beijing102249China Exploration&Development Institute Xinjiang Oil Field CompanyKaramay834000XinjiangChina

The Fengcheng Formation is a crucial source rock and the primary reservoir for oil accumulation in the Mahu *** oils are distributed throughout the Fengcheng Formation,ranging from the edge to the interior of the sag in the southern Mahu *** crude oils originate from in-situ source rocks in shallowly buried areas and the inner deep *** migration,the crude oil from the inner deep sag affects the source rocks close to carrier beds,leading to changes in the organic geochemical characteristics of the source *** changes might alter source rock evaluations and oil-source *** on data such as total organic carbon(TOC),Rock-Eval pyrolysis of source rocks,and gas chromatography-mass spectrometry(GC-MS)of the saturated fraction,and considering the geological characteristics of the study area,we define the identification characteristics of source rock affected by migrated hydrocarbons and establish the various patterns of influence that migrated hydrocarbons have on the source rock of the Fengcheng Formation in the southern Mahu *** source rocks of the Fengcheng Formation are mostly fair to good,containing mainly Type II organic matter and being thermally mature enough to generate *** rocks affected by migrated hydrocarbons exhibit relatively high hydrocarbon contents(S1.TOC>1.0 mg HC/g TOC,Extract/TOC>30%,HC:hydrocarbon),relatively low Rock-Eval Tmax values,and relatively high tricyclic terpane contents with a descending and mountain-shaped ***,biomarker composition parameters indicate a higher thermal maturity than in-situ source *** a comparison of the extract biomarker fingerprints of adjacent reservoirs and mudstones in different boreholes,three types of influence patterns of migrated hydrocarbons are identified:the edge-influence of thin sandstone-thick mudstone,the mixed-influence of sandstone-mudstone interbedded,and the full-influence of thick sandstone-thin *** finding reminds

关键词： Organic geochemistry Source rock Influence of migrated hydrocarbons Fengcheng Formation Southern Mahu Sag

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Highly Aromatic Norditerpenoid Heterodimers and Monomers from Trigonostemon fragilis

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Engineering 2024年第7期38卷 144-154页

作者： Jun-Su Zhou long Cheng Yuan Gao Zhan-Peng Ge Bin Zhou Jing-Ya Li Jin-{1. Zhao Jian-Min Yue State Key Laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China Shandong Laboratory of Yantai Drug Discovery Bohai Rim Advanced Research Institute for Drug DiscoveryYantai 264117China

Four new norditerpenoid heterodimers with different dimerization patterns-namely,trigofragiloids A-C(denoted as compounds 1.3)and(+)-and(-)-trigofragiloid D(compound 4)-and three new phenanthrenone norditerpenoids-namely,trigofragiloids E-G(compounds 5-7)-were isolated from Trigonostemon *** 1.and 2 feature a novel heterodimeric carbon skeleton formed by the conjugation of a tetra-norditerpenoid and an ennea-norditerpenoid;they have been identified as class 2 atropisomers by means of quantum chemical *** 3 is an unprecedented phenylpropanoid-norditerpenoid adduct with a new dimerization ***(+)-and(-)-4 are the first example of S-shaped 1.4-dioxane-fused norditerpenoid *** by the structure elucidation of compound 4,two co-occurring analogues,actephilol A and epiactephilol A,were structurally revised as a pair of geometrical isomers and were identified as two pairs of enantiomers,(+)-and(-)-8 and(+)-and(-)-9,*** structures were characterized using a combined ***,compound 7 exhibits remarkable adenosine triphosphate-citrate lyase(ACLY)inhibition with a halfmaximal inhibition concentration(IC50)value of(0.46±0.1.)lmol·L^(-1.,as active as the positive control BMS-3031.1.and a molecular docking study offers deep insight into the interaction between compound 7 and ACLY.

关键词： Norditerpenoid heterodimer Trigonostemon fragilis Euphorbiaceae Trigofragiloid Structural revision Adenosine triphosphate-citrate lyase(ACLY) inhibitory activity

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Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy

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Chinese Chemical Letters 2024年第10期35卷 516-520页

作者： A-Yang Wang Sheng-Hua Zhou Mao-Yin Ran xin-Tao Wu Hua Lin Qi-{1. Zhu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences (CAS) Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China College of Chemistry Fuzhou University University of Chinese Academy of Sciences

Recently, non-centrosymmetric（NCS） Hg-based chalcogenides have garnered significant interest due to their strong second-harmonic-generation intensities(deff), making them attractive candidates for infrared nonlinear optical（IR-NLO） application. However, achieving both wide band gaps（Eg） and large phasematched deffsimultaneously in these materials remains a challenge due to their inherent constraints on each other. In this research, we have successfully obtained two quaternary NCS Hg-based chalcogenides, Rb2HgGe3S8and Cs2HgGe3S8, by implementing a bandgap engineering strategy that involves alkali metal introduction and Hg/Ge ratio regulation. Both compounds consist of 2D [Hg Ge3S8]2–anionic layers made of 1. [HgGeS6]6–chains and dimeric [Ge2S6]4–polyhedra arranged alternately, and the charge-balanced Rb+/Cs+cations located between these layers. Remarkably, Rb2HgGe3S8and Cs2HgGe3S8exhibit overall properties required for promising IR-NLO materials, including sufficient PM deff（0.55–0.70 × AgGaS2@2050 nm）, large Eg（3.27–3.41.e V）, giant laser-induced damage thresholds（1..4–1..7 ×AgGaS2@1.64 nm）, broad optical transmission intervals（0.32–1..5 μm）, and suitable theoretical birefringence（0.069–0.086@2050 nm）. Furthermore, in-depth theoretical analysis reveals that the exceptional IRNLO performance is attributed to the synergy effects of distorted [HgS4] and [GeS4] tetrahedra. Our study provides a useful strategy for enhancing the Egand advancing Hg-based IR-NLO materials, which is expected to extended and implemented in other chalcogenide systems.

关键词： Bandgap engineering strategy Hg-based chalcogenides IR nonlinear material Structure-activity relationship Wide energy gap

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