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Cucurbit[6]uril-based supramolecular assembly: its syntheses,structures, capture of heavy metal ions, and sensing properties

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Science China chemistry 2024年

作者： Yefang Yang Dechao Li ShaoWen Qie Shuai Su Ruijie Xu Wenting Li Wenping Hu Ming Hu School of chemistry and Chemical Engineering Inner Mongolia University Inner Mongolia Key Laboratory of Chemistry and Physics of Rare Earth Materials

Multidimensional supramolecular assembly（CB[6]-PA） based on cucurbit[6]uril（CB[6]） was constructed via the outer-surface interactions of CB[6] with a structure-directing agent of pamoic acid（H2PA）. Most impressively, crystal CB[6]-PA exhibited satisfactory selectivity for the capture of Cd2+and Hg2+cations, and released Cd2+and Hg2+cations under acidic condition. This reversible process allows for capturing applications of Cd2+and Hg2+cations. Furthermore, crystalline CB[6]-PA-Cd demonstrated enhanced fluorescence properties compared with H2PA ligands. CB[6]-PA-Cd could be employed for the precise detection of methylmalonic acid（EA or MMA） as a biomarker of septicemia. The introduction of EA resulted in the fluorescence quenching of CB[6]-PA-Cd, the mechanism of sensing EAwas clearly elucidated. A portable detection platform was designed to augment the efficiency of EA detection. To promote biological applications, the exceptional probe capable of exactly detecting EA in serum samples had been substantiated. CB[6]-PA-Cd exhibited a negligible cytotoxicity, favorable cytocompatibility, and good hemocompatibility. Thus, these results will bring about new enlightenment for the fabrication of light-emitting materials and high-resolution bio-imaging probes based on cucurbit[n]urils.

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Synthesis,chemical bonding and reactivity of new medium-sized polyarsenides

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Chinese Chemical Letters 2024年第7期35卷 497-501页

作者： Xu-Hui Yue Xiang-Wen Zhang Hui-Min He Lei Qiao Zhong-Ming Sun State Key Laboratory of Element-Organic chemistry Tianjin Key Lab for Institution Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Department of physics Institute of Computational and Applied PhysicsTaiyuan Normal UniversityJinzhong 030619China

Gaining an understanding of the growth mechanism from single atoms to clusters and bulk materials continues to present a ***,it is important to explore the evolving trends of clusters in the structure and properties during the size *** this work,we report the synthesis and characterization of two medium-sized chain-like polyarsenic anions.[As_(21)]^(3-)represents a trimeric example of polyarsenic anion assembled through oxidative coupling of As_(7)^(3-)*** anion As_(18)^(4-)included in[As_(18)MO_(2)(CO)_(8)]^(4-)is regarded as formed by two realgar-type As_(8)subunits connected by a dinuclear AsAs *** As_(18)cluster was previously predicted by theory,and this is the first time successfully synthesized using wet chemistry ***,small-sized polyarsenides As_(2)^(2-)and As_(10)^(2-)were found in compound[K(18-crown-6)]_(3)[As_(10)]_(0.5)[As_(4){Mo(CO)_(3)}_(2)]_(0.5)·*** these,the former exhibits coordination with metal ***-crystal X-ray diffraction combined with quantum chemical calculations revealed the formation of double bonded As_(2)^(2-)stabilized by metal carbonyl *** work demonstrates a novel synthetic approach for the preparation of new polyarsenides and highlights their intriguing bonding characteristics,laying the foundation for the synthesis of such compounds and paving the way for their potential applications.

关键词： Polyarsenide Zintl anions Chain-like cluster DFT calculations AdNDP

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Reversing free-electron transfer of sulfide cocatalyst for exceptional photocatalytic H_(2)evolution

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Journal of materials Science & Technology 2024年第4期171卷 147-149页

作者： Yanfeng Zhang Zhenyi Zhang National Experimental chemistry Teaching Center Hebei Key Laboratory of Inorganic Nano-materialsCollege of Chemistry and Materials ScienceHebei Normal UniversityShijiazhuang 050024China Key Laboratory of New Energy and Rare earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials and Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Minzu UniversityDalian 116600China

Recently,Yu and co-workers deeply explore the potential impact of free electron transfer between co-catalysts and photocatalyst carriers on H_(2)evolution efficiency of active sites over MoS_(2+x).They pro-pose an electron-reversal tactics to evade the unexpected electron transfer and synchronously regulate the above transfer in a beneficial orientation for weakening hydrogen adsorption on S ***,this highlight not only discusses and summarizes the essences of electron reversal and the optimized H ad-sorption/desorption mechanism,but also emphasizes the significance of femtosecond transient absorp-tion spectroscopy(fs-TAS)and in-situ irradiated X-ray photoelectron spectroscopy(ISI-XPS)for revealing charge transfer dynamics and *** anticipate that this highlight can disseminate a new per-spective on the roles of photocatalyst carriers in improving cocatalytic H_(2)-production kinetics.

关键词： Photocatalysis Cocatalyst Electron reversal Antibonding-orbital occupancy S–H bonds

A DFT study on Pt single atom loaded COF for efficient photocatalytic CO_(2)reduction

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Journal of materials Science & Technology 2024年第3期170卷 87-94页

作者： Fei Xie Chuanbiao Bie Jian Sun Zhenyi Zhang Bicheng Zhu Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan430078China Key Laboratory of New Energy and Rare earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials and Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Minzu UniversityDalian116600China

Photocatalytic CO_(2)reduction provides a promising strategy for the alleviation of greenhouse effect and energy shortage *** single atom modification is an effective method to improve the CO_(2)reduction performance of covalent organic framework(COF)photocatalysts,while the intrinsic mechanism is not revealed in ***,a Pt-COF photocatalytic system was constructed by embedding Pt single atom in TFPT-TMT-COF(TFPT:1,3,5-tris(4-formylphenyl)-triazine,TMT:2,4,6-trimethyl-1,3,5-triazine).Based on density functional theory(DFT)calculation,the geometric structure and electronic property of Pt-COF were investigated,and the CO_(2)adsorption and reduction reaction process on Pt-COF were *** results show that the Pt atom can be steadily anchored in COF via the formation of Pt-N and Pt-C ***,there is strong electronic interaction between Pt and *** incorporation of Pt atom benefits the CO_(2)reduction activity of COF from multiple aspects:(ⅰ)reducing the band gap and improving light absorption;(ⅱ)enhancing CO_(2)adsorption and activating the CO_(2)molecule;(ⅲ)decreasing the energy barrier in the hydrogenation step of CO_(2)→COOH,thus facilitating CO_(2)conversion to CO;(ⅳ)inhibiting the hydrogenation of CO,thereby increasing the selectivity of *** work brings a novel insight into the excellent CO_(2)reduction performance of Pt modified COF,and provides useful references for the design of single atom photocatalysts.

关键词： Photocatalysis Carbon dioxide reduction Covalent organic framework Pt single atom Theoretical calculation

Universal insertion of molecules in ionic compounds under pressure

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National Science Review 2024年第1期11卷 120-128页

作者： Feng Peng Yanming Ma Chris J.Pickard Hanyu Liu Maosheng Miao College of physics and Electronic Information Luoyang Normal University Department of chemistry and Biochemistry California State University Northridge State Key Laboratory of Superhard materials & Key Laboratory of Material Simulation Methods and Software of Ministry of Education College of Physics Jilin University International Center of Future Science Jilin University Department of materials Science & Metallurgy University of Cambridge Advanced Institute for materials Research Tohoku University Department of earth Science University of California Santa Barbara

Using first-principles calculations and crystal structure search methods, we found that many covalently bonded molecules such as H2, N2, CO2, NH3, H2O and CH4may react with NaC l, a prototype ionic solid,and form stable compounds under pressure while retaining their molecular structure. These molecules,despite whether they are homonuclear or heteronuclear, polar or non-polar, small or large, do not show strong chemical interactions with surrounding Na and Cl ions. In contrast, the most stable molecule among all examples, N2, is found to transform into cyclo-N5-anions while reacting with NaC l under high pressures. It provides a new route to synthesize pentazolates, which are promising green energy materials with high energy density. Our work demonstrates a unique and universal hybridization propensity of covalently bonded molecules and solid compounds under pressure. This surprising miscibility suggests possible mixing regions between the molecular and rock layers in the interiors of large planets.

关键词： molecule-solid hybrid materials high-pressure crystal structure prediction density functional theory planet interior

Sustainable all-weather CO2 utilization by mimicking natural photosynthesis in a single material

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National Science Review 2024年第2期11卷 177-187页

作者： Xianjin Shi Yu Huang Ran Long Zhenyu Wang Liqin Wang Junji Cao Gangqiang Zhu Yujie Xiong State Key Laboratory of Loess and Quaternary Geology(SKLLQG) Key Laboratory of Aerosol Chemistry and Physics Institute of Earth EnvironmentChinese Academy of Sciences Center of Excellence in Quaternary Science and Global Change Chinese Academy of Sciences University of Chinese Academy of Sciences Hefei National Research Center for Physical Sciences at the Microscale School of Chemistry and Materials Science and National Synchrotron Radiation Laboratory University of Science and Technology of China Institute of Atmospheric physics Chinese Academy of Sciences School of physics and Information Technology Shaanxi Normal University

Solar-driven CO2conversion into hydrocarbon fuels is a sustainable approach to synchronously alleviating the energy crisis and achieving net ***,the dependence of the conversion process on solar illumination hinders its practical application due to the intermittent availability of sunlight at night and on cloudy or rainy ***,we report a model material of Pt-loaded hexagonal tungsten trioxide（Pt/h-WO3） for decoupling light and dark reaction processes,demonstrating the sustainable CO2conversion under dark conditions for the first *** such a material system,hydrogen atoms can be produced by photocatalytic water splitting under solar illumination,stored together with electrons in the h-WO3through the transition of W6+to W5+and spontaneously released to trigger catalytic CO2reduction under dark ***,we demonstrate using natural light that CH4production can persist at night and on rainy days,proving the accomplishment of all-weather CO2conversion via a sustainable way.

关键词： sustainable CO2 utilization artificial photosynthesis all-weather application charge storage

Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting

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Nano Research 2024年第3期17卷 1114-1122页

作者： Chao-Peng Wang Hao Sun Gang Bian Jia-Xi Wang Xixi Pang Guoqi Wang Jian Zhu Xian-He Bu School of materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Tianjin Key Laboratory of Metal and Molecule-Based Material chemistry Nankai UniversityTianjin 300350China Tianjin Key Laboratory for Rare earth materials and Applications Nankai UniversityTianjin 300350China

Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient ***,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)*** particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 ***,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V *** study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.

关键词： layer-by-layer(LbL)assembly layered double hydroxides(LDH) two-dimensional(2D)electrocatalysts oxygen evolution reaction(OER) water splitting

Recent progress in CdS-based S-scheme photocatalysts

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Journal of materials Science & Technology 2024年第4期171卷 162-184页

作者： Yajing Ren Yunfeng Li Guixu Pan Ning Wang Yan Xing Zhenyi Zhang College of Environmental and Chemical Engineering Xi’an Polytechnic UniversityXi’an 710048China Jilin Provincial Key Laboratory of Advanced Energy materials Department of ChemistryNortheast Normal UniversityChangchun 130024China Key Laboratory of New Energy and Rare earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials and Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Minzu UniversityDalian 116600China

Photocatalytic technology with sunlight as driving force can convert solar energy into other energy sources for storage and further *** sulfide(CdS),as a typical reducing semiconductor of metal sulfides,represents an interesting research hotspot in photocatalysis due to its suitable bandgap(2.4 eV)for utilizing visible light and strong reducing ability for inducing surface catalytic ***,the photocatalytic performance of CdS is still limited by its fast carrier recombination and serious *** far,CdS semiconductor has been widely developed as a typical reducing photocatalyst in constructing novel S-scheme heterojunction to overcome the above *** this review,the de-sign concepts,basic principles,and charge transfer characteristics of CdS-based S-scheme heterojunction photocatalysts have been comprehensively *** advanced and effective characterization methods for studying the mechanism of CdS-based S-scheme heterojunction are analyzed in ***-thermore,we also summarize the typical applications of CdS-based S-scheme heterojunctions for water splitting,CO_(2) reduction,pollutant degradation,***,according to the current investigation sta-tus,some drawbacks in the current synthetic strategy,mechanism exploration,and application prospect of CdS-based S-scheme heterojunction are proposed,which need to be addressed by further expansion and innovative research.

关键词： Photocatalysis CdS semiconductor Heterojunction S-scheme Metal sulfide

High temperature superconductor Na2B2H stabilized by hydrogen intercalation under ambient pressure

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Science China(physics,Mechanics & Astronomy) 2024年第11期Mechanics & Astronomy) .卷 145-152页

作者： Wendi Zhao Defang Duan Zhengtao Liu Zihao Huo Shumin Guo Decheng An Maosheng Miao Tian Cui State Key Laboratory of Superhard materials Key Laboratory of Material Simulation Methods & Software of Ministry of Education College of Physics Jilin University Department of chemistry and Biochemistry California State University Department of earth Science University of California Institute of High Pressure physics School of Physical Science and Technology Ningbo University

Hydrogenated metal borides have attracted much attention due to their potential high-temperature superconductivity. Here, we propose a new strategy for hydrogen intercalation tuning the stability and superconductivity of the boron honeycomb sublattice,and predict an unprecedented layered compound Na2B2H, which hosts excellent superconductivity. Strikingly, the superconducting transition temperature（Tc） of Na2B2H reaches 42 K at ambient pressure. The Tcvalue can be further increase to 63 K under 5% biaxial tensile strain. The excellent superconductivity originates from the strong electron-phonon coupling between theσ-bonding bands near the Fermi level and the B-B stretching optical E modes. The interstitial electron localization and crystal orbitals of the H-intercalated Na ion layer well match the boron honeycomb lattice and act as a chemical template to stabilize the B layer. Furthermore, the introduction of hydrogen tuned the Fermi level, and the coupling vibration of Na and H ions effectively enhanced the dynamic stability of the structure. Na2B2H represents a new family of layered high-temperature superconductors,and the strategy of stabilizing the honeycomb boron sublattice via chemical template hosts great potential for application to more layered compounds.

关键词： superconductivity hydrogenation metal borides electron-phonon coupling