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An efficient Ag/MIL-100(Fe)catalyst for photothermal conversion of CO_(2)at ambient temperature

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Chinese Chemical Letters 2021年第11期32卷 3505-3508页

作者： Peng Jing Boyuan Wu zongsu han Wei Shi Peng Cheng Key Laboratory of Advanced Energy Materials Chemistry(MOE) College of ChemistryNankai UniversityTianjin 300071China Renewable Energy Conversion and Storage Center Nankai UniversityTianjin 300071China

The conversion of CO_(2)under mild condition is of great importance because these reactions involving CO_(2)can not only produce value-added chemicals from abundant and inexpensive CO_(2)feedstock but also close the carbon ***,the chemical inertness of CO_(2)requires the development of high-performance ***,Ag nanoparticles/MIL-100(Fe)composites were synthesized by simple impregnation-reduction method and employed as catalysts for the photothermal carboxylation of terminal alkynes with CO_(2).MIL-100(Fe)could stabilize Ag nanoparticles and prevent them from aggregation during catalytic *** the advantages of photothermal effects and catalytic activities of both Ag nanoparticles and MIL-100(Fe),various aromatic alkynes could be converted to corresponding carboxylic acid products(86%-92%yields)with 1 atm CO_(2)at room temperature under visible light irradiation when using Ag nanoparticles/MIL-100(Fe)as photothermal *** catalysts also showed good recyclability with almost no loss of catalytic activity for three consecutive *** importantly,the catalytic performance of Ag nanoparticles/MIL-100(Fe)under visible light irradiation at room temperature was comparable to that upon heating,showing that the light source could replace conventional heating method to drive the *** work provided a promising strategy of utilizing solar energy for achieving efficient CO_(2)conversion to value-added chemicals under mild condition.

关键词： Ag nanoparticles Metal-organic frameworks Photothermal catalysis CO_(2)conversion Carboxylation

Rapid detection of nanoplastic particles by a luminescent Tb-based coordination polymer

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Chinese Chemical Letters 2024年第5期35卷 529-533页

作者： Tiankai Sun Hui Min zongsu han Liang Wang Peng Cheng Wei Shi Department of Chemistry College of ChemistryNankai UniversityTianjin 300071China State Key Laboratory of Separation Membranes and Membrane Processes School of Environmental Science and EngineeringTiangong UniversityTianjin 300387China Key Laboratory of Advanced Energy Materials Chemistry(MOE) Frontiers Science Center for New Organic Matter and Renewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Nanoplastics(NPs)in aqueous environment have become a category of emerging pollutants on account of their potential risks to both human health and *** detection of NPs is a great challenge due to the lack of sensitive and selective sensing materials with fast response time and wide sensing range of particle ***,a Tb-based coordination polymer has been synthesized for luminescent detection of nanopolystyrene with different particle sizes in aqueous solutions,showing a low limit of detection,fast response time within 10 s and high selectivity in the presence of other ***“turn-on”sensing mechanism is studied in *** work provides a facile method for the fast detection of NPs.

关键词： Coordination polymer Nano polystyrene Luminescent detection Sensing mechanism Water safety

Observation of oxygen evolution over a {Ni12}-cluster-based metal-organic framework

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Science China Chemistry 2022年第6期65卷 1088-1093页

作者： zongsu han Zheng Yan Kunyu Wang Xinchen Kang Kai Lv Xiaoping Zhang Zhen Zhou Sihai Yang Wei Shi Peng Cheng Department of Chemistry Key Laboratory of Advanced Energy Materials Chemistry(MOE)Renewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin300071China College of Biological Chemical Sciences and EngineeringJiaxing UniversityJiaxing314001China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190China Department of Chemistry University of ManchesterManchesterM139PLUK School of Materials Science and Engineering Institute of New Energy Material ChemistryNankai UniversityTianjin300350China

The development of efficient electrocatalysts based on non-noble metals for oxygen evolution reaction(OER) remains an important and challenging task. Multinuclear transition-metal clusters with high structural stability are promising OER catalysts but their catalytic role is poorly understood. Here we report the crystallographic observation of OER activity over robust {Ni12}-clusters immobilised in a porous metal-organic framework, NKU-100, by single-crystal X-ray diffraction as a function of external applied potential. We observed the aggregation of confined oxygen species around the {Ni12}-cluster as a function of applied potential during the electrocatalytic process. The refined occupancy of these oxygen species shows a strong correlation with the variation of current density. This study demonstrates that the enrichment of oxygen species in the secondary coordination sphere of multinuclear transition-metal clusters can promote the OER activity.

关键词： metal-organic framework oxygen evolution reaction secondary coordination sphere X-ray diffraction binding site

Dynamic-static coupled sensing of trace biomarkers by molecularly imprinted metal-organic frameworks

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Science China Chemistry 2023年第12期66卷 3511-3517页

作者： Hui Min zongsu han Tiankai Sun Kunyu Wang Jun Xu Peiyu Yao Sihai Yang Peng Cheng Wei Shi Department of Chemistry Key Laboratory of Advanced Energy Materials Chemistry(MOE)and Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin 300071China School of Materials Science and Engineering&National Institute for Advanced Materials Center for Rare Earth and Inorganic Functional Materials Tianjin Key Lab for Rare Earth Materials and ApplicationsNankai UniversityTianjin 300350China Department of Emergency Tianjin Union Medical CenterTianjin 300121China Department of Chemistry University of ManchesterManchester M139PLUK College of Chemistry and Molecular Engineering Beijing National Laboratory for Molecular SciencesPeking UniversityBeijing 100871China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Accommodating target analytes within the pores of metal-organic frameworks(MOFs)to improve the sensing performance is an important but challenging ***,we report a novel molecular imprinting strategy to create target recognition sites in a tailored multicomponent MOF with the inter-ligand synergistic antenna effect to lanthanide ions,enabling selective recognition of trace biomarkers,which is critical to the early diagnosis of age-related diseases in blood samples with high sensitivity and ultralow limit of detection(LOD)of 69 nmol L^(-1).Compared with MOF-based sensors without imprinted recognition sites,the significantly enhanced sensing performance(both sensitivity and LOD)was attributed to a dynamic-static coupled sensing mechanism:the dynamic interactions involve concentrating the trace biomarkers at the imprinted recognition sites to enhance the sensing performance at ultralow concentration,and the static interactions are derived from electron/energy exchange between the molecularly imprinted MOF and the biomarker to govern the sensing *** work establishes a new molecular imprinting strategy to attain advanced materials for sensing trace bio-analytes.

关键词： molecularly imprinted metal-organic frameworks dynamic-static coupled sensing biomarker recognition

A Multicenter Metal–Organic Framework for Quantitative Detection of Multicomponent Organic Mixtures

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CCS Chemistry 2022年第10期4卷 3238-3245页

作者： zongsu han Kunyu Wang Yinlin Chen Jiangnan Li Simon JTeat Sihai Yang Wei Shi Peng Cheng Department of Chemistry Key Laboratory of Advanced Energy Materials Chemistry(MOE)and Renewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071 Department of Chemistry The University of ManchesterManchester M139PL Advanced Light Source Lawrence Berkeley National LaboratoryBerkeleyCA 94720

Instant recognition and quantification of multicomponent organicmixtures,especially the oneswith similar characteristics,remains a key challenge in the chemical *** luminescence sensing is considered a rapid and facile method for the detection of various chemical substances,the simultaneous and quantitative detection of three or more components has not yet been ***,we report a rationally designed white-light-emitting metal–organic framework(MOF)EuTb@NKU-102,and demonstrate its application in the simultaneous discrimination of multicomponent organic mixtures.

关键词： multicenter emission multicomponent mixture isomer sensing material metal–organic framework

稀土金属-有机框架在同分异构体传感材料中的应用

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中国稀土学报 2021年第1期39卷 110-127页

作者：韩宗甦师唯程鹏南开大学化学学院天津300071

基于稀土金属离子独特的电子结构,稀土金属-有机框架的光致发光具有发射峰尖锐、量子产率高和发光寿命长等特点,可应用于针对特定功能化学物种的光学传感材料。稀土金属离子高的配位数和丰富的配位模式,使得稀土金属-有机框架具有结构... 详细信息

基于稀土金属离子独特的电子结构,稀土金属-有机框架的光致发光具有发射峰尖锐、量子产率高和发光寿命长等特点,可应用于针对特定功能化学物种的光学传感材料。稀土金属离子高的配位数和丰富的配位模式,使得稀土金属-有机框架具有结构多样性和可调性,可与不同的化学物种在结构和能级两个方面相匹配,是其具有传感功能的基础。关于同分异构体的识别,尤其是针对同类同分异构体的快速识别,在化工和制药等领域均具有重要的价值。本文综述了稀土金属-有机框架针对具有特定功能同分异构体的传感性质,并讨论了其相关传感机制。

关键词：稀土金属-有机框架同分异构体传感材料

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手性金属-有机框架的设计、合成及应用

化学学报 2020年第12期78卷 1336-1348页

作者：陈中杭韩宗甦师唯程鹏南开大学化学学院

手性金属-有机框架具有框架结构多样性和功能可调性等特点,在对映异构体的识别与分离和不对称催化等领域中具有重要的应用.近年来,关于手性金属-有机框架的应用还扩展到其它研究领域,如在圆偏振荧光和手性铁电体等方面的研究中.与非手... 详细信息

手性金属-有机框架具有框架结构多样性和功能可调性等特点,在对映异构体的识别与分离和不对称催化等领域中具有重要的应用.近年来,关于手性金属-有机框架的应用还扩展到其它研究领域,如在圆偏振荧光和手性铁电体等方面的研究中.与非手性金属-有机框架相比,手性金属-有机框架的设计不但要考虑手性的引入途径,还要考虑其结晶与纯化,因此在合成上相对困难.本综述论述了三种构筑手性金属-有机框架的有效策略,包括直接利用手性配体合成、非手性配体的自发拆分或手性模板诱导合成和非手性金属-有机框架的手性化.对近年来手性金属-有机框架在手性分子识别、对映异构体分离、不对称催化、圆偏振荧光以及手性铁电体等方面的研究进展进行了讨论.

关键词：手性金属-有机框架设计与合成性质

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一个基于偶氮六酸的稀土金属-有机框架

高等学校化学学报 2022年第1期43卷 16-21页

作者：韩宗甦于晓泳闵辉师唯程鹏南开大学化学学院天津300071

采用1,2,3-三羧基-(1′,2′,3′-三羧基偶氮苯)-苯(H_(6)TTAB)连接线性四核铕配位单元,组装形成具有{4^(14)·6^(20)·8^(11)}{4^(3)}_(2){4^(5)·6}拓扑结构的稀土金属-有机框架***-TTAB具有高的热和溶剂稳定性,在紫外光激发下具有发... 详细信息

采用1,2,3-三羧基-(1′,2′,3′-三羧基偶氮苯)-苯(H_(6)TTAB)连接线性四核铕配位单元,组装形成具有{4^(14)·6^(20)·8^(11)}{4^(3)}_(2){4^(5)·6}拓扑结构的稀土金属-有机框架***-TTAB具有高的热和溶剂稳定性,在紫外光激发下具有发光性质,且其发光性能可以被铽离子调控并被银离子大幅度提升.

关键词：稀土金属-有机框架发光性质

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发光稀土配合物的生物功能分子传感研究进展

中国稀土学报 2023年第3期41卷 476-496,I0003页

作者：孙天凯闵辉韩宗甦师唯南开大学化学学院天津300071

基于稀土离子独特的电子组态和有机配体的敏化作用,稀土中心发光的配合物具有发光寿命长、发射峰尖锐和Stokes位移大等特点,可在复杂环境中针对特定的分析物进行快速和便捷的检测。稀土配合物与生物功能分子如生命必需分子、疾病标志物... 详细信息

基于稀土离子独特的电子组态和有机配体的敏化作用,稀土中心发光的配合物具有发光寿命长、发射峰尖锐和Stokes位移大等特点,可在复杂环境中针对特定的分析物进行快速和便捷的检测。稀土配合物与生物功能分子如生命必需分子、疾病标志物分子和药物分子等相互作用引起其光学信息的变化可以实现对生物功能分子的快速传感,在监测生命体的生理状态和公共卫生安全等方面具有重要的意义。本文综述了稀土配合物针对生物功能分子的传感性质研究进展,讨论了设计稀土配合物材料的传感策略,提出了稀土配合物作为生物功能分子先进传感材料的发展建议。

关键词：稀土配合物生物功能分子传感材料