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Construction of a Metallacyclopentadiene Ring through the Attack of Carbanions to M≡C Bond Followed by C—H Activation

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Chinese Journal of chemistry 2024年第3期42卷 235-242页

作者： Chun Tang Shengjie zhang Zhengyu Lu Qian Li ming luo Dafa Chen haiping xia state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringCollaborative Innovation Center of Chemistry for Energy MaterialsXiamen UniversityXiamenFujian361005 China Shenzhen Grubbs Institute and Guangdong Provincial key laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenGuangdong518055 China

Metallacyclopentadienes are important metallacycles and regarded as intermediates in many reactions,therefore,new methods to achieve them are *** this study,a formal[3+2]method,through the reactions of an osmapentalyne with benzyl carbanions,was *** reactions underwent a nucleophilic attack of carbanions to the Os≡C bond,followed by C—H activation to form the five-membered osmacyclopentadiene *** of the reactions were carried out at room temperature,the substituents on the aromatic rings of benzyl carbanions are diverse,and the resulting products contain an Os—H bond,representing a novel type of 10C-carbolong *** work provides a new convenient route to construct metallacyclopentadienes,which is expected to further promote the development of such a type of substances.

关键词： Metallacyclopentadiene Carbolong chemistry Osmium C–H activation Nucleophilic addition

General strategy for evaluating the d-band center shift and ethanol oxidation reaction pathway towards Pt-based electrocatalysts

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Science China chemistry 2023年第1期66卷 279-288页

作者： Jin-hong Zheng Guang Li Jun-ming zhang Ningyan Cheng Li-Fei Ji Jian Yang Jialin zhang Bin-Wei zhang Yan-xia Jiang Shi-Gang Sun state key laboratory of physical chemistry of solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing 400044China key laboratory of Magnetic Molecules&Magnetic Information Materials Ministry of Education School of Chemical and Material ScienceShanxi Normal UniversityTaiyuan 030031China Information Materials and Intelligent Sensing laboratory of Anhui Province Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information TechnologyAnhui UniversityHefei 230039China

The catalytic performance of Pt-based catalysts depends sensitively on their d-band ***,there are still huge challenges to evaluate their d-band centers from experimental technologies,and modulate them to analyze their selectivity in ethanol oxidation reaction(EOR).Here,Pt1Au1alloy supported on the commercial carbon material(Pt_(1)Au_(1)/C)is employed as a typical example to investigate its d-band center shift of surface Pt,and as electrocatalysts to study its selectivity towards ***,a highly reliable in situ Fourier-transform infrared spectroscopy CO-probe strategy is developed to characterize the d-band center shift of surface *** modified electronic effect and site effect of Pt_(1)Au_(1)/C dictated the adsorption configuration of intermediate species and the OH species coverage,thereby influencing its *** importantly,we developed a universal cyclic voltammetry peak differentiation fitting method as an electrochemical analysis technique to investigate CO_(2)selectivity,which is potentially extendable to other Pt-based electrocatalysts.

关键词： PtAu in situ FTIRS d-band center ethanol oxidation reaction CV peak differentiation fitting method

Alternative photothermal/electrothermal hierarchical membrane for hypersaline water treatment

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SusMat 2022年第6期2卷 679-688页

作者： Miao Wang Wen He Yuhui Hua Xinwen Xie Shiyan Chen Lei Zhou Yunmao zhang Yaqi Hou Shihong lin haiping xia Jing Zheng Xu Hou state key laboratory of physical chemistry of solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenChina College of Materials Xiamen UniversityXiamenChina Research Institute for Biomimetics and Soft Matter Fujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamenChina Shenzhen Grubbs Institute and Guangdong Provincial key laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenChina Collaborative Innovation Center of chemistry for Energy Materials(iChEM) Xiamen UniversityXiamenChina Department of Civil and Environmental Engineering Vanderbilt UniversityNashvilleTennesseeUSA Interdisciplinary Material Science Program Vanderbilt UniversityNashvilleTennesseeUSA Tan Kah Kee Innovation laboratory Xiamen UniversityXiamenChina Engineering Research Center of Electrochemical Technologies of Ministry of Education Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenChina

Over the last decades,the treatment of the large quantities of hypersaline wastewater generated by conventional industries,inland desalination,and fossil-fueled power plants has been an important economic issue and also an inescapable green ***,we developed a versatile interfacial heating membrane with alternating utilization of electricity or solar energy for hypersaline water *** hierarchical membrane functions both as a separation membrane and an interface heater,which can quickly(line *** 10wt% hyper-saline water,the freshwater production rate can reach 16.8kg/m^(2)⋅h by applying a voltage of 10 V and 1.36 kg/m^(2)⋅h under 1-sun ***,it exhibits high electrochemical resistance to corrosion and therefore remains stable tack-ling hypersaline water(>5 wt%),with a high salt rejection rate of 99.99%.This system shows an efficient desalination strategy that can provide fresh water from brines for agriculture and industry,and even for daily life.

关键词： carbon nanotubes electrothermal hypersaline water treatment interface evaporate pho-tothermal

Syntheses,Crystal Structures and Properties of Two New Zn Based Boron Imidazolate Frameworks

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Chinese Journal of Structural chemistry 2021年第7期40卷 865-870,838页

作者： BI ming-Yue WEN Yi-Hang zhang Hai-xia zhang Jian Zhejiang key laboratory for Reactive chemistry on solid surfaces Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China state key laboratory of Structural chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Two new boron imidazolate frameworks(BIFs),Zn2[HBH(2-mim)3]2(1,2-PEA)2(EG)2(BIF-120,EG=ethylene glycol)and Zn[BH(2-mim)3](1,2-HPEA)(BIF-121),were successfully synthesized by mixing the KBH(2-mim)3 ligand and the semirigid aromatic dicarboxylate ligand 1,2-benzenediacetic acid(1,2-H2PEA)under solvothermal *** this paper,the two samples were structurally characterized by single-crystal X-ray diffraction and tested by infrared spectroscopy(IR),UV-visible spectroscopy(UV-Vis),thermogravimetric analysis TGA and X-ray powder *** addition,the solid-state luminescent properties of these crystals were also investigated.

关键词： boron imidazolate frameworks crystal structure X-ray crystallography luminescent

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纯碳链与过渡金属的螯合化学

厦门大学学报（自然科学版） 2020年第5期59卷 864-878页

作者：郑雪娟张弘夏海平厦门大学化学化工学院固体表面物理化学国家重点实验室能源材料化学协同创新中心福建厦门361005

碳-金属键的形成与断裂是金属有机化学的核心问题,也是金属参与各种有机化学反应的关键步骤.然而,传统的金属有机化合物多数不稳定且合成条件苛刻,制约了碳-金属键构建的相关研究.近10多年来,夏海平团队始终致力于在一个金属中心上构筑... 详细信息

碳-金属键的形成与断裂是金属有机化学的核心问题,也是金属参与各种有机化学反应的关键步骤.然而,传统的金属有机化合物多数不稳定且合成条件苛刻,制约了碳-金属键构建的相关研究.近10多年来,夏海平团队始终致力于在一个金属中心上构筑尽可能多的碳-金属σ键,发现了一系列全新的芳香性金属杂环结构基元,逐步建立了“碳龙化学”.本文主要对一系列含2~5个碳-金属σ键的金属杂环化合物进行综述.

关键词：金属杂环化合物碳龙化学多齿配体碳-金属σ键

调控Pt_(3)Zn合金化程度改善酸性氧还原活性与稳定性

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电化学 2022年第4期28卷 19-29页

作者：张天恩颜雅妮张俊明瞿希铭黎燕荣姜艳霞厦门大学化学化工学院固体表面物理化学国家重点实验室福建厦门361005

Pt基催化剂是氧还原反应的优良催化剂,改善其活性和稳定性是燃料电池商业化的关键。本文利用金属有机框架衍生的氮掺杂碳材料为载体,通过浸渍、冻干和简单热处理的方法合成了Pt/NC、Pt3Zn/NC-L和Pt3Zn/NC-H催化剂,平均粒径均在2 nm左右... 详细信息

Pt基催化剂是氧还原反应的优良催化剂,改善其活性和稳定性是燃料电池商业化的关键。本文利用金属有机框架衍生的氮掺杂碳材料为载体,通过浸渍、冻干和简单热处理的方法合成了Pt/NC、Pt3Zn/NC-L和Pt3Zn/NC-H催化剂,平均粒径均在2 nm左右。在Pt中引入Zn元素引起其晶格收缩,使Pt-Pt键变短,优化了Pt与含氧中间体的结合,增强氧还原反应的活性。在高合金化程度的Pt3Zn/NC-H催化剂上,氧还原反应的半波电位为0.903 V,较商业Pt/C正移57 mV。0.9 V下的质量活性和面积比活性分别是商业Pt/C的4.50倍和3.33倍。在O2饱和的0.1 mol·L^(-1) HClO4溶液,0.6~1.0 V(***)进行10000周稳定性测试,商业Pt/C的质量活性和面积比活性分别衰减25.00%和23.80%,而在Pt3Zn/NC-H催化剂上未观察到衰减。

关键词：金属有机框架氮碳载体电催化剂 Pt_(3)Zn合金氧还原反应