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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 anticipated.In this study,a formal[3+2]method,through the reactions of an osmapentalyne with benzyl carbanions,was developed.The reactions underwent a nucleophilic attack of carbanions to the Os≡C bond,followed by C—H activation to form the five-membered osmacyclopentadiene ring.Most 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 complexes.This 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

Experimental and theoretical evidences for the formation of transition metal complexes with five coplanar metal–carbon σ bonds

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National Science Review 2023年第12期10卷 174-180页

作者： Yuhui Hua Ming Luo Zhengyu Lu Hong Zhang Dafa Chen haiping xia Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis Department of ChemistrySouthern University of Science and Technology Department of Chemistry College of Chemistry and Chemical EngineeringXiamen University

The σ bond is an important concept in chemistry, and the metal–carbon(M–C) σ bond in particular is a central feature in organometallic chemistry. Synthesis of stable complexes with five coplanar M–C σ bonds is challenging. Here, we describe the synthesis of two different types of stable complexes with five coplanar M–C σ bonds, and examine the stability of such complexes which use rigid conjugated carbon chains to chelate with the metal center. Density functional theory(DFT) calculations show that the M–C σ bonds in these complexes have primarily a covalent character. Besides the σ nature, there are also a π conjugation component among the metal center and carbons, which causes delocalization. This work expanded the coplanar M–C σ bonds to five.

关键词： M–C bond polydentate ligands metallaaromatics DFT calculations aromaticity

Synergistic Optimization of Buried Interface by Multifunctional Organic-Inorganic Complexes for Highly Efficient Planar Perovskite Solar Cells

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Nano-Micro Letters 2023年第9期15卷 505-519页

作者： Heng Liu Zhengyu Lu Weihai Zhang Hongkang Zhou Yu xia Yueqing Shi Junwei Wang Rui Chen haiping xia Hsing-Lin Wang School of Materials Science and Engineering Harbin Institute of TechnologyHarbin 150001People’s Republic of China Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055GuangdongPeople’s Republic of China Shenzhen Grubbs Institute and Department of Chemistry Southern University of Science and TechnologyShenzhen 518055GuangdongPeople’s Republic of China Department of Electrical and Electronic Engineering Southern University of Science and TechnologyShenzhen 518055GuangdongPeople’s Republic of China Key University Laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of Guangdong Southern University of Science and TechnologyShenzhen 518055GuangdongPeople’s Republic of China

For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is challenging to effectively optimize this interface as it is buried beneath the perovskite film.Herein,we have designed and synthesized a series of multifunctional organic-inorganic(OI)complexes as buried interfacial material to promote electron extraction,as well as the crystal growth of the perovskite.The OI complex with BF4−group not only eliminates oxygen vacancies on the SnO_(2) surface but also balances energy level alignment between SnO_(2) and perovskite,providing a favorable environment for charge carrier extraction.Moreover,OI complex with amine(−NH_(2))functional group can regulate the crystallization of the perovskite film via interaction with PbI2,resulting in highly crystallized perovskite film with large grains and low defect density.Consequently,with rational molecular design,the PSCs with optimal OI complex buried interface layer which contains both BF4−and−NH_(2) functional groups yield a champion device efficiency of 23.69%.More importantly,the resulting unencapsulated device performs excellent ambient stability,maintaining over 90%of its initial efficiency after 2000 h storage,and excellent light stability of 91.5%remaining PCE in the maximum power point tracking measurement(under continuous 100 mW cm−2 light illumination in N2 atmosphere)after 500 h.

关键词： Perovskite solar cells Organic Inorganic complexes Multifunctional interfacial material Buried interface layer

Formal[2+1]Cycloadditions of a Metallacyclopentadiene Unit with Alkynes:Constructing Tetracyclic Conjugated Frameworks with Bridgehead Metals

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Chinese Journal of Chemistry 2023年第16期41卷 1987-1993页

作者： Zhenwei Chu Jinhua Li Dafa Chen Zhengyu Lu Weiran Meng Ming Luo haiping xia Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenGuangdong 518055China

Comprehensive Summary Metallacyclopentadienes play a vital role in transition-metal mediated and catalyzed cycloaddition reactions of alkynes.Though versatile reactions of metallacyclopentadienes with alkynes have been disclosed,[2+1]cycloadditions of metallacyclopentadienes and alkynes have never been discovered.In present work,we report the formal[2+1]cycloadditions of a metallacyclopentadiene unit with a broad scope of commercial alkynes,providing a facile strategy to construct tetracyclic conjugated compounds.The deuterated experiment indicates a metal vinylidene intermediate has been involved in[2+1]cycloaddition.Moreover,the electrophilic substitution reaction of the tetracyclic conjugated compound with the aid of density functional theory(DFT)calculated Fukui functions is investigated.

关键词： Metallacycle Cycloaddition Alkynes Electrophilic substitution Conjugation

A One-Pot Strategy for the Synthesis of β-Substituted Rhoda-and Irida-Carbolong Complexes

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Chinese Journal of Chemistry 2022年第15期40卷 1777-1784页

作者： Binbin Xu Wei Mao Chengcheng Wu Jinhua Li Zhengyu Lu Ming Luo Liu Leo Liu Lingling Mao Dafa Chen haiping xia Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenGuangdong 518055China

Comprehensive Summary Starting from an organic multiyne,three steps are normally needed for the preparation of non-βphosphonium functionalized rhodaand irida-carbolong complexes.Herein,a one-pot strategy,by mixing a multiyne,a nucleophile,and Rhcl(CO)(PPh_(3))_(2)/AgBF_(4)or[Ir(CH:CN)(CO)(PPh_(3))_(2)]BF_(4),was developed to achieve a series ofβfunctionalized rhoda-and irida-carbolong complexes.Theβ-substituents in these complexes can be various C-,N-and O-centered groups,dependent on the nucleophiles used.This strategy provides a new convenient route to construct carbolong complexes,which is important for the further development of carbolong chemistry.

关键词： Carbolong chemistry Metallacycles Rhodium Iridium Tridentate ligands

Metallafurans and their synthetic chemistry

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Science Bulletin 2016年第6期61卷 430-442页

作者： Guomei He Jiangxi Chen haiping xia Key Laboratory of High Performance Ceramic Fibers ofMinistry of Education Department of Materials Science and Engineering College of Materials Xiamen University State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University

Based on isolobal analogy,the definition of metallafuran was described and its synthetic chemistry was briefly summarized.In the structure of furan,when one of CH groups was replaced by an isolobal metal fragment ML n(M=metal;L=ligand),the corresponding organometallic complex was called metallafuran,which should be two possible isomers called a-metallafuran(metal fragment at a-carbon of original furan)and b-metallafuran(metal fragment at b-carbon of original furan).As an organometallic complex,a-metallafuran has two resonant forms:one can be viewed as carbonyl coordinated vinyl metal complex and the other can be viewed as alkoxymetal carbene.Therefore,a-metallafuran was also called chelated vinyl ketone metal complex or oxametallacyclopentadiene in the early literatures.For synthesis of metallafurans,a-metallafurans were very common and easily prepared,for example,from alkynes insertion into acyl metal complexes and so on.While there were rare examples reported for b-metallafurans.In this mini review,the synthetic chemistry of metallafuran was mainly focused on its formation mechanism.

关键词：合成化学有机金属配合物等瓣相似乙烯酮呋喃异构体基团配体

Metallaaromatics Containing Main-group Heteroatoms

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Chinese Journal of Chemistry 2018年第2期36卷 93-105页

作者： Hongjian Wang xiaoxi Zhou haiping xia College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China

Metallaaromatics are metallacycles that are derived from the formal replacement of a carbon atom in the framework of organic aromatics with a metal fragment. As an important subclass of metallaaromatics, metallaaromatics that contain main-group heteroatoms have attracted considera- ble attention. In the past ten years, we have developed several new methods to construct metallaaromatics as well as those containing main-group het- eroatoms, such as metallapyridine, metallapyridinium, metallapyridyne, metallafuran, metallabenzothiazole, metallabenzoxazole, metallabenzthiophene, aza-metallapentalene and some novel tricyclic/tetracyclic metallaaromatics. In addition, interesting reactions such as the first hetero-Diels Aider reaction between 1-metalla-1,3-dienes and nitriles, the first intramolecular nucleophilic aromatic substitution （SNAr） reaction of metallabenzene, and the first iodine-mediated electrophilic cyclizations of a metallabenzene complex were demonstrated. In this account, recent and novel approaches for their synthesis and property analyses are summarized. The structural diversity and unique properties of metallaaromatics containing main-group heteroatoms will strongly inspire further investigation of these species and provide a wide range of potential applications.

关键词： metallacycles aromatic heteroatom fused ring synthesis

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 issue.Here,we developed a versatile interfacial heating membrane with alternating utilization of electricity or solar energy for hypersaline water treat-ment.This hierarchical membrane functions both as a separation membrane and an interface heater,which can quickly(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

Photoluminescence properties of Tm^(3+)/Tb^(3+)/Sm^(3+) tri-doped Na_(5)Y_(9)F_(32) single crystal with high thermal stability for white light-emitting diodes

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Journal of Rare Earths 2021年第5期39卷 512-519页

作者： Yang Qiao Xiong Zhou Jianli Zhang haiping xia Hongwei Song Baojiu Chen Key Laboratory of Photo-electronic Materials Ningbo UniversityNingbo 315211China State Key Laboratory on Integrated Optoelectronics College of Electronic Science and Engineering and College of PhysicsJilin UniversityChangchun 130012China Department of Physics Dalian Maritime UniversityDalian 116026China

A novel Tm^(3+)/Tb^(3+)/Sm^(3+)tri-doped Na_(5)Y_(9)F_(32)single crystal was synthesized by a modified Bridgman method for the propose of white light emitting diodes.The fluorescence spectra of various Sm^(3+)ion concentrations and fixed 0.4 mol%Tm^(3+)and 0.5 mol%Tb^(3+)were measured and studied systematically excited by near-ultraviolet light of 355 nm.The Sm3+ion concentration takes apparent effect on the relative intensity of peaks in the visible region and the color coordinate combining from these emission bands.A near pure white light emission with color coordinates(0.3295,0.3057)and color temperature(5657 K)can be obtained when the concentrations of Tm^(3+),Tb^(3+)and Sm^(3+)ions are 0.4 mol%,0.5 mol%and 0.8 mol%,respectively.Furthermore,the practical down-conversion internal quantum yield was measured by integrating spheres at about 14.39%.The tri-doped Na_(5)Y_(9)F_(32)single crystal shows a high thermal stability inferring from the temperature dependent emission in which the integrated emission intensities are reduced only by^3%with the increase of temperature from 280 to 450 K.The present results demonstrate that the Tm^(3+)/Tb^(3+)/Sm^(3+)tri-doped Na_(5)Y_(9)F_(32)single crystal may provide a promising candidate for white light-emitting diodes,luminescent materials and fluorescent display devices.

关键词： Na_(5)Y_(9)F_(32)single crystal Tm^(3+)/Tb^(3+)/Sm^(3+) Bridgman method White light emission Rare earths

White Light Emission Characteristics of Tb3+/Sm3+Co-Doped Glass Ceramics Containing YPO4 Nanocrystals

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Journal of Materials Science & Technology 2017年第5期33卷 432-437页

作者： Zhixiong Zhang Yuepin Zhang Cheng Wang Zhigang Feng Weihuan Zhang haiping xia Key Laboratory of Photo-electronic Materials Ningbo UniversityNingbo 315211China

The Tb3＋/Sm3＋ single-doped and co-doped glasses and glass ceramics containing YPO4 nanocrystals have been synthesized by melt quenching method. The structural and luminescent properties of these glass specimens were investigated. Under 375 nm wavelength excitation, the emission spectra combined with blue, green and red bands were observed, which achieved the white light emission. Moreover, the energy transfer between Tb3＋ and Sm3＋ ions was validated by decay lifetime measurement and energy level diagram. The color coordinates （x = 0.333, y = 0.333）, correlated color temperature （5595 K） and the color render- ing index （Ra = 80.5） indicated that the glass ceramics were considered to be good lighting source. Hence, the YPO4-based Tb3＋/Sm3＋ co-doped glass ceramics can act as potential matrix materials for white light- emitting diodes under ultraviolet excitation.

关键词： Glass ceramicsYPO4 Tb3＋/Sm3＋ co-dopedLuminescent propertiesWhite light-emitting diodes