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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

A case study of comparing two dimerized acceptor molecules built by different branch-connected and terminal-connected approaches

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Science China chemistry 2024年第5期67卷 1687-1696页

作者： Kangqiao Ma Huazhe Liang Yuxin Wang Tengfei He Tainan Duan Xiaodong Si Wendi Shi Guankui Long Xiangjian Cao Zhaoyang Yao Xiangjian Wan Chenxi Li Bin Kan Yongsheng Chen State Key Laboratory and institute of Elemento-Organic chemistry Frontiers Science Center for New Organic MatterThe Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsInstitute of Polymer ChemistryRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China School of Materials Science and Engineering National Institute for Advanced MaterialsRenewable Energy Conversion and Storage Center(RECAST)Nankai UniversityTianjin 300350China Chongqing institute of Green and Intelligent Technology Chongqing SchoolUniversity of Chinese Academy of Sciences(UCAS Chongqing)Chinese Academy of SciencesChongqing 400015China

Dimerized small-molecule acceptors(SMAs) built by the conventional connection of terminal groups of monomers have contributed to exciting long-term stabilities of organic solar cells(OSCs). However, device efficiencies, especially fill factors(FFs), still need to be improved. This probably originates from unsymmetrical molecular structure/conformation-determined less compact/ordered molecular stackings, such as ineffective stackings of constraint terminals. Herein, an exotic dimerized SMA of BC-Th is established by bridging the branched groups(BC-type, branch coupling) of two monomers rather than conventional terminal units(TC-type, terminal coupling). Benefiting from the three-dimensional conformation and more uncurbed terminals,BC-Th exhibits multiple molecular orientations along with a larger dielectric constant and electron mobility compared with TCTh. Finally, an efficiency of 17.43% is achieved by BC-Th-based OSCs, along with the highest FF of 79.13% among all dimerized SMAs-based OSCs to date. When introducing L8-BO as the third component, overall enhanced efficiency of 18.05%and FF of 80.11% are further afforded. Contrarily, TC-Th-based OSCs exhibit much inferior PCE of 16.29% and FF of 74.81%,demonstrating the great advantages of “branch coupling” over “terminal coupling” when building dimerized SMAs.

关键词： organic solar cells dimerized acceptor molecules branch coupling morphology control stability

Dual-functional POM@IL complex modulate hole transport layer properties and interfacial charge dynamics for highly efficient and stable perovskite solar cells

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Chinese Chemical Letters 2024年第7期35卷 461-464页

作者： Boyuan Hu Jian Zhang Yulin Yang Yayu Dong Jiaqi Wang Wei Wang Kaifeng Lin Debin Xia MIIT Key Laboratory of Critical Materials Technology for New energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China

The severe interfacial charge recombination as well as the stability issues brought by the Li-TFSI still hinder the commercialization of high-performance perovskite solar cells(PSCs).Here,a polyoxometalates(POMs)-based complex,POM@ionic liquid(IL),is synthesized and applied as an effective additive that simultaneously enhances the performance and stability of *** interactions between POM@IL complex and Li-TFSI inhibit the aggregation of *** synergistic oxidation of POM@IL complex and Li-TFSI towards 2,2,7,7-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene(Spiro-OMeTAD)effectively enhances the electrical properties of hole transport layer film and the photovoltaic performances of *** champion device modified with the POM@IL complex yields an excellent power conversion efficiency(PCE)of 22.73%.Moreover,the incorporation of POM@IL improves the humidity stability of *** storing under high humidity conditions(25℃,60%RH)for 1200 h,the POM@IL modified device retained a remarkable 81.2%of its initial *** work provides new insight into constructing POMs-based materials for high-performance photovoltaic devices.

关键词： Polyoxometalates Ionic liquid Perovskite solar cells energy alignment Humidity stability

Towards the insights into the deactivation behavior of acetylene hydrogenation catalyst

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Petroleum Science 2024年第2期21卷 1405-1414页

作者： Hai-Xia Su Yang Jiao Jian-Gong Shi Zhi-Wei Yuan Di Zhang Xu-Peng Wang Jing Ren Dan Liu Jian-Zhou Gui Hai-Yang Gao Xiao-Li Xu State Key Laboratory of Separation Membranes&Membrane processes Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringSchool of Material Science and EngineeringTiangong UniversityTianjin300387China institute of Engineering Technology Sinopec Catalyst Co.LtdBeijing101100China State Key Laboratory of Separation Membranes and Membrane processes Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringSchool of ChemistryTiangong UniversityTianjin300387China

A series of model catalysts were obtained by treating commercial fresh and spent catalysts unloaded from the factory with different methods, including green oil dipping, extraction and high-temperature regeneration;finally, the deactivation behavior of the commercial catalyst for acetylene hydrogenation were studied. The influence of various possible deactivation factors on the catalytic performance was elucidated via detailed structural characterization, surface composition analysis, and activity *** results showed that green oil, carbon deposit and sintering of active metal were the main reasons for deactivation, among which green oil and carbon deposit led to rapid deactivation, while the activity could be recovered after regeneration by high-temperature calcination. The sintering of active metal components was attributed to the high-temperature regeneration in hydrothermal conditions, which was slow but irreversible and accounted for permanent deactivation. Thus, optimizing the regeneration is expected to extend the service life of the commercial catalyst.

关键词： Acetylene Hydrogenation Green oil Carbon deposit Sintering Catalyst deactivation

Decarboxylative cyanation and thiocyanation via catalytic electron donor-acceptor complex with copper catalysis

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Science China chemistry 2024年第9期67卷 3019-3028页

作者： Hongping Zhao Xiaoxiang Xi Tianbao Wu Zimin Chen Minyan Wang Weiming Yuan Key Laboratory of Material chemistry for energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Bioinorganic Chemistry and Materia MedicaSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074China State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China Shenzhen Huazhong University of Science and Technology Research institute Shenzhen 518000China

A new catalytic decarboxylative cyanation and thiocyanation via a synergistic Na I/Cu catalysis is *** photoexcited electron donor-acceptor complex by assembly of Na I,R3P,and N-acyloxy-phthalimide ester(NHPI ester)triggers the generation of alkyl radical species,which then engages in Cu-catalyzed radical coupling *** to success of this dual catalytic transformation is the reliable charge transfer between I·and Cu(I).This dual catalytic platform can eliminate the use of expensive iridium-based photocatalyst or synthetically elaborate organic dyes.A series of primary,secondary,and tertiary alkyl nitriles and thiocyanates are easily ***,an asymmetric decarboxylative cyanation by applying a chiral Cu catalyst is also developed to afford chiral nitriles in high *** mechanistic details and the origin of the high enantioselectivity are further investigated by the mechanistic experiments and the density functional theory calculations.

关键词： electron donor-acceptor catalysis copper catalysis cyanation thiocyanation asymmetric synthesis

A new route towards polarized luminescence:0D/2D nanocomposites

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Light(Science & Applications) 2024年第2期13卷 175-177页

作者： Andries Meijerink Debye institute for Nanomaterials Science Department of ChemistryUtrecht UniversityPrincetonplein 13584CCUtrechtThe Netherlands School of Materials and energy Lanzhou UniversityLanzhouGansuChina

Combining wide bandgap 2D inorganic materials and blue-light-emitting 0D carbon dots in 0D/2D heterojunction nanocomposites was shown to give rise to unique optical properties and a multifunctional prototype device wa... 详细信息

关键词： polarized luminescence nanocomposites

Tuning electrochemical water activation over NiIr single-atom alloy aerogels for stable electrochemiluminescence

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Science Bulletin 2024年第15期69卷 2387-2394页

作者： Ling Ling Mengzhen Xi Hengjia Wang Runshi Xiao Lirong Zheng Liuyong Hu Wenling Gu Chengzhou Zhu State Key Laboratory of Green Pesticide International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079China Hubei Key Laboratory of Plasma chemistry and Advanced Materials Hubei Engineering Technology Research Center of Optoelectronic and New Energy MaterialsWuhan Institute of TechnologyWuhan 430205China institute of High energy Physics Chinese Academy of SciencesBeijing 100049China

The anodic oxygen evolution reaction is a well-acknowledged side reaction in traditional aqueous electrochemiluminescence(ECL) systems due to the generation and surface aggregation of oxygen at the electrode, which detrimentally impacts the stability and efficiency of ECL emission. However, the effect of reactive oxygen species generated during water oxidation on ECL luminophores has been largely overlooked. Taking the typical luminol emitter as an example, herein, we employed NiIr single-atom alloy aerogels possessing efficient water oxidation activity as a prototype co-reaction accelerator to elucidate the relationship between ECL behavior and water oxidation reaction kinetics for the first time. By regulating the concentration of hydroxide ions in the electrolyte, the electrochemical oxidation processes of both luminol and water are finely tuned. When the concentration of hydroxide ions in electrolyte is low,the kinetics of water oxidation is attenuated, which limits the generation of oxygen, effectively mitigates the influence of oxygen accumulation on the ECL strength, and offers a novel perspective for harnessing side reactions in ECL systems. Finally, a sensitive and stable sensor for antioxidant detection was constructed and applied to the practical sample detection.

关键词： Electrochemiluminescence Luminol Water activation Single-atom doping Sensing

Insight into demand-driven preparation of single-atomic mediators for lithium–sulfur batteries

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Journal of energy chemistry 2024年第3期90卷 205-219,I0007页

作者： Miaoyu Lu Yifan Ding Zaikun Xue Ziang Chen Yuhan Zou Jingyu Sun College of energy Soochow Institute for Energy and Materials InnovationsKey Laboratory for Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina Beijing Graphene institute Beijing 100095China

Lithium-sulfur(Li-S) batteries have attracted considerable attention as one of the most appealing energy storage *** efforts have been devoted to tackling the tremendous challenges,mainly pertaining to the severe shuttle effect,sluggish redox kinetics and lithium dendritic ***-atomic mediators as promising candidates exhibit impressive performance in addressing these intractable *** research often utilizes a trial-and-error approach,proposing solutions to fabricate single-atomic materials with diversified ***,comprehensive review articles especially targeting demand-driven preparation are still in a nascent *** by these considerations,this review summarizes the design of single-atomic mediators based on the application case-studies in LiS batteries and other metal-sulfur *** preparation routes represented by chemical vapor deposition technology are introduced in a demand-oriented ***,future research directions are proposed to foster the advancement of single-atomic mediators in Li-S realm.

关键词： Single-atom catalyst Lithium–sulfur battery Chemical vapor deposition Demand-driven preparation

Electrocatalytic performance of CNTs/graphene composited rare earth phthalocyanines(M=La,Y,Yb,Sc)

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Journal of Rare Earths 2024年第2期42卷 323-333,I0004页

作者： Tingting Jiang Caixia Ou Luyi Wang Jun Chen Sydorov Dmytro Qian Zhang Jintian Luo Hua Wang Jiangxi Key Laboratory of Power Batteries and Materials Faculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou341000China Joint Department of Electrochemical energy Systems Institute of Bioorganic Chemistry and PetrochemistryNational Academy of Sciences of Ukraine38A VernadskyAveKiev03142Ukraine Guangdong Jiana energy Technology Co. Ltd.Qingyuan511500China

In this study,a class of rare earth composite sandwich phthalocyanines(MPcs,M=La,Y,Yb,Sc) were prepared and compounded with graphene and carbon nanotubes to obtain MPc/Gr and MPc/CNTs *** electrocatalytic behaviors of MPc/Gr and MPc/CNTs electrodes were further *** results show that the central rare earth metal has a large influence on the electrocatalytic *** the MPcs/Gr samples,ScPc with the smallest ionic radius and molecular size can be more uniformly dispersed in graphene,and the hydrogen precipitation overpotential of ScPc/Gr electrode is514 mV,corresponding to a Tafel slope of 148 mV/dec,with better electrocatalytic performance than other rare earth metal *** for the MPc/CNTs composites,LaPc,which has the largest ionic radius and molecular size,is more uniformly dispersed on the surface of CNTs,so that the LaPc/CNT electrode exhibits the best LSV performance with the smallest corresponding Tafel slope(176 mV/dec).The main reason is the different binding modes of MPcs molecules in Gr and *** rare earth phthalocyanine is combined with layered graphene,the smallest size of rare earth phthalocyanine(ScPc)is more easily embedded in the graphene layer,resulting in better homogeneity of the composite,larger effective contact area and better electrocatalytic *** contrast,when rare earth phthalocyanine is bound to carbon nanotubes in a tubular structure,it is mainly bound by attaching to the surface or being entangled by the carbon *** this case,the rare-earth phthalocyanine molecules(LaPc)with larger layer spacing can provide more contact area with CNTs,forming a more uniform and effective composite,which eventually provides more active sites and better electrocatalytic performance.

关键词： Electrocatalysis Rare earth phthalocyanines Graphene(Gr) Carbon nanotubes(CNTs) Composite

Co-enhancement of thermal conduction and radiation through morphologies controlling of graphene functional layer for chip thermal management

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Nano Research 2024年第10期17卷 8885-8892页

作者： Shuting Cheng Kun Wang Shichen Xu Yi Cheng Ruojuan Liu Kewen Huang Hao Yuan Wenjuan Li Yuyao Yang Fushun Liang Fan Yang Kangyi Zheng Zhiwei Liang Ce Tu Mengxiong Liu Xiaomin Yang Jingnan Wang Xuzhao Gai Yuejie Zhao Xiaobai Wang Yue Qi Zhongfan Liu State Key Laboratory of Heavy Oil Processing College of ScienceChina University of PetroleumBeijing 102249China Centre for Nanochemistry Beijing Science and Engineering Centre for NanocarbonsBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing Graphene institute(BGI) Beijing 100095China College of energy Soochow Institute for Energy and Materials Innovations(SIEMIS)Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy TechnologiesSoochow UniversitySuzhou 215006China Department of chemistry College of Chemistry and Materials EngineeringBeijing Technology and Business UniversityBeijing 100048China

With the continuous advancements in electronics towards downsizing and integration,efficient thermal dissipation from chips has emerged as a critical factor affecting their lifespan and operational *** fan-less chip cooling system has two critical interfaces for thermal transport,which are the contact interface between the base and the chip dominated by thermal conduction,and the surface of the fins dominated by thermal *** different thermal transfer modes of these two critical interfaces pose different requirements for thermal management *** the study,a novel approach was proposed by developing graphene thermal transport functional material whose morphology could be intentionally designed via reformed plasmaenhanced chemical vapor deposition(PECVD)methods to meet the diverse requirements of heat transfer ***,graphene with multilevel branching structure of vertical graphene(BVG)was fabricated through the hydrogenassisted PECVD(H_(2)-PECVD)strategy,which contributed a high emissivity of~*** was deposited on the fins’surface and functioned as the radiation enhanced layer to facilitate the rapid radiation of heat from the heat sinks into the surrounding ***,the well-oriented vertical graphene(OVG)was successfully prepared through the vertical electric field-assisted PECVD process(EF-PECVD),which showed a high directional thermal conductivity of~53.5 W·m^(-1)·K^(-1).OVG was deposited on the contact interface and functioned as the thermal conduction enhanced layer,allowing for the quick transmission of heat from the chip to the heat *** this design concept,the two critical interfaces in the chip cooling system can be jointly enhanced,resulting in a remarkable cooling efficiency enhancement of~30.7%,demonstrating that this novel material possessed enormous potential for enhancing the performance of cooling ***,this research not only provided new design concepts for the cooling system

关键词： chip thermal management thermal conduction thermal radiation graphene morphology control