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Molecular engineering binuclear copper catalysts for selective CO_(2) reduction to C_(2) products

Journal of Energy chemistry 2024年第6期93卷 166-173,I0005页

作者： Qi Zhao Kai Lei Bao Yu Xia Rachel Crespo-Otero Devis Di Tommaso Department of chemistry School of Physical and Chemical SciencesQueen Mary University of LondonLondonE14NSUK Key laboratory of Material {1. for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureState Key Laboratory of Materials Processing and Die&Mould TechnologySchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074HubeiChina Department of chemistry University College LondonLondonWC1H 0AJUK Digital Environment Research Institute Queen Mary University of LondonEmpire HouseLondon E11HHUK

Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal *** investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular *** modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)*** findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R *** rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular *** placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) *** research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products.

关键词： Molecular catalyst design Selective CO_(2)reduction C_(2)products Density functional theory calculations

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Efficient and stable PtFe alloy catalyst for electrocatalytic methanol oxidation with high resistance to CO

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Journal of Energy chemistry 2024年第3期90卷 327-336,I0008页

作者： Qian Yang Sifan Zhang Fengshun Wu Lihua Zhu Guang Li Mingzhi Chen An Pei Yingliang Feng Jiangxi Provincial Key laboratory of Functional Molecular Materials {1. College of Chemistry and Chemical EngineeringFaculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou 341000JiangxiChina College of chemistry and Chemical Engineering Xiamen UniversityXiamen 361005FujianChina

Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in terms of surface CO toxicity in long-term ***,the PtFe alloy nanoparticles(NPs) with small particle size(~4.1. nm) supported on carbon black catalysts with different Pt/Fe atomic ratios(Pt_(1.Fe_(2)/C,Pt_(3)Fe_(4)/C,Pt_(1.Fe_(1./C,and Pt_(2)Fe_(1./C) are successfully prepared for enhanced anti-CO poisoning during methanol oxidation reaction(MOR).The optimal atomic ratio of Pt/Fe for the MOR is 1.2,and the mass activity of Pt_(1.Fe_(2)/C(5.40 A mg_(Pt)^(-1.) is 1..5 times higher than that of conventional commercial Pt/C(Pt/C-JM)(0.40 A mg_(Pt)^(-1.).The introduction of Fe into the Pt lattice forms the PtFe alloy phase,and the electron density of Pt is reduced after forming the PtFe ***-situ Fourier transform infrared results indicate that the addition of oxyphilic metal Fe has reduced the adsorption of reactant molecules on Pt during the *** doping of Fe atoms helps to desorb toxic intermediates and regenerate Pt active sites,promoting the cleavage of C-O bonds with good selectivity of CO_(2)(58.1.).Moreover,the Pt_(1.Fe_(2)/C catalyst exhibits higher CO tolerance,methanol electrooxidation activity,and long-term stability than other Pt_(x)Fe_(y)/C catalysts.

关键词： Alloy catalyst PtFe Methanol oxidation In-situ FTIR CO resistance

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Interface engineering enabled sintering-resistant metal nanocatalysts via reverse Ostwald ripening

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Science China chemistry 2024年第9期67卷 2789-2791页

作者： Ying Sun Wenhui Fang Jieshan Qiu Institute of Clean Energy chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning ProvinceCollege of ChemistryLiaoning UniversityShenyang 110036China State Key laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

The design and fabrication of advanced nanocatalysts with the high activity,selectivity,and superior durability remains a big challenge in industrial catalysis[1.2].The sintering of nanocatalysts under the thermally and/or chemically triggered conditions is a bottle-neck issue,which seriously decreases the amount of the exposed active sites and changes the original electronic structure of catalysts,resulting in the irreversible catalyst deactivation and high capital and time cost in industrial operation[3].

关键词： durability irreversible catalysis

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Advancing microarray fabrication:One-pot synthesis and highresolution patterning of UV-crosslinkable perovskite quantum dots

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Nano Research 2024年第9期17卷 8600-8609页

作者： Linfeng Yuan Dejian Chen Kun He Jiamin Xu Kunyuan Xu Jie Hu Sisi Liang Haomiao Zhu CAS Key laboratory of Design and {1. of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation laboratory for Optoelectronic Information of China Fuzhou 350108China University of Chinese Academy of Sciences Beijing 100049China College of chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Xiamen Key laboratory of Rare Earth Photoelectric Functional Materials Xiamen Research Center of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021China

The development of highly efficient,solution-processable,and environmentally stable perovskite quantum dots(PQDs)is crucial for their accurate high-resolution patterning and subsequently enabling the practical deployment of PQD based emissive display *** study presents an innovative strategy for integrating all-inorganic PQDs and ultraviolet(UV)crosslinkable acrylate polymer at a structural and functional *** achievement is accomplished by meticulous design and one-pot synthesis of UV-crosslinkable CsPbX_(3)(X=Cl,Br,I)PQDs solution,which exhibit outstanding environmental *** the solution-processable characteristics of the resulting UV-crosslinkable PQDs,precise patterning of high-resolution(2μm,7608 pixels·in.^(-1.)and colorful PQDs microarrays can be readily achieved through inkjet printing and high-throughput photolithography(~2μm in pitch line/space patterning).The UV cross-linked process guarantees a homogeneous distribution of PQDs,effectively mitigating coffee ring effect and improving the overall quality of stereoscopic *** photo-cured PQDs film,which undergoes free radical photopolymerization,displays an impressive photoluminescence quantum yield(PL QY)of up to 89.2%,reaching 98%of the value observed in the solution *** approach outlined in this research is both cost-effective and pragmatic,exhibiting tremendous promise for diverse system-level integrated optoelectronic devices,such as ultra-high-resolution micro-light-emitting device(micro-LED)displays.

关键词： perovskite quantum dots microarrays cross-linking strategy Inkjet printing photolithography

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Anionic covalent organic framework electrolyte with tailored ion channels for high-areal-capacity solid-state lithium metal battery

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Science China chemistry 2024年

作者： Xu Zhuang Yangdan Hui Yangyang Feng Jiajie Chen Junlan Chen Yaobing Wang College of chemistry Institute of Molecular Engineering Plus Fuzhou University CAS Key laboratory of Design and {1. of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsState Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fujian College University of Chinese Academy of Sciences University of Chinese Academy of Sciences Fujian Science and Technology Innovation laboratory for Optoelectronic Information of China

Covalent organic frameworks（COFs） are an emerging class for solid-state electrolytes due to their ordered and customizable ion transport nanochannels. Although high ionic conductivity(σLi+) and Li+transference number(tLi+) are achieved, the high-arealcapacity solid-state lithium metal battery（LMB） still encountered challenges, which is mainly determined by homogeneous Li+flux through channels and interfaces. Herein, we design a COF coupling anionic skeletons with branched ion-conductive chains（COF-S） as tailored fast ion-transport channels to achieve high-areal-capacity solid-state LMB. Then the dispersed COF-S-based electrolyte is further obtained by incorporating ethoxylated trimethylolpropane triacrylate（ETPTA） and LiFSI（ETPTA-COF-S）via in situ light solidification. In this way, the abundant SO-3groups promote Li+adsorption and facilitate axial transport via 1. channels, thus enabling high σLi+of 1.29 mS cm-1.nd tLi+of 0.83. The branched chains can tailor ion channels to suppress largesize anions transport, disperse and uniform Li+flux, thus leading to high average Coulombic efficiency（CE） up to 98.43 % for1.0 cycles（～800 h） at 0.5 mA cm-2under the high areal capacity of 2 mAh cm-2. When paired with 2 mAh cm-2LiFePO4（LFP）cathode and thin Li anode of 20 μm, Li||ETPTA-COF-S||LFP exhibits superior cyclic stability for 80 cycles.

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Rational design of new in situ reduction of Ni(II)catalytic system for low-cost and large-scale preparation of porous aromatic frameworks

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Carbon Energy 2024年第5期6卷 105-113页

作者： Shanshan Wang Yue Wu Wenxiang Zhang Hao Ren Guangshan Zhu Heping Ma School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anChina State Key laboratory of Inorganic Synthesis and Preparative {1. College of ChemistryJilin UniversityChangchunChina College of chemistry Northeast Normal UniversityChangchunChina

Porous aromatic framework 1.PAF-1.is an extremely representative nanoporous organic framework owing to its high stability and exceptionally high surface ***,the synthesis of PAF-1.is catalyzed by the Ni(COD)2/COD/bpy system,suffering from great instability and high ***,we developed an in situ reduction of the Ni(II)catalytic system to synthesize PAF-1.in low cost and high *** active Ni(0)species produced from the NiCl_(2)/bpy/NaI/Mg catalyst system can effectively catalyze homocoupling of tetrakis(4-bromophenyl)methane at the room temperature to form PAF-1.with high Brunauer-Emmett-Teller(BET)-specific surface area up to 4948 m^(2) g^(−1.(Langmuir surface area,6785 m2 g−1..The possible halogen exchange and dehalogenation coupling mechanisms for this new catalytic process in PAF's synthesis are discussed in *** efficiency and universality of this innovative catalyst system have also been demonstrated in other PAFs'*** work provides a cheap,facile,and efficient method for scalable synthesis of PAFs and explores their application for high-pressure storage of Xe and Kr.

关键词： adsorption carbon material nickel catalysis porous aromatic framework porous organic polymer

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Copper/Photoredox-Catalyzed Regioselective 1.4-Addition to 1.3-Enynes: A Convenient Access to Perfluoroalkylated Allenes

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Chinese Journal of chemistry 2024年第17期42卷 2023-2028页

作者： Ya Chen Quanyuan Wang Keyi Peng Lilei Cheng Ziyi She Guo-Jun Deng Key laboratory for Green Organic Synthesis and Application of Hunan Province Key Laboratory of EnvironmentallyFriendly Chemistry andApplication of Ministryof EducationCollege of ChemistryXiangtan UniversityXiangtanHunan 411105China Department School of chemistry and Chemical Engineering Henan Normal UniversityXinxiangHenan 453007China

A general and broadly applicable copper and photoredox dual-catalyzed multicomponent 1.4-perfluoroalkylcyanation of 1.3-enynes has been *** protocol enjoys success with high regioselectivity,mild reaction conditions,and excellent functional-group tolerance,allowing the facile synthesis of structurally diverse perfluoroalkylated allenes from readily available fluoroalkyl halides,1.3-enynes and TMscN in a one-pot manner.A reasonable mechanism has been proposed according to a series of control experiments.

关键词： Fluorinated allenes 1 3-Enynes Photoredox Fluoroalkylation Multicomponent reactions Difunctionalization Radicals Regioselectivity

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Enhancing blocking temperature using inverse hydrogen bonds for non-radical bridged dimeric Dy(Ⅲ)single-molecule magnets

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Science China chemistry 2024年第10期67卷 3328-3338页

作者： Peng-Bo Jin Qian-Cheng Luo Ye-Ye Liu Yan-Zhen Zheng Frontier Institute of Science and Technology State Key Laboratory of Electrical Insulation and Power EquipmentMOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed MatterXi’an Key Laboratory of Electronic Devices and Material Chemistry and School of ChemistryXi’an Jiaotong UniversityXi’an 710054China

Single-molecule magnets(SMMs)are a kind of nanosized magnetic materials that are capable of storing massive bytes of *** coupling the spin centers in a proper manner is a usual approach to promote the working temperature(or blocking temperature)for *** delocalized radicals have been widely employed to accomplish this ***,we show a new manner by using weak but multiple B–H^(δ-)···Dy^(3+)inverse hydrogen bonding(IHB)interactions to control the magnetic couplings in a series of dimeric dysprosiacaborane *** approach leads to a record high T_(B)^(1.0s)of 1. K among non-radical bridged dimeric SMMs,which is mainly ascribed to strong ferromagnetic coupling(4.38 cm^(-1.)and the proper alignment of the magnetic principle axes of the adjacent dysprosium(Ⅲ)*** verifying by theoretical calculations,these results demonstrate that IHB interactions can be used to construct strong axial ferromagnetic coupling and enhancing magnetic blocking temperature for SMMs.

关键词： single-molecule magnets carborane dysprosium ferromagnetic coupling inverse hydrogen bond

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Enhancing the deep-red/near-infrared fluorescence of higher rylene diimides via the chalcogen-annulation strategy

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Science China chemistry 2024年第4期67卷 1324-1333页

作者： Kai Chen Xiao Chen Ke Hu Yilun Zhao Yujian Liu Guogang Liu Jinquan Chen Wei Jiang Zhigang Shuai Da-Hui Qu Zhaohui Wang Key laboratory for Advanced Materials and Joint International Research laboratory of Precision chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Key laboratory of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China State Key laboratory of Precision Spectroscopy East China Normal University500 Dongchuan RoadShanghai 200241China

Deep-red/near-infrared fluorescence is highly suitable for bioimaging owing to its ability to deeply penetrate tissues,organs,and live ***,developing organic fluorophores with high deep-red/near-infrared fluorescence quantum yield(Φ_(FL))and fluorescent brightness remain a significant challenge owing to the energy gap ***,we developed a straightforward and effective chalcogen-annulation strategy by introducing O,S and Se into the bay region of TDI and QDI fluorophores,realizing the increase ofΦFLand fluorescent brightness up to 1. *** our best knowledge,this study potentially stands as the pioneering instance showcasing the anti-heavy-atom effect of chalcogens,and the absoluteΦFL(93%)and fluorescent brightness(1.8,200 cm^(-1.mol^(-1.L)of Se-TDI is among top deep-red/near-infrared organic fluorophores currently *** femtosecond transient absorption(fs-TA)measurements show the absence of obvious changes of the excited state lifetime after the introduction of chalcogens in TDI and QDI fluorophores,indicating that intersystem crossing(ISC)can be neglected in TDI and QDI *** calculations further reveal the chalcogen-annulation strategy increase the radiative rates and reduce the reorganization energy of several accepting modes at the ground state in TDI fluorophores,leading to the suppression of internal conversion(IC)*** chalcogen-annulation strategy,which effectively increases the Φ_(FL)and restricts the IC processes,while remaining unaffected by the heavy-atom effect,offers novel insights and theoretical support for the design and synthesis of deep-red/near-infrared organic fluorophores with high Φ_(FL)and fluorescent brightness.

关键词： π-extended rylene diimides chalcogen-annulation strategy deep-red/near-infrared fluorescence

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The 2^(nd)Asian Conference on Porphyrins,Phthalocyanines and Related Materials

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Chinese Chemical Letters 2024年第7期35卷 1-3页

作者： Gaojie Zhu Zhen Yang Shijun Li Weihua Zhu Rui Cao Junlong Zhang Jianzhang Zhao Jonathan L.Sessler Xunjin Zhu Jianxin Song Yongshu Xie Jianzhuang Jiang Key laboratory for Advanced Materials and Institute of Fine Chemicals School of Chemistry and Molecular EngineeringEast China University of Science&TechnologyShanghai 200237China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material Technology of Ministry of EducationHangzhou Normal UniversityHangzhou 311121China School of chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China Key laboratory of Applied Surface and Colloid {1. Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an 710119China Beijing National laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China State Key laboratory of Fine Chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China Department of chemistry The University of TexasAustinTexas 78712-1224United States Department of chemistry and Institute of Advanced Materials Hong Kong Baptist UniversityHong Kong 999077China Key laboratory of Chemical Biology and Traditional Chinese Medicine(Ministry of Educational of China) Key Laboratory of the Assembly and Application of Organic Functional Molecules of Hunan ProvinceCollege of Chemistry and Chemical EngineeringHunan Normal UniversityChangsha 410081China Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

In the past decades,porphyrins,phthalocyanines and related materials have attracted significant attention due to their diverse and brilliant structures[1.2],as well as their unique electronic structures and photophysi... 详细信息

关键词： cyanine phthalocyanine Porphyrin

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