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Photoinduced copper-catalyzed alkoxyl radical-triggered ring-expansion/aminocarbonylation cascade

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Chinese Chemical Letters 2024年第6期35卷 331-336页

作者： Jing-Qi Tao Shuai Liu Tian-Yu Zhang Hong Xin Xu Yang Xin-Hua Duan Li-Na Guo Department of chemistry School of ChemistryXi’an Key Laboratory of Sustainable Energy Material Chemistry and Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an 710049China School of Electrical Engineering Xi’an Jiaotong UniversityXi’an 710049China State Key Laboratory of Applied Organic chemistry Lanzhou UniversityLanzhou 730000China

A photoinduced copper-catalyzed alkoxyl triggered C-C bond cleavage/aminocarbonylation cascade is presented.Through adjusting the structure of alkoxyl radical precursors,functionalized lactones and ketoamides were synthesized with good yields and excellent functional group tolerance under redox-neutral conditions.Notably,this protocol enables the integration of lactone fragments with many amine drugs and drug fragments.

关键词： Copper catalysis Ring-expansion Aminocarbonylatioin Macrolactones Keto-amides

Stabilizing perovskite precursors with the reductive natural amino acid for printable mesoscopic perovskite solar cells

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Journal of energy chemistry 2024年第3期90卷 32-39,I0003页

作者： Wenjing Hu Jian Yang Chuang Yang Xufeng Xiao Chaoyang Wang Zhaozhen Cui Qiaojiao Gao Jianhang Qi Minghao Xia Yaqiong Su Anyi Mei Hongwei Han Michael Gratzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for OptoelectronicsKey Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Huazhong University of Science and TechnologyWuhan 430074HubeiChina School of chemistry Xi'an Key Laboratory of Sustainable Energy Materials ChemistryState Key Laboratory of Electrical Insulation and Power EquipmentXi'an Jiaotong UniversityXi'an 710049ShaanxiChina

Solution processability significantly advances the development of highly-efficient perovskite solar cells.However,the precursor solution tends to undergo irreversible degradation reactions,impairing the device performance and reproducibility.Here,we utilize a reductive natural amino acid,Nacetylcysteine(NALC),to stabilize the precursor solution for printable carbon-based hole-conductorfree mesoscopic perovskite solar cells.We find that I_(2) can be generated in the aged solution containing methylammonium iodide(MI) in an inert atmosphere and speed up the MA-FA^(+)(formamidinium) reaction which produces large-size cations and hinders the formation of perovskite phase.NALC effectively stabilizes the precursor via its sulfhydryl group which reduces I_(2) back to I^(-)and provides H^(+).The NALC-stabilized precursor which is aged for 1440 h leads to devices with a power conversion efficiency equivalent to 98% of that for devices prepared with the fresh precursor.Furthermore,NALC improves the device power conversion efficiency from 16.16% to 18.41% along with enhanced stability under atmospheric conditions by modifying grain boundaries in perovskite films and reducing associated defects.

关键词： Perovskite solar cells Perovskite precursor Degradation Stabilization Reductive natural amino acid

Lone pair-π interaction induced regioselective sulfonation of ethers under light irradiation

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Green Synthesis and Catalysis

Green Synthesis and Catalysis 2024年第2期5卷 117-121页

作者： Chonglong He Min Wang Bowu Dong Yaqiong Su Xin-Hua Duan Le Liu School of chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi'an Key Laboratory of Sustainable Energy Material ChemistryXi’an Jiaotong UniversityXi’an 710049China

Non-covalent interactions are of significance in supramolecular chemistry and biochemistry,while synthetic procedures driven by these weak interactions remain challenging and rare.Inspired by the lone pair-π interaction presence in the Z-DNA structure,a light-induced regioselective sulfonation of ethers taking advantage of the lone pair-π interaction between the oxygen of ethers and sulfonyl chlorides has been disclosed.Moreover,this strategy is also applicable to the sulfonation of aniline derivatives.Features of the methods include readily accessible starting materials,high atom-economy,green and photocatalyst-free conditions and broad functional group tolerance.Mechanism studies suggest that the lone pair-πinteraction plays an important role to initiate the transformation.

关键词： Non-covalent interactions Lone-pair-πinteractions Sulfonyl radical Photocatalysis Ethers

Single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates

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Carbon energy 2024年第3期6卷 64-117页

作者： Karl Adrian Gandionco Juwon Kim Lieven Bekaert Annick Hubin Jongwoo Lim Department of chemistry Seoul National UniversitySeoulRepublic of Korea Research group Electrochemical and Surface Engineering(SURF) Department of Materials and ChemistryVrije Universiteit BrusselBrusselsBelgium

The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.

关键词： electrocatalysis electrochemical CO_(2)reduction hydrocarbons oxygenates single-atom catalysts

Selective nickel-electrocatalyzed benzylic C-H oxygenation of functionalized alkyl arenes

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Chinese Chemical Letters 2024年第2期35卷 396-401页

作者： Shunyao Tang Siyi Wang Dongmei Zhang Xinxing Zhang Guang Yang Yanwei Wang Youai Qiu State Key Laboratory of Elemento-Organic chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin 300071China College of chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Renewable Energy Conversion and Storage Center (RECAST)Frontiers Science Center for New Organic MatterNankai UniversityTianjin 300071China

Herein, a site-selective paired electrochemical C–H oxidation of functionalized alkyl arenes promoted by nickel catalyst is disclosed. A Ni(Ⅱ)-dioxygen species formed in situ efficiently enable the oxidation process under mild conditions with a broad substrate scope with excellent functional group compatibilities,such as free carboxylic acid, aldehyde, halogen(including aryl iodide), amide and amino acid. The use of the nickel catalyst in combination with water provides a safe, green and economical method for oxidation of a range of molecules varying in complexity and drug derivatives, demonstrating its potential application in organic synthesis and the pharmaceutical industry. Reaction outcomes and mechanistic studies revealed the key role of the in situ Ni(Ⅱ)-dioxygen species for the subsequent oxidation of C(sp^(3))–H bonds,and short-lived reactive intermediates(aryl radical cation) was rapidly captured by the combination of a bipolar ultramicroelectrode(BUME) with nano-electrospray ionization mass spectrometry.

关键词： Electrochemical C-H oxidation Functionalized alkyl arenes Paired nickel-electrocatalysis H_(2)O oxidation Ketones

Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of Environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao Institute of Catalysis for energy and Environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high photosensitivity.This study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) clusters.To further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and NO.Meanwhile,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate complexes.The H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/mol.The calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational results.Interestingly,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) clusters.Comparison indicted that the chemisorptions of aldehyde oxygen have largest energies.The results suggested adsorption conformations have a respectable impact on the catalysis barrier.This study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

Optical responses of metallic plasmonic arrays under the localized excitation

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Nano Research 2024年第3期17卷 1571-1577页

作者： Sen Yan Hao Ma Yi-Fan Bao Maofeng Cao Chuan Liu Kaifeng Zhang Xiaowei Wu Jianbo He Xiang Wang Bin Ren State Key Laboratory of Physical chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation Laboratory for Sciences and Technologies of energy Materials of Fujian Province(IKKEM) Xiamen 361005China Research&Development group HitachiLtd.Yokohama 244-0817KanagawaJapan Department of Electronic Science and Engineering Kyoto UniversityKyoto 615-8510Japan

The metallic plasmonic array that can support both propagating surface plasmon polaritons(PSPPs)and localized surface plasmon resonance(LSPR)possesses rich optical properties and remarkable optical performance,making it a powerful platform for applications in photonics,chemistry,and materials.For practical applications,the excitation spot is usually smaller than the area of metal arrays.It is thus imperative to address“how many array units are enough?”towards a rational design of plasmonic nanostructures.Herein,we employed focused ion beam(FIB)to precisely fabricate a series of plasmonic array structures with increased unit number.By utilizing photoluminescence(PL)and surface-enhanced Raman spectroscopy(SERS),we found that the array units outside the excitation spot still have a significant impact on the optical response within the spot.Combined with the numerical simulation,we found that the boundary of the finite array leads to the loss of PSPP outside the excitation point,which subsequently affects the coupling of PSPP and LSPR in the excitation spot,leading to variations in PL and SERS intensity.Based on the findings,we further tuned the LSPR mode of the metal arrays by electrodeposition to obtain strong near-field enhancement without any influence on the PSPP mode.This work advances the understanding of near-field and far-field optical behavior in finite-size array structures and provides guidance for designing highly-efficient photonic devices.

关键词： plasmonic periodic array finite-size effects dark field scattering surface-enhanced Raman spectroscopy(SERS)

Selective photocatalytic oxidation of methane to C1 oxygenates by regulating sizes and facets over Au/ZnO

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Nano Research 2024年第5期17卷 3810-3818页

作者： Qiang Zhou Xinyu Wang Xiaojie Tan Qinhua Zhang Hao Yang Tao Xing Mingqing Wang Mingbo Wu Wenting Wu State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical Engineering&Institute of New EnergyChina University of Petroleum(East China)Qingdao 266580China National Engineering Research Center of Coal Gasification and Coal-Based Advanced Materials ShanDong Energy Group CO.LTDJinan 250101China

Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions,nevertheless confronting great challenges in efficiently activating C-H bonds and inhibiting over-oxidation.Herein,we propose a comprehensive strategy for the selective generation of reactive oxygen species(ROS)by regulating the sizes and facets of Au nanoparticles loaded on ZnO.For photocatalytic methane oxidation at ambient temperature,a high oxygenates yield of 36.4 mmol·g^(-1)·h^(-1) with a nearly 100%selectivity has been achieved over the optimized 1.0%Au/ZnO-9.6(1%Au with(111)facet and 9.6 nm size on ZnO)photocatalyst,exceeding most reported literatures.Mechanism investigations reveal that 1.0%Au/ZnO-9.6 with the medium size and Au(111)facet guarantees the favourable formation of superoxide radicals(·OOH)through mild oxygen reduction,ultimately leading to excellent photocatalytic methane oxidation performance.This work provides some guidance for the delicate design of photocatalysts for efficient photocatalytic methane oxidation and oxygen utilization.

关键词： photocatalysis methane oxidation radical regulation oxygen activation nanomaterial

Apically guiding electron/mass transfer reaction induced by Ag/FeNx Mott-Schottky effect within a hollow star reactor toward high performance zinc-air batteries

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Journal of energy chemistry 2024年第8期95卷 106-116页

作者： Kaixiang Shi Kaixin Wang Tong Li Junhao Li Jie Ren Xu Li Yonggang Min Zhouguang Lu Wei Tan Quanbing Liu Guangdong Provincial Laboratory of chemistry and Fine Chemical Engineering Jieyang Center(Rongjiang Laboratory) Guangdong University of Technology Guangzhou Key Laboratory of Clean Transportation energy chemistry Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology Key Laboratory of Electrochemical energy Storage and energy Conversion of Hainan Province School of Chemistry and Chemical Engineering Hainan Normal University School of Materials and energy Guangdong University of Technology Department of Materials Science and Engineering Southern University of Science and Technology

The disparity in the transfer of carriers（electrons/mass） during the reaction in zinc-air batteries（ZABs）results in sluggish kinetics of the oxygen reduction reaction（ORR） and oxygen evolution reaction（OER）,along with elevated overpotentials,thereby imposing additional constraints on its utilization.Therefore,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently needed.In this work,an apically guiding dual-functional electrocatalyst（Ag-FeNx-N-C） was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional（3D） hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride（FeNx） nanoparticles.Theoretical calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeNx,of which electron accumulation in the FeNxphase region and electron depletion in the Ag phase region promote orientated-guiding charge migration.The effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/OER.Additionally,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass transfer.Experimental results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm-2.A rechargeable ZAB with Ag-FeNx-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles（500 h）,with a power density of 180 mW cm-2.Moreover,when employing AgFeNx-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm-2.Ag-FeNx-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the exploration prospects of ZABs.

关键词： Apically guiding effect Bifunctional catalysis Hollow star structure Mott-Schottky effect Zinc-air batteries