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Boosting Fischer-Tropsch Synthesis via Tuning of N Dopants in TiO_(2)@CN-Supported Ru Catalysts

Transactions of Tianjin University 2024年第1期30卷 90-102页

作者： Xincheng Li Yunhao Liu Dejian Zhao Shuaishuai Lyu Jingwei Ye Xiaoshen Li Peipei Wu Ye Tian Yingtian Zhang Tong Ding Song Song Qingpeng Cheng Xingang Li State Key Laboratory of Chemical Engineering Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Haihe Laboratory of Sustainable Chemical TransformationsTianjin Key Laboratory of Applied Catalysis Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Zhejiang institute of Tianjin University Shaoxing 312300China Sinopec research institute of Petroleum Processing Co. LTDBeijing 100083China Physical Sciences and Engineering Division Advanced Membranes and Porous Materials(AMPM)CenterKing Abdullah University of Science and Technology(KAUST)23955-6900 ThuwalSaudi Arabia

Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)*** regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru ***,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic *** addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed ***,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain ***,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%.

关键词： Fischer-Tropsch synthesis N-doped carbon materials Ruthenium catalyst Pyridinic N Metal-N interaction

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Li-air batteries:air stability of lithium metal anodes

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Science China Chemistry 2024年第1期67卷 122-136页

作者： Renfei Cao Kai Chen Jianwei Liu Gang Huang Wanqiang Liu Xinbo Zhang School of materials Science and Engineering Changchun University of Science and TechnologyChangchun 130022China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChangchun 130022China

Aprotic rechargeable lithium-air batteries(LABs)with an ultrahigh theoretical energy density(3,500 Wh kg^(-1))are known as the‘holy grail’of energy storage systems and could replace Li-ion batteries as the next-generation high-capacity batteries if a practical device could be ***,only a few researches focus on the battery performance and reactions in the ambient air environment,which is a major obstacle to promote the practical application of ***,we have summarized the recent research progress on LABs,especially with respect to the Li metal *** chemical and electrochemical deteriorations of the Li metal anode under the ambient air are discussed in detail,and the parasitic reactions involving the cathode and electrolyte during the charge-discharge processes are *** also provide stability perspectives on protecting the Li metal anodes and propose design principles for realizing high-performance LABs.

关键词： parasitic reaction lithium metal anode anode protection Li-air batteries

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Lattice Boltzmann simulation study of anode degradation in solid oxide fuel cells during the initial aging process

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International Journal of Minerals,Metallurgy and materials 2024年第2期31卷 405-411页

作者： Shixue Liu Zhijing Liu Shuxing Zhang Hao Wu Hydrogen Energy Industrial Technology Innovation Center China Nuclear Power Technology Research InstituteShenzhen 518031China Shenzhen Engineering research Center for Hydrogen Safety Shenzhen 518031China

For present solid oxide fuel cells(SOFCs),rapid performance degradation is observed in the initial aging process,and the dis-cussion of the degradation mechanism necessitates quantitative ***,focused ion beam-scanning electron microscopy was em-ployed to characterize and reconstruct the ceramic microstructures of SOFC *** lattice Boltzmann method(LBM)simulation of multiphysical and electrochemical processes in the reconstructed models was *** samples collected from industrial-size cells were characterized,including a reduced reference cell and a cell with an initial aging *** parameters of the reconstructed microstructures revealed a significant decrease in the active triple-phase boundary and Ni connectivity in the aged cell compared with the reference *** LBM simulation revealed that activity degradation is dominant compared with microstructural degradation during the initial aging process,and the electrochemical reactions spread to the support layer in the aged *** microstructural and activity de-gradations are attributed to Ni migration and coarsening.

关键词： solid oxide fuel cell anode degradation focused ion beam-scanning electron microscopy lattice Boltzmann method

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调控动态生长过程以构筑嵌段可换和光谱可调的有机异质结构

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Science China materials 2024年第7期67卷 2153-2160页

作者：赵帅许超飞余悦夏星宇王磊王雪东廖良生 Jiangsu Key Laboratory for Carbon-Based Functional materials&Devices Institute of Functional Nano&Soft Materials(FUNSOM)Soochow UniversitySuzhou 215123China Macao institute of materials Science and Engineering Macao University of Science and TechnologyMacao 999078China

与单一结构相比,有机嵌段异质结构具有特殊的光电性能.然而,有机分子间的相互作用主导了异质结构构建单元的生长顺序,如有机单元A、B会自发形成BAB型结构而不是相反的ABA型结构,不能可控生长.在此,我们提出了次序结晶工程,结合晶种逐步... 详细信息

与单一结构相比,有机嵌段异质结构具有特殊的光电性能.然而,有机分子间的相互作用主导了异质结构构建单元的生长顺序,如有机单元A、B会自发形成BAB型结构而不是相反的ABA型结构,不能可控生长.在此,我们提出了次序结晶工程,结合晶种逐步自组装,控制共晶R与共晶N在彼此的两端纵向外延生长,从而精确合成具有可逆嵌段构型的有机嵌段异质结构:RNR和***有机嵌段异质结构,由于其逐渐掺杂的异质结而表现出渐变色的发射和波导特性,而NRN有机嵌段异质结构由于其明显的构筑异质结界限而表现出纯双色发射和波导特性.本工作实现了有机嵌段异质结构中嵌段块的有序可控生长,为未来光子学发展提供了制备合理复杂有机嵌段异质结构的途径.

关键词： organic heterostructure charge transfer cocrystal crystallization optical waveguide

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Theory,technology and application of grouted bolting in soft rock roadways of deep coal mines

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International Journal of Minerals,Metallurgy and materials 2024年第7期31卷 1463-1479页

作者： Hongpu Kang Jianwei Yang Pengfei Jiang Fuqiang Gao Wenzhou Li Jiafeng Li Huiyuan Chen Coal Mining research institute China Coal Technology and Engineering Group Co.Ltd.Beijing 100013China Coal Mining Branch China Coal Research InstituteBeijing 100013China State Key Laboratory of Intelligent Mining and Strata Control Beijing 100013China

The grouted bolt,combining rock bolting with grouting techniques,provides an effective solution for controlling the surrounding rock in deep soft rock and fractured *** has been extensively applied in numerous deep mining areas characterized by soft rock roadways,where it has demonstrated remarkable control *** article systematically explores the evolution of grouted bolting,covering its theoretical foundations,design methods,materials,construction processes,monitoring measures,and methods for assessing its *** overview encompassed several key elements,delving into anchoring theory and grouting reinforcement *** new principle of high pretensioned high-pressure splitting grouted bolting collaborative active control is introduced.A fresh method for dynamic information design is also *** discussion touches on both conventional grouting rock bolts and cable bolts,as well as innovative grouted rock bolts and cables characterized by their high pretension,strength,and sealing hole *** examination of the merits and demerits of standard inorganic and organic grouting materials versus the new inorganic–organic composite materials,including their specific application conditions,was ***,the article presents various methods and instruments to assess the support effect of grouting rock bolts,cable bolts,and grouting ***,it provides a foundation for understanding the factors influencing decisions on grouted bolting timing,the sequence of grouting,the pressure applied,the volume of grout used,and the strategic arrangement of grouted rock bolts and cable *** application of the high pretensioned high-pressure splitting grouted bolting collaborative control technology in a typical kilometer-deep soft rock mine in China—the soft coal seam and soft rock roadway in the Kouzidong coal mine,Huainan coal mining area,was ***,the existing problems in grouted bolting control

关键词： deep coal mine soft rock roadway grouted bolting rock bolt and cable grouting material high-pressure splitting grouting collaborative control technology

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Direct recycling of Li-ion batteries from cell to pack level:Challenges and prospects on technology,scalability,sustainability,and economics

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Carbon Energy 2024年第6期6卷 1-39页

作者： Joseph Jegan Roy Do Minh Phuong Vivek Verma Richa Chaudhary Michael Carboni Daniel Meyer Bin Cao Madhavi Srinivasan Energy research institute@NTU(ERI@N) SCARCE LaboratoryNanyang Technological UniversitySingaporeSingapore School of materials Science and Engineering Nanyang Technological UniversitySingaporeSingapore CEA CNRSENSCMUniversity of MontpellierUMR 5257(ICSM)Bagnols-sur-Cèze CedexFrance School of Civil and Environmental Engineering Nanyang Technological UniversitySingaporeSingapore

Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent *** primary objective of directly recycling LIBs is to efficiently recover and restore the active electrode materials and other components in the solid phase while retaining electrochemical *** technology's advantages over traditional pyrometallurgy and hydrometallurgy are costeffectiveness,energy efficiency,and sustainability,and it preserves the material structure and morphology and can shorten the overall recycling *** review extensively discusses the advancements in the direct recycling of LIBs,including battery sorting,pretreatment processes,separation of cathode and anode materials,and regeneration and quality enhancement of electrode *** encompasses various approaches to successfully regenerate high-value electrode materials and streamlining the recovery process without compromising their electrochemical ***,we highlight key challenges in direct recycling when scaled from lab to industries in four perspectives:(1)battery design,(2)disassembling,(3)electrode delamination,and(4)commercialization and *** on these challenges and changing market trends,a few strategies are discussed to aid direct recycling efforts,such as binders,electrolyte selection,and alternative battery designs;and recent transitions and technological advancements in the battery industry are presented.

关键词： battery design cathode regeneration direct recycling graphite recycling lithium-ion battery,scaling-up

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Quantum-mechanical effects in photoluminescence from thin crystalline gold films

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Light(Science & Applications) 2024年第4期13卷 783-794页

作者： Alan R.Bowman Alvaro Rodríguez Echarri Fatemeh Kiani Fadil Iyikanat Ted V.Tsoulos Joel D.Cox Ravishankar Sundararaman F.Javier García de Abajo Giulia Tagliabue Laboratory of Nanoscience for Energy Technologies(LNET) STIÉcole Polytechnique Fédérale de Lausanne(EPFL)LausanneSwitzerland ICFO–Institut de Ciencies Fotoniques The Barcelona Institute of Science and TechnologyCastelldefels(Barcelona)Spain. MBI–Max-Born-Institut BerlinGermany. POLIMA–Center for Polariton-driven Light–Matter Interactions University of Southern DenmarkOdense MDenmark. Danish institute for advanced Study University of Southern DenmarkOdense MDenmark. Department of materials Science&Engineering Rensselaer Polytechnic InstituteTroyNYUSA. Department of Physics Applied Physicsand AstronomyRensselaer Polytechnic InstituteTroyNYUSA. ICREA–Institucio Catalana de Recerca i Estudis Avancats BarcelonaSpain

Luminescence constitutes a unique source of insight into hot carrier processes in metals,including those in plasmonic nanostructures used for sensing and energy ***,being weak in nature,metal luminescence remains poorly understood,its microscopic origin strongly debated,and its potential for unraveling nanoscale carrier dynamics largely ***,we reveal quantum-mechanical effects in the luminescence emanating from thin monocrystalline gold ***,we present experimental evidence,supported by first-principles simulations,to demonstrate its photoluminescence origin(i.e.,radiative emission from electron/hole recombination)when exciting in the interband *** model allows us to identify changes to the measured gold luminescence due to quantum-mechanical effects as the gold film thickness is ***,such effects are observable in the luminescence signal from flakes up to 40 nm in thickness,associated with the out-of-plane discreteness of the electronic band structure near the Fermi *** qualitatively reproduce the observations with first-principles modeling,thus establishing a unified description of luminescence in gold monocrystalline flakes and enabling its widespread application as a probe of carrier dynamics and light-matter interactions in this *** study paves the way for future explorations of hot carriers and charge-transfer dynamics in a multitude of material systems.

关键词： luminescence quantum crystalline

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Asymmetric Cu Sites for Enhanced CO_(2)Electroreduction to C_(2+)Products

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CCS Chemistry 2024年第5期6卷 1231-1239页

作者： Weiwei Guo Xingxing Tan Shunhan Jia Shoujie Liu Xinning Song Xiaodong Ma Limin Wu Lirong Zheng Xiaofu Sun Buxing Han Beijing National Laboratory for Molecular Sciences Key Laboratory of Colloid and Interface and ThermodynamicsCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190 institute of Molecular Metrology College of Chemistry and Chemical EngineeringQingdao UniversityQingdao 266071 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 School of materials Science and Engineering Anhui UniversityHefei 230601 institute of High Energy Physics Chinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green Chemistry and Chemical processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062

Cu-based electrocatalysts can have excellent activity for the generation of C_(2+)products from a CO_(2)reduction reaction(CO_(2)RR).Cuδ+species is crucial in tuning the performance of the ***,we discovered that Si-doped Cu catalysts had excellent performance for electrochemical CO_(2)to C_(2+)products.A high Faradaic efficiency(FE)of 84.7%was achieved with a current density of 289mA cm^(−2)in the flow-cell *** situ experimental results showed that the significant reconstruction occurred during the electrolysis,resulting in the formation of the asymmetric Cu sites(Cu^(0)-Cu^(+)).The ratio of Cu^(0)and Cu^(+)could be tuned by changing Si *** experiments and theoretical calculations demonstrated that the asymmetric Cu sites caused by the appropriate Si doping promoted CO_(2)activation and strengthened the adsorption of^(*)CO *** was beneficial to the subsequent^(*)CO–^(*)CO dimerization step,and thus,accounted for the enhancement of C_(2+)selectivity.

关键词： carbon dioxide electrocatalysis asymmetric Cu sites C-C coupling green chemistry

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Progress in in-situ electrochemical nuclear magnetic resonance for battery research

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Magnetic Resonance Letters 2024年第2期4卷 13-21页

作者： Yong Jiang Mengmeng Zhao Zhangquan Peng Guiming Zhong Laboratory of advanced Spectro-electrochemistry and Li-ion Batteries Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China University of Chinese Academy of Sciences Beijing100049China Tianmu Lake institute of advanced Energy Storage Technologies Co. Ltd.Liyang213300China

A thorough understanding of the fundamental electrochemical and chemical processes in batteries is crucial to advancing energy density and power ***,the characterizations of such processes are ***-situ electrochemical nuclear magnetic resonance(EC-NMR)offers the capability to collect real-time data during battery operation,furnishing insights into the local structures and ionic dynamics of materials by monitoring changes in the chemical environment around the ***-NMR also has the advantages of being both quantitative and *** paper systematically reviews the design of EC-NMR approach,and delves into the applications and progress of EC-NMR concerning battery reaction mechanisms,failure mechanisms,and overall battery *** review culminates in a comprehensive summary of the perspective and challenges associated with EC-NMR.

关键词： In-situ NMR Reaction mechanism Failure mechanism Battery systems Ionic dynamics

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Anodic Electrosynthesis of Amide from Alcohol and Ammonia

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CCS Chemistry 2024年第1期6卷 125-136页

作者： Yuxuan Lu Yingying Li Bo Zhou Jingcheng Wu Ling Zhou Yuping Pan Zhongcheng Xia Ming Yang Yandong Wu Zhenran Yuan Rixin Peng Zhijie Kong Shuangyin Wang Yuqin Zou State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082 Shenzhen institute of Hunan University Shenzhen 518057 School of Chemistry and Chemical Engineering Jishou UniversityJishouHunan 416000

Amide is essential in biologically active compounds,synthetic materials,and building ***,conventional amide production relies on energyintensive consumption and activating agents that modulate processes to construct the C–N ***,for the first time,we have successfully realized the formation of amides at industrial current density via the anodic coelectrolysis of alcohol and ammonia under ambient *** have proved thatmodulation of the interface microenvironment concentration of nucleophile by electrolyte engineering can regulate the reaction pathways of amides rather than acetic *** C-N coupling strategy can be further extended to the electrosynthesis of the long-chain and aryl-ring amide with high selectivity by replacing ammonia with *** work opens up a vast store of information on the utilization of biomass alcohol for high-value N-containing chemicals via an electrocatalytic C-N coupling reaction.

关键词： electrocatalysis electrocatalysts biomass upgrading elctrochemical oxidation coupling amide production

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