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Effect of reduction pretreatment on the structure and catalytic performance of Ir-In_(2)O_(3)catalysts for CO_(2) hydrogenation to methanol

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Journal of Environmental Sciences 2024年第6期140卷 2-11页

作者： Changyu Ding Feifei Yang Xue Ye Chongya Yang Xiaoyan Liu Yuanlong Tan Zheng Shen Hongmin Duan Xiong Su Yanqiang Huang CAS Key Laboratory of Science and Technology on Applied catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

In_(2)O_(3)has been found a promising application in CO_(2)hydrogenation to methanol,which is beneficial to the utilization of CO_(2).The oxygen vacancy(O_(v))site is identified as the catalytic active center of this ***,there remains a great challenge to understand the relations between the state of oxygen species in In_(2)O_(3)and the catalytic performance for CO_(2)hydrogenation to *** the present work,we compare the properties of multiple In_(2)O_(3)and Ir-promoted In_(2)O_(3)(Ir-In_(2)O_(3))catalysts with different Ir loadings and after being pretreated under different reduction *** CO_(2)conversion rate of Ir-In_(2)O_(3)is more promoted than that of pure In_(2)O_(3).With only a small amount of Ir loading,the highly dispersed Ir species on In_(2)O_(3)increase the concentration of O_(v)sites and enhance the *** finely tuning the catalyst structure,Ir-In_(2)O_(3)with an Ir loading of 0.16 wt.%and pre-reduction treatment under 300℃exhibits the highest methanol yield of 146 mgCH_(3)OH/(gcat·hr).Characterizations of Raman,electron paramagnetic resonance,X-ray photoelectron spectroscopy,CO_(2)-temperature programmed desorption and CO_(2)-pulse adsorption for the catalysts confirm that more O_(v)sites can be generated under higher reduction temperature,which will induce a facile CO_(2)adsorption and desorption *** performance for methanol production requires an adequate dynamic balance among the surface oxygen atoms and vacancies,which guides us to find more suitable conditions for catalyst pretreatment and reaction.

关键词： Carbon dioxide Hydrogenation Methanol In_(2)O_(3) Fixed-bed Reduction temperature

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Electrochemical Oxygen Evolution Performance of Nitrogen-Doped Ultra-Thin Carbon Nanosheets Composite Ru1Co Single Atom Alloy Catalysts

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Chinese Journal of Chemistry 2024年第9期42卷 973-979页

作者： Ziwei Deng Zhiyi Sun Yaqiong Li Jiajing Pei Wenxing Chen Energy&catalysis Center Schoolof Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 00049China

Energy transformation is imminent,and hydrogen energy is one of the important new energy *** of the keys to increasing the rate of hydrogen evolution during electrolysis is the use of high-performance catalysts for oxygen evolution reactions(OER).Single-atom alloys(SAAs)have garnered significant attention because they partially reduce costs and combine the advantages of both single-atom catalysts(SACs)and alloy ***,an efficient pyrolysis strategy based on a mixing and drying process is designed to anchor ultra-small Co cluster particles,combined with Ru single atoms dispersed on nitrogen-doped ultra-thin carbon nanosheets(Ru_(1)Co SAA/NC).The prepared electrocatalyst exhibits superior OER activity and superb stability,demonstrating an overpotential of 238 mV for OER with a current density of 10 mA·cm^(-2) in 0.5 mol/L H_(2)SO_(4).And we also utilized in-situ XAS to detect the oxidation state of Ru sites during *** in all,this method achieves cost reductions and efficiency improvements through the design of SAAs,offering new prospects for the structural transformation of clean energy.

关键词： Oxygen evolution reaction Single alloy catalyst Ultra-thin carbon nanosheets Electrocatalyst Pyrolysis RuiCo SAA/NC

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Combinations of electron and proton donors in transition-metal complex mediated nitrogen reduction reactions

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Science China Chemistry 2024年第7期67卷 2136-2154页

作者： Delong Han Li Yang Hao Huang Priyanka Chakraborty Shashikant U.Dighe Kuo-Wei Huang KAUST catalysis Center and Division of Physical Science and Engineering King Abdullah University of Science and TechnologyThuwal 23955Saudi Arabia Agency for Science Technologyand ResearchInstitute of Materials Research and Engineering and Institute of Sustainability for ChemicalsEnergy and EnvironmentSingapore 138634Singapore

Nitrogen fixation is a complex process involving the transfer of six electrons and *** from the conventional Haber-Bosch process,which relies on hydrogen(H_(2))to provide both electrons and protons to reduce nitrogen(N_(2)),homogeneous transition metal complex-catalyzed N_(2)reduction reactions(NRR)employ an array of electron and proton donors or even electron donors combined with *** the synthesis of diverse catalytic progress,the categories of donors have seen rapid ***,existing literature only provides summaries regarding the metal,ligands,and *** the significance of electron and proton donor combinations in nitrogen reduction reactions,no literature has thoroughly reviewed this ***,we hereby compiled a comprehensive list of commonly used reagents in N_(2)reduction and classified them according to their specific donor *** review presents clear and organized information about these combinations,along with a summary of their general performance trend in NRR with related ***,we conclude the discussion by highlighting key points for researchers to consider when selecting catalysts and donor combinations,with the ultimate goal of advancing the field of nitrogen fixation.

关键词： dinitrogen reduction reaction reducing donor combination transition metal complexes homogeneous catalysis

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Tailoring Ni based catalysts by indium for the dehydrogenative coupling of ethanol into ethyl acetate

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Green Energy & Environment 2024年第8期9卷 1321-1331页

作者： Ming Yin Jifeng Pang Jin Guo Xianquan Li Yujia Zhao Pengfei Wu Mingyuan Zheng CAS Key Laboratory of Science and Technology on Applied catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences University of Chinese Academy of Sciences School of Materials Science and Engineering Dalian Jiaotong University

Exploring stable and robust catalysts to replace the current toxic CuCr based catalysts for dehydrogenative coupling of ethanol to ethyl acetate is a challenging but promising ***,novel NiIn based catalysts were developed by tailoring Ni catalysts with Indium （In） for this *** the optimal Ni0.1Zn0.7Al0.3InOx catalyst,the ethyl acetate selectivity reached 90.1%at 46.2%ethanol conversion under the conditions of 548 K and a weight hourly space velocity of 1.9 h-1in the 370 h time on ***,the ethyl acetate productivity surpassed1.1 gethyl acetateg-1catalysth-1,one of the best performance in current *** to catalyst characterizations and conditional experiments,the active sites for dehydrogenative coupling of ethanol to ethyl acetate were proved to be Ni4In *** presence of In tailored the chemical properties of Ni,and subsequently inhibited the C±C cracking and/or condensation reactions during ethanol *** Ni4In alloy sites,ethanol was dehydrogenated into acetaldehyde,and then transformed into acetyl species with the removal of H ***,the coupling between acetyl species and surface-abundant ethoxyde species into ethyl acetate was achieved,affording a high ethyl acetate selectivity and catalyst stability.

关键词： Dehydrogenative coupling Ethanol Ethyl acetate Nickel and indium alloys

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High-Voltage and Fast-Charging Lithium Cobalt Oxide Cathodes: From Key Challenges and Strategies to Future Perspectives

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Engineering 2024年第6期37卷 105-127页

作者： Gongrui Wang Zhihong Bi Anping Zhang Pratteek Das Hu Lin Zhong-Shuai Wu State Key Laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China

Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable ***,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high ***,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this *** and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial *** provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.

关键词： Lithium cobalt oxide High energy/power density Fast-charging High-voltage Lithium-ion battery

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Tuning interaction strength between CeO_(2) and iridium to promote CO oxidation over Ir/TiO_(2)

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Journal of Rare Earths 2024年第4期42卷 651-659页

作者： Lu Dai Binghua Li Yuhan Peng Xianwei Hao Runquan Xuan Hua Huang Yiming Bi Liping Xu Yanhui Zhang Yun Guo Fangqi Du Li Wang Hui Wang Technology Center China Tobacco Zhejiang Industrial Co.Ltd.Hangzhou310024China Research institute of Industrial catalysis East China University of Science and TechnologyShanghai200237China

The interaction between support and noble metal plays a crucial role in heterogeneous catalysis ***,how to tune metal support interactions to optimize the activity still needs further ***_(2) was introduced to promote CO oxidation ove r Ir/TiO_(2) by adjusting the interaction strength between iridium(Ir)and CeO_(2).The strong interaction between Ir and CeO_(2) blocks CO adsorption and causes low CO oxidation ***,introducing CeO_(2) on Ir/TiO_(2) produces localized interaction between Ir and CeO_(2),which can tune the surface electronic state of Ir,so a"volcano curve"relationship between CO oxidation activity and electronic state is *** amount of CeO_(2) on Ir/TiO_(2)(Ir/Ce_(0.2)Ti)leads to CO complete oxidization at 22℃,and a new pathway for CO oxidation was *** study demonstrates that the utilization of tuning interaction strength between active metal and support is a potential method to increase the catalytic activity.

关键词： CO oxidation CeO_(2) Localized interaction Interaction strength Supported Ir catalysts Rareearths

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TiO_(2) nanofiber-supported copper nanoparticle catalysts for highly efficient methane conversion to C1 oxygenates under mild conditions

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Nano Research 2024年第5期17卷 3844-3852页

作者： Wencui Li Yu Ren Zean Xie Yipeng Wang Hang Zhang Dianxiang Peng Hengfang Shen Hongfei Shi Jiaxin Cai Peng Wang Tongxin Zhang Zhen Zhao State Key Laboratory of Heavy Oil Processing China University of Petroleum(Beijing)Beijing 102249China institute of catalysis for Energy and Environment College of Chemistry&Chemical EngineeringShenyang Normal UniversityShenyang 110034China institute of Petrochemical Technology Jilin Institute of Chemical TechnologyJilin 132022China

The selective oxidation of methane under mild conditions remains the“Holy Grail of catalysis”.The key to activating methane and inhibiting over-oxidation of target oxygenates lies in designing active *** nanoparticles were loaded onto TiO_(2) nanofibers using the photo-deposition *** resulting catalysts were found to effectively convert methane into C1 oxygenated products under mild *** with previously reported catalysts,it delivers a superior performance of up to 2510.7 mmol·g_(Cu)^(-1)·h^(-1) productivity with a selectivity of around 100%at 80℃for 5 *** characterizations and density functional theory(DFT)calculations indicate that TiO_(2) in the mixed phase of anatase and rutile significantly increases the Cu^(+)/CuO ratio of the supported Cu species,and this ratio is linearly related to the formation rate of oxygen-containing *** CuI site promotes the generation of active O species from H_(2)O_(2) dissociation on Cu_(2)O(111).These active O species reduce the energy barrier for breaking the C-H bond of CH_(4),thus boosting the catalytic *** methane conversion mechanism was proposed as a methyl radical pathway to form CH_(3)OH and CH_(3)OOH,and then the generated CH_(3)OH is further oxidized to HOCH_(2)OOH.

关键词： TiO_(2)nanofiber copper nanoparticles photo-deposition method methane oxidation C1 oxygenates

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Hydrodechlorination of trifluoro-trichloroethane to chlorotrifluoroethylene:Revealing the deactivation mechanism and regeneration strategy of Pd-Cu/AC catalyst

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Chinese Journal of Chemical Engineering 2024年第6期70卷 261-268页

作者： Song Tian Yicheng Chen Xiaoyu Wen Bingcheng Li Jian Lu Zile Li Feng Feng Qingtao Wang Qunfeng Zhang Xiaonian Li State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology Institute of Industrial Catalysis of Zhejiang University of TechnologyHangzhou 310014China State Key Laboratory of Fluorine&Nitrogen Chemicals Xi'an Modern Chemistry Research InstituteXi'an 710065China

Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly ***,hydrodechlorination catalysts for olefin production often suffer from poor *** Pd/AC catalyst and Pd-Cu/AC catalyst prepared by co-impregnation method exhibited poor stability,Pd-Cu/AC catalyst with CFC-113 conversion dropping to around 37%after 50 h of hydrodechlorination ***-Emmett-Teller,transmission electron microscopy,X-ray photoelectron spectroscopy,and X-ray diffraction of fresh and deactivated Pd/AC catalysts indicate that the deactivation of Pd/AC catalysts is due to high-temperature agglomeration of *** analysis of fresh and deactivated Pd-Cu/AC catalysts using Brunauer-Emmett-Teller,transmission electron microscopy,and thermogravimetric analysis techniques revealed decreased dispersion of active sites,reduced surface area,catalyst aggregation deactivation,and a significant decrease in Cu ***,the results of NH3-TPD revealed that the acid sites of the catalyst increased significantly.X-ray diffraction spectra indicated the formation of new species,basic copper chloride(Cu_(2)(OH)_(3)Cl),during the *** the reaction progressed,these new species agglomerated,leading to a gradual loss of catalyst ***,the deactivated catalyst was successfully reactivated using a simple alkaline washing method.

关键词： CFC-113 Hydrodechlorination Chlorotrifluoroethylene Catalyst deactivation

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Stabilization and detection of labile reaction intermediates in supramolecular containers

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Chinese Chemical Letters 2024年第6期35卷 47-52页

作者： Rui Wang Yang Liang Julius Rebek Jr. Yang Yu Center for Supramolecular Chemistry&catalysis and Department of Chemistry College of ScienceShanghai UniversityShanghai 200444China Skaggs institute for Chemical Biology and Department of Chemistry The Scripps Research InstituteLa JollaCA 92037United States

Detection and observation of reactive intermediates is an essential step in investigation of reaction ***,most reactive intermediates are unstable and present at low concentrations;their short lifetimes make them difficult to detect and *** containers offer opportunities for the stabilization and characterization of those labile species,through isolation from the media and protection inside the cavity of the *** this review,we summarize the examples of labile reaction intermediates that are stabilized and characterized with the help of supramolecular *** container compounds include carcerands,deep cavitands and amide *** focus on unstable guest species-cyclobutadiene,benzocyclopropenone,o-benzyne,1,2,4,6-cycloheptatetraene,anti-Bredt's olefin,fluorophenoxycarbene,O-acylisoamide,and hemiaminalthat act as intermediates in certain organic reactions.

关键词： Supramolecular containers Reaction intermediates Labile species stabilization Short-lived species detection Supramolecular chemistry

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Intensification of bituminous coal and lignite oxidation by copper-based activating additives

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International Journal of Coal Science & Technology 2021年第1期8卷 141-153页

作者： K.B.Larionov I.V.Mishakov K.V.Slyusarskiy A.A.Vedyagin National Research Tomsk Polytechnic University TomskRussia634050 boreskov institute of catalysis sb ras NovosibirskRussia630090

The oxidation of lignite and bituminous coal samples modified by 5 wt%(in terms of dry salt)addition of copper salts Cu(NO_(3))_(2),CuSO_(4),and Cu(CH_(3)COO)_(2) was *** samples’reactivity was studied by thermogravimetry within a temperature range of 45–600℃ at a heating rate of 2.5℃/min in an oxidizing *** introduction of activating additives has resulted in a significant decrease in the temperature of intense oxidation onset(ΔT_(i)=20/94℃),in a reduction in the sample residence time in the volatile matter release region(Δt_(e)=2/22 min)and the total duration of the coal combustible mass oxidation(Δt_(f)=8/14 min).The Friedman method was used to calculate the activation energy values for the oxidation process of the modified *** maximum change in activation energy values was observed for the bituminous coal *** possible mechanism behind the action of the copper-salt additives,which activate the oxidation of lignite and bituminous coal,is *** to the data of mass spectrometric analysis,the concentration of NOx in the reaction products decreases as the temperature of the activated oxidation process is shifted towards the low-temperature region.

关键词： Coal Activated oxidation Copper nitrate Copper sulfate Copper acetate Thermo-gravimetric and mass spectrometry analysis

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