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Construction of highly dispersed Pt single sites and high-efficiencyheterocatalysis silylation of alcohols with silanes

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Nano Research 2023年第4期16卷 4643-4649页

作者： Qiulian Wei Yunqiang Sun Shan Wang Zunfu Hu Qingyun Liu Xiuwen Zheng School of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266510China Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong College of Chemistry and Chemical EngineeringLinyi UniversityLinyi 276000China

The construction of silicon-oxygen bonds has been highlighted as an exciting achievement in organosilicon and green chemistry,but their synthetic efficiency has great improvement potential,so it is crucial to explore and achieve an effective approach for synthesizing such *** this study,we successfully prepared the highly dispersed platinum single-atom catalyst(Pt SAC/N-C)through a coordination-assisted strategy with a mixture of ligands(H2bpdc and H2bpydc),which were used for the Osilylation of alcohols with *** strong coordination between Pt2+and the Pyridine N at the skeleton of UiO-67 plays a critical role in accessing the atomically isolated dispersion of Pt *** the assistance of the H2bpydc ligands,the Pt/UiO-67-bpdc precursor is prone to aggregation during the pyrolysis process,resulting in the formation of Pt *** by advanced characterization techniques of high-angle annular dark-field scanning transmission electron microscopy(HAADFSTEM)and X-ray absorption fine structure(XAFS)spectroscopy,it has been demonstrated that atomically dispersed Pt was formed on the UiO-67 through a local structure of four-coordinated Pt-N4,exhibiting a high actual Pt loading content(0.6962 wt.%).In the oxidation of silanes,the Pt SAC/N-C catalyst showed a high turnover frequency(TOF)value(up to 9,920 h−1)when the catalyst loading decreased to 0.005%.Excellent performance was maintained during recycling experiments,indicating high stability of the catalyst.

关键词： high-dispersion single-atom catalysis O-silylation heterogeneous catalysis

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Electrospinning engineering of gas electrodes for high-performance lithium-gas batteries

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Carbon Energy 2024年第10期6卷 353-398页

作者： Jingzhao Wang Xin Chen Jianan Wang Xiangming Cui Ze Wang Guangpeng Zhang Wei Lyu Maxim Shkunov S.Ravi P.Silva Yaozu Liao Kai Yang Wei Yan State Key Laboratory of Multiphase Flow in Power Engineering Department of Environmental Science and EngineeringSchool of Energy and Power EngineeringXi'an Jiaotong UniversityXi'anChina Advanced Technology Institute University of SurreyGuildfordSurreyUK State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghaiChina

Lithium-gas batteries(LGBs)have garnered significant attention due to their impressive high-energy densities and unique gas conversion ***,the practical application of LGBs faces substantial challenges,including sluggish gas conversion kinetics inducing in low-rate performance and high overpotential,along with limited electrochemical reversibility leading to poor cycle *** imperative task is to develop gas electrodes with remarkable catalytic activity,abundant active sites,and exceptional electrochemical ***,a versatile and well-established technique for fabricating fibrous nanomaterials,has been extensively explored in LGB *** this work,we emphasize the critical structure-property for ideal gas electrodes and summarize the advancement of employing electrospun nanofibers(NFs)for performance enhancement in *** elucidating the fundamental principles of LGBs and the electrospinning technique,we focus on the systematic design of electrospun NF-based gas electrodes regarding optimal structural fabrication,catalyst handling and activation,and catalytic site optimization,as well as considerations for large-scale *** demonstrated principles and regulations for electrode design are expected to inspire broad applications in catalyst-based energy applications.

关键词： carbon nanofibers electrocatalyst electrospinning gas electrodes metal-gas batteries

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Synthesis of chiral allylic phosphonates via asymmetric reductive cross-coupling of α-bromophosphonates and vinyl bromides

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Science China Chemistry 2023年第9期66卷 2621-2625页

作者： Hepan Wang Xinxuan Li Tao XU Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China

Chiral phosphine-containing skeletons play a pivotal role in bioactive natural products, pharmaceuticals, chiral catalysts, and ligands. Despite considerable progress has been made in the synthesis of chiral phosphorus compounds, the development of facile and modular methods to access chiral allylic phosphorus compounds remains challenging due to the simultaneous control required for reactivity, enantioselectivity, and stereoselectivity. Herein, we present a general and modular platform to achieve the asymmetric reductive cross-coupling of α-bromophosphonates and vinyl bromides, enabling the synthesis of highly valuable chiral allylic phosphonate products with remarkable yields, enantioselectivities, and stereoselectivities.

关键词： chiral phosphorus compound reductive cross-coupling α-alkenyl phosphonate nickel asymmetric reaction

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Extractive distillation of cycloalkane monomers from the direct coal liquefaction fraction

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Frontiers of chemical Science and engineering 2024年第11期18卷 269-279页

作者： Shuo-Shuo Zhang Xing-Bao Wang Wen-Ying Li State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China College of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuan 030024China

Separating monomeric cycloalkanes from naphtha obtained from direct coal liquefaction not only facilitates the valuable utilization of naphtha but also holds potential for addressing China’s domestic chemical feedstock market demand for these *** extractive distillation processes of naphtha,relative volatility serves as a crucial parameter for extractant ***,determining relative volatility through conventional vapor-liquid equilibrium experiments for extractant selection proves challenging due to the complexity of naphtha’s compound *** address this challenge,a prediction model for the relative volatility of n-heptane/methylcyclohexane in various extractants has been developed using machine-learning quantitative structure-property relationship *** model enables rapid and cost-effective extractant *** statistical analysis of the model revealed favorable performance indicators,including a coefficient of determination of 0.88,cross-validation coefficient of 0.94,and root mean square error of *** such asα,EHOMO,ρ,and logPoct/water collectively influence relative *** of standardized coefficients in the multivariate linear regression equation identified density as the primary factor affecting the relative volatility of n-heptane/methylcyclohexane in the different *** with higher densities,devoid of branched chains,exhibited increased relative volatility compared to their counterparts with branched ***,the process of separating cycloalkane monomers from direct coal liquefaction products via extractive distillation was optimized using Aspen Plus software,achieving purities exceeding 0.99 and yields exceeding 0.90 for cyclohexane and methylcyclohexane ***,energy consumption,and environmental assessments were *** acid emerged as the most suitable extractant for purifying cycloalkanes in direct coal liquefaction naphtha due to its super

关键词： naphtha relative volatility molecular descriptor quantitative structure-property relationship model

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Unlocking new possibilities in ionic thermoelectric materials: a machine learning perspective

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National Science Review 2025年第1期12卷 195-206页

作者： Yidan Wu Dongxing Song Meng An Cheng Chi Chunyu Zhao Bing Yao Weigang Ma Xing Zhang Key Laboratory for Thermal Science and Power Engineering of Ministry of Education Department of Engineering Mechanics Tsinghua University Key Laboratory of Process Heat Transfer and Energy Saving of Henan Province School of Mechanics and Safety Engineering Zhengzhou University College of Mechanical and Electrical Engineering Shaanxi University of Science and Technology Key Laboratory of Power Station Energy Transfer Conversion and System of Ministry of Education School of Energy Power and Mechanical Engineering North China Electric Power University School of Materials and Chemical Engineering Xuzhou University of Technology

The high thermopower of ionic thermoelectric(i-TE) materials holds promise for miniaturized waste-heat recovery devices and thermal sensors. However, progress is hampered by laborious trial-and-error experimentations, which lack theoretical underpinning. Herein, by introducing the simplified molecular-input line-entry system, we have addressed the challenge posed by the inconsistency of i-TE material types, and present a machine learning model that evaluates the Seebeck coefficient with an R2of0.98 on the test dataset. Using this tool, we experimentally identify a waterborne polyurethane/potassium iodide ionogel with a Seebeck coefficient of 41.39 m V/K. Furthermore, interpretable analysis reveals that the number of rotatable bonds and the octanol-water partition coefficient of ions negatively affect Seebeck coefficients, which is corroborated by molecular dynamics simulations. This machine learning-assisted framework represents a pioneering effort in the i-TE field, offering significant promise for accelerating the discovery and development of high-performance i-TE materials.

关键词： thermoelectric conversion ionic thermoelectric materials machine learning interpretable analysis

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Enabling nickel ferrocyanide nanoparticles for highperformance ammonium ion storage

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Frontiers of chemical Science and engineering 2023年第2期17卷 226-235页

作者： Haoxiang Yu Leiyu Fan Chenchen Deng Huihui Yan Lei Yan Jie Shu Zhen-Bo Wang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringState Key Lab of Urban Water Resource and EnvironmentHarbin Institute of TechnologyHarbin 150001China School of Materials Science and Chemical Engineering Ningbo UniversityNingbo 315211China

Prussian blue and its analogs are extensively investigated as a cathode for ammonium-ion ***,they often suffer from poor electronic ***,we report a Ni_(2)Fe(CN)_(6)/multiwalled carbon nanotube composite electrode material,which is prepared using a simple coprecipitation *** obtained material consists of nanoparticles with sizes 30-50 nm and the multiwalled carbon nanotube embedded in *** existence of multiwalled carbon nanotube ensures that the Ni_(2)Fe(CN)_(6)/multiwalled carbon nanotube composite shows excellent electrochemical performance,achieving a discharge capacity of 55.1 mAh·g^(-1)at 1 C and 43.2 mAh·g^(-1)even at 15 *** increase in the ammoniumion diffusion coefficient and ionic/electron conductivity based on kinetic investigations accounts for their high ***,detailed ex situ characterizations demonstrate that Ni_(2)Fe(CN)_(6)/multiwalled carbon nanotube composite offers three advantages:negligible lattice expansion during cycling,stable structure,and the reversible redox ***,the Ni_(2)Fe(CN)_(6)/multiwalled carbon nanotube composite presents a long cycling life and high rate ***,our study reports a desirable material for ammonium-ion batteries and provides a practical approach for improving the electrochemical performance of Prussian blue and its analogs.

关键词： nickel ferrocyanides NH_(4)^(+) electrochemistry Prussian blue aqueous ammonium ion batteries

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“In-N-out” design enabling high-content triethyl phosphate-based non-flammable and high-conductivity electrolytes for lithium-ion batteries

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Science China Chemistry 2024年第2期67卷 724-731页

作者： Mengchuang Liu Fenfen Ma Zicheng Ge Ziqi Zeng Qiang Wu Hui Yan Yuanke Wu Sheng Lei Yanli Zhu Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan430074China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan430074China GuSu Laboratory of Materials Suzhou215123China Institute of Metal Research Chinese Academy of SciencesShenyang110000China State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081China

Safety issues related to flammable electrolytes in lithium-ion batteries(LIBs) remain a major challenge for their extended *** use of non-flammable phosphate-based electrolytes has proved the validity in inhibiting the combustion of ***,the strong interaction between Li^(+) and phosphate leads to a dominant solid electrolyte interphase(SEI) with limited electronic shielding,resulting in the poor Li^(+) intercalation at the graphite(Gr) anode when using high-phosphate-content *** mitigate this issue and improve Li^(+) insertion,we propose an “In-N-Out” strategy to render phosphates “noncoordinative”.By employing a combination of strongly polar solvents for a “block effect” and weakly polar solvents for a “drag effect”,we reduce the Li^(+)–phosphate *** a result,phosphates remain in the electrolyte phase(“In”),minimizing their impact on the incompatibility with the Gr electrode(“Out”).We have developed a non-flammable electrolyte with high triethyl phosphate(TEP) content(>60 wt.%),demonstrating the excellent ion conductivity(5.94 mS cm^(-1) at 30 ℃) and reversible Li^(+) intercalation at a standard concentration(~1 mol L^(-1)).This approach enables the manipulation of multiple electrolyte functions and holds the promise for the development of safe electrochemical energy storage systems using non-flammable electrolytes.

关键词： lithium-ion batteries graphite anode high-phosphate-content electrolytes non-flammable electrolyte excellent ion conductivity standard concentration

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Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction

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Nano Research 2024年第6期17卷 4807-4814页

作者： Runze Chen Xiaoying Wang Jianfei Dang Songjie Yun Liqiang Wang Fangong Kong You-Nian Liu State Key Laboratory of Biobased Material and Green Papermaking Qilu University of TechnologyJinan 250353China School of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Hunan Provincial Key Laboratory of Micro&Nano Materials Interface Science College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Carbon-supported single-atom catalysts were found to suffer reversible deactivation in catalytic hydrogenation,but the mechanism is still ***,nitro compounds hydrogenation catalyzed by N-doped carbon-supported Co single atom(Co1/NC)was taken as a model to uncover the mechanism of the reversible deactivation ***1/NC exhibited moderate adsorption towards the substrate molecules(i.e.,nitro compounds or related intermediates),which could be strengthened by the confinement effect from the porous ***,substrate molecules tend to accumulate within the pore channel,especially micropores that host Co1,making it difficult for the reactants to access the active sites and finally leading to their *** situation could be even worse when the substrate molecules possess a large ***,the catalytic activity of Co1/NC could be restored via a simple thermal treatment,which could remove the adsorbates within the pore channel,hence releasing active sites that were originally inaccessible to reactants.

关键词： single-atom catalysts porous carbon support reversible deactivation mechanistic study hydrogenation reaction

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Tuning active sites in MoS_(2)-based catalysts via H_(2)O_(2)etching to enhance hydrodesulfurization performance

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Petroleum Science 2023年第6期20卷 3875-3886页

作者： Shui-Sen He Ting-Ting Huang Chao Chen Yu Fan State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China State Key Laboratory Base for Eco-Chemical Engineering in College of Chemical Engineering Qingdao University of Science and TechnologyZhengzhou Road 53Qingdao266042ShandongChina

A H_(2)O_(2)etching strategy was adopted to introduce coordinatively unsaturated sites(CUS)on MoS_(2)-based catalysts for dibenzothiophene(DBT)hydrodesulfurization(HDS).The CUS concentrations on MoS_(2) slabs were finely regulated by changing the concentrations of H_(2)O_(2)*** the increasing H_(2)O_(2)concentrations(0.1–0.3 mol/L),The CUS concentrations on MoS_(2) slabs increased ***,the high-concentration H_(2)O_(2)etching(0.5 mol/L)increased the MoOxSy and MoO_(3) contents on MoS_(2) slabs compared to etching with the H_(2)O_(2)concentration of 0.3 mol/L,which led to the less CUS concentration in the sulfided Mo–H-0.5 catalyst than in the sulfided Mo–H-0.3 catalyst.A microstructure-activity correlation indicated that the CUS introduced by H_(2)O_(2)etching on MoS_(2) slabs significantly enhanced DBT *** Co loadings were further introduced into Mo–H-0.3,which had the most CUS concentration,and the corresponding 0.2-CoMo catalyst with the highest CoMoS content(3.853 wt%)exhibited the highest reaction rate constant of 6.95×10^(−6)mol g^(−1)s^(−1)among these CoMo catalysts.

关键词： H_(2)O_(2)etching Coordinatively unsaturated site concentrations CoMoS Hydrodesulfurization

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Machine learning models coupled with ionic fragmentσ-profiles to predict ammonia solubility in ionic liquids

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Green chemical engineering 2025年第2期6卷 223-232页

作者： Kaikai Li Yuesong Zhu Sensen Shi Yongzheng Song Haiyan Jiang Xiaochun Zhang Shaojuan Zeng Xiangping Zhang Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Mesoscience and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China College of Chemical and Engineering University of Chinese Academy of SciencesBeijing100049China College of Chemical Engineering and Environment China University of PetroleumBeijing102249China Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of EducationEast China University of Science and TechnologyShanghai200237China

Emitting NH_(3)into the atmosphere leads to significant air pollution,while NH_(3)itself serves as an essential component for fertilizers and refrigerants in ***,recovering and reusing NH_(3)is highly *** liquids(ILs)have shown great potential for NH_(3)capture,where the accurate prediction of solubility is a critical point for selecting ILs and designing a separation *** work combined the Ionic Fragment Contribution(IFC)strategy with machine learning(ML)to develop four models(IFC-ML)to predict NH_(3)solubility in ILs.A dataset containing 785 solubility data points,covering 10 cations and 10 anions,was *** this dataset,the S1–S6 descriptors based on the IFC method were used as inputs for the ML models,together with temperature(T)and pressure(P).Among the models,the IFC-GBR model was recommended for predicting NH_(3)solubility in ILs due to its higher coefficient of determination(R^(2))of 0.9945 and lower mean squared error(MSE)of 0.0003 than the ***,in comparison with previous conductor-like screening model for real solvents(COSMO-RS)and extreme learning machine(ELM)methods,the IFC-GBR(gradient boosting regressor)method showed a more accurate prediction of the NH_(3)solubility in ILs over a wider range of temperatures and pressures,providing additional chemical insights into IL-NH_(3)system that cations played a more important role for NH_(3)*** results highlighted the developed IFC-GBR model offered valuable insights for helping guide the process design of absorbing NH_(3)through IL-based technology.

关键词： Ionic liquids Ionic fragments contribution NH_(3)solubility Machine learning

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