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Elucidating Confinement and Microenvironment of Ru Clusters Stably Confined in MFI Zeolite for Efficient Propane Oxidation

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Angewandte Chemie 2024年第5期137卷

作者： Jingjing Wang Dr. Zeyu Jiang Hengyue Xu Prof. Xinzhe Li Dr. Yanfei Jian Dr. Lianghui Xia Dr. Pei Su Qiyuan Liu Prof. Shouning Chai Dr. Mudi Ma Dr. Abdallah Amedlous Dr. Mathias Barreau Prof. Zhengping Hao Prof. Jiaguo Yu Prof. Chi He State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 Shaanxi P.R. China Laboratoire Catalyse & Spectrochimie Normandie Univ ENSICAEN UNICAEN CNRS Caen 14000 France Department of Chemistry Tsinghua University Beijing 100084 P.R. China College of Environmental and Chemical Engineering Yanshan University Qinhuangdao 066004 P.R. China National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing 101408 P.R. China Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences Wuhan 430078 P.R. China

Achieving active and stable heterogeneous catalysts by encapsulating noble metal species within zeolites is highly promising for high utilization and cost efficiency in thermal and environmental catalytic reactions. Ru, considered an economical noble metal alternative with comparable performance, faces great challenges within MFI-type microporous zeolites due to its high cohesive energy and mobility. Herein, an innovative strategy was explored that couples hydrothermal in situ ligand protection with stepwise calcination in a flowing atmosphere to embed ultrasmall Ru clusters anchored at K + -healed silanol sites (≡Si−Ru δ+ −O−K complexes) within 10-membered ring sinusoidal channels of MFI. Comprehensive experiments and theoretical calculations unveiled that the interplay between confined Ru clusters and MFI induces local strain in MFI, creating a unique catalytic microenvironment around the Ru clusters. This synergy interaction enhances alkane deep oxidation as the confined Ru clusters and the MFI microenvironment collectively pre-activate C 3 H 8 and O 2 , facilitate the cleavage of C−H and C−C bonds at low temperatures. Notably, the stable geometric and electronic properties of the confined Ru show exceptional thermal stability up to 1000 °C, rivaling fresh catalysts. These findings shed vital methodological and mechanistic insights for developing efficacious heterogeneous catalysts for thermal catalysis.

关键词： heterogeneous catalysis microenvironment Ruthenium strain zeolite

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Front Cover: Decoupled Water Electrolysis Driven by 1 cm2Single Perovskite Solar Cell Yielding a Solar-to-Hydrogen Efficiency of 14.4 % (ChemSusChem 1/2023)

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ChemSusChem 2022年第1期16卷

作者： Fei Lv Dr. Zhixiao Qin Jiazhe Wu Lixia Pan Longjie Liu Prof. Yubin Chen Prof. Yixin Zhao International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Shaanxi 710049 P. R. China School of Environmental Science and Engineering Frontiers Science Center for Transformative Molecules Shanghai Jiao Tong University Shanghai 200240 P. R. China

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A study of a computational BVP for heat transfer and friction drag in magnetohydrodynamics viscous flow of a nanofluid subject to the curved surface

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Proceedings of the Institution of Mechanical Engineers, Part E: Journal of Process Mechanical engineering 2021年

作者： Khan, M Riaz Saleel, C Ahamed Saeed, Tareq Allehiany, F.M. El-Refaey, Adel M Jing, Dengwei Mahmoud, Emad E LSEC and ICMSEC Academy of Mathematics and Systems Science Chinese Academy of Sciences China School of Mathematical Science University of Chinese Academy of Sciences China Department of Mechanical Engineering College of Engineering King Khalid University Saudi Arabia -Research Group Department of Mathematics Faculty of Science King Abdulaziz University Saudi Arabia Department of Mathematical Sciences College of Applied Sciences Umm Al-Qura University Saudi Arabia Department of Basic and Applied Science College of Engineering and Technology Arab Academy for Science Technology Maritime Transport Smart Village Campus Egypt State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong University China Department of Mathematics and Statistics College of Science Taif University Taif Saudi Arabia

The ongoing work investigates the features of Joule heating and convective condition over a magnetohydrodynamic stagnation point flow of (Formula presented.) nanofluid moving across a curved surface. Moreover, mass suction is supposed through the stretching/shrinking surface. The initially developed model of partial differential equations is transformed into the ordinary ones assisted by suitable similarity variables. Subsequently, the ultimate nonlinear model of ordinary differential equations is solved with the help of a built-in function bvp4c package in MATLAB. Several graphical results are plotted to see the influence of various dimensionless parameters over the velocity, temperature, heat transfer, and friction drag. We found that there exists an escalation in temperature with increasing values of curvature, Eckert number, Hartmann number, and Biot number;however, the velocity profile declines with large curvature, ratio parameter, and high concentration of nanoparticles. It is also important to note that the friction drag rises with the mass suction, and reduces with vast curvature, whereas the rate of heat transfer improves with suction and Biot number but lowers with Eckert number and Hartmann number. © IMechE 2021.

关键词： Magnetohydrodynamics

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Novel Cu_3P/g-C_3N_4 p-n heterojunction photocatalysts for solar hydrogen generation

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Science China Materials 2018年第6期61卷 861-868页

作者： Zhixiao Qin Menglong Wang Rui Li Yubin Chen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University

Developing efficient heterostructured photocatalysts to accelerate charge separation and transfer is crucial to improving photocatalytic hydrogen generation using solar energy. Herein, we report for the first time that p-type copper phosphide（Cu3P） coupled with n-type graphitic carbon nitride（g-C3N4） forms a p-n junction to accelerate charge separation and transfer for enhanced photocatalytic *** optimized Cu3P/g-C3N4 p-n heterojunction photocatalyst exhibits 95 times higher activity than bare g-C3N4, with an apparent quantum efficiency of 2.6% at 420 nm. A detail analysis of the reaction mechanism by photoluminescence,surface photovoltaics and electrochemical measurements revealed that the improved photocatalytic activity can be ascribed to efficient separation of photo-induced charge carriers. This work demonstrates that p-n junction structure is a useful strategy for developing efficient heterostructured photocatalysts.

关键词： photocatalysis copper phosphide p-n junction heterostructure hydrogen production

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Vapor condensation with low air mass fraction inside water seal branch tube under free convection

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Nuclear engineering and Design 2021年 379卷

作者： Bing Tan Xi Wang Y.W. Wu W.X. Tian S.Z. Qiu G.H. Su School of Nuclear Science and Technology State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong University 28 Xianning West Road Xi an 710049 China School of Electric Power South China University of Technology Guangzhou 510640 China

The pressure vessel has used a newly designed water seal structure, and the sealed water is from condensation at low hydrogen concentration. To get the condensation capacity of the water seal branch tube under the pressure vessel normal operation, the experimental loop named WASETEL was constructed, which is aimed at studying the heat transfer during the process of air-steam mixture condensation inside the inclined branch tube at the condition of low air mass fraction. The inner tube is diameter 0.134 m with length 0.68 m which is connected with diameter 1.4 m, high 2.5 m pressure vessel. A canon camera was set to record the images and videos of the condensate height through glass tube in communicating vessel liquidometer. The experiment was conducted under the pressure ranged from 0.2 to 0.6 MPa, air mass concentration ranged from 0.49 to 6.42% and wall subcooling ranged from 11 to 40 K. The test showed HTC (heat transfer coefficient) would sharply deteriorate with the small air fraction, compared with pure steam condensation, about 0.49% mass fraction of the air will reduce heat transfer coefficient by 70–80%. When air concentration is relatively small, those widely used relations can not predict the condensation well, therefore, a new heat transfer empirical correlation with air mass fraction, pressure and subcooling is proposed, covered all the experimental data within the error band ±13%.

关键词： Natural condensation New empirical correlation Water seal

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Synthesis of AgI/Bi2MoO6 nano-heterostructure with enhanced visible-light photocatalytic property

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Progress in Natural Science:Materials International 2018年第2期28卷 235-241页

作者： Li Zhang Hongcheng Teng Jiancheng Zhou Yueming Sun Naixu Li Maochang Liu Dengwei Jing School of Chemistry and Chemical Engineering Southeast University Department of Chemical and Pharmaceutical Engineering Southeast University Chengxian College Jiangsu Province Hi-Tech Key Laboratory for Bio-medical Research Southeast University International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Suzhou Academy of Xi'an Jiaotong University

A novel nano-heterostructure of Ag I/Bi2MoO6photocatalyst was successfully synthesized via a facile depositionprecipitation method. The samples were systematically characterized by X-ray diffraction, scanning and transmission electron microscopy, X-ray photoemission spectroscopy, UV–Vis absorption spectroscopy, and photoluminescence spectra. While sole Bi2MoO6or Ag I showed poor activity toward photocatalytic rhodamine B degradation, the nano-heterostructure was found with superior performance. The AgI/Bi2MoO6composite with an optimal content of 20 wt% Ag I exhibited the highest photocatalytic degradation rate. Rhodamine B was totally degraded within 75 min visible-light irradiation. Moreover, the hybrid photocatalyst also showed a fairly good stability for several-cycle reuse. This study indicates that the AgI/Bi2MoO6nano-heterostructure can be used as an effective candidate for photocatalytic degradation of organic pollutants.

关键词： Heterostructure Photocatalyst RhB-degradation

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Experimental Study on Deliquification with Atomizing Nozzle in Gas Well

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IOP Conference Series: Earth and Environmental Science 2020年第1期555卷

作者： Yutang Gao Xiaobai Li Peng Chang Lei Liu State Key Laboratory of Multiphase Flow in Power Engineering Xi'an 710049 Shaanxi P.R. China

Gas is a clean energy resource in comparison with oil and coal. Liquid-loading problem is frequently encountered in the process of gas production. It would directly cause the production of gas wells decreasing, even off production. A number of deliquification techniques have been suggested for solving this kind of problem, but the available techniques are not yet widely applicable. Based on the analysis, the method of deliquification with atomizing nozzle in gas wells was put forward. The test bench was designed for studying the atomization of nozzles and the liquid entrainment of gas flow. The size distribution of atomized droplets was measured by Malvern laser grain size analyzer. The Sauter mean diameters of atomized droplets were analysed under different two-phase flow conditions. The results indicate that the designed nozzles have good atomization performances and show potential application for reducing liquid loading in gas wells.

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Photocatalytic water oxidation over BiVO_4 with interface energetics engineered by Co and Ni-metallated dicyanamides

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Chinese Journal of Catalysis 2018年第3期39卷 502-509页

作者： Yi Shang Fujun Niu Shaohua Shen International Research Centre for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’an 710049 Shaanxi China

Photocatalytic water oxidation based on semiconductors usually suffers from poor charge transfer from the bulk to the interface,which is necessary for oxygen ***,we construct a hybrid artificial photosynthesis system for photocatalytic water *** system consists of BiVO4as the light harvester,a transitional metal complex(M(dca)2,M=Co,Ni,dca:dicyanamide)as the water oxidation catalyst,and S2O82?as a sacrificial electron *** system exhibits enhanced oxygen evolution activity when M(dca)2is *** BiVO4/Co(dca)2and Bi‐VO4/Ni(dca)2systems exhibit excellent oxygen evolution rates of508.1and297.7μmol/(h·g)compared to the pure BiVO4which shows a photocatalytic oxygen evolution rate of252.2μmol/(h·g)during6h of photocatalytic ***(dca)2is found to be more effective than Ni(dca)2as a water oxidation *** enhanced photocatalytic performance is ascribed to the M(dca)2‐engineered BiVO4/electrolyte interface energetics,and to the M(dca)2‐catalyzed surface water *** two factors lead to a decrease in the energy barrier for hole transfer from the bulk to the surface of BiVO4,which promotes the water oxidation kinetics.

关键词： Metal complex BiVO4 Water oxidation Photocatalysis Interfacial kinetics

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Current Density Regulating Lithium Metal Directional Deposition for Long Cycle Life Lithium Metal Batteries

SSRN

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SSRN 2020年

作者： Mao, Heng Yu, Wei Cai, Zhuanyun Liu, Guixian Liu, Limin Wen, Rui Su, Yaqiong Xi, Kai Li, Benqiang Da, Xinyu Kou, Huari Yan, Wei Ding, Shujiang Xi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Xi’an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power Xi’an Jiaotong University Xi’an710049 China State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen361005 China Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Beijing100190 China Cambridge Graphene Centre Department of Engineering University of Cambridge CambridgeCB3 0FA United Kingdom Department of Mechanical Engineering University of Michigan-Dearborn DearbornMI48128 United States Department of Environmental Science and Engineering State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong University Xi’an710049 China

Uncontrolled dendrite formation in the high energy density of lithium metal batteries (LMBs) may pose serious safety risks. Numerous works have been reported to protect separator. However, these methods still couldn’t inhibit the dendrite upward growth to protect the separator, effectively. Here, we introduce a novel “orientated-growth” strategy that makes the depositional interface transfer to the anode/current collector interface from the anode/separator interface. We placed a layer of cellulose/graphene carbon composite aerogel (CCA) between the current collector and the anode (CCA-Li). This layer works as the charge organizer;it induces a higher current density distribution and makes Li prefer to deposit in the bottom CCA layer of CCA-Li electrode. Both in-situ and ex-situ images of the electrode demonstrate the anode part of the cell has been flipped;with the new deposited particles facing the current collector and smooth surface facing the separator. Electrochemical characterization of the electrode in half and full cells showed outstanding cyclic stability and rate capability, with the CCA-Li/LPF full cell able to maintain 94% of its initial capacity after 1000 cycles. We believe that the innovative strategy would promote the leapfrog development for LMBs. © 2020, The Authors. All rights reserved.

关键词： Electric current collectors

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Carbon-Confined Indium Oxides for Efficient Carbon Dioxide Reduction in a Solid-state Electrolyte flow Cell

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Angewandte Chemie 2022年第21期134卷

作者： Zhitong Wang Yansong Zhou Dongyu Liu Ruijuan Qi Chenfeng Xia Prof. Mingtao Li Prof. Bo You Prof. Bao Yu Xia School of Chemistry and Chemical Engineering Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure Hubei Engineering Research Center for Biomaterials and Medical Protective Materials Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology (HUST) 1037 Luoyu Rd Wuhan 430074 China International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE) Xi'an Jiaotong University (XJTU) 28 Xianning West Road Xi'an 710049 China HSE University 101000 Moscow Russia Key Laboratory of Polar Materials and Devices (MOE) Department of Electronics School of Physics and Electronic Science East China Normal University Shanghai 200241 China

Developing robust electrocatalysts and advanced devices is important for electrochemical carbon dioxide (CO 2 ) reduction toward the generation of valuable chemicals. We present herein a carbon-confined indium oxide electrocatalyst for stable and efficient CO 2 reduction. The reductive corrosion of oxidative indium to the metallic state during electrolysis could be prevented by carbon protection, and the applied carbon layer also optimizes the reaction intermediate adsorption, which enables both high selectivity and activity for CO 2 reduction. In a liquid-phase flow cell, the formate selectivity exceeds 90 % in a wide potential window from −0.8 V to −1.3 V vs. RHE. The continuous production of ca. 0.12 M pure formic acid solution is further demonstrated at a current density of 30 mA cm −2 in a solid-state electrolyte mediated reactor. This work provides significant concepts in the parallel development of electrocatalysts and devices for carbon-neutral technologies.

关键词： Carbon Dioxide Reduction Corrosion-Resistant Electrocatalyst Indium Oxide Solid-state Electrolyte

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