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Room‐Temperature Activation of H2by a Surface Frustrated Lewis Pair

Angewandte Chemie 2019年第28期131卷

作者： Lu Wang Tingjiang Yan Rui Song Wei Sun Yuchan Dong Jiuli Guo Zizhong Zhang Xuxu Wang Geoffrey A. Ozin Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S3H6 Canada College of Chemistry and Chemical Engineering Qufu Normal University Qufu Shandong 273165 P. R. China International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an Shanxi 710049 P. R. China Department of Chemistry Nankai University Tianjin 300071 P. R. China State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University Fuzhou 350108 P. R. China

Surface frustrated Lewis pairs (SFLPs) have been implicated in the gas‐phase heterogeneous (photo)catalytic hydrogenation of CO 2 to CO and CH 3 OH by In 2 O 3− x (OH) y . A key step in the reaction pathway is envisioned to be the heterolysis of H 2 on a proximal Lewis acid–Lewis base pair, the SFLP, the chemistry of which is described as In⋅⋅⋅In‐OH + H 2 → In‐OH 2 + ⋅⋅⋅In‐H − . The product of the heterolysis, thought to be a protonated hydroxide Lewis base In‐OH 2 + and a hydride coordinated Lewis acid In‐H − , can react with CO 2 to form either CO or CH 3 OH. While the experimental and theoretical evidence is compelling for heterolysis of H 2 on the SFLP, all conclusions derive from indirect proof, and direct observation remains lacking. Unexpectedly, we have discovered rhombohedral In 2 O 3− x (OH) y can enable dissociation of H 2 at room temperature, which allows its direct observation by several analytical techniques. The collected analytical results lean towards the heterolysis rather than the homolysis reaction pathway.

关键词： Gasphasenreaktionen Heterolytische H2-Dissoziation Indiumoxid Oberflächenchemie Oberflächenfrustriertes Lewis-Paar

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Dynamics and energy harvesting of a flow-induced snapping sheet with nonuniform stiffness distribution

International Journal of Fluid Engineering

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International Journal of Fluid engineering 2024年第4期1卷 44-55页

作者： Zhaokun Wang Jingyu Cui Fuwang Zhao M.N.Mumtaz Qadri Yuanye Zhou Hui Tang Department of Mechanical Engineering The Hong Kong Polytechnic UniversityKowloonHong KongChina School of Fashion and Textiles The Hong Kong Polytechnic UniversityKowloonHong KongChina Zhejiang Key Laboratory of Multiphase Flow and Fluid Machinery Zhejiang Sci-Tech UniversityHangzhou 310018China Department of Aerospace Engineering School of Mechanical and Manufacturing EngineeringNUSTIslamabad 44000Pakistan Shenzhen Research Institute of Shandong University A301 Virtual University Park in South District of ShenzhenShenzhenChina

Energy harvesting through periodic snap-through of a buckled sheet has recently gained considerable attention because of its potential applications in energy harvesting in low incoming *** the snapping dynamics of uniform buckled sheets has been extensively studied,the present work focuses on the energy harvesting and dynamics of a nonuniform snapping sheet with both of its ends clamped in a channel *** analysis reveals that the sheet undergoes periodic snap-through oscillations,with its rear half consistently serving as the main contributor to effective energy harvesting,and the potential energy contributing significantly more than the kinetic *** the stiffness differenceΔEI^(*)shows that increasing the stiffness of the rear part and decreasing that of the fore part shifts the deformation wave toward upstream and enhances the snapping amplitude of the fore part,optimizing energy *** a length compression ratioΔL^(*)=0.3,the maximum potential energy is observed forΔEI^(*)=1,and the total energy peaks atΔEI^(*)=*** study also identifies an optimalΔL^(*)=0.4that maximizes both total and potential energies,and triples the potential energy in comparison withΔL^(*)=***,the enhancement of nonuniformity disappears atΔL^(*)>0.3 for the total energy andΔL^(*)>0.2 for the potential *** findings provide insights to aid optimization of the design and performance of snapping sheet energy harvesters.

关键词： stiffness energy harvesting

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flow behaviors of shale oil in kerogen slit by molecular dynamics simulation

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Chemical engineering Journal 2022年 434卷

作者： Jie Liu Yongfei Yang Shuyu Sun Jun Yao Jianlong Kou Physical Science and Engineering Division (PSE) Computational Transport Phenomena Laboratory King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia Key Laboratory of Unconventional Oil & Gas Development (China University of Petroleum (East China)) Ministry of Education Qingdao 266580 PR China Research Center of Multiphase Flow in Porous Media School of Petroleum Engineering China University of Petroleum (East China) Qingdao 266580 PR China Institute of Condensed Matter Physics Zhejiang Normal University Jinhua 321004 PR China

In the last decades, shale oil, mainly distributed in the nanopores of shale, has been considered as the representative of unconventional energy to alleviate the energy crisis. But the ideal pore models greatly overestimate the flowing capability of shale oil. To get more accurate and reasonable flow behavior, the multicomponent shale oil in the realistic kerogen channel is studied by using molecular dynamic simulation. Both density and velocity distributions that along and perpendicular to the flow direction are studied in kerogen channel, where the influence of branch chain of kerogen is also took into consideration. The heavy component tends to form the adsorbed layers on the kerogen wall, as a result of the extremely strong affinity between kerogen and hydrocarbons, and some asphaltene molecules in bulk phase form the cluster in middle of slit. On the flow direction, the velocity profile preforms the peristaltic behavior due to the effect of branch chain of kerogen, and the toluene and asphaltene components contribute it mostly. According to the heterogeneous characteristics of shale oil flow, we define the fictitious slip boundary, which corresponds to the boundary between bulk phase and adsorbed phase, to describe shale oil flow precisely. We also examine the effects of driving pressure gradient, temperature and pore size on the flow behaviors. The enhancements of driving force and temperature both facilitate shale oil flow, and the maximum velocity reaches the stable value within larger kerogen pores. The potential energy distribution and the interaction force contour verified the peristaltic flow behavior and the validity of fictitious slip boundary.

关键词： Shale oil Kerogen flow behavior Molecular simulation

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Adsorption behaviors of shale oil in kerogen slit by molecular simulation

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Chemical engineering Journal 2020年 387卷

作者： Yongfei Yang Jie Liu Jun Yao Jianlong Kou Zheng Li Tianhao Wu Kai Zhang Lei Zhang Hai Sun Key Laboratory of Unconventional Oil & Gas Development China University of Petroleum (East China) Ministry of Education Qingdao 266580 PR China Research Center of Multiphase Flow in Porous Media School of Petroleum Engineering China University of Petroleum (East China) Qingdao 266580 PR China Institute of Condensed Matter Physics Zhejiang Normal University Jinhua 321004 PR China Reservoir Engineering Research Institute 595 Lytton Avenue Suite B Palo Alto CA 94301 USA

Shale oil is widely distributed in organic nanopores, while kerogen plays a complex and key role for adsorption behavior of shale oil, and thus it is crucial to identify the associated storage mechanisms. In this paper, molecular dynamic (MD) simulation had been performed to quantify the adsorption behavior of shale oil in kerogen slits. Both the distribution of shale oil properties and potential of the mean force (PMF) were used to identify the interaction mechanisms between the light and heavy components respectively represented by methane and asphaltene. We also examined the effects of different temperatures and apertures on the adsorption behavior. Owning to the extremely strong adsorption capacity between the asphaltene and kerogen, the adsorbed asphaltene layers reduce the slit width, preventing the light components from adsorbing on the kerogen slits due to the energy barrier formed by heavy components. It is found that, with an increase in temperature, the distribution of hydrocarbons performs more homogeneously. In addition, the adsorption quantity of medium components displays a reduction in kerogen slit, while the heavy component shows a rising as its greater competitiveness, suggesting that the medium components are the most potential fraction in thermal exploitation, and the light components keep a steady quantity with the combined action of medium and heavy components. The small slit (aperture <2 nm) can be blocked by asphaltene molecules, and the adsorption density of hydrocarbons reaches the maximum at 2 nm aperture.

关键词： Adsorption behavior Shale oil Kerogen Molecular simulation

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Modulating the Electronic Metal-Support Interactions in Single-Atom Pt1−CuO Catalyst for Boosting Acetone Oxidation

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Angewandte Chemie 2022年第28期134卷

作者： Dr. Zeyu Jiang Dr. Mingjiao Tian Dr. Meizan Jing Prof. Shouning Chai Dr. Yanfei Jian Dr. Changwei Chen Prof. Mark Douthwaite Dr. Lirong Zheng Dr. Mudi Ma Prof. Weiyu Song Prof. Jian Liu 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 Department of Chemistry National University of Singapore Singapore 117543 Singapore Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences Wuhan 430074 P. R. China State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing 102249 P. R. China Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis School of Chemistry Cardiff University Cardiff CF10 3AT UK Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 P. R. China National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing 101408 P. R. China

The development of highly active single-atom catalysts (SACs) and identifying their intrinsic active sites in oxidizing industrial hazardous hydrocarbons are challenging prospects. Tuning the electronic metal-support interactions (EMSIs) is valid for modulating the catalytic performance of SACs. We propose that the modulation of the EMSIs in a Pt 1 −CuO SAC significantly promotes the activity of the catalyst in acetone oxidation. The EMSIs promote charge redistribution through the unified Pt−O−Cu moieties, which modulates the d -band structure of atomic Pt sites, and strengthens the adsorption and activation of reactants. The positively charged Pt atoms are superior for activating acetone at low temperatures, and the stretched Cu−O bonds facilitate the activation of lattice oxygen atoms to participate in subsequent oxidation. We believe that this work will guide researchers to engineer efficient SACs for application in hydrocarbon oxidation reactions.

关键词： Acetone Oxidation Electronic Metal-Support Interactions Intrinsic Mechanism Single-Atom Catalysts

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Formation damage evaluation of a sandstone reservoir via pore-scale X-ray computed tomography analysis

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Journal of Petroleum Science and engineering 2019年 183卷

作者： Yongfei Yang Yingwen Li Jun Yao Kai Zhang Stefan Iglauer Linda Luquot Zengbao Wang Key Laboratory of Unconventional Oil & Gas Development (China University of Petroleum (East China)) Ministry of Education Qingdao 266580 PR China Research Center of Multiphase Flow in Porous Media School of Petroleum Engineering China University of Petroleum (East China) Qingdao 266580 PR China Petroleum Engineering Department Edith Cowan University Joondalup Western Australia 6027 Australia Hydrosciences Montpellier - CNRS Hydrosciences Montpellier Montpellier France School of Energy Resources China University of Geosciences (Beijing) Beijing 100083 PR China

The incompatibility between workover fluid and reservoir rock is one of the causes of formation damage. Fines migration and clay swelling are considered as the major mechanisms responsible for formation damage, which results in declining productivity. However, there has been limited visualized evidence of pore structural changes during formation damage. This paper establishes a formation damage evaluation method for sandstone reservoirs based on X-ray micro-computed tomography (CT) analysis. We presented conclusive evidence for clay swelling and fines migration during workover fluid flooding and formation liquid flooding. Water sensitivity and flow rate sensitivity tests were performed on a Dongying sandstone (heterogeneous argillaceous sandstone) plug. In addition, the plug was micro-CT imaged before and after flooding with workover fluid and formation liquid at medium resolution (24 μm voxel size); the changes in core permeability and the associated changes in 2D and 3D pore space were analyzed. We found that the sandstone pore space was partially blocked by clay minerals and moving particles, leading to significantly decreased porosity (5.17%–4.19% for sample 1, 5.38%–2.76% for sample 2) and permeability (3.38 × 10 −3  μm 2 to 1.28 × 10 −3  μm 2 for sample 1, 13.30 × 10 −3  μm 2 to 3.15 × 10 −3  μm 2 for sample 2). This permeability decrease was caused by a decrease in the average pore radius and coordination number. Moreover, increased micro-CT intensity was measured by comparison of initial and final tomogram images, representing clay swelling & blockage of pores during the displacement and a generally lower porosity. This work visualized microscale formation damage, which reminds that incompatibility between workover fluid and reservoir rock damages formation seriously and the fluid injection rate should be lower than the critical flow rate when developing a reservoir with a strong water sensitivity and flow rate sensitivity.

关键词： X-ray computed tomography In-situ imaging Permeability change Fines migration Clay swelling Formation damage

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Corrigendum to: “One-pot synthesis of amorphous/crystalline SnO 2 /BaSO 4 composite sensitized with Eosin Y for enhanced photocatalytic H 2 production” [J. Environ. Chem. Eng. 12 (2024) 112770/JECE112770]

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Journal of Environmental Chemical engineering 2024年第5期12卷

作者： Cheng Cheng Jinfeng Zhang Haiping Jia Xutao Ding Gongyue Dong Feng Chen Yuchao Hu Jinwen Shi School of Chemical Engineering and Technology International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE) Xi’an Jiaotong University (XJTU) 28 West Xianning Road Xi’an 710049 China Shaanxi Key Laboratory of Advanced Stimulation Technology for Oil & Gas Reservoirs Xi’an Shiyou University Xi’an 710065 China Shaanxi Gas Group Fuping Energy Technology Co. Ltd 2 Kaiyuan Road Xi'an 710016 China Integrated Energy Institute Sichuan Digital Economy Industry Development Research Institute 88 Jiefang Road Chengdu 610036 China West Pipeline Company PipeChina 666 Beijing Middle Road Urumqi 830013 China School of Materials and Energy University of Electronic Science and Technology of China Chengdu 611731 China

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A ‐Oriented Hittorf's Phosphorus Nanorods/Polymeric Carbon Nitride Heterostructure for Boosting Wide‐Spectrum‐Responsive Photocatalytic Hydrogen Evolution from Pure Water

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Angewandte Chemie 2019年第2期132卷

作者： Yukun Zhu Chunxiao Lv Zhuocheng Yin Jun Ren Xianfeng Yang Chung‐Li Dong Hongwei Liu Rongsheng Cai Yu‐Cheng Huang Wolfgang Theis Shaohua Shen Dongjiang Yang State Key Laboratory of Bio-fibers and Eco-textiles Shandong Collaborative Innovation Center of Marine Biobased Fibers and Ecological Textiles Institute of Marine Biobased Materials School of Environmental Science and Engineering Qingdao University Qingdao 266071 P. R. China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 P. R. China School of Chemical and Environmental Engineering North University of China Taiyuan 030051 P. R. China Analytical and Testing Centre South China University of Technology Guangzhou 510640 P. R. China Research Center for X-ray Science & Department of Physics Tamkang University Tamsui 25137 Taiwan The Australian Centre for Microscopy & Microanalysis The University of Sydney Sydney New South Wales 2006 Australia Nanoscale Physics Research Laboratory School of Physics and Astronomy University of Birmingham Birmingham B15 2TT UK

Red phosphorus is a promising photocatalyst with wide visible‐light absorption up to 700 nm, but the fast charge recombination limits its photocatalytic hydrogen evolution reaction (HER) activity. Now, [001]‐oriented Hittorf's phosphorus (HP) nanorods were successfully grown on polymeric carbon nitride (PCN) by a chemical vapor deposition strategy. Compared with the bare PCN and HP, the optimized PCN@HP hybrid exhibited a significantly enhanced photocatalytic activity, with HER rates reaching 33.2 and 17.5 μmol h −1 from pure water under simulated solar light and visible light irradiation, respectively. It was theoretically and experimentally indicated that the strong electronic coupling between PCN and [001]‐oriented HP nanorods gave rise to the enhanced visible light absorption and the greatly accelerated photoinduced electron–hole separation and transfer, which benefited the photocatalytic HER performance.

关键词： Heterostrukturen Nanostäbe Hittorfscher Phosphor Kohlenstoffnitrid Wasserspaltung

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Pore-scale simulation of gas-water two-phase flow in volcanic gas reservoir based on Volume of Fluid method

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Journal of Natural Gas Science and engineering 2022年 106卷

作者： Yongfei Yang Quan Xu Xinze Li Lianjin Zhang Xuemei Lan Junjie Wang Kai Zhang Hai Sun Lei Zhang Jun Yao Key Laboratory of Unconventional Oil & Gas Development (China University of Petroleum (East China)) Ministry of Education Qingdao 266580 PR China Research Center of Multiphase Flow in Porous Media School of Petroleum Engineering China University of Petroleum (East China) Qingdao 266580 PR China Sichuan Oil and Gas Mine of Southwest Oil and Gas Field Company of PetroChina Chengdu 629000 Sichuan China Exploration and Development Research Institute of PetroChina Southwest Oil & Gas Field Company Cheng du 610041 Sichuan China

Understanding the transport process of gas-water flow in volcanic gas reservoir is of key importance for natural gas production . However, there is still limited evidence on the precise influence of volcanic reservoir type, capillary number and wettability . We thus performed gas-water flow simulations (using Volume of Fluid method) at different capillary numbers under different wettability conditions directly on microcomputed tomography (μ-CT) images. The simulation results demonstrated that the eddy current in dead-end corners is the main mechanism for the formation of residual gas . The gas phase near the wall of fractured porous medium was mainly dominated by drag force, resulting in lower residual gas saturation. Moreover, it is generally believed that a low capillary number facilitates the displacement of residual gas in dead-end corners. However, we found that under high temperature (>100 °C) and high pressure (>100 MPa), less residual gas distributed in dead-end corners at higher capillary number. This showed that the conventional percolation law was unlikely to provide reliable predictions in fluid distribution under high temperature and high pressure . The wettability of rock affected the shape of displacement front. The water-gas flow dynamics under water-wet condition was piston like. However, fingering flow occurred under non-hydrophilic condition, and snap-off trapping was more likely to occur, resulting in higher residual gas saturation. This work provides fundamental data on the influence of pore structure, capillary number and wettability on gas-water flow and aids in the further advancements of improved nature gas recovery in volcanic reservoirs.

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Solar Hydrocarbons: Single-Step, Atmospheric-Pressure Synthesis of C2−C4Alkanes and Alkenes from CO2

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Angewandte Chemie 2023年第27期135卷

作者： Rui Song Zhao Li Jiuli Guo Paul N. Duchesne Chenyue Qiu Chengliang Mao Jia Jia Sanli Tang Yang-Fan Xu Wenzhe Zhou Lu Wang Wei Sun Xiaoliang Yan Liejin Guo Dengwei Jing Geoffrey A. Ozin International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an Shaanxi 710049 China Solar Fuels Group Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 Canada Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (equal) Contribution: Data curation (supporting) Formal analysis (equal) Writing - original draft (supporting) School of Chemistry and Chemical Engineering Anyang Normal University Anyang Henan 455000 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (equal) Software (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Software (lead) Department of Materials Science and Engineering University of Toronto Toronto Ontario M5S 3E4 Canada Contribution: Data curation (supporting) Contribution: Conceptualization (supporting) Contribution: Formal analysis (supporting) Contribution: Methodology (supporting) State Key Laboratory of Silicon Materials and School of Materials Science and Engineering Zhejiang University Hangzhou Zhejiang 310058 China Contribution: Project administration (supporting) Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (equal) Project administration (equal) Supervision (equal) Writing - original draft (lead) Contribution: Conceptualization (lead) Funding acquisition (equal) Project administration (equal) Writing - original draft (lead)

Cobalt ferrite (CoFe 2 O 4 ) spinel has been found to produce C 2 −C 4 hydrocarbons in a single-step, ambient-pressure, photocatalytic hydrogenation of CO 2 with a rate of 1.1 mmol g −1 h −1 , selectivity of 29.8 % and conversion yield of 12.9 %. On stream the CoFe 2 O 4 reconstructs to a CoFe−CoFe 2 O 4 alloy-spinel nanocomposite which facilitates the light-assisted transformation of CO 2 to CO and hydrogenation of the CO to C 2 −C 4 hydrocarbons. Promising results obtained from a laboratory demonstrator bode well for the development of a solar hydrocarbon pilot refinery.

关键词： C2−C4 Hydrocarbons CO2 Hydrogenation Cobalt Ferrite Photocatalysis

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