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Interface engineering of Z-scheme heterojunction for photocatalytic water splitting

Fundamental Research 2024年

作者： Daming Zhao Yuxiao Yang Vasileios Binas Shaohua Shen School of Advanced Energy Shenzhen Campus of Sun Yat-sen University Shenzhen 518107 China Institute of Electronic Structure and Laser (IESL) FORTH P.O. Box 1527 Vasilika Vouton GR-71110 Heraklion Greece Physical Chemistry Laboratory Chemistry Department Aristotle University of Thessaloniki 54124 Thessaloniki Greece International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China

Photocatalytic water splitting technology can directly convert solar energy into H 2 via a zero-carbon route, offering a sustainable solution for solar utilization and H 2 supply. Among various developed photocatalysts, Z-scheme heterojunction mimicking natural photosynthesis by combining two dissimilar semiconductors for redox reactions in series has unequivocally demonstrated its superiority in enhanced charge transfer, robust redox driving force, and wide optical absorption range. A comprehensive understanding on the fundamental principles of interface engineering between semiconductor components is the key to construct an efficient Z-scheme heterojunction. By focusing on different types of semiconductors, this article thoroughly expounds the coupling principles of components in binary mediator-free and ternary solid-mediator Z-scheme heterojunctions for photocatalytic water splitting, from the viewpoint of band structure alignment and interfacial electric field design. In addition to the well summarized research progresses in recent years, perspectives on the challenges and opportunities for developing advanced Z-scheme heterojunctions are provided.

关键词： Interface engineering Z-scheme heterojunction Water splitting Photocatalysis Solar energy conversion

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Photo-Triggered Fluorescence Polyelectrolyte Nanoassemblies: Manipulate and Boost Singlet Oxygen in Photodynamic Therapy

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Angewandte Chemie 2024年第2期137卷

作者： Dr. Yongkang Yao Dr. Shangjun Chen Dr. Chenxu Yan Prof. Dr. Junyou Wang Prof. Dr. Jianjun Liu Prof. Dr. Wei-Hong Zhu Prof. Dr. Chunhai Fan Prof. Dr. Zhiqian Guo Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Shanghai Key Laboratory of Functional Materials Chemistry Feringa Nobel Prize Scientist Joint Research Center Institute of Fine Chemicals Frontiers Science Center for Materiobiology and Dynamic Chemistry School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 China Institute of Molecular Medicine Renji Hospital School of Medicine Shanghai Jiao Tong University Shanghai 200127 China Key Laboratory of Resource Chemistry of Ministry of Education Shanghai Key Laboratory of Rare Earth Functional Materials Department of Chemistry Shanghai Normal University Shanghai 200234 China State Key Laboratory of Chemical Engineering and Shanghai Key Laboratory of Multiphase Materials Chemical Engineering East China University of Science and Technology Shanghai 200237 China State Key Laboratory of Bioreactor Engineering Shanghai Frontier Science Research Base of Optogenetic Techniques for Cell Metabolism East China University of Science and Technology Shanghai 200237 China

Photodynamic therapy (PDT) is a clinically approved therapeutic modality that has shown great potential for cancer treatment. However, there exist two major problems hindering PDT applications: the nonspecific phototoxicity requiring patients to stay in dark post-PDT, and the limited photodynamic efficiency. Herein, we report a photo-triggered porphyrin polyelectrolyte nanoassembling (photo-triggered PPN) strategy, in which porphyrin photosensitizer and photoswitchable energy accepter are assembled into polyelectrolyte micelles by a combined force of charge interaction and metal-ligand coordination. The polyelectrolyte-based PPN exhibits good biocompatibility, and bestows a unique “confining isolated” inner microenvironment for fully overcoming the π–π stacking of porphyrins with significant photodynamic efficiency (123-fold enhancement). Due to the high Förster resonance energy transfer (FRET) (91.5 %) between porphyrin and photoswitch in closed-form, we could use light as a specific trigger to modulate photoswitch between closed- and open-form, and manipulate the 1 O 2 generation in three stages: pre-PDT (quenching 1 O 2 generation), during PDT (activating 1 O 2 generation), and post-PDT (silencing 1 O 2 generation). This de novo strategy has for the first time realized remotely manipulating and boosting 1 O 2 generation in PDT, well resolving the critical and general challenges of limited photodynamic efficiency and side effects from nonspecific phototoxicity.

关键词： fluorescent probe near-infrared fluorescence photodynamic therapy polyelectrolyte

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Excess thermodynamic properties and FTIR studies of binary of 1, 3-dichlorobenzene with alkyl acetates (C1–C5) at different temperatures

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Chemical Data Collections 2020年 29卷

作者： R. Raju S. Ravikumar R. Gerald Arokiaraj S. Karlapudi K. Sivakumar V. Pandiyan Department of Physics Nehru Memorial College (Autonoums) Puthanampatti 621 007Tamil Nadu India. State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Shaanxi 710049 P. R. China. Department of Chemistry S.V.Arts Degree & P.G.College (T.T.D'S) Tirupati 517502 A.P India

Densities ( ρ ) and speed of sound ( u ) have been reported for the binary mixtures containing 1, 3- dichlorobenzene (1, 3-DCB) with methyl acetate, ethyl acetate, propyl acetate, butyl acetate and pentyl acetate at four different temperatures ( T = 303.15, 308.15, 313.15 and 318.15 K) and at atmospheric pressure. The experimental data of densities and speeds of sound has been further utilized to calculate excess molar volume ( V m E ) and excess isentropic compressibility ( κ S E ) the excess properties have been fitted to Redlich-Kister equation. Further, V m E results have also been discussed by using Prigogine–Flory–Patterson (PFP). The experimental speeds of sound data in the present investigated mixtures were compared with various theoretical models like collision factor theory (CFT) and free length theory (FLT) to check their relative merits of pure component properties. Moreover, the experimental excess functions were correlated in terms of FTIR spectral analysis.

关键词： Binary mixtures Densities Ester Halogenated benzene Speed of sound FTIR

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Pore-scale simulation of remaining oil distribution in 3D porous media affected by wettability and capillarity based on volume of fluid method

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International Journal of multiphase flow 2021年 143卷

作者： Yongfei Yang Shaobin Cai Jun Yao Junjie Zhong Kai Zhang Wenhui Song Lei Zhang Hai Sun Vadim Lisitsa 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 Petroleum Geology and Geophysics SB RAS Novosibirsk 630090 Russia

Characterizing the trapped phase in porous media is essential for many engineering applications, such as enhanced oil recovery, nuclear storage, and geological sequestration of CO 2 . This study aims to study the distribution, evolution, and influencing factors of the remaining oil in the process of water flooding at the pore scale. The single-connected pore space model was established by reconstructing the real micron CT scanned images of carbonate rocks. The VOF (volume of fluid) method using FSF (filtered surface force) formulation was adopted on OpenFOAM platform to simulate the oil-water two-phase flow process at the pore scale. Different wettability and capillary number were considered in the model. The accuracy of the model was proved by comparing with previous experimental results. The results showed that in the process of water flooding, the complex pore structure would lead to the generation of remaining oil, and the phase circulation phenomenon can be observed in the remaining oil and presents two distribution forms: co-current driven flow and lid-cavity driven flow. It also revealed that the phase recirculation increases the viscous dissipation. Further research also showed that the two forms of recirculation could be transferred by changing the wettability and that a higher capillary number was more beneficial for reducing the remaining oil saturation.

关键词： Pore-scale modeling VOF Remaining oil Phase recirculation Capillary number Wettability

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Corrigendum to “Assessing the capability of continuum and discrete particle methods to simulate gas-solids flow using DNS predictions as a benchmark” [Powder technology 321 (2017) 301–309]

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Powder Technology 2019年 349卷 109-109页

作者： Liqiang Lu Xiaowen Liu Tingwen Li Limin Wang Wei Ge National Energy Technology Laboratory Morgantown 26507 West Virginia United States State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering (IPE) Chinese Academy of Sciences (CAS) Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China AECOM Morgantown 26505 West Virginia United States

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Ausgeprägte Nahordnung in kleinen amorphen Calciumcarbonat‐Clustern (<2 nm)

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Angewandte Chemie 2016年第40期128卷

作者： Shengtong Sun Daniel M. Chevrier Peng Zhang Denis Gebauer Helmut Cölfen Physikalische Chemie Universität Konstanz Universitätsstraße 10 78457 Konstanz Deutschland School of Chemical Engineering State Key Laboratory of Chemical Engineering Shanghai Key Laboratory of Multiphase Materials Chemical Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 Volksrepublik China Department of Chemistry and Institute for Research in Materials Dalhousie University Halifax Nova Scotia B3H 4R2 Kanada

Amorphe Zwischenphasen sind wichtige Vorstufen bei der Kristallisation vieler biogener Minerale. Obwohl bereits gezeigt werden konnte, dass amorphe Calciumcarbonate (ACC) eine inhärente Nahordnung aufweisen, die unterschiedlichen kristallinen Formen zugeordnet werden kann, wurde bisher noch nie experimentell bestätigt, ob solche Nahordnungen bereits in sehr kleinen Clustern (<2 nm) vorkommen. Hier wurde die Stabilität und Struktur von 10,12‐Pentacosadiinsäure(PCDA)‐geschützten ACC‐Clustern untersucht, die eine Kerngröße von ca. 1.4 nm aufweisen und aus nur 7 CaCO 3 ‐Einheiten bestehen. Die Ligandenkonzentration und ‐struktur spielt eine Schlüsselrolle bei der Stabilisierung dieser ACC‐Cluster. Schon solch kleine CaCO 3 ‐Einheiten weisen eine Proto‐Calcit‐Nahordnung auf, wenn auch mit relativ hoher Unordnung. Dies legt nahe, dass ein struktureller Zusammenhang zwischen Pränukleationsclustern, amorphen Zwischenstufen und dem fertigen kristallinen Polymorph besteht.

关键词： Amorphe Materialien Calciumcarbonat-Cluster Carboxylatliganden EXAFS Nahordnung

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Poly(ionic liquid)-Armored MXene Membrane: Interlayer engineering for Facilitated Water Transport

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Angewandte Chemie 2022年第27期134卷

作者： Ming Yi Mi Wang Prof. Yan Wang Prof. Yanlei Wang Jian Chang Atefeh Khorsand Kheirabad Hongyan He Prof. Jiayin Yuan Dr. Miao Zhang Key Laboratory of Material Chemistry for Energy Conversion and Storage Huazhong University of Science and Technology Wuhan 430074 P. R. China Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 P. R. China Department of Materials and Environmental Chemistry Stockholm University Stockholm 10691 Sweden Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China

Two-dimensional (2D) MXene-based lamellar membranes bearing interlayers of tunable hydrophilicity are promising for high-performance water purification. The current challenge lies in how to engineer the pore wall's surface properties in the subnano-confinement environment while ensuring its high selectivity. Herein, poly(ionic liquid)s, equipped with readily exchangeable counter anions, succeeded as a hydrophilicity modifier in addressing this issue. Lamellar membranes bearing nanochannels of tailorable hydrophilicity are constructed via assembly of poly(ionic liquid)-armored MXene nanosheets. By shifting the interlayer galleries from being hydrophilic to more hydrophobic via simple anion exchange, the MXene membrane performs drastically better for both the permeance (by two-fold improvement) and rejection (≈99 %). This facile method opens up a new avenue for building 2D material-based membranes of enhancing molecular transport and sieving effect.

关键词： Anion Exchange Assembly MXene Nanochannel Hydrophilicity Poly(Ionic Liquid)

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Machine Learning and Physics-Driven Modelling and Simulation of multiphase Systems

SSRN

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SSRN 2024年

作者： Basha, Nausheen Arcucci, Rossella Angeli, Panagiota Anastasiou, Charitos Abadie, Thomas Casas, César Quilodrán Chen, Jianhua Cheng, Sibo Chagot, Loïc Galvanin, Federico Heaney, Claire E. Hossein, Fria Hu, Jinwei Kovalchuk, Nina Kalli, Maria Kahouadji, Lyes Kerhouant, Morgan Lavino, Alessio Liang, Fuyue Nathanael, Konstantia Magri, Luca Lettieri, Paola Materazzi, Massimiliano Erigo, Matteo Pico, Paula Pain, Christopher C. Shams, Mosayeb Simmons, Mark Traverso, Tullio Valdes, Juan Pablo Wolffs, Zef Zhu, Kewei Zhuang, Yilin Matar, Omar K. Department of Chemical Engineering Imperial College London United Kingdom Department of Earth Science & Engineering Imperial College London United Kingdom Department of Chemical Engineering University College London United Kingdom School of Chemical Engineering University of Birmingham United Kingdom Data Science Institute Department of Computing Imperial College London United Kingdom State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing China Centre for AI-Physics Modelling Imperial-X White City Campus Imperial College London United Kingdom The Alan Turing Institute British Library 96 Euston Road LondonNW1 2DB United Kingdom Department of Aeronautics Imperial College London United Kingdom Institute of Physics University of Amsterdam Science Park Amsterdam904 Netherlands Nikhef Science Park Amsterdam105 Netherlands Department of Computer Science University of York United Kingdom

We highlight the work of a multi-university collaborative programme, PREMIERE (PREdictive Modelling with QuantIfication of UncERtainty for multiphase Systems), which is at the intersection of multi-physics and machine learning, aiming to enhance predictive capabilities in complex multiphase flow systems across diverse length and time scales. Our contributions encompass a variety of approaches, including the Design of Experiments for nanoparticle synthesis optimisation, Generalised Latent Assimilation models for drop coalescence prediction, Bayesian regularised artificial neural networks, eXtreme Gradient Boosting for microdroplet formation prediction, and a sub-sampling based adversarial neural network for predicting slug flow behaviour in two-phase pipe flows. Additionally, we introduce a generalised latent assimilation technique, Long Short-Term Memory networks for sequence forecasting mixing performance in stirred and static mixers, active learning via Bayesian optimisation to recover coalescence model parameters for high current density electrolysers, Gaussian process regression for drop size distribution predictions for sprays, and acoustic emission signal inversion using gradient boosting machines to characterise particle size distribution in fluidised beds. We also offer perspectives on the development of a shape optimisation framework that leverages the use of a multi-fidelity multiphase emulator. The results presented have applications in chemical synthesis, microfluidics, product manufacturing, and green hydrogen generation. © 2024, The Authors. All rights reserved.

关键词： Forecasting

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Changes in relative permeability curves for natural gas hydrate decomposition due to particle migration

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Journal of Natural Gas Science and engineering 2020年 84卷

作者： Yushu Wang Yongfei Yang Ke Wang Liu Tao Jie Liu Chenchen Wang Jun Yao Kai Zhang Wenhui Song 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 Hubei Cooperative Innovation Center of Unconventional Oil and Gas Yangtze University Wuhan 430100 China

It is very important to study the fluid flow in a natural gas hydrate (NGH) reservoir for hydrate exploitation. During the decomposition of NGH, some particles fall off and flow with the fluid as a result of poor cementation , which usually leads to sand production in the hydrate mining process. In this study, a three-dimensional pore network model (PNM) was established to simulate the three-phase flow of the gas phase (CH 4 ), water phase, and solid phase (particles). Relevant parameters were set considering the deposition, blockage, and flow in the process of particle migration. Then, the gas–water relative permeability curves under different hydrate saturations, particle diameters, and particle numbers were obtained, considering the influence of the change in the pore-throat space during the hydrate decomposition process . The results showed that the gas–water relative permeability equal points (isotonic points) first turned toward the left and then to the right. The analysis results showed that particle deposition and blockage mainly influenced the relative permeability curves during the early period of the hydrate decomposition process. An increase in the pore-throat space was the main factor affecting the relative permeability curves in the late period of the hydrate decomposition process. Moreover, increasing the particle diameter and number of particles caused the isosmotic points of the relative permeability curves moving to the left as a whole because the pore-throat space decreased. Increasing the number of particles first affected the fluid flow in the hydrate reservoir when the temperature was 280 K, pressure was 5.76 MPa, and hydrate saturation was 0.48. In the actual hydrate mining process, this could cause sudden changes in the relative permeability and production. Thus, this condition needs to be avoided. It has important significance in reference to the process of hydrate mining with sand production.

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Calcined [email protected] @Rh x Ni 1- x : A novel hierarchically oriented composition tunable catalyst for green and sustainable hydrogen generation

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Journal of Environmental Chemical engineering 2022年第3期10卷

作者： Yasir Abbas Zareen Zuhra Sahresh Majeed Muhammad Shuaib Khan Majid Basharat Deependra Tyagi Shafqat Ali Zhanpeng Wu Zhaojun Liu Department of Electrical and Electronic Engineering Southern University of Science and Technology 1088 Xueyuan Blvd Nanshan District Shenzhen 518055 PR China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 PR China Department of Environment and Civil Engineering Dongguan University of Technology Dongguan 523808 PR China Institute of Chemical Sciences Bahauddin Zakariya University Multan 60800 Pakistan International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MPFE) Xi’an Jiaotong University Xi’an 710049 PR China Institute for Advanced Study Shenzhen University Nanhai Avenue 3688 Shenzhen 518060 PR China

The ever decreasing amount of fossil fuels and increasing environmental pollution are alarming threats for green and sustainable future. Designing a new catalyst is, therefore, of paramount significance in the quest to discover sustainable, robust, and environmentally benign materials for clean and sustainable energy generation. Herein, we developed a hierarchically oriented catalyst of calcined poly(ferrocenedimethano)-cyclotriphosphazene-microspheres (CPFC-MS) supported with nickel-aluminum layered double hydroxide and decorated with nanoparticles (NPs) of rhodium-nickel, [email protected] x Ni 1 - x ( x = 2.06–6.75), for H 2 generation from ammonia borane (AB) hydrolysis . The highly active catalyst was characterized by scanning electron microscopy (SEM), Raman spectroscopy , high-resolution transmission electron microscopy (HRTEM) and TEM, energy dispersive X-ray spectroscopy (EDX), fourier transform infrared (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS). The as-fabricated [email protected] @Rh x Ni 1- x ( x = 2.06–6.75) catalysts were tested for AB hydrolysis and the results showed remarkable performance and higher stability for H 2 generation. The [email protected] @Rh 2.06 Ni 7.32 catalyst, having the lowest Rh-contents, exhibited maximum H 2 generation with a turn over frequency (TOF) of 780 mol H 2 hr −1 mol Rh −1 and an activation energy (E a ) of 40.3 kJ/mol with excellent sustainability . The superior activity is ascribed to the synergetic effect between RhNi NPs and their well-dispersion over hierarchically oriented [email protected] support, while higher stability due to LDH-AlNi/RhNi attractions. This work will provide new opportunities for polyphosphazenes and LDH derived hierarchically oriented sustainable catalysts for green energy production for sustainable future.

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