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Single-atom catalysis for organic reactions

Chinese Chemical Letters 2023年第6期34卷 121-129页

作者： Hanyu Hu Jiangbo Xi Key Laboratory of Novel Biomass-Based Environmental and Energy Materials in Petroleum and Chemical Industry Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemistry and Environmental EngineeringWuhan Institute of TechnologyWuhan 430205China

Metal-based catalysis,including homogeneous and heterogeneous catalysis,plays a significant role in the modern chemical *** catalysis is widely used due to the high efficiency,easy catalyst separation and ***,the metal-utilization efficiency for conventional heterogeneous catalysts needs further improvement compared to homogeneous *** tackle this,the pursing of heterogenizing homogeneous catalysts has always been attractive but *** a recently emerging class of catalytic material,single-atom catalysts(SACs)are expected to bridge homogeneous and heterogeneous catalytic process in organic reactions and have arguably become the most active new frontier in catalysis *** this review,a brief introduction and development history of single-atom catalysis and SACs involved organic reactions are *** addition,recent advances in SACs and their practical applications in organic reactions such as oxidation,reduction,addition,coupling reaction,and other organic reactions are thoroughly *** understand structure-property relationships of single-atom catalysis in organic reactions,active sites or coordination structure,metal atom-utilization efficiency(e.g.,turnover frequency,TOF calculated based on active metal)and catalytic performance(e.g.,conversion and selectivity)of SACs are comprehensively ***,the application limitations,development trends,future challenges and perspective of SAC for organic reaction are discussed.

关键词： Single-atom catalysis Active site Metal utilization Organic reaction Catalytic performance

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Highly selective kinetic resolution of D/L-syn-p-sulfone phenylserine catalyzed by D-threonine aldolase in two-phase ionic solvent

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Green Chemical engineering 2023年第2期4卷 212-216页

作者： Fengfan Liu Zhihao Shi Jinmei Zhu Xiaobin Liang Mingming Liang Yuanyuan Xie Weike Su Jiequn Wu National Engineering Research Center for Process Development of Active Pharmaceutical Ingredients Collaborative Innovation Center of Yangtze River Delta Region Green PharmaceuticalsZhejiang University of TechnologyHangzhou310014China Key Laboratory for Green Pharmaceutical Technologies and Related Equipment of Ministry of Education and Pharmaceutical Engineering of Zhejiang Province College of Pharmaceutical SciencesZhejiang University of TechnologyHangzhou310014China

In the chemical synthesis of L-syn-p-methylsulfoxide phenylserine ethyl ester(D-ethyl ester),L-tartaric acid or enzymatic resolution is employed to resolve the racemate,and thus obtain the target compound,and the remaining isomer can be recycled to obtain the raw *** this study,high-purity L-syn-p-methylsulfoxide phenylserine(L-syn-MPS)was *** kinetics of the D-threonine aldolase enzymatic hydrolysis reaction reveals that D-syn-p-sulfoxylphenylserine resolves well in[BMIM][BF 4]ionic *** D/L-syn-MPS racemate was resolved using a two-phase ionic solvent[BMIM][NTf 2]to afford L-syn-MPS(ee(enantiomeric excess)>99%)and a white solid in 41.7%***,this system is suitable for the separation of insoluble aldehydes and successfully avoids the condensation of hydroxyl aldehydes to form D-anti-MPS.

关键词： Kinetic resolution Ionic solvent Enzymatic resolution D/L-p-sulphoxyl phenylserine ethyl ester Biphasic reaction system

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Unveiling the geometric site dependent activity of spinel Co_(3)O_(4)for electrocatalytic chlorine evolution reaction

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Journal of Energy Chemistry 2024年第5期92卷 95-103页

作者： Linke Cai Yao Liu Jingfang Zhang Qiqi Jia Jiacheng Guan Hongwei Sun Yu Yu Yi Huang Key Laboratory of Pesticide&Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079HubeiChina Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering&PharmacyWuhan Institute of TechnologyWuhan 430205HubeiChina College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108FujianChina School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601AnhuiChina

Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost ***,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the Co_(Oh) site acts as the main active site for CER in spinel Co_(3)O_(4),which shows better Cl^(-)adsorption and more moderate intermediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condition at applied *** by above findings,the oxygen vacancies were further introduced into the Co_(3)O_(4) to precisely manipulate the electronic configuration of Co_(Oh) to boost Cl^(-)adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity *** work figures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.

关键词： Chlorine evolution reaction Geometry effects Active chlorine Electronic configuration optimization Spinel oxides

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Green and selective hydrogenation of aromatic diamines over the nanosheet Ru/g-C_(3)N_(4)-H_(2) catalyst prepared by ultrasonic assisted impregnation-deposition method

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Green Energy & Environment 2022年第6期7卷 1361-1376页

作者： Huanhuan Yang Liguo Wang Shuang Xu Yan Cao Peng He Jiaqiang Chen Zheng Zheng Huiquan Li Key Laboratory of Green Process and Engineering National Engineering Laboratory for Hydrometallurgical Cleaner Production TechnologyInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China Chemical and Biochemical Engineering Technical University of DenmarkLyngby 2800 KgsDenmark Sino-Danish College University of Chinese Academy of SciencesBeijing100049China Sino-Danish Center for Education and Research University of Chinese Academy of SciencesBeijing100049China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Dalian National Laboratory for Clean Energy Dalian116023China

In this study,nanosheet g-C_(3)N_(4)-H_(2) was prepared by thermal exfoliation of bulk g-C_(3)N_(4) under hydrogen.A series of Ru/g-C_(3)N_(4)-H_(2) catalysts with Ru species supported on the nanosheet g-C_(3)N_(4)-H_(2) were synthesized via ultrasonic assisted impregnation-deposition *** Ru nanoparticles(<2 nm)were highly dispersed on nanosheet g-C_(3)N_(4)-H_(2).Strong interaction due to Ru-Nx coordination facilitated the uniform distribution of Ru ***,the involvement of surface basicity derived from abundant nitrogen sites was favourable for enhancing the selective hydrogenation performance of bi-benzene ring,i.e.,almost complete 4,40-diaminodiphenylmethane(MDA)conversion and>99%4,40-diaminodicyclohexylmethane selectivity,corresponding to a reaction activity of 35.7 mol_(MDA) mol_(Ru)^(-1) h^(-1).Moreover,the reaction activity of catalyst in the fifth run was 36.5 mol_(MDA) mol_(Ru)^(-1) h^(-1),which was comparable with that of the fresh *** computational results showed that g-C_(3)N_(4) as support was favorable for adsorption and dissociation of H_(2) ***,the substrate scope can be successfully expanded to a variety of other aromatic ***,this work provides an efficient and green catalyst system for selective hydrogenation of aromatic diamines.

关键词： Nanosheet carbon nitride Ultrafine Ru species Selective hydrogenation Aromatic diamine Alicyclic diamine

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State-of-the-art evolution of g-C_(3)N_(4)-based photocatalytic applications:A critical review

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Chinese Journal of Structural Chemistry 2024年第12期43卷 113-129页

作者： Yanghanbin Zhang Dongxiao Wen Wei Sun Jiahe Peng Dezhong Yu Xin Li Yang Qu Jizhou Jiang School of Environmental Ecology and Biological Engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan430205PR China Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan430074PR China College of Forestry and Landscape Architecture South China Agricultural UniversityGuangzhou510642PR China Key Laboratory of Functional Inorganic Materials Chemistry(Ministry of Education) School of Chemistry and Materials ScienceInternational Joint Research Center for Catalytic TechnologyHeilongjiang UniversityHarbin150080PR China

g-C_(3)N_(4)is a promising non-metallic photocatalyst recognized for its unique structural and physicochemical *** reviews have addressed g-C_(3)N_(4)-based photocatalysis;however,the rapid progress in big data and artificial intelligence has significantly accelerated the design,synthesis,and optimization of these *** learning,theoretical simulations,and advanced in-situ characterization techniques have deepened our understanding of their photocatalytic *** review critically evaluates advancements in g-C_(3)N_(4)-based photocatalysts over the last two to three years,focusing on strategies to improve photogenerated charge sepa-ration,expand light absorption,and enhance stability and catalytic *** discusses cutting-edge in-situ characterization methods alongside machine learning approaches for predicting and optimizing applications in photocatalytic H_(2)evolution,CO_(2)reduction,pollutant degradation,H_(2)O_(2)production,and nitrogen ***,it proposes prospective strategies for further enhancing the performance of g-C_(3)N_(4)-based photocatalysts,aiming to guide the design of high-performance two-dimensional carbon-based photocatalysts.

关键词： g-C_(3)N_(4) Photocatalysis Enhancement strategies In-situ characterization Theoretical simulations

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Excess pore pressure behavior and evolution in deep coalbed methane reservoirs

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International Journal of Mining Science and Technology 2024年第6期34卷 763-781页

作者： Changqing Liu Zhaobiao Yang Yong Qin Xia Yan Yunhai Wang Zhe Wang Key Laboratory of Coalbed Methane Resources and Reservoir Formation Process Ministry of EducationChina University of Mining and TechnologyXuzhou 221008China School of Resources and Geosciences China University of Mining and TechnologyXuzhou 221116China National Engineering Research Center of Coalbed Methane Development&Utilization Beijing 100095China PetroChina Coalbed Methane Company Limited Beijing 102200China SINOPEC East China Oil and Gas Company Nanjing 210000China

Deep coalbed methane(DCBM),an unconventional gas reservoir,has undergone significant advancements in recent years,sparking a growing interest in assessing pore pressure dynamics within these *** some production data analysis techniques have been adapted from conventional oil and gas wells,there remains a gap in the understanding of pore pressure generation and evolution,particularly in wells subjected to large-scale hydraulic *** address this gap,a novel technique called excess pore pressure analysis(EPPA)has been introduced to the coal seam gas industry for the first time to our knowledge,which employs dual-phase flow principles based on consolidation *** technique focuses on the generation and dissipation for excess pore-water pressure(EPWP)and excess pore-gas pressure(EPGP)in stimulated deep coal *** have been developed respectively and numerical solutions have been provided using the finite element method(FEM).Application of this model to a representative field example reveals that excess pore pressure arises from rapid loading,with overburden weight transferred under undrained condition due to intense hydraulic fracturing,which significantly redistributes the weight-bearing role from the solid coal structure to the injected fluid and liberated gas within artificial pores over a brief ***,field application indicates that the dissipation of EPWP and EPGP can be actually considered as the process of well production,where methane and water are extracted from deep coalbed methane wells,leading to consolidation for the artificial ***,history matching results demonstrate that the excess-pressure model established in this study provides a better explanation for the declining trends observed in both gas and water production curves,compared to conventional practices in coalbed methane reservoir engineering and petroleum *** research not only enhances the understanding of DCBM re

关键词： Deep coalbed methane Consolidation Excess pore-water pressure Excess pore-gas pressure Production data analysis

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Carbon nanofiber catalysts containing high-entropy metal phosphides with low-content Ru for highly efficient hydrogen evolution reaction

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Rare Metals 2025年第1期44卷 324-335页

作者： Peng Wang Jie Zheng Xue-Hao Li Wen-Bo Cui Jin-Hua Liu Yong Wan Jun Zhang Yusuke Yamauchi Zhong-Li Wang Mang Niu Yun-Ze Long Shandong Key Laboratory of Medical and Health Textile Materials College of PhysicsQingdao UniversityQingdao 266071China Industrial Research Institute of Nonwovens and Technical Textiles Shandong Center for Engineered Nonwovens(SCEN)College of Textiles ClothingQingdao UniversityQingdao 266071China State Key Laboratory of Bio-Fibers and Eco-textiles Institute of Biochemical EngineeringCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology(AIBN) The University of QueenslandBrisbaneQLD 4072Australia Department of Chemical and Biomolecular Engineering Yonsei UniversitySeoul 03722Republic of Korea Department of Materials Process Engineering Graduate School of EngineeringNagoya UniversityNagoya 464-8603Japan Tianjin Key Laboratory of Applied Catalysis Science and Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

High-entropy metal phosphide(HEMP)has considerable potential as an electrocatalyst owing to its beneficial properties,including high-entropy alloy synergy as well as the controllable structure and high conductivity of ***,electrospinning and in situ phosphating were employed to prepare three-dimensional(3D)networks of self-supporting HEMP nanofibers with varying degrees of phosphate *** characterizations via X-ray diffraction and X-ray photoelectron spectroscopy,as well as density functional theory calculations,demonstrate that the introduction of phosphorus(P)atoms to HEMP carbon nanofibers mediates their electronic structure,leads to lattice expansion,which in turn enhances their catalytic performance in the hydrogen evolution reaction(HER).Moreover,the formation of metal-P bonds weakens metal-metal interaction and decreases the free energy of hydrogen adsorption,contributing to the exceptional activity observed in the HEMP *** measurements demonstrate that the HEMP-0.75 catalyst with an ultralow loading of 1.22 wt%ruthenium(Ru)exhibits the highest HER catalytic activity and stability in a 1 M KOH electrolyte,achieving a minimal overpotential of 26 mV at a current density of 10 mA·cm^(-2)and Tafel slope of 50.9 mV·dec^(-1).

关键词： High-entropy metal phosphide Electrospinning Hydrogen evolution reaction Self-supporting carbon nanofibers

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Designing lab-on-a-chip systems with attribute dependency graphs

Designing lab-on-a-chip systems with attribute dependency gr...

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2024 International Design Society Conference, Design 2024

作者： Soika, Johannes Wanninger, Tobias Muschak, Patrick Schwaminger, Sebastian Berensmeier, Sonja Zimmermann, Markus Laboratory for Product Development and Lightweight Design TUM School of Engineering and Design Technical University of Munich Germany Bioseparation Engineering TUM School of Engineering and Design Technical University of Munich Germany Division of Medicinal Chemistry Otto Loewi Research Center Medical University of Graz Austria Munich Institute for Integrated Materials Energy and Process Engineering Technical University of Munich Germany

Lab-on-a-Chip (LOC) products for point-of-care diagnostics have gained significant attention. However, there is a lack of systematic approaches for LOC product development. To address this, we introduce an Attribute Dependency Graph exemplary for a magnetophoretic LOC system for pathogen detection. This model organizes dependencies between the design variables and crucial quantities of interest, such as detectability, cost per test, and test duration. The obtained model helps to manage design complexity and can be adapted to other LOC approaches. © 2024 Proceedings of the Design Society. All rights reserved.

关键词： Lab-on-a-chip

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Bioactive Ions-Loaded Bioinks Primed for 3D Printing of Artificial Tissues

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Biomedical Materials and Devices 2024年第2期2卷 811-833页

作者： Jo, Hyo Jung Kang, Moon Sung Kim, Jeong Min Raja, Iruthayapandi Selestin Jang, Hee Jeong Park, Kyung Min Han, Dong-Wook Department of Cogno-Mechatronics Engineering College of Nanoscience and Nanotechnology Pusan National University Department of Bioengineering and Nano-Bioengineering College of Life Sciences and Bioengineering Incheon National University Institute of Nano-Bio Convergence Pusan National University Research Center for Bio Materials & amp Process Development Incheon National University

Bioactive ions have become increasingly important in tissue engineering due to their ability to improve cellular activity by modifying both cell–material and cell–cell interactions. Inorganic biomaterials have additional attributes such as mechanical properties and drug delivery. Recently, many studies have focused on fabricating three-dimensional (3D) scaffolds utilizing inorganic ions, such as bioceramics and bioactive glass, using 3D bioprinting technology. 3D bioprinting has emerged as a focal point for innovative tissue and organ reconstruction approaches. The aim of this review is to summarize the mechanisms by which inorganic ions affect the regeneration of tissues and to summarize research on 3D-printed scaffolds utilizing bioactive ions. The review summarizes how recently used inorganic ions induce biological responses in tissue regeneration through signal transduction pathways. Studies on 3D-printed scaffolds using newly developed inorganic ion-releasing hydrogels were summarized, focusing on functions that improved cell proliferation and differentiation ability or increased effectiveness in in-vivo experiments. Finally, the review discusses the difficulties and prospects for scaffolds using these inorganic ion-releasing bioinks. © The Author(s), under exclusive licence to Springer Science+Business Media, LLC 2024.

关键词： 3D bioprinting Bioactive ions Bioinks Hydrogel Tissue engineering

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Machine Learning-Based Sobol Sensitivity Analysis for Building Energy Assessment without Monte Carlo Integral 18

Machine Learning-Based Sobol Sensitivity Analysis for Buildi...

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18th IBPSA Conference on Building Simulation, BS 2023

作者： Zhang, Hu Tian, Wei Sambatmaryde, Kheng Tan, Jingyuan Chen, Bo College of Mechanical Engineering Tianjin University of Science and Technology China Tianjin International Joint Research and Development Center of Low-Carbon Green Process Equipment Tianjin China College of Economics and Management Tianjin University of Science and Technology China

Sensitivity analysis would be very useful to prioritize energy-saving measures for both new and existing buildings. The variance-based Sobol sensitivity analysis can provide reliable sensitivity results at the expense of high computational costs. The BASS (Bayesian Adaptive Spline Surfaces) method is one of the efficient approaches to reduce computational time without Monte Carlo integrals. The performance of this new type of sensitivity analysis is much less studied in building energy assessment. An office building is used to demonstrate the performance of BASS sensitivity analysis by combining the EnergyPlus program. Results indicate that the BASS method can provide robust and reliable sensitivity results compared to the conventional sampling-based Sobol sensitivity analysis. Sufficient data is required to obtain stable results of the BASS sensitivity analysis and the variations of total effects using the bootstrap technique. © 2023 *** rights reserved.

关键词： Sensitivity analysis

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