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Balancing electron transfer and intermediate adsorption ability of metallic Ni-Fe-RE-P bifunctional catalysts via 4f-2p-3d electron interaction for enhanced water splitting

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Journal of Energy Chemistry 2024年第7期94卷 458-465页

作者： Hong-Rui Zhao Cheng-Zong Yuan Chenliang Zhou Wenkai Zhao Lunliang Zhang Cong-Hui Li Lei Xin Fuling Wu Shufeng Ye Xiaomeng Zhang Yunfa Chen School of Rare Earths University of Science and Technology of ChinaHefei 230026AnhuiChina Jiangxi Province Research Institute of Rare Earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou 341119JiangxiChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking efficient ***,one efficient and universal strategy is developed to greatly regulate electronic structures of the metallic Ni-Fe-P catalysts via in-situ introducing the rare earth(RE)atoms(Ni-Fe-RE-P,RE=La,Ce,Pr,and Nd).Accordingly,the as-prepared optimal Ni-Fe-Ce-P/CC self-supported bifunctional electrodes exhibited superior electrocatalytic activity and excellent stability with the low overpotentials of 247 and 331 mV at 100 mA cm^(-2) for HER and OER,*** the assembled electrolyzer,the Ni-Fe-Ce-P/CC as bifunctional electrodes displayed low operation potential of 1.49 V to achieve a current density of 10 mA cm^(-2),and the catalytic performance can be maintained for 100 *** results combined with density functional theory(DFT)calculation reveal that Ce doping leads to electron decentralization and crystal structure distortion,which can tailor the band structures and d-band center of Ni-Fe-P,further increasing conductivity and optimizing intermediate adsorption *** work not only proposes a valuable strategy to regulate the electron transfer and intermediate adsorption of electrocatalysts via RE atoms doping,but also provides a deep under-standing of regulation mechanism of metallic electrocatalysts for enhanced water splitting.

关键词： RE atoms Electron transfer Adsorption energy Oxygen evolution Hydrogen evolution

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Fluidization of Swelling Particles at Elevated Temperatures

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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 2023年第19期62卷 7671-7681页

作者： Xu, Qiushi Guan, Xiaoping Yang, Ning Chinese Acad Sci Inst Proc Engn State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China Univ Chinese Acad Sci Sch Chem Engn Beijing 100049 Peoples R China

Semicrystalline polymer (e.g., polyethylene and polypropylene) particles may swell in solvent at elevated temper-atures, inducing flow instability in operation, reactor blockage, and undesired product. Understanding the fluidization behavior of swelling particles at elevated temperatures is therefore of great significance. This work conducts an experimental study on the fluidization of polyethylene particles in an elevated-temperature liquid-solid fluidized bed. With the increase in temperature, particle swelling develops over two phases, i.e., non-cohesive swelling and cohesive swelling, which is different from the fluidization of cohesive particles in gas-solid systems. Four regimes can be identified through static bed height and pressure drop measurements, i.e., stable fluidization, noncohesive-swelling fluidization, cohesive-swelling fluidization, and full defluidization. A phase diagram was then obtained to demarcate these regimes. Furthermore, an energy balance model was proposed to predict the initial agglomerating temperature Tag of swelling particles for early warning of abnormal fluidization in practical operation.

关键词： Fluidization

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Universality class of machine learning for critical phenomena

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Science China(Physics,Mechanics & Astronomy) 2023年第12期66卷 63-70页

作者： Gaoke Hu Yu Sun Teng Liu Yongwen Zhang Maoxin Liu Jingfang Fan Wei Chen Xiaosong Chen School of Systems Science and Institute of Nonequilibrium Systems Beijing Normal UniversityBeijing 100875China Data Science Research Center Faculty of ScienceKunming University of Science and TechnologyKunming 650500China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Herein,percolation phase transitions on a two-dimensional lattice were studied using machine learning *** reveal that different phase transitions belonging to the same universality class can be identified using the same neural networks(NNs),whereas phase transitions of different universality classes require different *** on this finding,we proposed the universality class of machine learning for critical ***,we investigated and discussed the NNs of different universality *** research contributes to machine learning by relating the NNs with the universality class.

关键词： universality class machine learning percolation

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Preparation of Antibacterial Biobased Fibers by Triaxial Microfluidic Spinning Technology Using Ionic Liquids as the Solvents

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ACS APPLIED MATERIALS & INTERFACES 2024年第14期16卷 18063-18074页

作者： Zhao, Zhimin Wang, Junlei Yuan, Hanmeng Xu, Jie Gao, Hongshuai Nie, Yi Chinese Acad Sci Inst Proc Engn Beijing Key Lab Ion Liquids Clean Proc CAS State Key Lab Multiphase Complex SystCAS Key Beijing 100190 Peoples R China Univ Chinese Acad Sci Sch Chem Engn Beijing 100049 Peoples R China Zhengzhou Inst Emerging Ind Technol Zhengzhou 450000 Peoples R China

Bacterial infections have become a serious threat to public health. The utilization of antibacterial textiles offers an effective way to combat bacterial infections at the source, instead of relying solely on antibiotic consumption. Herein, efficient and durable antibacterial fibers based on quercetin and cellulose were prepared by a triaxial microfluidic spinning technology using ionic liquids (ILs) as the solvents. It was indicated that the structure and properties of the antibacterial fibers were affected by the type of IL and the flow rates during the triaxial microfluidic spinning process. Quercetin regenerated from [Emim]Ac underwent structural transformation and obtained an increased water solubility, while quercetin regenerated from [Emim]DEP remained unchanged, which was proven by FI-IR, XRD, and UV analyses. Furthermore, antibacterial fibers regenerated from [Emim]Ac exhibited the highest antibacterial activity of 96.9% against S. aureus, achieved by reducing the inner-to-outer flow rate ratio to 0 and concentrating quercetin at the center of fibers. On the other hand, when [Emim]DEP was used as the solvent, balancing the inner-to-outer flow rate ratio to concentrate quercetin in the middle layer of the fiber was optimal for achieving the best antibacterial activity of 93.3% because it promised both the higher encapsulation efficiency and release rate. Computational fluid dynamics (CFD) mathematically predicted the solvent exchange process during triaxial spinning, explaining the influence of IL types and flow rates on quercetin distribution and encapsulation efficiency. It was indicated that optimizing the distribution of antibacterial agents within the fibers can fully unleash its antibacterial potential while preserving the mechanical properties of the fiber. Therefore, the proposed simple triaxial spinning strategy provides valuable insights into the design of biomedical materials.

关键词： antibacterial fibers triaxial microfluidic spinningtechnology ionic liquid regenerated cellulosefibers computational fluid dynamics

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Liquid-phase esterification of methacrylic acid with methanol catalyzed by cation-exchange resin in a fixed bed reactor:Experimental and kinetic studies

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Chinese Journal of Chemical Engineering 2023年第6期58卷 1-10页

作者： Junyang Liu Luming Wang Yuhang Bian Chunshan Li Zengxi Li Jie Li School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Beijing Key Laboratory of Ionic Liquids Clean Process Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Langfang Technological Center of Green Industry Langfang 065801China

The kinetic behavior of esterification between methacrylic acid and methanol catalyzed by NKC-9 resin was studied in a fixed bed *** reaction was conducted in the temperature range of 323.15 to 368.15 K with the molar ratio of reactants from 0.8 to 1.4 under certain *** measurement data were regression with the pseudo-homogeneous(P-H),Eley-Rideal(E-R),and Langmuir-Hinshelwood(L-H)heterogeneous kinetic *** adsorption experiments were implemented to gain the adsorption equilibrium constants of four *** the above three models,the L-H model exhibited the best fitting *** stability of NKC-9 was evaluated by long-term running with the yield of methyl methacrylate no decrease during 3000 h *** structure and physicochemical properties of the new and used catalyst were performed by several characterizations including thermogravimetric analysis(TG),scanning electron microscope(SEM),X-ray diffraction(XRD)and Fourier transform infrared spectroscopy(FT-IR)and so on.

关键词： Kinetics Esterification Methyl methacrylate Cation-exchange resin Fix bed reactor

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Facile synthesis of Ni-phyllosilicate assisted by polyacrylamide at room temperature for CO2 hydrogenation to methane

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 2024年 71卷 81-87页

作者： Bi, Wenhui Guo, Qingbin Zhang, Tengfei He, Yan Liu, Qing Shandong Univ Sci & Technol Key Lab Low Carbon Energy & Chem Engn Qingdao 266590 Peoples R China Chinese Acad Sci State Key Lab Multiphase Complex Syst Inst Proc Engn Beijing 100190 Peoples R China Guangxi Univ Sch Chem & Chem Engn Guangxi Key Lab Petrochem Resource Proc & Proc Int Nanning 530004 Peoples R China

To elucidate the effect of solution viscosity on the synthesis of Ni-phyllosilicate, polyacrylamide was incorporated to create a viscous aqueous medium containing of sodium metasilicate, nickel nitrate and NH4F. The enhanced viscosity promotes the dispersion of the initial formed crystal seeds and the growth of Ni-phyllosilicate, culminating in a Ni-rich NiPs-RT-6 of a high Ni content of up to 55.2 wt%. Residual polyacrylamide elimination was accomplished via calcination, concurrently enhancing metal-support interaction. The as-synthesized samples display a nanoflower morphology with nanospheres overlaid with numerous thin nanosheets. The relatively small Ni particles around 5.7 nm were obtained after reduction even at a very high Ni loading, owing to its strong metal-support interaction. NiPs-RT-6 achieves a CO2 conversion of 75.9% at 450 degrees C, 0.1 MPa, 60 L g- 1 center dot h- 1, which closely approximates thermodynamic equilibrium. The turn over frequency for CO2 (TOFCO2) was substantial, calculated at 3.7 x 10- 3 s- 1, accompanied by activation energy (Ea) of 80.6 kJ center dot mol-1. In-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) further disclosed that m-HCOO- serves as a crucial intermediate following a formate reaction pathway. With its high Ni content, finely distributed Ni particles, and strong metal-support interaction, NiPs-RT-6 demonstrates promising catalytic activity in CO2 methanation.

关键词： Ni-phyllosilicate Polyacrylamide Stirring CO 2 methanation

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Resolving Ultraviolet-Visible Spectra for complex Dissolved Mixtures of Multitudinous Organic Matters in Aerosols

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ANALYTICAL CHEMISTRY 2024年第5期96卷 1834-1842页

作者： Xu, Nan Hu, Min Li, Xiao Song, Kai Qiu, Yanting Sun, Hao Xuan Wang, Yujue Zeng, Linghan Li, Mengren Wang, Hui Hu, Shuya Zong, Taomou Bai, Yao Zhang, Zhou Li, Shuangde Shuai, Shijin Chen, Yunfa Guo, Song Peking Univ Coll Environm Sci & Engn State Key Joint Lab Environm Simulat & Pollut Cont Int Joint Lab Reg Pollut Control Beijing 100871 Peoples R China Tsinghua Univ State Key Lab Automot Safety & Energy Beijing 100084 Peoples R China Chinese Acad Sci Inst Proc Engn State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China Peking Univ Ctr Data Sci Beijing 100871 Peoples R China

Light-absorbing organic aerosols, referred to as brown carbon (BrC), play a vital role in the global climate and air quality. Due to the complexity of BrC chromophores, the identified absorbing substances in the ambient atmosphere are very limited. However, without comprehensive knowledge of the complex absorbing compounds in BrC, our understanding of its sources, formation, and evolution mechanisms remains superficial, leading to great uncertainty in climatic and atmospheric models. To address this gap, we developed a constrained non-negative matrix factorization (NMF) model to resolve the individual ultraviolet-visible spectrum for each substance in dissolved organic aerosols, with the power of ultrahigh-performance liquid chromatography-diode array detector-ultrahigh-resolution mass spectrometry (UHPLC-DAD-UHRMS). The resolved spectra were validated by selected standard substances and validation samples. Approximately 40,000 light-absorbing substances were recognized at the MS1 level. It turns out that BrC is composed of a vast number of substances rather than a few prominent chromophores in the urban atmosphere. Previous understanding of the absorbing feature of BrC based on a few identified compounds could be biased. Weak-absorbing substances missed previously play an important role in BrC absorption when they are integrated due to their overwhelming number. This model brings the property exploration of complex dissolved organic mixtures to a molecular level, laying a foundation for identifying potentially significant compositions and obtaining a comprehensive chemical picture.

关键词： Absorption Aerosols Alcohols Mixtures Quantum mechanics

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Electrocatalytic reduction of furfural for selective preparation of 2-methylfuran over a trace Ni assisted Cu catalyst

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CATALYSIS SCIENCE & TECHNOLOGY 2023年第6期13卷 1846-1854页

作者： Cui, Yiming Wang, Ze Li, Songgeng Chinese Acad Sci Inst Proc Engn State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China Univ Chinese Acad Sci Sino Danish Coll Beijing 100190 Peoples R China

The electrocatalytic reduction (ECR) of furfural (FF) for the synthesis of 2-methylfuran (MF) with high octane number and calorific value is investigated, using a carbon-paper-supported Ni-Cu bimetallic material as a catalytic electrode. It is found that the Cu in the electrode plays a basic role in the generation of MF from the ECR of FF, while the existence of Ni in a trace amount can remarkably enhance the activity of the Cu electrode. A low pH value is more favorable for the generation of MF than for the formation of furfuryl alcohol (FA). At the optimal pH value of 0.5, the Faradaic efficiency (FE) and the production rate of MF first increase with an increase in current density and then decline after 10 mA cm(-2). The existence of Ni2+ in the electrolyte benefits the formation of MF, while the addition of Cu2+ ions is more useful to promotion of the generation of FA. At the optimal concentration of Ni2+ (10(-7) M) in the electrolyte, the total FE of the organics (88%), the FE of MF (82%) and the production rate of MF (77 mu mol cm(-2) h(-1)) reach their highest levels. Kinetic analysis shows that the route by which MF is directly generated from FF is preferable to a consecutive route with an intermediate of FA.

关键词： Furfural

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Advanced 3D ordered electrodes for PEMFC applications: From structural features and fabrication methods to the controllable design of catalyst layers

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Green Energy & Environment 2024年第9期9卷 1336-1365页

作者： Kaili Wang Tingting Zhou Zhen Cao Zhimin Yuan Hongyan He Maohong Fan Zaiyong Jiang School of Chemistry&Chemical Engineering and Environmental Engineering Weifang UniversityWeifang261061China Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex SystemsCAS Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China College Engineering and Physical Sciences and School of Energy ResourcesUniversity of WyomingLaramieWY 82071USA

The catalyst layers(CLs) electrode is the key component of the membrane electrode assembly(MEA) in proton exchange membrane fuel cells(PEMFCs). Conventional electrodes for PEMFCs are composed of carbon-supported, ionomer, and Pt nanoparticles, all immersed together and sprayed with a micron-level thickness of CLs. They have a performance trade-off where increasing the Pt loading leads to higher performance of abundant triple-phase boundary areas but increases the electrode cost. Major challenges must be overcome before realizing its wide commercialization. Literature research revealed that it is impossible to achieve performance and durability targets with only high-performance catalysts, so the controllable design of CLs architecture in MEAs for PEMFCs must now be the top priority to meet industry goals. From this perspective, a 3D ordered electrode circumvents this issue with a support-free architecture and ultrathin thickness while reducing noble metal Pt loadings. Herein, we discuss the motivation in-depth and summarize the necessary CLs structural features for designing ultralow Pt loading electrodes. Critical issues that remain in progress for 3D ordered CLs must be studied and characterized. Furthermore, approaches for 3D ordered CLs architecture electrode development, involving material design, structure optimization, preparation technology, and characterization techniques, are summarized and are expected to be next-generation CLs for PEMFCs. Finally, the review concludes with perspectives on possible research directions of CL architecture to address the significant challenges in the future.

关键词： PEMFC 3D ordered electrode Structural features Preparation technology Ultralow Pt loading

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Dual hydrogen bond donor functionalized hierarchical porous poly(ionic liquid)s for efficient CO2 fixation into cyclic carbonates

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SEPARATION AND PURIFICATION TECHNOLOGY 2024年 344卷

作者： Fu, Mengqian Ding, Weilu Zhao, Qianmeng Xu, Zhenyang Hua, Wei Li, Yunong Yang, Zifeng Dong, Li Su, Qian Cheng, Weiguo Chinese Acad Sci CAS Key Lab Green Proc & Engn State Key Lab Multiphase Complex Syst Beijing Key Lab Ion Liquids Clean ProcInst Proc E Beijing 100190 Peoples R China Univ Chinese Acad Sci Sch Chem Engn Beijing 100049 Peoples R China Sinopec Beijing Yanshan Petrochem Co Beijing 102500 Peoples R China

CO2 capture and conversion to high-value-added products is critical for the purposes of environmental preservation and carbon resource utilization. In this study, a novel class of porous poly(ionic liquid)s has been synthesized, incorporating dual hydrogen bond donors (amide and hydroxyl groups) and nucleophiles (Br-) as multiple effective active sites for the cycloaddition reaction between CO2 and epoxides. The presence of dual hydrogen bond donors not only provides two active sites for synergistic catalysis with epoxides but also enhances the capacity for CO2 adsorption. Comprehensive characterization has been conducted to elucidate the structural features and properties of these innovative materials. By regulating the ratio between ionic liquid monomer and divinylbenzene, a hierarchical porous structure favorable for the reaction was constructed, resulting in optimized catalytic activity comparable to that of bulk ionic liquid monomers. Furthermore, this catalyst exhibits remarkable structural stability with minimal activity loss even after five consecutive use cycles. Combining density functional theory calculations with in-situ Fourier transform infrared spectroscopy analysis, the catalytic mechanism was proposed that the dual hydrogen bond donors and Br- synergistically promote ring-opening reactions of epoxides, while amide groups serve as basic sites to enhance CO2 adsorption during the reaction process.

关键词： Poly(ionic liquid)s Cycloaddition reaction Carbon dioxide utilization Hydrogen bond donor

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