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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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Chemical and engineering bases for green H2O2 production and related oxidation and ammoximation of olefins and analogues

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National Science Review 2024年第8期11卷 304-321页

作者： Minghua Qiao Xinggui Zhou Zexue Du Peng Wu Baoning Zong Collaborative Innovation Center of Chemistry for Energy Materials Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University State Key Laboratory of Chemical Engineering East China University of Science and Technology State Key Laboratory of Petroleum Molecular& Process Engineering Research Institute of Petroleum ProcessingSINOPEC State Key Laboratory of Petroleum Molecular& Process Engineering School of Chemistry and Molecular Engineering East China Normal University

Plastics,fibers and rubber are three mainstream synthetic materials that are essential to our daily lives and contribute significantly to the quality of our *** production of the monomers of these synthetic polymers usually involves oxidation or ammoximation reactions of olefins and ***,the utilization of C,O and N atoms in current industrial processes is <80%,which represents the most environmentally polluting processes for the production of basic *** innovation and integration of catalytic materials,new reaction pathways,and reaction engineering,the Research institute of Petroleum processing,Sinopec Co.,Ltd.（RIPP） and its collaborators have developed unique H2O2-centered oxidation/ammoximation technologies for olefins and analogues,which has resulted in a ￥500 billion emerging industry and driven trillions of ￥s' worth of downstream *** chemical and engineering bases of the production technologies mainly involve the integration of slurry-bed reactors and microsphere catalysts to enhance H2O2production,H2O2propylene/chloropropylene epoxidation for the production of propylene oxide/epichlorohydrin,and integration of H2O2cyclohexanone ammoximation and membrane separation to innovate the caprolactam production *** review briefly summarizes the whole process from the acquisition of scientific knowledge to the formation of an industrial production technology by ***,the scientific frontiers of H2O2production and related oxidation/ammoximation processes of olefins and analogues are reviewed,and new technological growth points are envisaged,with the aim of maintaining China's standing as a leader in the development of the science and technologies of H2O2production and utilization.

关键词： hydrogen peroxide oxidation ammoximation propylene oxide epichlorohydrin cyclohexanone oxime

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Ionic liquid-trimetallic electrocatalytic system for C–O bond cleavage in lignin model compounds and lignin under ambient conditions

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Nano Research 2024年第4期17卷 2420-2428页

作者： Guangyong Liu Yumiao Lu JunFeng Lu Yanlei Wang Shijing Liang Hongyan He Lilong Jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex SystemsBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial TechnologyZhengzhou 450000China

Electrocatalytic depolymerization of lignin into value-added chemicals offers a promising technique to make biorefining ***,we report a robust trimetallic PdNiBi electrocatalyst for reductive C–O bond cleavage of different lignin model dimers and oxidized lignin under mild *** reduction reaction proceeds with complete substrate conversion and excellent yields toward monomers of phenols(80%–99%)and acetophenones(75%–96%)in the presence of an ionic liquid electrolyte with operational *** experimental investigations together with density functional theory(DFT)calculations reveal that the outstanding performance of the catalyst results from the synergistic effect of the metal elements,which facilitates the easier formation of a key Cαradical intermediate and the facile desorption of the as-formed products at the *** results open up new opportunities for lignin valorization through the green electrocatalytic approach.

关键词： electrocatalytic depolymerization lignin Ionic liquids density functional theory(DFT)calculation

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Selective cyclohexane oxidation enhancement by electronic structures regulation of metal-poly(ionic liquid)s

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Green Chemical engineering 2024年第2期5卷 213-221页

作者： Ying Jin Shengxin Chen Ruirui Wang Yumei Liu Xinxin Li Yingwei Li Ruirui Zhang Ruixia Liu Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou450001China Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringInnovation Academy for Green ManufactureCASBeijing100190China

Poly(ionic liquids)(PILs)combined with the macromolecular structure and unique properties of ionic liquids show unlimited potential in *** this work,a series of metal-based PIL with different ionic ratios were prepared for the selective oxidation of *** analysis reveals that different degrees of ionization could adjust the Co-N sites of the catalysts efficiently,leading to significant changes in their electronic structure,which strongly relate to catalytic performance in oxidation.20.07%cyclohexane conversion and 13.06%cyclohexanone and cyclohexanol(KA oil)yield can be achieved by metal-based PILs that are better than other commercial *** with CoCl_(2),metal-based PILs perform well,with superior conversion and KA oil *** interestingly,the catalyst created in this study features a malleable Co-N site,which may potentially have an impact on how oxygen species adsorb and desorb from the ***,the catalyst studied in this work is used as molecular oxygen for the selective oxidation of cyclohexane to produce KA oil,and its application prospect is promising.

关键词： Metal-PILs Cyclohexane oxidation C-H activation Co-N sites

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A brief review of preparation and applications of monolithic aerogels in atmospheric environmental purification

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Journal of Environmental Sciences 2025年第3期149卷 209-220页

作者： Linfeng Nie Shuangde Li Mengjie Cao Ning Han Yunfa Chen State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Key Laboratory of Science&Technology on Particle Materials Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Monolithic aerogels are promising candidates for use in atmospheric environmental purification due to their structural advantages,such as fine building block size together with high specific surface area,abundant pore structure,***,monolithic aerogels possess a unique monolithic macrostructure that sets them apart from aerogel powders and nanoparticles in practical environmental clean-up *** review delves into the available synthesis strategies and atmospheric environmental applications of monolithic aerogels,covering types of monolithic aerogels including SiO_(2),graphene,metal oxides and their combinations,along with their preparation *** particular,recent developments for VOC adsorption,CO_(2)capture,catalytic oxidation of VOCs and catalytic reduction of CO_(2)are ***,challenges and future opportunities for monolithic aerogels in the atmospheric environmental purification field are *** reviewprovides valuable insights for designing and utilizing monolithic aerogel-based functional materials.

关键词： Monolithic aerogel Environmental purification Catalysis Adsorption

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Mn-modified nitrogen-doped Pt-based electrocatalyst for efficient oxygen reduction in aluminum-air batteries

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Nano Research 2024年第8期17卷 7126-7135页

作者： Li Gao Yang Song Xuebing Xu Chang Li Chaoquan Hu State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Zhongke Nanjing Institute of Green Manufacturing Industry Nanjing 211135China

In this study,a Mn-modified Pt-based catalyst loaded on nitrogen-doped Ketjen black(Mn-Pt/NKB)is prepared using a simple ethylene glycol reduction *** size of Pt nanoparticles(NPs)is effectively controlled by doping with Mn and *** the smallest average particle size of 1.7 nm,Mn-Pt/NKB demonstrates half-wave potentials of 0.890 and 0.688 V in the alkaline and neutral electrolytes,respectively,which are superior to those of commercial platinum on activated carbon(Pt/C).When applied as an air cathode in aluminum-air battery,it exhibits ultra-high power densities of 190(alkaline)and 26.2 mW·cm^(−2)(neutral).Moreover,the voltage remains stable after 5 h of *** practical application performance of the Mn-Pt/NKB catalyst in an aluminum-air battery is better than that of commercial Pt/***,the oxygen reduction reaction(ORR)mechanism on surfaces with different particle sizes is analyzed using density functional *** cracking is the major pathway on the surface of the small particles with lower energy consumption of 0.5 eV,while water molecule cleavage is the major pathway on the surface of the large particles with higher energy consumption of 0.97 *** lower energy consumption of the oxygen cracking pathway further confirms the ORR mechanism for higher activity on small-sized *** study provides a direction for the rational design of Pt-based catalysts for ORR and sheds light on the commercial development of aluminum-air batteries.

关键词： oxygen reduction reaction precious metal catalysts aluminum-air battery density functional theory(DFT)calculations reaction pathway

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Significant enhancement in local thermal conductivity of erythritol at interface with nanoparticles due to their interaction

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Nano Research 2024年第8期17卷 7726-7736页

作者： Ning Cao Yanhui Feng Kening Yan Zihan Liu Jiawei Wan Lin Qiu School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China State Key Laboratory of Biochemical Engineering Key Laboratory of Biopharmaceutical Preparation and DeliveryInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

When nano-fillers are used to enhance the thermal conductivity of organic phase change materials(PCMs),the naturally formed interface is considered to hinder thermal transport of the composite ***,the effect of the interface on the thermal properties of surrounding PCM has not been fully *** this paper,three composite PCMs(Ery@SiC,Ery@SiO_(2) and Ery@Si_(3)N_(4))were prepared by melt-blending *** local thermal conductivity and reduced Young’s modulus(E^(*))of the erythritol at the interface and far away from the interface in the composite PCMs were simultaneously measured by scanning thermal microscopy(SThM).The results revealed significant enhancement in local thermal conductivity of erythritol at the interface and its obvious positive correlation with E^(*).For different composite PCMs,molecular dynamics(MD)simulations suggested that the increase in intrinsic thermal conductivity and E^(*)of erythritol is attributed to the increase in interaction energy between erythritol and nanoparticles,as more erythritol phonon vibrations transform from localized mode to delocalized mode and erythritol has a higher density at the *** findings will provide new ideas for the design of PCM for energy storage.

关键词： scanning thermal microscopy phase change materials thermal conductivity reduced Young’s modulus interaction energy phonon participation ratio

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Synthesis of NaY zeolite from a submolten depolymerized perlite:Alkalinity effect and crystallization kinetics

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Chinese Journal of Chemical engineering 2024年第6期70卷 130-138页

作者： Yanli Qu Peng Dong Li Yang Yuanyuan Yue Haoliang Wang Jingcai Cheng Chao Yang CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Petroleum Molecular&Process EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100190China Qingyuan Innovation Laboratory Quanzhou 362801China National Engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350108China

NaY zeolites are synthesized using submolten salt depolymerized natural perlite mineral as the main silica and alumina sources in a 0.94 L stirred *** of alkalinity ranging from 0.38 to 0.55(n(Na_(2)O)/n(SiO_(2)))on the relative crystallinity,textural properties and crystallization kinetics were *** results show that alkalinity exerts a nonmonotonic influence on the relative crystallinity and textural properties,which exhibit a maximum at the alkalinity of *** nucleation kinetics are studied by fitting the experimental data of relative crystallinity with the Gualtieri *** is shown that the nucleation rate constant increases with increasing alkalinity,while the duration period of nucleation decreases with increasing *** n(Na_(2)O)/n(SiO_(2))ratios ranging from 0.38 to 0.55,the as-synthesized NaY zeolites exhibit narrower crystal size distributions with the increase in *** growth rates determined from the variations of average crystal size with time are 51.09,157.50,46.17 and 24.75 nm·h^(-1),*** is found that the larger average crystal sizes at the alkalinity of 0.38 and 0.43 are attributed to the dominant role of crystal growth over ***,the combined action of prominent crystal growth and the longer duration periods of nucleation at the alkalinity of 0.38 and 0.43 results in broader crystal size *** findings demonstrate that control of the properties of NaY zeolite and the crystallization kinetics can be achieved by conducting the crystallization process in an appropriate range of alkalinity of the reaction mixture.

关键词： NaY zeolite Submolten salt depolymerized perlite Alkalinity Crystallization kinetics

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Steady-state multiscale CFD simulation of a circulating fluidized bed riser

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Particuology 2024年第10期93卷 54-64页

作者： Zhaojie Ke Yujie Tian Fei Li Bona Lu Wei Wang State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Compared to transient simulation,steady-state simulation of circulating fluidized bed risers is more efficient,but is also harder to perform due to the complex scale-dependency of dense gas-solid *** this work,steady-state computational fluid dynamics(CFD)simulation of a riser is performed using the steady energy-minimization multi-scale(EMMS)*** is found that the steady state corresponds to an extremely large scale of length and time,thus the grid size required in steady-state simulation is larger than that in transient *** time-averaged two-fluid model(TFM)coupled with the steady-state EMMS/1M drag model enables a good prediction of the S-shaped,axial solids distribution and the choking transition,whereas the two-phase turbulence and solids stress models are important in predicting the radially core-annular distribution of *** far as we know,this is the first time that one can predict the choking transition in a steady-state CFD *** improvement may need an EMMS modeling of the time-averaged solid stresses.

关键词： Fluidization Drag force Steady state Simulation Mesoscale

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Gas–solid reactor optimization based on EMMS-DPM simulation and machine learning

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Particuology 2024年第6期89卷 131-143页

作者： Haolei Zhang Aiqi Zhu Ji Xu Wei Ge State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing 100190China

Design,scaling-up,and optimization of industrial reactors mainly depend on step-by-step experiments and engineering experience,which is usually time-consuming,high cost,and high *** numerical simulation can reproduce high resolution details of hydrodynamics,thermal transfer,and reaction process in reactors,it is still challenging for industrial reactors due to huge computational *** this study,by combining the numerical simulation and artificial intelligence(AI)technology of machine learning(ML),a method is proposed to efficiently predict and optimize the performance of industrial reactors.A gas–solid fluidization reactor for the methanol to olefins process is taken as an example.1500 cases under different conditions are simulated by the coarse-grain discrete particle method based on the Energy-Minimization Multi-Scale model,and thus,the reactor performance data set is *** develop an efficient reactor performance prediction model influenced by multiple factors,the ML method is established including the ensemble learning strategy and automatic hyperparameter optimization technique,which has better performance than the methods based on the artificial neural ***,the operating conditions for highest yield of ethylene and propylene or lowest pressure drop are searched with the particle swarm optimization algorithm due to its strength to solve non-linear optimization *** show that decreasing the methanol inflow rate and increasing the catalyst inventory can maximize the yield,while decreasing methanol the inflow rate and reducing the catalyst inventory can minimize the pressure *** two objectives are thus conflicting,and the practical operations need to be compromised under different circumstance.

关键词： Discrete particle method Artificial intelligence Machine learning Particle swarm optimization Industrial reactor optimization

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