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A hybrid spatial-temporal deep learning prediction model of industrial methanol-to-olefins process

Frontiers of Chemical Science and Engineering 2024年第4期18卷 73-85页

作者： Jibin Zhou Xue Li Duiping liu Feng Wang Tao Zhang Mao Ye zhongmin liu National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Yulin Innovation Institute for Clean Energy Clean Energy Innovation Institute of Chinese Academy of SciencesYulin 719053China Xuelang Industrial Intelligence Technology Co. Ltd.Wuxi 214000China

Methanol-to-olefins,as a promising non-oil pathway for the synthesis of light olefins,has been successfully industrialized.The accurate prediction of process variables can yield significant benefits for advanced process control and optimization.The challenge of this task is underscored by the failure of traditional methods in capturing the complex characteristics of industrial processes,such as high nonlinearities,dynamics,and data distribution shift caused by diverse operating conditions.In this paper,we propose a novel hybrid spatial-temporal deep learning prediction model to address these issues.Firstly,a unique data normalization technique called reversible instance normalization is employed to solve the problem of different data distributions.Subsequently,convolutional neural network integrated with the self-attention mechanism are utilized to extract the temporal patterns.Meanwhile,a multi-graph convolutional network is leveraged to model the spatial interactions.Afterward,the extracted temporal and spatial features are fused as input into a fully connected neural network to complete the prediction.Finally,the outputs are denormalized to obtain the ultimate results.The monitoring results of the dynamic trends of process variables in an actual industrial methanol-to-olefins process demonstrate that our model not only achieves superior prediction performance but also can reveal complex spatial-temporal relationships using the learned attention matrices and adjacency matrices,making the model more interpretable.Lastly,this model is deployed onto an end-to-end Industrial Internet Platform,which achieves effective practical results.

关键词： methanol-to-olefins process variables prediction spatial-temporal self-attention mechanism graph convolutional network

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Designing ABC-6 family small pore zeolites by epitaxial growth approach

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Chinese Chemical Letters 2024年第3期35卷 508-512页

作者： Xiaohui Cui Jia Lv Chao Ma Yujiao Wang Zhenghao Jia Daliang Zhang Peng Guo zhongmin liu Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450001China National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Multi-scale Porous Materials Center Institute of Advanced Interdisciplinary Studies&School of Chemistry EngineeringChongqing UniversityChongqing 400044China University of Chinese Academy of Sciences Beijing 100049China Division of Energy Research Resources Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Aluminosilicate small pore zeolites belonging to ABC-6 family play crucially important roles in the high methanol conversion with the high selectivity of light olefins,gas separation and storage,and selective catalytic reduction of NO_(x).In this work,we report a general method,called the epitaxial growth approach,for designing ABC-6 family small pore zeolites.It is mainly realized through the epitaxial growth on the nonporous SOD-type zeolite in the presence of inorganic cations(Na^(+)and K^(+))combined with a variety of organic structure directing agents(OSDAs).In this case,a series of ABC-6 family small pore zeolites such as ERI-,SWY-,LEV-,AFX-,and PTT-type zeolites have been successfully synthesized within a few hours.More importantly,the advanced focused ion beam(FIB)and the low-dose high-resolution transmission electron microscopy(HRTEM)imaging technique have been utilized for unraveling the zeolite heterojunction at the atomic level during the epitaxial growth process.It turns out(222)crystallographic planes of the SOD-type zeolite substrate provide unique pre-building units,which facilitate the growth of targeted ABC-6 family small pore zeolites along its c-axis.Moreover,the morphologies of ERI-type zeolite can also be tuned through the epitaxial growth approach,achieving a longer lifetime in the methanol conversion.

关键词： Zeolite structure Zeolite synthesis Structural characterizations Low-dose imaging Focused ion beam

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High-silica faujasite zeolite-tailored metal encapsulation for the low-temperature production of pentanoic biofuels

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Journal of Energy Chemistry 2024年第1期88卷 552-560,I0012页

作者： Wenhao Cui Yuanshuai liu Pengfei Guo Zhijie Wu Liqun Kang Huawei Geng Shengqi Chu Linying Wang Dong Fan Zhenghao Jia Haifeng Qi Wenhao Luo Peng Tian zhongmin liu National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101ShandongChina College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina State Key Laboratory of Heavy Oil Processing and Key Laboratory of Catalysis of CNPC China University of PetroleumBeijing 102249China Department of Inorganic Spectroscopy Max Planck Institute for Chemical Energy ConversionMülheim an der Ruhr 45470Germany Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Division of Energy Research Resources Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Leibniz-Institut für Katalyse Albert-Einstein-Straβe 29aRostock 18059Germany

Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge.Herein,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation.Compared with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.

关键词： High-silica zeolite Y Metal encapsulation Bifunctional catalysis Hydrodeoxygenation Biofuels

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IoV environment exploring coordination:A federated learning approach

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Digital Communications and Networks 2024年第1期10卷 135-141页

作者： Tong Ding Lei liu Yi Zhu Lizhen Cui zhongmin Yan School of Software Shandong UniversityJinan250101China

Exploring open fields with coordinated unmanned vehicles is popular in academia and industries.One of the most impressive applicable approaches is the Internet of Vehicles(lov).The IoV connects vehicles,road infrastructures and communication facilities to provide solutions for exploration tasks.However,the coordination of acquiring information from multi-vehicles may risk data privacy.To this end,sharing high-quality experiences instead of raw data has become an urgent demand.This paper employs a Deep Reinforcement Learning(DRL)method to enable IoVs to generate training data with prioritized experience and states,which can support the IoV to explore the environment more efficiently.Moreover,a Federated Learning(FL)experience sharing model is established to guarantee the vehicles'privacy.The numerical results show that the proposed method presents a better successful sharing rate and a more stable convergence within the comparison of fundamental methods.The experiments also suggest that the proposed method could support agents without full information to achieve the tasks.

关键词： Internet of vehicle Deep reinforcement learning Federated learning Data privacy

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Cavity-controlled methanol conversion over zeolite catalysts

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National Science Review 2023年第9期10卷 72-91页

作者： Wenna Zhang Shanfan Lin Yingxu Wei Peng Tian Mao Ye zhongmin liu National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian National Laboratory for Clean Energy iChEM(Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences Energy College University of Chinese Academy of Sciences State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

The successful development and application in industry of methanol-to-olefins(MTO) process brought about an innovative and efficient route for olefin production via non-petrochemical resources and also attracted attention of C1 chemistry and zeolite catalysis.Molecular sieve catalysts with diversified microenvironments embedding unique channel/cavity structure and acid properties,exhibit demonstrable features and advantages in the shape-selective catalysis of MTO.Especially,shape-selective catalysis over8-MR and cavity-type zeolites with acidic supercage environment and narrow pore opening manifested special host-guest interaction between the zeolite catalyst and guest reactants,intermediates and products.This caused great differences in product distribution,catalyst deactivation and molecular diffusion,revealing the cavity-controlled methanol conversion over 8-MR and cavity-type zeolite catalyst.Furthermore,the dynamic and complicated cross-talk behaviors of catalyst material(coke)-reaction-diffusion over these types of zeolites determines the catalytic performance of the methanol conversion.In this review,we shed light on the cavity-controlled principle in the MTO reaction including cavity-controlled active intermediates formation,cavity-controlled reaction routes with the involvement of these intermediates in the complex reaction network,cavity-controlled catalyst deactivation and cavity-controlled diffusion.All these were exhibited by the MTO reaction performances and product selectivity over 8-MR and cavity-type zeolite catalysts.Advanced strategies inspired by the cavity-controlled principle were developed,providing great promise for the optimization and precise control of MTO process.

关键词： methanol-to-olefins cavity-controlled principle reaction intermediates and routes deactivation and diffusion shape-selective catalysis

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Achieving high conversion of syngas to aromatics

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Journal of Energy Chemistry 2022年第3期31卷 597-602,I0016页

作者： Yi Fu Youming Ni Zhiyang Chen Wenliang Zhu zhongmin liu National Engineering Laboratory for Methanol to Olefins Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Realizing high CO conversion and high aromatics selectivity simultaneously in syngas-to-aromatics(STA)reaction is still challenging.Herein,we report a 57.5%CO conversion along with 74%aromatics selectivity over a composite catalyst consisting of Fe/ZnCr_(2)O_(4)(Fe modified ZnCr_(2)O_(4)spinel)oxide and H-ZSM-5 zeolite.Impregnation of only 3 wt%of Fe onto ZnCr_(2)O_(4)can remarkably increase CO conversion without sacrificing the aromatics selectivity.Oxygen vacancy concentration is improved after impregnating Fe.The highly dispersed iron carbide species is formed during the reaction over Fe/ZnCr_(2)O_(4)spinel oxide.The synergistic effect of oxygen vacancy and iron carbide results in a rapid formation of abundant oxygenated intermediate species,which can be continuously transformed to aromatics in H-ZSM-5.This study provides a new insight into the design of highly efficient catalyst for syngas conversion.

关键词： Syngas Aromatics Fe/ZnCr_(2)O_(4)oxide H-ZSM-5 zeolite High conversion

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Defined organic-octamolybdate crystalline superstructures derived Mo_(2)C@C as efficient hydrogen evolution electrocatalysts

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Chinese Chemical Letters 2024年第6期35卷 201-205页

作者： Jiao Li Chenyang Zhang Chuhan Wu Yan liu Xuejian Zhang Xiao Li Yongtao Li Jing Sun zhongmin Su School of Materials Science and Engineering Jilin Jianzhu UniversityChangchun 130018China School of Chemical and Environmental Engineering Changchun University of Science and TechnologyChangchun 130022China

Hydrogen evolution electrocatalysts derived from metal-organic crystalline frameworks can inherit the merits of ordered and adjustable structures with high surface area.In this paper,organic-octamolybdate crystalline superstructures(OOCS)with a fixed stoichiometric ratio of Mo_(8)(L)_(2) and high Mo content(>40 wt%)were synthesized using flexible ligands with controllable lengths(named as OOCS-1-3).Then,molybdenum carbides coated with carbon layers as electrocatalysts(Mo_(2)C@C-1-3)can be obtained directly from a one-step high-temperature carbonization process using OOCS-1-3 as precursors.As a typical example,Mo_(2)C@C-3 exhibits satisfactory hydrogen evolution activity with a low overpotential of 151 m V(1.0 mol/L KOH)at 10 m A/cm^(2) and stability for 24 h.The electrocatalytic activity is mainly from the synergistic interactions between the carbon layers and molybdenum carbide species.Furthermore,compared with the initial content of C,N,Mo in OOCS and Mo_(2)C@C,the catalytic activity increases with the N amount.This work makes organic-octamolybdate crystalline superstructures used as general precursors to product high Mo content electrocatalysts applied in energy storage and conversion fields.

关键词： Molybdenum carbides Electrocatalysts Organic-octamolybdate crystalline superstructures Synergistic interactions Hydrogen evolution reaction(HER)

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Enhancing the aromatic selectivity of cyclohexane aromatization by CO_(2)coupling

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Frontiers of Chemical Science and Engineering 2023年第11期17卷 1801-1808页

作者： Xiangxiang Ren Zhong-Pan Hu Jingfeng Han Yingxu Wei zhongmin liu National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Improving the aromatic selectivity in the alkane aromatization process is of great importance for its practical utilization but challenge to make because the high H/C ratio of alkanes would lead to a serious hydrogen transfer process and a large amount of light alkanes.Herein,CO_(2)is introduced into the cyclohexane conversion process on the HZSM-5 zeolite,which can improve the aromatic selectivity.By optimizing the reaction conditions,an improved aromatic(benzene,toluene,xylene,and C9+)selectivity of 48.2%can be obtained at the conditions of 2.7 MPa(CO_(2)),450℃,and 1.7 h^(−1),which is better than that without CO_(2)(aromatic selectivity=43.2%).In situ transmission Fourier transform infrared spectroscopy spectra illustrate that many oxygenated chemical intermediates(e.g.,carboxylic acid,anhydride,unsaturated aldehydes/ketones or ketene)would be formed during the cyclohexane conversion process in the presence of CO_(2).13C isotope labeling experimental results demonstrate that CO_(2)can enter into the aromatics through the formation of oxygenated chemical intermediates and thereby improve the aromatic selectivity.This study may open a green,economic,and promising way to improve the aromatic selectivity for alkane aromatization process.

关键词： aromatics carbon dioxide aromatization coupling reaction ZSM-5 zeolite

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Multiscale dynamical cross-talk in zeolite-catalyzed methanol and dimethyl ether conversions

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National Science Review 2022年第9期9卷 28-39页

作者： Shanfan Lin Yuchun Zhi Zhiqiang liu Jiamin Yuan Wenjuan liu Wenna Zhang Zhaochao Xu Anmin Zheng Yingxu Wei zhongmin liu National Engineering Laboratory for Methanol to Olefins Dalian National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy Materials(iChEM) Dalian Institute of Chemical Physics Chinese Academy of Sciences Energy College University of Chinese Academy of Sciences National Center for Magnetic Resonance in Wuhan State Key Laboratory of Magnetic Resonance and Atomic and Molecular PhysicsKey Laboratory of Magnetic Resonance in Biological SystemsWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of Sciences Key Laboratory of Separation Science for Analytical Chemistry Dalian Institute of Chemical PhysicsChinese Academy of Sciences State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Establishing a comprehensive understanding of the dynamical multiscale diffusion and reaction process is crucial for zeolite shape-selective catalysis and is urgently demanded in academia and industry. So far,diffusion and reaction for methanol and dimethyl ether(DME) conversions have usually been studied separately and focused on a single scale. Herein, we decipher the dynamical molecular diffusion and reaction process for methanol and DME conversions within the zeolite material evolving with time, at multiple scales, from the scale of molecules to single catalyst crystal and catalyst ensemble. Microscopic intracrystalline diffusivity is successfully decoupled from the macroscopic experiments and verified by molecular dynamics simulation. Spatiotemporal analyses of the confined carbonaceous species allow us to track the migratory reaction fronts in a single catalyst crystal and the catalyst ensemble. The constrained diffusion of DME relative to methanol alleviates the high local chemical potential of the reactant by attenuating its local enrichment, enhancing the utilization efficiency of the inner active sites of the catalyst crystal. In this context, the dynamical cross-talk behaviors of material, diffusion and reaction occurring at multiple scales is uncovered. Zeolite catalysis not only reflects the reaction characteristics of heterogeneous catalysis, but also provides enhanced, moderate or suppressed local reaction kinetics through the special catalytic micro-environment, which leads to the heterogeneity of diffusion and reaction at multiple scales,thereby realizing efficient and shape-selective catalysis.

关键词： MTO reaction diffusion multiscale dynamical cross-talk shape-selective catalysis zeolite

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Insights into the size effect of ZnCr_(2)O_(4)spinel oxide in composite catalysts for conversion of syngas to aromatics

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Green Energy & Environment 2023年第2期8卷 530-537页

作者： Yi Fu Youming Ni Wenhao Cui Xudong Fang Zhiyang Chen Zhaopeng liu Wenliang Zhu zhongmin liu National Engineering Laboratory for Methanol to Olefins Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023LiaoningChina University of Chinese Academy of Sciences Beijing100049China

Direct conversion of syngas to aromatics(STA)over oxide-zeolite composite catalysts is promising as an alternative method for aromatics production.However,the structural effect of the oxide component in composite catalysts is still ambiguous.Herein,we investigate the size effect by selecting ZnCr_(2)O_(4)spinel,as a probe oxide,mixing with H-ZSM-5 zeolite as a composite catalyst for STA reaction.The CO conversion,aromatics selectivity and space-time yield(STY)of aromatics are all significantly improved with the crystal size of ZnCr_(2)O_(4)oxide decreases,which can mainly attribute to the higher oxygen vacancy concentration and thus the rapid generation of more C1oxygenated intermediate species.Based on the understanding of the size-performance relationship,ZnCr_(2)O_(4)-400 with a smaller size mixing with H-ZSM-5 can achieve32.6%CO conversion with 76%aromatics selectivity.The STY of aromatics reaches as high as 4.79 mmol g_(cat)^(-1)h^(-1),which outperforms the previously reported some typical catalysts.This study elucidates the importance of regulating the size of oxide to design more efficient oxidezeolite composite catalysts for conversion of syngas to value-added chemicals.

关键词： Size effect Syngas conversion Aromatics ZnCr_(2)O_(4)oxide H-ZSM-5 zeolite

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