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Towards the insights into the deactivation behavior of acetylene hydrogenation catalyst

Petroleum Science 2024年第2期21卷 1405-1414页

作者： Hai-Xia Su Yang Jiao Jian-Gong Shi Zhi-Wei Yuan Di Zhang Xu-Peng Wang Jing Ren Dan Liu Jian-Zhou Gui Hai-Yang Gao Xiao-Li Xu State Key Laboratory of Separation Membranes&Membrane Processes Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringSchool of Material Science and EngineeringTiangong UniversityTianjin300387China Institute of Engineering Technology Sinopec Catalyst Co.LtdBeijing101100China State Key Laboratory of Separation Membranes and Membrane Processes Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringSchool of ChemistryTiangong UniversityTianjin300387China

A series of model catalysts were obtained by treating commercial fresh and spent catalysts unloaded from the factory with different methods, including green oil dipping, extraction and high-temperature regeneration;finally, the deactivation behavior of the commercial catalyst for acetylene hydrogenation were studied. The influence of various possible deactivation factors on the catalytic performance was elucidated via detailed structural characterization, surface composition analysis, and activity *** results showed that green oil, carbon deposit and sintering of active metal were the main reasons for deactivation, among which green oil and carbon deposit led to rapid deactivation, while the activity could be recovered after regeneration by high-temperature calcination. The sintering of active metal components was attributed to the high-temperature regeneration in hydrothermal conditions, which was slow but irreversible and accounted for permanent deactivation. Thus, optimizing the regeneration is expected to extend the service life of the commercial catalyst.

关键词： Acetylene Hydrogenation Green oil Carbon deposit Sintering Catalyst deactivation

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The infinite separation principle

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Green Energy & Environment 2023年第5期8卷 1229-1231页

作者： Suojiang Zhang Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China

In this paper,we propose“The Infinite Separation Principle”.This principle contains two implications:firstly,even exhausting all separation approaches,including chemical techniques,it is impossible to achieve 100%pu... 详细信息

关键词： Separation Thermodynamics Purity Mixture

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Enhanced light harvesting ability in hollow Pt/TiO2 nanoreactor for boosting tetracycline photodegradation

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Progress in Natural Science:Materials International 2024年第4期34卷 767-775页

作者： Danyang Li Yongqi Li Dagui Liao Mengqing Cao Lulu Zhang Shasha Zhang Ling Chen Yawen Chen Huan Wang Jian Qi Feifei You College of Textile and Clothing Yancheng Institute of Technology Hebei Key Laboratory of Flexible Functionals Materials School of Materials Science and Engineering Hebei University of Science and Technology State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences School of Chemical Engineering University of Chinese Academy of Sciences

Utilizing solar energy to decompose tetracycline（TC） is a green strategy to treat wastewater. Herein, a heterogeneous hollow structured TiO2decorated Pt nanoparticles were successfully designed and synthesized via hardtemplate approach and photo-deposition process toward TC photodegradation. The Pt nanoparticles loaded on the surface of hollow structured TiO2can increase the visible light absorption due to the local surface plasmon resonance（LSPR） effect. Furthermore, owing to the tough electron oscillation of the LSPR excitation, the plasmonic hot holes on the surface of Pt nanoparticles can capture the electrons of TiO2, effectively facilitating the separation of photo-excited charge carriers because of the formation of Schottky junction constructed between Pt and TiO2. Combined the natural merits of shorten conveying path of charge carriers and physical structural stability for hollow structure, the optimal Pt/TiO2hetero-junction hybrid showed superior photocatalytic activity and durability for TC photodegradation with the degradation efficiency of 93.8 % after 30 min and the rate constant of 0.09196 min-1under 300 W Xe lamp irradiation. This work displays a heterogeneous hybrids catalyst based on eco-friendly metal and semiconductor materials which can be used in the fields including without limitation TC photodegradation.

关键词： Pt/TiO2 Hollow structure Photodegradation Tetracycline Hetero-junction

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Activating lithium storage in 2D CaSi_(2) anode via enhancing pseudocapacitive properties with oxygen modification engineering

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Nano Research 2025年第4期18卷 199-206页

作者： Yongzheng Zhang Lu Sun Kailin Yang Youwang Ye Liang Zhan Qi Wei Jianan Gu Institute of Energy Power Innovation North China Electric Power UniversityBeijing 100096China State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Aviation Key Laboratory of Science and Technology on Advanced Surface Engineering AVIC Manufacturing Technology InstituteBeijing 100024China

Silicon(Si)has emerged as a promising anode material for lithium-ion batteries(LIBs)due to its extremely high theoretical capacity of 4200 mAh·g^(-1).However,its practical application is limited by several critical challenges,including severe volume expansion and poor electrical ***,we employ a two-dimensional(2D)oxygen modification engineering approach to fabricate 2D oxygen-functionalized CaSi_(2)(CaSi_(2)O_(x))*** the preparation of 2D CaSi_(2) layers,O atoms are gradually incorporated onto their *** resulting 2D CaSi_(2)O_(x) layers have a thickness of 3-5 nm,closely matching the theoretical thickness of 6-10 *** used as lithium anodes,the 2D CaSi_(2)O_(x) layers exhibit exceptional electrochemical performance,maintaining stability over 3000 cycles at an ultrahigh current density of 30 A·g^(-1).By tailoring the surface properties,their pseudocapacitive charge storage mechanism is significantly enhanced,effectively overcoming the intrinsic limitations of traditional Si *** study highlights the promise of 2D surface engineering in the development of advanced materials for next-generation LIBs.

关键词： two-dimensional(2D)CaSi_(2)O_(x) Si anode volume change pseudocapacitive surface modification lithium storage

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Adsorption removal of mercury from flue gas by metal selenide:A review

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Journal of Environmental Sciences 2025年第2期148卷 420-436页

作者： Yang Zheng Guoliang Li Yi Xing Wenqing Xu Tao Yue School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China CAS Key Laboratory of Green Process and Engineering Institute of Process EngineeringInnovation Academy for Green ManufactureChinese Academy of SciencesBeijing 100190China

Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the *** intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas *** the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury *** paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium *** on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial *** addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.

关键词： Non-conventional pollutants Adsorbents Metal selenides Flue gas Mercury removal

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Exploring the role of cationic lipids in modulating immunogenicity and vaccine efficacy of mRNA-LNP

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Particuology 2025年第2期97卷 1-11页

作者： Yan Zhou Xiangfei Shan Renji Gu Yufei Xia Xiaonan Huang State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100081China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing10090China

The mRNA vaccines have become a transformative platform in medicine,with their success during the COVID-19 pandemic accelerating research in viral prevention and cancer *** nanoparticles(LNPs)enhance the stability and efficacy of mRNA vaccines,but achieving an optimal balance between innate immune activation and mRNA expression is crucial for their *** cationic lipids,although largely replaced by ionizable lipids due to concerns over excessive immunogenicity,have demonstrated potential in cancer immunotherapy by inducing strong immune *** this study,we investigated whether incorporating cationic lipids into mRNA-LNP formulations could enhance immunogenicity without requiring new lipid *** introduced varying proportions of cationic lipids into D-Lin-MC3-DMA and SM-102-based LNPs and evaluated their impact on innate immune activation,along with long-term humoral and cellular immune *** results showed that in MC3-based LNPs,cationic lipids significantly improved anti-tumor efficacy,though slightly diminished long-term humoral and cellular *** contrast,in SM-102-based LNPs,cationic lipids enhanced anti-tumor effects without negatively impacting long-term *** findings suggest that adding cationic lipid as an additional component allows for the fine-tuning of mRNA-LNP immunogenicity,expanding the potential applications of mRNA vaccines and simplifying LNP design.

关键词： Lipid nanoparticle mRNA vaccine Immunogenicity Cationic lipids Immune response

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Upcycling of polyethylene terephthalate to 1,4-cyclohexanedimethanol in water

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Science China Chemistry 2025年第5期68卷 2101-2109页

作者： Shuhui Fang Zhiwen Gao Xinrui Shi Min Zhang Wei Zhang Yue Liu State Key Laboratory of Petroleum Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular EngineeringEast China Normal University Engineering Center for Sustainable Carbon Science and Technology East China Normal University Institute of Eco-Chongming

The recycling of waste polyethylene terephthalate（PET）, an extensively used polymer as plastic and fiber materials, has become an urgent topic due to the rapid generation and accumulation of plastic waste into the environment. Current chemical recycling approaches to depolymerize and convert PET into 1,4-cyclohexanedimethanol（CHDM）, an important chemical in the production of advanced polyesters, predominantly use organic solvents, such as alcohols or dioxane. Herein, we developed an environmentally friendly and economically viable pathway for converting PET to CHDM using water as the solvent. In this process, PET is sequentially hydrolyzed in water, hydrogenated to 1,4-cyclohexane dicarboxylic acid（CHDA）, and then reduced to CHDM. The PET conversion rate is self-enhanced in aqueous medium via acid-catalyzed hydrolysis by the generated CHDA intermediate. A Pd-based catalyst（e.g., Pd/C） selectively hydrogenates the arene ring of the PET monomer, terephthalic acid intermediate, and a Ru-Sn/C bimetallic catalyst reduces its COOH to CH2OH group. At optimized reaction conditions, a complete conversion of PET and 80.1% yield of CHDM are obtained. Alternatively, this approach can also efficiently produce CHDA from PET, with a yield up to 86.4%.

关键词： polyethylene terephthalate (PET) 1,4-cyclohexanedimethanol (CHDM) hydrogenation hydrogenolysis

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Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

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Nano Research 2024年第6期17卷 5298-5304页

作者： Yuwei He Yueguang Chen Renjie Wu Zhihe Xiao Mengxian Li Chunfeng Shi Leyu Wang State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China State Key Laboratory of Petroleum Molecular and Process Engineering SINOPEC Research Institute of Petroleum Processing Co.Beijing 100083China

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains ***,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the *** NWs possess uniform sizes and well-controlled atomic *** to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based ***,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/*** ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.

关键词： ligand effect oxygen reduction reaction group VI B transition metal ultrathin nanowires multiple oxygen species

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Dodecylamine-mediated synthesis of caron-supported platinum-ruthenium alloy nanoparticles with ultrafine sizes towards high-efficiency methanol oxidation electrocatalysis

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Progress in Natural Science:Materials International 2025年第1期35卷 215-221页

作者： Liang Chu Zheng Rong Mengyuan Ma Feng Guo Shaonan Tian Jun Yang School of Electronics and Information & Institute of Carbon Neutrality and New Energy Hangzhou Dianzi University State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences

For fully leveraging the advantages of PtRu alloys as electrocatalysts to catalyze methanol oxidation reaction（MOR）, we herein report an ambient-temperature method for directly synthesizing carbon-supported PtRu alloy nanoparticles with ultrafine sizes in an organic medium towards high-efficiency MOR. This strategy involves the dodecylamine（DDA）-mediated extraction of Pt and Ru ions from water to toluene, and then mixing them with carbon substrate, followed by NaBH4reduction in the same organic medium. Profiting from their ultrafine sizes of ca. 1.68 nm, the as-prepared PtRu nanoparticles supported on carbon substrate show a mass activity of 0.93 A mg-1and a specific activity of 10.56 mA cm-2, respectively, both of which are much higher than those of the commercial PtRu/C catalyst.

关键词： Carbon substrate Dodecylamine-mediated extraction Methanol oxidation reaction PtRu alloy nanoparticles Ultrafine size

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An improved EMMS model for turbulent flow in pipe and its solution

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Particuology 2023年第5期76卷 1-12页

作者： Lin Zhang Wen Lai Huang Jianhua Chen State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China

Based on the existing energy-minimization multi-scale(EMMS)model for turbulent flow in pipe,an improved version is proposed,in which not only a new radial velocity distribution is introduced but also the quantification of total dissipation over the cross-section of pipe is improved for the dominant mechanism of fully turbulent flow in *** four dynamic equality constraints and some other constraints are constructed but there are five parameters involved,leading to one free variable *** the compromise in competition between dominant mechanisms for laminar and fully turbulent flow in pipe respectively,the above four constructed dynamic equality constraints can be ***,the cases for turbulent flow in pipe with low,moderate and high Reynolds number are simulated by the improved EMMS *** numerical results show that the model can obtain reasonable results which agree well with the data computed by the direct numerical simulation and those obtained by *** illustrates that the improved EMMS model for turbulent flow in pipe is reasonable and the compromise in competition between dominant mechanisms is indeed a universal governing principle hidden in complex ***,one more EMMS model for a complex system is offered,pro-moting the further development of mesoscience.

关键词： Mesoscience EMMS Compromise in competition Dominant mechanism Turbulent flow in pipe

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