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Cobalt-modified MCM-41 catalysts with multiple acidic sites for energy-efficient CO2 desorption of functionalized ionic liquid absorbents

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Separation and Purification Technology 2025年 373卷

作者： Chu, Haozhan Zeng, Shaojuan Zhang, Xiangping Zhan, Guoxiong Wang, Bo Zhang, Hongyu Zhong, Sheng Liu, Wei Beijing Key Laboratory of Solid State Battery and Energy Storage Process State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China School of Future Technology University of Chinese Academy of Sciences Beijing101408 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing101408 China National Key Laboratory of Heavy Oil China University of Petroleum Beijing102249 China

Ionic liquids (ILs) show great application potentials in CO2 capture due to extremely low vapor pressures, tunable structures, and strong CO2 affinity. Up to date, many efforts have been focused on the design and absorption performance of novel functionalized ILs, rather than desorption performance. In our previous work, the IL solvent [Cho][Triz]/TMS exhibited exceptional CO2 absorption performance. As a successive study on decreasing regeneration energy consumption, this work focused on the design and synthesis of novel metal-modified MCM-41 catalysts with multiple acidic sites to enhance CO2 catalytic desorption in the nonaqueous [Cho][Triz]/TMS (80 wt%/20 wt%) absorbent under lower temperatures. Among all the composite MCM-41 catalysts, the CoM-1/4 catalyst exhibits superior catalytic performance because of the increase of Brønsted acid sites by 232.3 % and Lewis acid sites by 56.2 % compared with pristine MCM-41, which promote CO2 desorption by accelerating C-N bond breaking. The CO2 desorption rate and amount increased by 180.2 % and 95.7 %, and the activation energy reduced by 46.7 % compared to the non-catalysis. Therefore, the theoretical regeneration energy consumption of the catalyst-added system was 0.88 GJ/t CO2, representing a 76.7 % reduction compared with the 30 wt% MEA solution. Furthermore, the CoM-1/4 catalyst maintained high catalytic activity after 20 cycles. This work indicated that the CoM-1/4 catalyst effectively enhanced the regeneration performance of IL absorbent, facilitating the development of an energy-efficient CO2 capture process for industrial applications. © 2025 Elsevier B.V.

关键词： Energy utilization

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Synthesis of High Entropy Oxides Derived from Metal Organic Frame and Catalytic Performance for Total Toluene Oxidation

SSRN

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SSRN 2024年

作者： Hussain, Abid Zheng, Yuhua Wang, Qianyu Cui, Yanbin State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China University of Chinese Academy of Sciences Beijing100049 China State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing102249 China

In this work, a series of high-entropy oxides (HEOs) was successfully prepared by the calcination of identical metal organic framework (MOF) precursor. Thermal treatment above 400 °C led to the complete transformation of MOFs to HEOs. The performance of the obtained HEOs catalysts in the removal of volatile organic compounds (VOCs) was studied with the catalytic oxidation of toluene as the probe reaction. The optimized Ce-HEO-400 catalyst showed impressive activity and stability over toluene catalytic oxidation, which resulted from the vast quantity of surface oxygen vacancies and the relative variable metal valence. The T50 and T90 values of Ce-HEO-400 were 180 and 255 °C. Moreover, it also showed excellent stability for 120 h with 98.5% toluene conversion rate at 260 °C. Combined with the characterizations of XRD, SEM, TEM, BET, H2-TPR and XPS, it was found that the high dispersion of active high entropy structure and the synergistic effect of different metal are the key factors for improving the catalytic performance of the Ce-HEO-400 catalyst. This work not only presents a facile method for synthesizing HEO materials at low temperature but also provides valuable technical support for the application of HEO catalysts in VOCs removal. The findings of this study open up new possibilities for the development of efficient catalysts for the removal of VOCs. © 2024, The Authors. All rights reserved.

关键词： Catalytic oxidation

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Hydrothermal pretreatment of protein-rich substrate:Modified physicochemical properties and consequent responses in its anaerobic digestion

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Carbon Resources Conversion 2023年第1期6卷 1-10页

作者： Fa Qiao Guangyi Zhang Jie Fan Hang Zhang Bowen Shi Jiancheng Yang Jianling Zhang Zhennan Han Shenyang University of Chemical Technology Shenyang 110142Liaoning ProvinceChina School of Ecology and Environment Beijing Technology and Business UniversityBeijing 100048China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Urban Construction Wuhan University of Science and TechnologyWuhan 430081Hubei ProvinceChina China Power Engineering Consulting Group Co. LtdBeijing 100120China

Wasted tofu rich in protein was subject to hydrothermal pretreatment(HTPT)under different conditions(at 120,140,160 and 180℃;for 0,30,60 and 90 min)followed by biochemical methane potential(BMP)tests,and 140℃and 0 min were found to be respectively the best temperature and duration for HTPT of tofu in terms of its biogas *** the under the optimal conditions(140℃,0 min)the accumulative methane yield reached up to 510.9 mL⋅(gVS)-1,which was 26.98%higher than that without HTPT(402.3 mL⋅(gVS)-1).The start-up process of continuous anerobic digestion(AD)of the tofu before and after hydrothermal treated(HT)at the optimal HTPT conditions(140℃,0 min)was examined,to investigate and compare how their consequent AD responded to *** was found that,for start-up of continuous AD,the HT tofu delivered more balanced nutrients and thus led to more stable AD and quicker biogas ***,HTPT generated products refractory to biodegradation,to slightly decrease the total biogas *** AD of HT tofu some weak ammonia-tolerant microbes,such as methylotrophic methanogens,survived and played indispensable *** of living microbial community structure indicated that,some hydrolytic acidification bacteria intolerant to ammonia nitrogen(such as Proteobacteria)were always active and appeared at high *** viable methylotrophic methanogens,*** M2,took obvious responsibilities in start-up of the AD for HT tofu.

关键词： Hydrothermal pretreatment(HTPT) Protein-rich substrate Anaerobic digestion(AD) Biogas Microbial community structure

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Corrosion studies of 90Cu-10Ni alloy tubes in simulated sulfide-polluted seawater under dynamic flow conditions

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Safety in Extreme Environments 2023年第3期5卷 221-242页

作者： Ekerenam, Okpo O. Emori, Wilfred Ma, Aili Obike, Anthony I. CAS Key Laboratory of Nuclear Materials and Safety Assessment Institute of Metal Research CAS Shenyang 110016 China Department of Biochemistry Federal University of Technology Ikot Abasi Nigeria School of Materials Science and Engineering Sichuan University of Science and Engineering Zigong 643000 China Department of Pure and Industrial Chemistry Abia State University Uturu Nigeria

A comprehensive corrosion study of two commercial 90Cu-10Ni alloy tubes, named Tube A and Tube B, in simulated sulfide-polluted seawater under dynamic flow conditions has been conducted to understand their service lives. Electrochemical techniques involving a rotating cylinder electrode were used to evaluate the effect of sulfide concentration on the corrosion behaviors of both tubes, while combined surface analytical techniques (SEM/EDS, XRD, and) were useful for the characterization of the corrosion product films on both tubes. Sulfide exhibited good corrosion inhibition abilities on both tubes under static flow condition (0 rpm). This is attributed to the spontaneous formation of protective film layers and the enrichment of the corrosion product films by the alloying elements. However, the inhibitive property gradually depleted with increasing flow speed due to the effect of hydrodynamic forces. Comparatively, due to the nature of the corrosion product films formed on the exposed surfaces of both tubes, Tube A demonstrated lower corrosion rates under static flow while Tube B exhibited lower corrosion rates at higher flow speeds. After 15 days exposure to the test system, the corrosion product films on both tubes were characterized to consist mainly of copper (I) sulfide (Cu₂S), copper (II) sulfide (CuS), copper (I) oxide (Cu₂O), nickel (II) hydroxide (Ni(OH)₂), nickel (II) oxide (NiO), nickel (III) oxide (Ni₂O₃), and copper (ii) oxide (CuO). Furthermore, traces of copper (II) chloride (CuCl₂), copper (II) hydroxide (Cu(OH)₂), nickel (II) sulfide (NiS), iron (II) sulfide (FeS), and iron (I) sulfide (FeS₂) were also characterized. The mechanism of their formation and effects on the corrosion processes were also discussed. © The Author(s), under exclusive licence to Springer Nature Switzerland AG 2023.

关键词： 90Cu-10Ni alloy Corrosion product film EIS Polarization Seawater Sulfide

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Structural architectures of polymer proton exchange membranes suitable for high-temperature fuel cell applications

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Science China Materials 2022年第2期65卷 273-297页

作者： Junming Dai Yu Zhang Gang Wang Yongbing Zhuang State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemistry and Chemical Engineering Henan University of TechnologyZhengzhou 450001China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

High-temperature proton exchange membrane(HT-PEM)fuel cells offer more advantages than low-temperature PEM fuel *** ideal characteristics of HT-PEMs are high conductivities,low-humidity operation conditions,adequate mechanical properties,and competitive *** molecular moieties,such as benzimidazole,benzothiazole,imide,and ether ether ketone,have been introduced to polymer chain backbones to satisfy the application requirements for *** most common sulfonated polymers based on the main chain backbones have been employed to improve the *** group/chain engineering,including the introduction of SO_(3)^(-) on the side chain,grafting,branching,and crosslinking,has been widely applied to HTPEMs to further improve their proton conductivity,thermal stability,and mechanical ***,phosphoric acid-doped polybenzimidazole is the most successful polymer material for application in *** compositing/blending modification methods of polymers are effective in obtaining high PA-doping levels and superior mechanical *** this review,the current progress of various membrane materials used for HT-PEMs is *** synthesis and performance characteristics of polymers containing specific moieties in the chain backbones applied to HT-PEMs are discussed *** modification approaches and their deficiencies associated with HT-PEMs are analyzed and *** and future challenges are also presented.

关键词： proton exchange membranes high-temperature fuel cells structure-performance relationship proton conductivity

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Biodegradable and Biorecyclable Organic Glass

Research Square

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Research Square 2022年

作者： Xing, Ruirui Yuan, Chengqian Fan, Wei Ren, Xiaokang Yan, Xuehai State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences China

Glass is ubiquitous in life and widely used in various fields. However, there is an urgent need to develop biodegradable and biorecyclable glasses that have a minimal environmental footprint toward a sustainable society and a circular materials economy. Here, we report a family of eco-friendly organic glasses of biological origin fabricated using biologically-derived amino acids or peptides through the classic heating-quenching procedure. Amino acids and peptides with chemical modification at their ends are found able to form a supercooled liquid before decomposition and eventually glass upon quenching. These developed glasses exhibit excellent glass-forming ability and optical characteristics and are amenable to 3D printed additive manufacturing and mould casting. Crucially, the glasses show biocompatibility, biodegradability and biorecyclability beyond the currently used commercial glasses and plastic materials. © 2022, CC BY.

关键词： Biodegradability

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Machine learning models coupled with ionic fragment σ-profiles to predict ammonia solubility in ionic liquids

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Green Chemical engineering 2025年第2期 223-232页

作者： Kaikai Li Yuesong Zhu Sensen Shi Yongzheng Song Haiyan Jiang Xiaochun Zhang Shaojuan Zeng Xiangping Zhang Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Mesoscience and EngineeringInstitute of Process EngineeringChinese Academy of Sciences College of Chemical and Engineering University of Chinese Academy of Sciences Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of EducationEast China University of Science and Technology College of Chemical Engineering and Environment China University of Petroleum

Emitting NH3into the atmosphere leads to significant air pollution, while NH3itself serves as an essential component for fertilizers and refrigerants in industry. Thus, recovering and reusing NH3is highly valuable. Ionic liquids（ILs） have shown great potential for NH3capture, where the accurate prediction of solubility is a critical point for selecting ILs and designing a separation process. This work combined the Ionic Fragment Contribution（IFC） strategy with machine learning（ML） to develop four models（IFC-ML） to predict NH3solubility in ILs. A dataset containing 785 solubility data points, covering 10 cations and 10 anions, was collected. From this dataset,the S1–S6 descriptors based on the IFC method were used as inputs for the ML models, together with temperature（T） and pressure（P）. Among the models, the IFC-GBR model was recommended for predicting NH3solubility in ILs due to its higher coefficient of determination（R2） of 0.9945 and lower mean squared error（MSE） of 0.0003than the others. Additionally, in comparison with previous conductor-like screening model for real solvents（COSMO-RS） and extreme learning machine（ELM） methods, the IFC-GBR（gradient boosting regressor） method showed a more accurate prediction of the NH3solubility in ILs over a wider range of temperatures and pressures,providing additional chemical insights into IL-NH3system that cations played a more important role for NH3solubility. These results highlighted the developed IFC-GBR model offered valuable insights for helping guide the process design of absorbing NH3through IL-based technology.

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ReaxFF molecular dynamic simulation of primary and secondary reactions involving in sub-bituminous coal pyrolysis for tar production

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Carbon Resources Conversion 2021年第1期4卷 230-238页

作者： Yanan Qian Jin-Hui Zhan Wei Xu Zhennan Han Xiaoxing Liu Guangwen Xu State Key Laboratory of Safety and Control for Chemicals SINOPEC Research Institute of Safety Engineering Co.Ltd.Qingdao 266071China State Key Laboratory of Multiphase Complex System Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Key Laboratory on Resources Chemicals and Materials of Ministry of Education of China Shenyang University of Chemical TechnologyShenyang 110142China

ReaxFF molecular dynamic simulation combined with experimental verification was performed to understand the overall reaction mechanism,especially the primary and secondary reactions involving in tar formation of sub-bituminous coal *** relationship at atomic level is clarified between bond breakage of functional groups and products generation,revealing that the amount and order in forming each product are subject to the number of corresponding functional groups and their bond energies *** primary breakage of-C-O-and-C-C-bridge-bonds present in initial coal macromolecular generates molecular of heavy tar,whereas heavy tar can be converted into light tar through cracking side chain of aromatic rings and cyclic hydrocarbons at increased pyrolysis *** very high temperatures the cracking of short-chain hydrocarbons and residual atoms connecting to aromatic rings further occurs to generate light tar and *** remaining aromatic-ring fragments of heavy tar are likely cross-linked to form ***,the simultaneous evolution tendency of tar yield and tar quality under different pyrolysis temperatures and heating rates is obtained at molecular *** obtaining high yield and quality of tar,appropriately high temperature as well as suitable heating rate are needed to compromise the high yield of primary tar and high quality of secondarily upgraded products.

关键词： ReaxFF MD simulation Sub-bituminous coal pyrolysis Reaction paths Primary formation Secondary upgrading

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Exploring the regulatory effect of stacked layers on moiréexcitons in twisted WSe_(2)/WSe_(2)/WSe_(2)homotrilayer

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Nano Research 2023年第7期16卷 10573-10579页

作者： Haihong Zheng Biao Wu Chang-Tian Wang Shaofei Li Jun He Zongwen Liu Jian-Tao Wang Ji-an Duan Yanping Liu School of Physics and Electronics Hunan Key Laboratory for Super-microstructure and Ultrafast ProcessCentral South University932 South Lushan RoadChangsha 410083China State Key Laboratory of Precision Manufacturing for Extreme Service Performance Central South University932 South Lushan RoadChangsha 410083China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China School of Chemical and Biomolecular Engineering The University of SydneyNSW 2006Australia The University of Sydney Nano Institute The University of SydneyNSW 2006Australia Songshan Lake Materials Laboratory Dongguan 523808China Shenzhen Research Institute of Central South University Shenzhen 518057China

Moirésuperlattices in van der Waals structures have emerged as a powerful platform for studying the novel quantum properties of two-dimensional *** periodic moirépatterns generated by these structures lead to the formation of flat mini-bands,which alter the electronic energy bands of the *** resulting flat electronic bands can greatly enhance strong correlative interactions between electrons,leading to the emergence of exotic quantum phenomena,including moiréphonons and moiré*** extensive research has been conducted on the exotic quantum phenomena in twisted bilayers of transition metal dichalcogenides(TMDs),and the regulatory effect of stacked layers on moiréexcitons remains *** this study,we report the fabrication of a twisted WSe_(2)/WSe_(2)/WSe_(2) homotrilayer with two twist angles and investigate the influence of stacked layers on moiré*** experiments reveal multiple moiréexciton splitting peaks in the twisted trilayer,with moirépotential depths of 78 and 112 meV in the bilayer and trilayer homostructures,*** also observed the splitting of the moiréexcitons at 90 K,indicating the presence of a deeper moirépotential in the twisted ***,we demonstrate that stacked layers can tune the moiréexcitons by manipulating temperature,laser power,and magnetic *** results provide a new physical model for studying moirésuperlattices and their quantum properties,which could potentially pave the way for the development of quantum optoelectronics.

关键词： materials material field

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An experimental and computational investigation on structural evolution of the In_(2)O_(3)catalyst during the induction period of CO_(2)hydrogenation

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Chinese Journal of Catalysis 2025年第5期72卷 301-313页

作者： Zhangqian Wei Mingxiu Wang Xinnan Lu Zixuan Zhou Ziqi Tang Chunran Chang Yong Yang Shenggang Li Peng Gao Center for Low-Carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of the Chinese Academy of Sciences Beijing 100049China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049ShaanxiChina

As one of the most important industrially viable methods for carbon dioxide(CO_(2))utilization,methanol synthesis serves as a platform for production of green fuels and commodity *** sustainable methanol synthesis,In_(2)O_(3)is an ideal catalyst and has garnered significant ***,cubic In_(2)O_(3)nanoparticles were prepared via the precipitation method and evaluated for CO_(2)hydrogenation to produce *** the initial 10 h of reaction,CO_(2)conversion gradually increased,accompanied by a slow decrease of methanol selectivity,and the reaction reached equilibrium after 10-20 h on *** activation and induction stage may be attributed to the sintering of In_(2)O_(3)nanoparticles and the creation of more oxygen vacancies on In_(2)O_(3)*** experimental studies demonstrate that hydrogen induction created additional oxygen vacancies during the catalyst activation stage,enhancing the performance of In_(2)O_(3)catalyst for CO_(2)*** functional theory calculations and microkinetic simulations further demonstrated that surfaces with higher oxygen vacancy coverages or hydroxylated surfaces formed during this induction period can enhance the reaction rate and increase the CO_(2)***,they predominantly promote the formation of CO instead of methanol,leading to reduced methanol *** predictions align well with the above-mentioned experimental *** work thus provides an in-depth analysis of the induction stage of the CO_(2)hydrogenation process on In_(2)O_(3)nano-catalyst,and offers valuable insights for significantly improving the CO_(2)reactivity of In_(2)O_(3)-based catalysts while maintaining long-term stability.

关键词： In_(2)O_(3) CO_(2)hydrogenation Methanol production Induction and activation Structural evolution

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