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Thermal coupling study during the co-processing of coal and biomass in the lab-scale adiabatic reactor

Chinese Journal of Chemical Engineering 2025年第2期78卷 303-313页

作者： Laisong Wang Zhidi Du Jie Feng Xiaolong Shi Wenying Li State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China

A lab-scale adiabatic reactor has been self-made to characterize the coupled properties of heat and reactions during the co-thermal-processing of coal and biomass with steam or steam/O_(2) gasification *** showed that the synergistic effects caused by heat transfer between corncob and coal at different mixing ratios were heavily determined by coal rank and gasification *** steam co-processing,the heat transfer from corncob char to adjacent bituminous coal char promoted the water-gas reaction on coal char and contributed to synergistic effects;the heat transfer from anthracite char to adjacent corncob char reduced the kinetic rate of the water-gas reaction on coal char and contributed to inhibitory effects,and the inhibitory effect caused by heat transfer was greater than the promotion effects of biomass mass *** introduction of O_(2) diminished the impact of inter-particle heat transfer and altered the intensity of synergy,decreasing the values of synergy factor of bituminous coal/corncob blends by 17%and increasing the value of synergy factor of anthracite/corncob blends by 142.5%.This study provides sufficient support for the process conditions selection for the production of syngas with specific H_(2)/CO molar ratios and the desired level of gasification performance.

关键词： Co-processing Element utilization efficiency Reaction heat Heat transfer Synergistic effect

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Segregation mechanism of 0–1 mm fine coal in vibration separation fluidized bed and its influence on the fluidization stability

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Particuology 2025年第2期97卷 167-182页

作者： Ziyi Guo Rongmiao Zhang Yifan Wang Yu Wang Zhibin Guo Ruikang Fan Yadong Zhang Enhui Zhou Chenlong Duan Key Laboratory of Coal Processing&Efficient Utilization Ministry of EducationXuzhou221116China Jiangsu Key Laboratory for Clean Utilization of Carbon Resources Xuzhou221116China School of Chemical Engineering&Technology China University of Mining&TechnologyXuzhou221116China

This study investigates the impact of mixing 0–1 mm fine coal with 0.15–0.3 mm magnetite powder to form a binary dense *** aim is to examine how the 0–1 mm fine coal influences the stability of vibration separation in a fluidized bed and to achieve steady-state control of vibration *** vibration segregation behaviour of the binary dense medium under varying fine coal contents is analyzed in this *** study discovers that the primary contributor to segregation is coal particles smaller than 0.5 *** the proportion of fine coal increases,upward movement becomes more pronounced,especially for particles smaller than 0.15 mm,where the upward segregation is most noticeable,with a peak mixing index of *** study confirms that the larger the particle size of fine coal,the higher the content limit for mixing with magnetite *** to studies on the process of fine coal segregation,coal particles larger than 0.5 mm move with the magnetite powder,and the mixing index remains below *** particles smaller than 0.5 mm fine coal will separate at a uniform speed in a stable environment produced by low vibration energy,with the top-level mixing index remaining constant at 26 after 6 ***,the study also examines how the fluidization of vibration separation is influenced by the segregation of 0–1 mm fine *** evidence shows that longitudinal density segregation within the binary dense medium competes with instantaneous density *** longitudinal density distribution of the binary dense medium was found to be nearly uniform when the frequency was set to 25 Hz,amplitude to 2 mm,and upward gas velocity to 1.4 times the minimum fluidization *** density fluctuation was found to be between 0 and 0.1 g/cm^(3).The best separation effect was achieved with fine coal particles ranging from 6 to 1 mm in size under these conditions.

关键词： Vibration separation fluidization 0-1mm fine coal Segregation process Density fluctuation

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Effect of noble metal nanoparticle size on C–N bond cleavage performance in hydrodenitrogenation: a study of active sites

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Frontiers of Chemical Science and Engineering 2023年第12期17卷 1986-2000页

作者： Yi-Fan Xue Jie Feng Yun-Cai Song Wen-Ying Li State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China

Breakage of the C-N bond is a structure sensitive process,and the catalyst size significantly affects its *** the active metal nanoparticle scale,the role of catalyst size in C-N bond cleavage has not been clearly ***,Ru catalysts with variable nanoparticle sizes were obtained by modulating the reduction temperature,and the catalytic activity was evaluated using 1,2,3,4-tetrahydroquinoline and o-propylaniline with different C-N bond hybridization patterns as *** showed a 13 times higher reaction rate for sp3-hybridized C-N bond cleavage than sp2-hybridized C-N bond cleavage,while the reaction rate tended to increase first and then decrease as the catalyst nanoparticle size *** concentrations of terrace,step,and corner sites were found in different sizes of Ru *** relationship between catalytic site variation and C-N bond cleavage activity was further investigated by calculating the turnover frequency values for each *** analysis indicates that the variation of different sites on the catalyst is the intrinsic factor of the size dependence of C-N bond cleavage activity,and the step atoms are the active sites for the C-N bond *** Ru nanoparticles are smaller than 1.9 nm,they have a strong adsorption effect on the reactants,which will affect the catalytic performance of the Ru ***,these findings were also confirmed on other metallic Pd/Pt *** role of step sites in C-N bond cleavage was proposed using the density function theory *** reactants have stronger adsorption energies on the step atoms,and step atoms have d-band center nearer to the Fermi *** this case,the interaction with the reactant is stronger,which is beneficial for activating the C-N bond of the reactant.

关键词： sp3 sp2-hybridized C–N bond noble metal nanoparticle catalytic active site turnover frequency DFT

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Boron-doped lamellar porous carbon supported copper catalyst for dimethyl oxalate hydrogenation

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Chinese Journal of Chemical Engineering 2023年第3期55卷 222-229页

作者： Peipei Ai Li Zhang Jinchi Niu Huiqing Jin Wei Huang State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China

Doping heteroatoms on carbon materials could bring some special advantages for using as catalyst *** this work, a boron doped lamellar porous carbon(B-LPC) was prepared facilely and utilized as carbonbased support to construct Cu/B-LPC catalyst for dimethyl oxalate(DMO) hydrogenation. Doping boron could make the B-LPC own more defects on surface and bigger pore size than B-free LPC, which were beneficial to disperse and anchor Cu nanoparticles. Moreover, the interaction between Cu species and B-LPC could be strengthened by the doped B, which not only stabilized the Cu nanoparticles, but also tuned the valence of Cu species to maintain more Cu^(+). Therefore, the B-doped Cu/B-LPC catalyst exhibited stronger hydrogenation ability and obtained higher alcohols selectivity than Cu/LPC, as well as high stability without decrease of DMO conversion and ethylene glycol selectivity even after 300 h of reaction at 240℃.

关键词： Hydrogenation Cu-based catalyst Boron doping Porous carbon Catalyst support Alcohol

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Constructing hierarchical ZSM-5 coated with small ZSM-5 crystals via oriented-attachment and in situ assembly for methanol-to-aromatics reaction

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Frontiers of Chemical Science and Engineering 2024年第7期18卷 41-53页

作者： Ning Yang Tingjun Fu Chuntao Cao Xueqing Wu Huiling Zheng Zhong Li State Key Laboratory of Clean and Efficient Coal Utilization College of Chemical Engineering and TechnologyTaiyuan University of TechnologyTaiyuan 030024China

Developing hierarchical and nanoscale ZSM-5 catalysts for diffusion-limited reactions has received ever-increasing attention. Here, ZSM-5 architecture integrated with hierarchical pores and nanoscale crystals was successfully prepared via in situ self-assembly of nanoparticles-coated silicalite-1. First, the oriented attachment of amorphous nanoparticles on external surface of silicalite-1 was achieved by controlling the alkalinity of Si-Al coating solution. The partial exposure of the external surface of silicalite-1 ensured the uniform removal of silicon in the bulk phase for the creation of hierarchical pores during the subsequent desilication-recrystallization. The uniform removal of silicon species in the bulk phase was mainly due to the synergistic effect of surface protection and alkaline etching, which could be balanced by regulating the relative amount of tetrapropylammonium cation and OH– in desilication-recrystallization solution. Importantly, the removed silicon from silicalite-1 recrystallized and in situ assembled into final ZSM-5 nanocrystals induced by surface Si-Al nanoparticles. The hierarchical pores and nanoscale crystals on this integrated architecture not only promoted the removal of coke precursors from micropores but also provided large external specific surface (91 m^(2)·g^(-1)) for coke deposition. Consequently, a much longer catalytic lifetime was achieved for methanol-to-aromatics reaction compared to conventional hollow structure ZSM-5 (84 h vs 46 h), with relatively high stability.

关键词： hierarchical ZSM-5 nanocrystal integrated architecture diffusion coke

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A Z-scheme LaFeO_(3)-CuFe_(2)O4 composite for sulfate radical-based photocatalytic process:Synergistic effect and mechanism

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Chinese Journal of Chemical Engineering 2024年第9期73卷 256-269页

作者： Wenwen Gao Yuhuan Wang Wang Li Zhifang Zhang Ting Su Miao Mu Ying Gong Rui Dang Rui Bai E Zheng Wei Zhao Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization School Chemistry and Chemical EngineeringYulin UniversityYulin 71900China Key Laboratory of Coal Processing and Efficient Utilization Ministry of EducationChina University of Mining&TechnologyXuzhou 221116China High Value Utilization of Coal Based Semi-coke Derivatives of Shaanxi University Engineering Research Center Yulin UniversityYulin 71900China

The sulfate radical-based photocatalytic process is supposed to be the most promising way to degrade organic ***,the development of a suitable and efficient photocatalyst is very *** 40LaFeO_(3)-CuFe_(2)O_(4)(40LFO-CFO)nanocomposite was constructed and its catalytic performance was studied using Rhodamine B(RhB)as the target pollutant.40LFO-CFO exhibited excellent RhB degradation by the persulfate(PS)-assisted photocatalytic process compared to the pristine LFO and *** degradation rate constant for RhB by 40LFO-CFO in the Vis/PS system was 2.22h^(-1)which is 3.04 times and 5.05 times higher than the pristine LFO(0.73 h^(-1))and CFO(0.44h^(-1)),***,the trapping experiments and EPR spectra proved that h^(+) plays a leading role in the bleaching of RhB for the 40LFO-CFO/PS/Vis *** enhanced photocatalytic oxidation activity of 40LFO-CFO could be attributed to the unique charge carriers flow in 40LFO-CFO due to the Z-scheme and the cooperation effect between photocatalysis and PS *** recycle tests confessed the stability of ***,the intermediates and products of RhB are detected by liquid chromatographymass spectrometry(LC-MS),and the photocatalytic degradation routes of RhB for the 40LFO-CFO/Vis/PS system were ***,the 40LFO-CFO nanocomposite has a superior catalytic performance for other organics,suggesting that it is a promising heterocatalyst because of its high catalytic activity and stability for the PS-assisted photocatalytic process.

关键词： Interfacial charge transfer Sulfate radical-based photocatalytic process Z-scheme electron transfer Enhanced charge pair separation Organic pollutants degradation

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Synergistic CO_(2) mineralization using coal fly ash and red mud as a composite system

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International Journal of coal Science & Technology 2024年第3期11卷 149-158页

作者： Zhenchao Yao Yugao Wang Jun Shen Yanxia Niu Jiang Feng Yang Xianyong Wei School of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuanShanxi030024China Key Laboratory of Coal Processing and Efficient Utilization Ministry of EducationUniversity of Mining&Technology221116XuzhouJiangsuChina

CO_(2) mineralization plays a critical role in the storage and utilization of CO_(2).coal fly ash(CFA)and red mud(RM)are widely utilized as CO_(2) ***,the inert calcium species in CFA limit its carbonation capacity,meanwhile the substantial Ca^(2+)releasing of RM is hindered by a covering layer of calcium *** this study,CO_(2) mineralization in a composite system of CFA and RM was investigated to enhance the carbonation *** analyzers were employed to characterize the raw materials and resulting mineralization *** results demonstrated that a synergistic effect existed in the composite system of CFA and RM,resulting in improving CO_(2) mineralization rate and *** produced calcium carbonate was ectopically attached the surface of CFA in the composite system,thus slowing down its coverage on the surface of *** phenomenon facilitated further releasing Ca^(2+)from the internal RM,thereby enhancing CO_(2) mineralization ***,the inclusion of RM significantly improved the alkalinity of the composite system,which not only promoted the dissolution of Ca^(2+)of the inert CaSO_(4)(H_(2)O)_(2) in CFA,but also accelerated CO_(2) mineralization *** investigation would be beneficial to CO_(2) mineralization using industrial solid wastes.

关键词： CO_(2)mineralization coal fly ash Red mud Synergistic effect

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Fabrication of pollution-free coal gangue-based catalytic material utilizing ferrous chloride as activator for efficient peroxymonosulfate activation

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International Journal of coal Science & Technology 2024年第1期11卷 103-118页

作者： Zhiming Sun Xinlin Wang Shaoran Jia Jialin Liang Xiaotian Ning Chunquan Li School of Chemical and Environmental Engineering China University of Mining and Technology(Beijing)Beijing100083China Key Laboratory of Coal Processing and Efficient Utilization (China University of Mining and Technology)Ministry of EducationXuzhou221116China

Novel coal gangue-based persulfate catalyst(CG-FeCl_(2))was successfully synthesized by the means of calcinating under nitrogen atmosphere with the addition of ferrous chloride tetrahydrate(FeCl_(2)·_(4)H_(2)O).The phase transformation of the prepared materials and gas products during the heating process are thoroughly *** is suggested that ferrous chloride participated in the phase transformation and formed Si-O-Fe *** the main gaseous products are H_(2)O,H_(2),and HCl during the heating ***,the ability of CG-FeCl_(2) to activate peroxymonosulfate(PMS)for catalytic degradation of polycyclic aromatic hydrocarbons(PAHs)and phenol was deeply *** than 95%of naphthyl,phenanthrene and phenol were removed under optimizied *** addition,1O_(2),·OH,and SO_(4)·−were involved in the CG-FeCl_(2)/PMS system from the free radical scavenging experiment,where 1O_(2) played a major role during the oxidation ***,CG-FeCl_(2)/PMS system exhibited superior stability in a relatively wide pH range and the presence of common anion from related degradation ***,the novel CG-FeCl_(2) is an efficient and environmentally friendly catalyst,displaying potential application prospect in the field of PAHs and phenol-contaminated wastewater treatment.

关键词： coal gangue Persulfate activation Advanced oxidation processes Polycyclic aromatic hydrocarbons Phenol Ferrous chloride

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Enhancement of catalytic and anti-carbon deposition performance of SAPO-34/ZSM-5/quartz films in MTA reaction by Si/Al ratio regulation

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Chinese Journal of Chemical Engineering 2023年第4期56卷 314-324页

作者： Jiaxin Wu Chenxiao Wang Xianliang Meng Haichen Liu Ruizhi Chu Guoguang Wu Weisong Li Xiaofeng Jiang Deguang Yang School of Chemical Engineering and Technology China University of Mining&TechnologyXuzhou 221116China Key Laboratory of Coal Processing and Efficient Utilization of Ministry of Education Xuzhou 221116China

In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics(MTA)technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthesized via hydrothermal crystallization. The Si/Al ratio of SAPO-34 film was used as the only variable to study this material. The composite zeolite material with 0.6Si/Al ratio of SAPO-34 has the largest mesoporous specific surface area and the most suitable acid distribution. The catalytic performance for the MTA process showed that 0.6-SAPO-34/ZSM-5/quartz film has as high as 50.3% benzene-toluenexylene selectivity and 670 min lifetime. The MTA reaction is carried out through the path we designed to effectively avoid the hydrocarbon pool circulation of ZSM-5 zeolite, so as to improve the aromatics selectivity and inhibit the occurrence of deep side reactions to a great extent. The coke deposition behavior was monitored by thermogravimetric analysis and gas chromatograph/mass spectrometer, it is found that with the increase of Si/Al ratio, the active intermediates changed from low-substituted methylbenzene to high-substituted methylbenzene, which led to the rapid deactivation of the catalyst. This work provides a possibility to employ the synergy effect of composite zeolite film synthesizing anti-carbon deposition catalyst in MTA reaction.

关键词： Composite zeolite film Methanol to aromatics Anti-carbon deposition Si/Al ratio Hydrocarbon pool circulation mechanism

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Novel process for facile preparation of mesoporous silica-based materials with controllable pore structure from coal fly ash Author links open overlay panel

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Particuology 2024年第8期91卷 128-137页

作者： Jian-ming Gao Zhen Li Shujia Ma Yuanyuan Zhang Fangqin Cheng Institute of Resources and Environment Engineering State Environmental Protection Key Laboratory of Efficient Utilization Technology of Coal Waste ResourcesShanxi Collaborative Innovation Center of High Value-added Utilization of Coal-related WastesShanxi UniversityTaiyuan 030006China

Extraction of silica from fly ash to produce mesoporous silica materials is one of the most important utilization *** silica could not be synthesized on a large-scale by conventional sol-gel *** this paper,facile preparation of mesoporous silica with controllable pore structure from fly ash by the template-free process via two steps of mineral phase transformation and selective acid etching was *** influence of crystalline structure and acid etching degree on structure of as-synthesized mesoporous silica materials was revealed,as well as mechanism of crystalline structure transformation and pore structure *** results show that mullite and quartz could be transformed into acid-soluble kaliophilite when fly ash reacted with K_(2)CO_(3)at temperature of 800-1100℃.The hexagonal kaliophilite would be transformed into orthorhombic KAlSiO_(4)-O1 phase when the temperature is controlled at 1100℃.Mesoporous silica with specific surface area of 475.93 m^(2)/g and 642.57 m^(2)/g could be synthesized from activated fly ash with kaliophilite and KAlSiO_(4)-O1 phase crystalline *** controlling the degree of acid etching,mesoporous silica materials with different pore structures can be *** paper provides a cost-effective and large-scale process for the preparation of mesoporous silica materials with controllable pore structure from solid waste fly ash.

关键词： Fly ash Mesoporous silica Crystal transformation Acid etching Controllable pore structure

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