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Mg-Al-hydrotalcite with alkaline sites protects Ni/KIT-6 from formation of amorphous coke in glycerol steam reforming via tailoring reaction intermediates

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 25-39页

作者： Yunyu Guo Yiran Wang Yuewen Shao Shu Zhang Yi Wang Song Hu Jun Xiang Xun Hu School of Material Science and Engineering University of JinanJinan 250022China Joint International Research Laboratory of Biomass Energy and Materials College of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037China State Key Laboratory of coal Combustion Huazhong University of Science and TechnologyWuhan 430074China

During steam reforming,the performance of a catalyst and amount/property of coke are closely related to reaction intermediates reaching surface of a catalyst.Herein,modification of reaction intermediates by placing Mg-Al-hydrotalcite above Ni/KIT-6 catalyst in steam reforming of glycerol was conducted at 300 to 600°C.The results revealed that the catalytic activity of Ni/KIT-6 in the lower bed was enhanced with either Mg1-Al5-hydrotalcite(containing more acidic sites)or Mg5-Al1-hydrotalcite(containing more alkaline sites)as upper-layer catalyst.The in situ infrared characterization of steam reforming demonstrated that Mg-Al-hydrotalcite catalyzed the deoxygenation of glycerol,facilitating the reforming of the partially deoxygenated intermediates over Ni/KIT-6.Mg-Al-hydrotalcite as protective catalyst,however,did not protect the Ni/KIT-6 from formation of more coke.Nonetheless,this did not lead to further deactivation of Ni/KIT-6 while Mg5-Al1-hydrotalcite even substantially enhanced the catalytic stability,even though the coke was much more significant than that in the use of single Ni/KIT-6(52.7%vs.28.6%).The reason beneath this was change of the property of coke from more aliphatic to more aromatic.Mg5-Al1-hydrotalcite catalyzed dehydration of glycerol,producing dominantly reaction intermediates bearing C=C,which formed the catalytic coke of with carbon nanotube as the main form with smooth outer walls as well as higher aromaticity,C/H ratio,crystallinity,crystal carbon size,thermal stability,and resistivity toward oxidation on Ni/KIT-6 in the lower bed.In comparison,the abundance of acidic sites on Mg1-Al5-hydrotalcite catalyzed the formation of more oxygen-containing species,leading to the formation of carbon nanotubes of rough surface on Ni/KIT-6.

关键词： steam reforming of glycerol Mg-Alhydrotalcite sacrificial catalyst reaction intermediates property of coke

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Biodiesel from Palm Vegetable Oil

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Natural Resources 2024年第2期15卷 51-60页

作者： Bhawna Yadav Lamba Sapna Jain Shreya Jha Applied Science Cluster School of Engineering UPES Dehradun India Winchester High School Massachusetts USA

Energy obtained from a variety of non-renewable sources is considered unsustainable. Various fossil fuels, such as petroleum, coal, and natural gas, are among these sources. The combustion of fossil fuels resulted in the generation of greenhouse gases, which increased the amount of carbon dioxide in the atmosphere. Global warming and ozone layer degradation are the negative consequences. In a country like india, where consumable oils are still imported, it is sense to look at the possibility of using such unpalatable oils in CI engines that aren’t often utilized as cooking oil. Palm oil is a vegetable oil obtained from the monocarp of the oil palm’s crop. The main goal is to provide a low-cost, high-performance alternative to diesel. The possibility of palm oil as a realistic, modest, and effective hotspot for the generation of biodiesel is investigated in this research. The article is focused on the comparison of palm oil and diesel in terms of characteristics.

关键词： Biodiesel Transesterification Palm Oil Heterogeneous Catalyst Methyl Esters Sustainable Fuel Energy

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Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

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Nano-Micro Letters 2024年第7期16卷 402-440页

作者： Yizhe Li Yajie Li Hao Sun Liyao Gao Xiangrong Jin Yaping Li Zhi LV Lijun Xu Wen Liu Xiaoming Sun State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China Xinjiang coal Mine Mechanical and Electrical Engineering Technology Research Center Xinjiang Institute of EngineeringUrumqi 830023Xinjiang Uygur Autonomous RegionPeople’s Republic of China

The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance electro-catalysts.Currently,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications.Compared to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic activity.Of these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal atoms.DACs have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active sites.In this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related applications.The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction reaction.The future research challenges and opportunities are also raised in prospective section.

关键词： Dual-atom catalysts Synergetic effect Electrocatalysis Oxygen reduction reaction CO_(2)reduction reaction Hydrogen evolution reaction N2 reduction reaction

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Damage degradation mechanism and macro-meso structural response of mudstone after water wetting

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Journal of Mountain Science 2024年第8期 2825-2843页

作者： SHAO Zhixin SONG Yanqi ZHENG Junjie SHEN Fuxin LIU Chuanpeng YANG Juntao School of Mechanics and Civil Engineering China University of Mining and Technology (Beijing) State Key Laboratory of coal Resources and Safe Mining China University of Mining & Technology (Beijing)

The predominant presence of weak interlayers primarily composed of mudstone renders them highly susceptible to a reduction in bearing capacity due to the water-rock weakening effect, significantly impacting the safety of open-pit mining operations. This study focuses on the weak mudstone layers within open-pit mine slopes. The mineral composition of mudstone and the microstructure evolution characteristics before and after water wetting were analyzed by X-ray diffraction(XRD) and scanning electron microscope(SEM). The mesostructure and parameter variation characteristics of mudstone interior space after water-rock interaction were quantified by computed tomography scanning test, and the damage variable characterization method was proposed. Additionally, according to the uniaxial compression test, the degradation characteristics of the macroscopic mechanical behavior of mudstone under different water wetting time were explored, and the elastic modulus and strength attenuation model of mudstone based on mesoscopic damage were established. Finally, building upon the macro-meso structural response characteristics of mudstone, an exploration of the failure characteristics and deterioration mechanism under the influence of waterrock interactions was undertaken. The results show that the water-rock interaction makes the internal defects of mudstone gradually develop and form a fracture network structure, which eventually leads to the deterioration of its macroscopic mechanical properties. The porosity, fractal dimension and damage characteristics of mudstone show an exponential trend with the increase of water wetting time. Moreover, the deterioration mechanism of mudstone after water wetting are postulated to encompass factors such as the hydrophilicity of mineral molecular structures, hydration stress and expansion effects on clay particles, as well as the spatial distribution of microcracks and the phenomenon of fracture adsorption. The outcomes of this research endeavor aim to provide certain reference value for fur

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Actively tuning anisotropic light-matter interaction in biaxial hyperbolic materialα-MoO_(3) using phase change material VO_(2) and graphene

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Chinese Physics B 2024年第4期33卷 631-638页

作者：周昆胡杨吴必园仲晓星吴小虎 School of Safety Engineering China University of Mining and TechnologyXuzhou 221116China Key Laboratory of Gas and Fire Control for coal Mines China University of Mining and TechnologyXuzhou 221116China Shandong Institute of Advanced Technology Jinan 250100China School of Power and Energy Northwestern Polytechnical UniversityXi'an 710072China

Anisotropic hyperbolic phonon polaritons(PhPs)in natural biaxial hyperbolic materialα-MoO_(3) has opened up new avenues for mid-infrared nanophotonics,while active tunability ofα-MoO_(3) PhPs is still an urgent problem necessarily to be solved.In this study,we present a theoretical demonstration of actively tuningα-MoO_(3) PhPs using phase change material VO_(2) and graphene.It is observed thatα-MoO_(3) PhPs are greatly dependent on the propagation plane angle of PhPs.The insulator-to-metal phase transition of VO_(2) has a significant effect on the hybridization PhPs of theα-MoO_(3)/VO_(2) structure and allows to obtain actively tunableα-MoO_(3) PhPs,which is especially obvious when the propagation plane angle of PhPs is 900.Moreover,when graphene surface plasmon sources are placed at the top or bottom ofα-MoO_(3) inα-MoO_(3)/VO_(2)structure,tunable coupled hyperbolic plasmon-phonon polaritons inside its Reststrahlen bands(RB s)and surface plasmonphonon polaritons outside its RBs can be achieved.In addition,the above-mentionedα-MoO_(3)-based structures also lead to actively tunable anisotropic spontaneous emission(SE)enhancement.This study may be beneficial for realization of active tunability of both PhPs and SE ofα-MoO_(3),and facilitate a deeper understanding of the mechanisms of anisotropic light-matter interaction inα-MoO_(3) using functional materials.

关键词： light-matter interaction hyperbolic material phase change material graphene

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One-step conversion of methane and formaldehyde to ethanol over SA-FLP dual-active-site catalysts: A DFT study

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Chinese Chemical Letters 2024年第4期35卷 544-548页

作者： Tao Ban Xi-Yang Yu Hai-Kuo Tian Zheng-Qing Huang Chun-Ran Chang Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering and TechnologyXi'an Jiaotong UniversityXi'an 710049China Shaanxi Key Laboratory of Low Metamorphic coal Clean Utilization School of Chemistry and Chemical EngineeringYulin UniversityYulin 719000China

One-step conversion of methane and formaldehyde into ethanol is a 100% atom-efficient process for carbon resources utilization and environment protection but still faces eminent challenges due to the lacking of efficient catalysts. Therefore, developing active and stable catalysts is crucial for the co-conversion of methane and formaldehyde. Herein, twelve kinds of “Single-Atom”-“Frustrated Lewis Pair”(SA-FLP)dual-active-site catalysts are designed for the direct conversion of methane and formaldehyde to ethanol based on density functional theory(DFT) calculations and microkinetic simulations. The results show that the SA-FLP dual active sites can simultaneously activate methane at the SA site and activate formaldehyde at the FLP site. Among the twelve designed SA-FLP catalysts, Fe1-FLP shows the best performance in the co-conversion of methane and formaldehyde to ethanol with the rate-determining barrier of 1.15 e V.Ethanol is proved as the main product with the turnover frequency of 1.32 × 10^(-4)s^(-1)at 573 K and 3 bar.This work provides a universal strategy to design dual active sites on metal oxide materials and offers new insights into the effective conversion of methane and formaldehyde to desired C_(2) chemicals.

关键词： Single-atom Frustrated Lewis pairs Methane conversion Dual active sites Ethanol synthesis

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Engineering practice of CO2 ESGR in Nanchuan normal-pressure marine shale gas reservoirs

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Natural Gas Industry 2024年第4期44卷 83-92页

作者： Yao, Hongsheng Fang, Dazhi Lu, Yiyu Wang, Baixue Lu, Zhaohui Gu, Hongtao Yan, Zhuolin Miao, Shipu Sinopec East China Oil & Gas Company Jiangsu Nanjing 210011 China State Key Laboratory of coal Mine Disaster Dynamics and Control/ Chongqing University Chongqing 400044 China School of Resources and Safety Engineering Chongqing University Chongqing 400044 China

Current experimental researches and simulation have demonstrated the theoretical feasibility of CO2 flooding to enhance shale gas recovery, but its actual engineering effects have not been verified in field tests. Based on the geological occurrence and production behaviors of Nanchuan normal-pressure shale gas reservoir in the Sichuan Basin, this paper studies the mechanisms of shale isothermal adsorption and CO2-CH4 competitive adsorption, carries out the first field test of CO2 huff and puff in a normal-pressure marine shale gas attenuation well, and points out the research direction of establishing a set of technological system. And the following research results are obtained. First, in the late production period, a gas well enters the stage of low pressure and low production, presenting the characteristics of insufficient formation energy, so it is an important stage to improve the degree of reserve recovery of the well. Second, compared with low-pressure and high-pressure shale, normal-pressure shale is much higher in CH4 and CO2 adsorption capacity, so CO2 ESGR is feasible and necessary. Third, shale samples of normal, high and low pressure adsorb more CO2 than CH4 under the same conditions, and their gas adsorption capacities are ranked as Nanchuan (normal pressure) marine shale > Changning (high pressure) marine shale > Yanchang (low pressure) continental shale. Fourth, CO2 huff and puff shows a remarkable stimulation effect in the test well, with an increase of single-well estimated ultimate shale gas reserves (EUR) from 0.75×108 m3 to 0.90×108 m3, single-well controlled reserves of 5.186×108 m3 and a recovery factor increase by 2.9%. In conclusion, breakthrough progress has been made for the first time in the CO2 huff and puff test of a normal-pressure marine shale gas attenuation well in China, which provides important guidance and reference for the research & development and application of ESGR technologies for shale gas wells in China. What's more, it is in an urgent need to conduct the resource pote

关键词： Carbon dioxide

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Visualization and characterization of experimental hydraulic fractures interacting with karst fracture-cavity distributions

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第5期16卷 1667-1683页

作者： Hanzhi Yang Xin Chang Chunhe Yang Wuhao Guo Lei Wang Guokai Zhao Yintong Guo State Key Laboratory of coal Mine Disaster Dynamics and Control Chongqing UniversityChongqing400044China State Key Laboratory of Geomechanics and Geotechnical Engineering Institute of Rock and Soil MechanicsChinese Academy of SciencesWuhan430071China

Karst fracture-cavity carbonate reservoirs,in which natural cavities are connected by natural fractures to form cavity clusters in many circumstances,have become significant fields of oil and gas exploration and exploitation.Proppant fracturing is considered as the best method for exploiting carbonate reservoirs;however,previous studies primarily focused on the effects of individual types of geological formations,such as natural fractures or cavities,on fracture propagation.In this study,true-triaxial physical simulation experiments were systematically performed under four types of stress difference conditions after the accurate prefabrication of four types of different fracture-cavity distributions in artificial samples.Subsequently,the interaction mechanism between the hydraulic fractures and fracture-cavity structures was systematically analyzed in combination with the stress distribution,cross-sectional morphology of the main propagation path,and three-dimensional visualization of the overall fracture network.It was found that the propagation of hydraulic fractures near the cavity was inhibited by the stress concentration surrounding the cavity.In contrast,a natural fracture with a smaller approach angle(0°and 30°)around the cavity can alleviate the stress concentration and significantly facilitate the connection with the cavity.In addition,the hydraulic fracture crossed the natural fracture at the 45°approach angle and bypassed the cavity under higher stress difference conditions.A new stimulation effectiveness evaluation index was established based on the stimulated reservoir area(SRA),tortuosity of the hydraulic fractures(T),and connectivity index(CI)of the cavities.These findings provide new insights into the fracturing design of carbonate reservoirs.

关键词： Karst fracture-cavity reservoir Fracturing experiment Fracture propagation Cross-sectional morphology Stimulation effectiveness

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Design of Support Effect in the Catalytic Application of Ligand-Protect Gold Clusters

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Chinese Journal of Chemistry 2024年第1期42卷 73-86页

作者： Shuohao Li Shenguang Fu Yuqing Gong Nuojie Wu Lei Wang Liang Wang School of Safety Engineering China University of Mining and TechnologyXuzhouJiangsu 221116China Schoolof Chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsu 225009 Jiangsu Key Laboratory of coal-based Greenhouse Gas Control and Utilization China University of Mining and Technology XuzhouJiangsu 221008China

Ligand-protected gold(Au_(n))clusters sometimes need the removal of organic ligands to expose more active sites and reduce steric hindrance in catalytic reactions,and large amount of organic and inorganic materials usually need to be employed as supports to anchor Aun clusters through different interaction mechanisms.Whereas,less comprehensive summaries have been provided about the crucial contribution of various supports to the catalytic performance of the supported Aun clusters.Herein,this review firstly summarizes synthesis methods(e.g.,impregnation and encapsulation processes)for the supported Aun cluster catalysts,and then mainly points out specific contributions of support effect in a great diversity of catalytic reactions,as well as deep interaction mechanisms.Besides,opportunities and challenging issues will be stated towards supported Aun clusters,in terms of improving catalytic performance and structural stability of Aun clusters inthedemand of catalysis.

关键词： Gold clusters Synthesis Support effect Catalytic performance Interaction

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Catalytic hydrogenolysis of organosolv lignin: Cleaving C–O bonds over CuMgAlOx-layered porous metal oxide catalysts for oriented monophenols production

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Green Carbon 2024年第2期2卷 211-220页

作者： Juping Liu Yang Yang Ziyue Tang Yingquan Chen Hanping Chen Xianhua Wang Haiping Yang State Key Laboratory of coal Combustion Huazhong University of Science and Technology WuhanHubei 430074China

To understand the catalytic conversion of lignin into high-value products,lignin depolymerization was performed using a layered polymetallic oxide(CuMgAlOx)catalyst.The effects of the conversion temperature,hydrogen pressure,and reaction time were studied,and the ability of CuMgAlOx to break the C–O bond was evaluated.The CuMgAlOx(Mg/Al=3:1)catalyst contained acidic sites and had a relatively homogeneous elemental distribution with a high pore size and specific surface area.Theβ-O-4 was almost completely converted by disassociating the C–O bond,resulting in yields of 14.74%ethylbenzene,47.58%α-methylphenyl ethanol,and 36.43%phenol.The highest yield of lignin-derived monophenols was 85.16%under reaction conditions of 280°C and 3 Mpa for 4 h.As the reaction progressed,depolymerization and condensation reactions occurred simultaneously.Higher temperatures(>280℃)and pressures(>3 Mpa)tended to produce solid char.This study establishes guidelines for the high-value application of industrial lignin in the catalytic conversion of polymetallic oxides.

关键词： Lignin Catalytic depolymerization Monophenols CuMgAlOx Layered polymetallic oxide catalyst

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